Project

Improvements for circular economy: development of new physicochemical process wastewater treatment methods and their evaluation

Goal: 1. Comparison and evaluation of separation processes
2. Model development of separation processes and validation in flowsheet environment
3. Dynamic modelling and exergy analysis of separation processes
4. Comprehensive evaluation of separation processes
5. Improving the optimisation of separation processes



Subproject between 09.2017-09.2020:
Development of liquid waste treatment in the circular economy
(János Bolyai Research Scholarship of the Hungarian Academy of Sciences)


Subproject between 09.2018-06.2019:
Study of liquid waste treatment processes to design the best practicing technologies
(ÚNKP Bolyai+ Higher Education Young Researcher Scholarship)


Subproject between 09.2019-06.2020:
Comparison of process wastewater treatment methods: distillation and membrane processes
(ÚNKP Bolyai+ Higher Education Young Researcher Scholarship)


Subproject between 07.2020-06.2021:
Development of modelling of separation processes in process simulator environment
(National Talent Program – Scholarship for Young Talents of the Nation)


Subproject between 05.2021-08.2021:
Evaluation of process wastewater treatment processes by life cycle assessment
(Tempus Public Foundation – Hungarian State Eotvos Scholarship)


Subproject between 07.2021-06.2022:
Investigation of competitive membrane operations in the chemical industry: development of pervaporation method
(National Talent Program – Scholarship for Young Talents of the Nation)


Subproject between 01.2022-12.2022:
Comparative evaluation of process wastewater treatment methods: separation methods and incineration
(Scientific Patronage Program (Subprogram 1))

Methods: Distillation, Pervaporation, Flowsheet simulators

Date: 1 September 2017 - 30 November 2023

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Andras Jozsef Toth
added an update
Journal paper
Andras Jozsef Toth, Reka Ladanyi, Huyen Trang Do Thi, Botond Szilagyi, Eniko Haaz: Sustainable Technology Solutions for Reuse of Process Wastewaters from Fine Chemical Industries, Chemical Engineering Transactions, 91, 2022, pp. 187–192., doi: 10.3303/CET2291032
Huyen Trang Do Thi, Andras Jozsef Toth: Comparative evaluation of desalination methods by life cycle analysis: reverse osmosis and thermal processes, MASZESZ Hírcsatorna, 2, 2022, pp. 25–35.
Andras Jozsef Toth: Modelling of Organophilic Pervaporation for Separation of Acetone-Butanol-Ethanol Mixture, Computer Aided Chemical Engineering, 51, 2022, pp. 43–48., doi: 10.1016/B978-0-323-95879-0.50008-4
Presentation
Andras Jozsef Toth (speaker): Modelling of Organophilic Pervaporation for Separation of Acetone-Butanol-Ethanol Mixture, 32th European Symposium on Computer Aided Process Engineering (ESCAPE-32), Touluose, France, 12–15 June 2022.
 
Andras Jozsef Toth
added 2 research items
Napjainkban az ivóvízhiány egyre nagyobb méreteket ölt, elsősorban a gyors népességnövekedés, az éghajlatváltozás, a pazarló túlhasználat és a szennyezés miatt. A jelenlegi körülmények között a világ lakosságának egynegyede nem jut jó minőségű ivóvízhez. Sőt, 2050-re a világ népességének fele, akár 5 milliárd ember is érintett lehet. Ezért más megoldást kell alkalmazni azokon a területeken, ahol nincs elegendő édesvíz. Az egyik lehetséges irány a tengervíz sótalanítása, amely az egyik legpraktikusabb megoldás az ivóvízhiány problémájának megoldására a csekély édesvízkészlettel rendelkező olajkitermelő, gazdag országok esetében. A három leggyakrabban alkalmazott sómentesítési technológia a fordított ozmózis (RO), a többfokozatú gyors desztilláció (MSF) és a többszörös hatású desztilláció (MED). Két módszer alapján vizsgáltuk a tengervíz sótalanítását: életciklus elemzést (LCA) végeztünk a SimaPro Life Cycle Analysis szoftver 9.1-es verziójával, illetve karbonlábnyom (carbon footprint) elemzést készítettünk. A három sómentesítési technológia esetében elemeztük a fosszilis és megújuló energiaforrásokkal előállított ivóvíz üvegházhatásúgáz-kibocsátását (ÜHG). Ennek eredményeként megállapítottuk, hogy az RO-technológia CO2-kibocsátása jelentősen alacsonyabb, mint a termikus technológiáké (MSF és MED). Az RO kombinálása megújuló energiával minősült a leginkább környezetbarátnak; kiemelkedő előnyöket biztosít az emberi egészség és az ökoszisztéma minősége szempontjából. Ez a technológia a jövőben még fejlődhet a hosszabb élettartamú, olcsóbb membránok előállításával, továbbá a folyamat energiaigénye a modern energia-visszanyerő rendszerek alkalmazásával még alacsonyabb lehet.
In the fine chemical industries, especially in the pharmaceutical industry, production technology generates large amounts of liquid waste and industrial waste solvents. Separation of various organic substances used in industry, such as adsorbable organic halides (AOX), from industrial wastewater is an important task of environmental protection. In this work, two technologies were compared to investigate the recycling/reuse of organic material of process wastewaters. The analysis was based on real case study from fine chemical industry. The separation efficiency, operational parameters and cost analysis were carried out to examine stripping and distillation technologies. The calculation was achieved in professional flowsheet simulator environment. According to the results, it can be determined there is no significant difference in separation efficiency of wastewater output streams. However, in the case of distillation technology, the reuse of halides can be possible inside the factory, so this is the recommended procedure for environmental protection. The cost of recovery technologies is also compared with waste incineration. These calculations also demonstrate the effectiveness of the treatment methods, because with recovery technologies it is possible to obtain a reduction of up to 85% compared to incineration.
Andras Jozsef Toth
added an update
Journal paper
Eniko Haaz, Daniel Fozer, Ravikumar Thangaraj, Milan Szori, Peter Mizsey, Andras Jozsef Toth: Vapor−Liquid Equilibrium Study of the Monochlorobenzene–4,6-Dichloropyrimidine Binary System, ACS Omega, 2022, doi: 10.1021/acsomega.2c00525
Presentation
Andras Jozsef Toth (speaker), Reka Ladanyi, Huyen Trang Do Thi, Botond Szilagyi, Eniko Haaz: Sustainable technology solutions for reuse of process wastewaters from fine chemical industries, 10th International Conference on Safety & Environment in Process & Power Industry, Firenze, Italy, 8–11 May 2022.
 
Andras Jozsef Toth
added a research item
The number of newly synthesized and produced organic chemicals has increased extremely quickly. However, the measurements of their physical properties, including their vapor−liquid equilibrium (VLE) data, are time-consuming. It so happens that there is no physical property data about a brand-new chemical. Therefore, the importance of calculating their physicochemical properties has been playing a more and more important role. 4,6-Dichloropyrimidine (DCP) is also a relatively new molecule of high industrial importance with little existing data. Therefore, their measurements and the comparison with the calculated data are of paramount concern. DCP is a widespread heterocyclic moiety that is present in synthetic pharmacophores with biological activities as well as in numerous natural products. Isobaric VLE for the binary system of 4,6-dichloropyrimidine and its main solvent monochlorobenzene (MCB) was measured using a vapor condensate and liquid circulation VLE apparatus for the first time in the literature. Density functional-based VLE was calculated using the COSMO-SAC protocol to verify the laboratory results. The COSMO-SAC calculation was found to be capable of representing the VLE data with high accuracy. Adequate agreement between the experimental and calculated VLE data was acquired with a minimal deviation of 3.0 × 10 −3 , which allows for broader use of the results.
Andras Jozsef Toth
added an update
Journal paper
Florian Enyedi, Huyen Trang Do Thi, Agnes Szayi, Peter Mizsey, Andras Jozsef Toth, Tibor Nagy: Low-Cost and Efficient Solution for the Automation of Laboratory Scale Experiments: The Case of Distillation Column, Processes, 10/4, 2022, 737., doi: 10.3390/pr10040737
 
Andras Jozsef Toth
added a research item
Chemical laboratories badly need efficient support for human works when experiments are carried out. Process control and data acquisition at the laboratory scale are still practical challenges among others, due to equipment prices and the relative complexity of the different scientific disciplines. There is, however, a large demand recently for the so-called Internet of Things (IoT), intelligent/smart labeled solutions that also include laboratory equipment items. Such solutions have enormous potential in making research activity and routine laboratory work efficient and easy by implementing proper data acquisition and control for laboratory-scale equipment items. To solve these practical challenges, an efficient and simple solution was designed and completed for the control and data acquisition of a laboratory-scale rectification process by a well-known microcontroller connected to MATLAB/Simulink. The straightforward application of this solution is demonstrated in case study measurements. The data acquired were used also for process identification. The data were then further processed for various simple and more advanced tunings that were applied, evaluated , and compared. By implementing gain scheduling, significant improvements can be achieved compared to model-based PID tunings while the application of self-tuning by adaptive interaction demands too much consideration for better evaluation with low benefit. Furthermore, the developed device introduces the advantages of digitalization and the 4.0 industrial revolution in the laboratory as well as supports human laboratory work. It also narrows the gap between the laboratory and industrial environment items since the final design can provide a complete process control experience already at the laboratory scale.
Andras Jozsef Toth
added an update
Presentation
Huyen Trang Do Thi (speaker), Andras Jozsef Toth: Comparative evaluation of desalination methods: reverse osmosis and thermal processes (in Hungarian), Hungarian Water- and Wastewater Association Dr. Dulovics Dezső Junior Symposium, Budapest, Hungary, 9 March 2022.
 
Andras Jozsef Toth
added an update
Presentation
Botond Szilagyi (speaker), Andras Jozsef Toth: Development and evaluation of separation methods: distillation and membrane processes, MTA Chemical Unit and Mechanical Working Committee and MKE Technical Chemistry Professional Meeting, Budapest, Hungary, 8 February 2022.
 
Andras Jozsef Toth
added a research item
MTA Chemical Unit and Mechanical Working Committee and MKE Technical Chemistry Professional Meeting, Budapest, Hungary, 8 February 2022
Andras Jozsef Toth
added an update
Journal paper
Emese Cser, Andras Jozsef Toth, Agnes Szanyi, Eniko Haaz, Peter Mizsey, Daniel Fozer: Investigating the homogeneous catalytic hydrothermal carbonization of high moisture containing biomass, Circular Economy and Environmental Protection, 5/3, 2021, pp. 39–50.
Andras Jozsef Toth, Szilvia Schmidt: Method for efficient regeneration of solvent mixture: extractive heterogeneous-azeotropic distillation, Papers on Technical Science, 15, 2021, pp. 103-107., doi: 10.33894/mtk-2021.15.20
Jonathan Wavomba Mtogo, Andras Jozsef Toth, Agnes Szanyi, Peter Mizsey: Comparison of Controllability Features of Extractive and Pressure Swing Distillations on the Example of Tetrahydrofuran Dewatering, ACS Omega, 6/51, 2021, pp. 35355–35362., doi: 10.1021/acsomega.1c04606
Nora Kurcsik, Zsombor Mihaldy, Andras Jozsef Toth: Presentation of the European Green Deal, Circular Economy and Environmental Protection, 5/4, 2021, accepted for publication
Lilla Friedreich, Gyongyi Magyar, Andras Jozsef Toth: Impact of COVID-19 on the state of our environment: case studies in air and water quality and fauna, Circular Economy and Environmental Protection, 5/4, 2021, accepted for publication
Presentation
Andras Jozsef Toth (speaker): Implemented examples of the circular economy in the chemical industry: treatment of process wastewater by physicochemical methods, Mizsey Symposium, Miskolc, Hungary, 9 December 2021.
Eniko Haaz (speaker), Andras Jozsef Toth: Treatment of process wash waters by vacuum evaporation and membrane processes, Mizsey Symposium, Miskolc, Hungary, 9 December 2021.
 
Andras Jozsef Toth
added an update
Journal paper
Huyen Trang Do Thi, Peter Mizsey, Andras Jozsef Toth: Applicability of Membranes in Protective Face Masks and Comparison of Reusable and Disposable Face Masks with Life Cycle Assessment, Sustainability, 13/22, 2021, 12574., doi: 10.3390/su132212574
Presentation
Botond Szilagyi (speaker), Andras Jozsef Toth: Development of flux estimation model for pervaporation membrane operation, 37th Borsod Chemical Day, Miskolc, Hungary, 17 November 2021.
Szilvia Schmidt (speaker), Andras Jozsef Toth: Modeling of extractive heterogeneous-azeotropic distillation in process simulator: optimization and development possibilities, 37th Borsod Chemical Day, Miskolc, Hungary, 17 November 2021.
 
Andras Jozsef Toth
added a research item
In the COVID-19 pandemic period, the role of face masks is critical as a protective physical barrier to prevent droplets and filtrate exhalations coming from infected subjects or against various environmental threats, including the SARS-Cov-2 virus. However, the plastic and microplastic waste from the used face masks pollute the environment, cause a negative impact on human health and the natural ecosystem, as well as increase landfill and medical waste. The presented paper focuses on providing an overview of the application of membrane technology in face mask products as well as the development of protection mechanisms in the future. The authors performed an environmental analysis of reusable (cloth) masks and disposable masks (surgical masks and filtering facepiece respirators) using the Life Cycle Assessment methodology to assess the impacts on the environment, human health, and ecosystem. IMPACT 2002+ V2.14, ReCiPe 2016 Endpoint (H) V1.02, IPCC 2013 GWP 100a V1.03 methods were applied using specialized software (SimaPro V9.1). The disposable masks consistently provide higher protection, though they also carry several multiple environmental burdens. Conversely, reusable masks improve environmental performance, reduce 85% of waste, have a 3.39 times lower impact on climate change, and are 3.7 times cheaper than disposable masks.
Andras Jozsef Toth
added an update
Journal paper
Huyen Trang Do Thi, Tibor Pasztor, Daniel Fozer, Flavio Manenti, Andras Jozsef Toth: Comparison of Desalination Technologies using Renewable Energy Sources with Life Cycle, PESTLE and Multi-Criteria Decision Analyses, Water, 13/21, 2021, 3023., doi: 10.3390/w13213023
 
Andras Jozsef Toth
added a research item
Nowadays, desalination continues to expand globally, which is one of the most effective solutions to solve the problem of the global drinking water shortage. However, desalination is not a fail-safe process and has many environmental and human health consequences. This paper investigated the desalination procedure of seawater with different technologies, namely, multi-stage flash distillation (MSF), multi-effect distillation (MED), and reverse osmosis (RO), and with various energy sources (fossil energy, solar energy, wind energy, nuclear energy). The aim was to examine the different desalination technologies’ effectiveness with energy sources using three assessment methods, which were examined separately. The life cycle assessment (LCA), PESTLE, and multi-criteria decision analysis (MCDA) methods were used to evaluate each procedure. LCA was based on the following impact analysis and evaluation methods: ReCiPe 2016, IMPACT 2002+, and IPCC 2013 GWP 100a; PESTLE risk analysis evaluated the long-lasting impact on processes and technologies with political, economic, social, technological, legal, and environmental factors. Additionally, MCDA was based on the Technique for Order Preference by Similarity to the Ideal Solution (TOPSIS) method to evaluate desalination technologies. This study considered the operational phase of a plant, which includes the necessary energy and chemical needs, which is called “gate-to-gate” analysis. Saudi Arabia data were used for the analysis, with the base unit of 1 m3 of the water product. As the result of this study, RO combined with renewable energy provided outstanding benefits in terms of human health, ecosystem quality, and resources, as well as the climate change and emissions of GHGs categories.
Andras Jozsef Toth
added an update
Journal paper
Daniel Fozer, Andras Jozsef Toth, Petar Sabev Varbanov, Jiří Jaromír Klemeš, Peter Mizsey: Sustainability assessment of biomethanol production via hydrothermal gasification supported by artificial neural network, Journal of Cleaner Production, 318, 2021, 128606., doi: 10.1016/j.jclepro.2021.128606
 
Andras Jozsef Toth
added an update
Journal paper
Huyen Trang Do Thi, Botond Szilagyi, Eniko Haaz, Daniel Fozer, Andras Jozsef Toth: Optimization of hybrid distillation-hydrophilic and organophilic pervaporation systems, Chemical Engineering Transactions, 86, 2021, pp. 1027-1032., doi: 10.3303/CET2186172
 
Andras Jozsef Toth
added a research item
The hybrid distillation-pervaporation process is an efficient method for the removal or recovery of volatile organic compounds from their aqueous mixtures. The hybrid distillation-pervaporation process has not only shown its excellent performance in the purification of solvent mixtures but also proven to have a potential of saving energy. In this study, the hybrid distillation-pervaporation process is optimized for the treatment of low-alcohol waste solvents. Three combinations are examined: distillation with hydrophilic pervaporation, distillation with organophilic pervaporation and distillation with both pervaporation methods. The hybrid systems result in a better performance in term of energy-use compared to conventional distillation. It is observed that a combination of distillation and hydrophilic or/and organophilic pervaporation is suitable for the separation of ethanol-water mixtures and the most recommended is the third layout.
Andras Jozsef Toth
added an update
Presentation
Huyen Trang Do Thi (speaker), Andras Jozsef Toth: Optimization of a hybrid distillation-pervaporation process for methanol-water separation (in Hungarian), 21st PhD Conference of Association of Professors for the European Hungary, Budapest, Hungary, 5 May 2021.
Botond Szilagyi (speaker), Andras Jozsef Toth: Development of a flux estimation model for pervaporation processes (in Hungarian), 21st PhD Conference of Association of Professors for the European Hungary, Budapest, Hungary, 5 May 2021.
Szilvia Schmidt (speaker), Andras Jozsef Toth: Investigation of modeling of extractive heterogeneous-azeotropic distillation in process simulator (in Hungarian), 21st PhD Conference of Association of Professors for the European Hungary, Budapest, Hungary, 5 May 2021.
Huyen Trang Do Thi (speaker), Botond Szilagyi, Eniko Haaz, Daniel Fozer, Andras Jozsef Toth: Process wastewater treatment with hybrid procedure: Distillation and hydrophilic pervaporation (in English), 15th International Conference on Chemical and Process Engineering (ICHEAP 15), Naples, Italy, 23–26 May 2021.
Journal paper
Greta Sztancs, Attila Kovacs, Andras Jozsef Toth, Peter Mizsey, Pieter Billen, Daniel Fozer: Improving sustainability via low-carbon emissionpower generation: catalytic hydrothermalcarbonization of microalgae biomass andhydrochar co-firing, Fuel, 300, 2021, 120927, doi: 10.1016/j.fuel.2021.120927
 
Andras Jozsef Toth
added an update
Presentation
Andras Jozsef Toth (speaker), Nikolett Ocztos: Comparison of process wastewater treatment technologies, Hungarian Water- and Wastewater Association Dr. Dulovics Dezső Junior Symposium, Budapest, Hungary, 3–4. March 2021.
Huyen Trang Do Thi (speaker), Andras Jozsef Toth: Optimization of hybrid distillation-pervaporation processes for ethanol-water separation, Hungarian Water- and Wastewater Association Dr. Dulovics Dezső Junior Symposium, Budapest, Hungary, 3–4. March 2021.
Andras Jozsef Toth (speaker), Szilvia Schmidt: Method for efficient regeneration of solvent mixture: extractive heterogeneous-azeotropic distillation, 26th International Scientific Conference of Young Engineers, Cluj-Napoca, 18. March 2021.
 
Andras Jozsef Toth
added an update
Journal paper
Eniko Haaz, Daniel Fozer, Andras Jozsef Toth: Development of Anhydrous Ethanol Purification: Reduction of Acetal Content and Vapor−Liquid Equilibrium Study of the Ethanol−Acetal Binary System, ACS Omega, 6/2, 2021, pp. 1289–1298., doi: 10.1021/acsomega.0c04750
 
Andras Jozsef Toth
added a research item
Acetaldehyde diethyl acetal (herein called acetal) is an important pollutant of anhydrous ethanol. Isobaric vapor−liquid equilibrium (VLE) of an ethanol−acetal binary system was measured using a vapor condensate and liquid circulation VLE still. The experimental data were correlated with Wilson, nonrandom two-liquid (NRTL), and universal quasichemical (UNIQUAC) activity coefficient models, which were found suitable for representing the VLE data. Proper agreements between experimental and calculated VLE data were obtained, which were then confirmed with consistency tests. The applicability of the novel VLE data was demonstrated during an investigation of an anhydrous ethanol purification column. Reduction of the concentration of acetal and other pollutants was examined and optimized in a flowsheet environment. The modeling results were verified in a laboratory with an experimental distillation column, confirming a correct agreement between the results. It must be highlighted that the developed method is suitable for the production of pharmacopeial quality anhydrous alcohol, based on reliable, verified VLE data. The results show the importance of accurate VLE data in critical compositions (low pollutant content); moreover, aiming at high product purity, experimental validation has paramount importance. The consistency between the three platforms (VLE and distillation experiments and flowsheet simulation) confirms the accuracy of the developed method.
Andras Jozsef Toth
added an update
Journal paper
Asmaa Selim, Andras Jozsef Toth, Daniel Fozer, Karoly Suvegh, Peter Mizsey: Facile preparation of Laponite /PVA mixed matrix membrane for efficient and sustainable pervaporative dehydration of C1-C3 alcohols, ACS Omega, 5/50, 2020, pp. 32373–32385., doi: 10.1021/acsomega.0c04380
Botond Szilagyi, Andras Jozsef Toth: Improvement of Component Flux Estimating Model for Pervaporation Processes, Membranes, 10/12, 2020, 418., doi: 10.3390/membranes10120418
Asmaa Selim, Andras Jozsef Toth, Daniel Fozer, Agnes Szanyi, Peter Mizsey: Pervaporative Dehydration of Methanol using PVA/Nanoclay Mixed Matrix Membranes: Experiments and Modeling, Membranes, 10/12, 2020, 435., doi: 10.3390/membranes10120435
 
Andras Jozsef Toth
added a research item
Separating non-ideal mixtures by pervaporation (hence PV) is a competitive alternative to most traditional methods, such as distillation, which are based on the vapour-liquid equilibrium (VLE). It must be said, in many cases, accurate VLE data are already well known in the literature. They make the method of PV modelling a lot more complicated, and most of the viable models are (semi)empirical and focus on component flux (J i) estimation. The pervaporation model of Mizsey and Valentinyi, which is based on Rautenbach's works, is further improved in this work and tested rigorously by statistical means. Until now, this type of exponential modelling was only used for alcohol-water mixtures, but in this work, it was extended to an ethyl acetate-water binary mixture as well. Furthermore, a flowchart of modelling is presented for the first time in the case of an exponential pervaporation model. The results of laboratory-scale experiments were used as the basis of the study and least squares approximation was used to compare them to the different model's estimations. According to our results, Valentinyi's model (Model I) and the alternative model (Model III) appear to be the best methods for PV modelling, and there is no significant difference between the models, mainly in organophilic cases. In the case of the permeation component, Model I, which better follows the exponential function, is recommended. It is important to emphasize that our research confirms that the exponential type model seems to be universally feasible for most organic-water binary mixtures. Another novelty of the work is that after PDMS and PVA-based membranes, the accuracy of the semiempirical model for the description of water flux on a PEBA-based membrane was also proved, in the organophilic case.
Andras Jozsef Toth
added a research item
The exfoliation method was applied for the preparation of high-water selective mixed matrix membranes (MMMs), especially for the dehydration of C1−C3 alcohol−water solutions. Herein, a facile and easy method was employed to fabricate physically cross-linked Laponite nanosilicate clay−PVA MMMs without additional cross-linking by a one-step synthesis route for water dehydration from methanol, ethanol, and isopropanol aqueous solutions. The morphologies, chemical structures, thermal stabilities, and surface hydrophilicity of Laponite−PVA MMMs were investigated properly by different characterization techniques. The Laponite concentration has affected the fractional free volume of the membranes, as proven by positron annihilation lifetime spectroscopy analysis. The MMMs displayed both a significant improvement in the separation factor and remarkable enhancement in the permeation fluxes for the three alcohol systems. The influence of the operating temperature on the MMM performance was investigated for the methanol/water solution. The methanol permeability was 100-fold lower than that of the water, indicating that the membranes are more water selective. Particularly, the Laponite−PVA membrane with 5 mg/mL Laponite loading exhibits excellent separation efficiency for C1−C3 dehydration having water permeabilities higher than most other polymeric membranes from the other literature studies of 2.82, 2.08, and 1.56 mg m −1 h −1 kPa −1 for methanol, ethanol, and isopropanol/water systems, respectively. This membrane development allows a more efficient and sustainable separation of aqueous alcoholic mixtures.
Andras Jozsef Toth
added an update
Presentation
Daniel Fozer (speaker), Eniko Haaz, Andras Jozsef Toth, Peter Mizsey: Valorisation of high total organic carbon containing process water by hydrothermal gasification, The 4th Sustainable Process Integration Laboratory Scientific Conference (Energy, Water, Emission & Waste in Industry and Cities), Brno, Czech Republic, 18–20. November 2020.
Huyen Trang Do Thi (speaker), Andras Jozsef Toth: Hybrid process treatment of industrial wastewater: Optimization of distillation and pervaporation system, IX. Interdisciplinary Doctoral Student Conference (IDK2020), Pecs, Hungary, 27–28. November 2020.
Journal paper
Huyen Trang Do Thi, Peter Mizsey, Andras Jozsef Toth: Separation of Alcohol-Water Mixtures by a Combination of Distillation, Hydrophilic and Organophilic Pervaporation Processes, Membranes, 10/11, 2020, 345., doi: 10.3390/membranes10110345
 
Andras Jozsef Toth
added a research item
It can be stated that in the fine chemical industries, especially in the pharmaceutical industry, large amounts of liquid waste and industrial waste solvents are generated during the production technology. Addressing these is a key issue because their disposal often accounts for the largest proportion of the cost of the entire technology. There is need to develop regeneration processes that are financially beneficial to the plant and, if possible, reuse the liquid waste in the spirit of a circular economy, in a particular technology, or possibly elsewhere. The distillation technique proves to be a good solution in many cases, but in the case of mixtures with high water content and few volatile components, this process is often not cost-effective due to its high steam consumption, and in the case of azeotropic mixtures there are separation constraints. In the present work, the membrane process considered as an alternative; pervaporation is demonstrated through the treatment of low alcohol (methanol and ethanol) aqueous mixtures. Alcohol-containing process wastewaters were investigated in professional process simulator environment with user-added pervaporation modules. Eight different methods were built up in ChemCAD flowsheet simulator: organophilic pervaporation (OPV), hydrophilic pervaporation (HPV), hydrophilic pervaporation with recirculation (R-HPV), dynamic organophilic pervaporation (Dyn-OPV), dynamic hydronophilic pervaporation (Dyn-HPV), hybrid distillation-organophilic pervaporation (D + OPV), hybrid distillation-hydrophilic pervaporation (D + HPV), and finally hybrid distillation-hydrophilic pervaporation with recirculation (R-D + HPV). It can be stated the last solution in line was the most suitable in the terms of composition, however distillation of mixture with high water content has significant heat consumption. Furthermore, the pervaporation supplemented with dynamic tanks is not favourable due to the high recirculation rate in the case of tested mixtures and compositions.
Andras Jozsef Toth
added an update
Presentation
Andras Jozsef Toth (speaker): Complex optimisation of treatment of process wastewater with extractive heterogeneous-azeotropic distillation, CAPE Forum 2020, Kongens Lyngby, Denmark, 7–9. October 2020.
Andras Jozsef Toth (speaker), Do Thi Huyen Trang, Botond Szilagyi, Asmaa Selim, Eniko Haaz, Daniel Fozer: Investigation of batch pervaporation: removal of alcohols from process wastewaters, CAPE Forum 2020, Kongens Lyngby, Denmark, 7–9. October 2020.
 
Andras Jozsef Toth
added a research item
Pervaporation is a separation method that is considered as green technology because of its low energy consumption. The mechanism of component separation in a liquid mixture by pervaporation is complex but it can be explained with the solution-diffusion mechanism. The work is motivated by an industrial separation problem, that is, ethyl acetate removal from aqueous mixture. To complete this goal hybrid organophilic/hydrophilic pervaporation of ethyl acetate/water mixture through commercially available Sulzer PERVAP™ 4060 and 1510 membranes are investigated to obtain information about the removal of ethyl acetate. Our experimental data are evaluated with the pervaporation model of our improvement (Valentínyi et al., 2013) and it is found that the model can be applied also for both cases. The hybrid separation process is rigorously modelled in professional flowsheet environment, and optimized with the dynamic programming optimization method. The objective function is product purity of 99.0, 99.5 m/m% in water and ethyl acetate content and the total annual cost is also determined. It can be determined, this hybrid separation should be become the alternative of distillation if the energy prices are too high.
Andras Jozsef Toth
added a research item
Nowadays, there is increasing interest in advanced simulation methods for desalination. The two most common desalination methods are multi-stage flash distillation (MSF) and reverse osmosis (RO). Numerous research works have been published on these separations, however their simulation appears to be difficult due to their complexity, therefore continuous improvement is required. The RO, in particular, is difficult to model, because the liquids to be separated also depend specifically on the membrane material. The aim of this study is to model steady-state desalination opportunities of saline process wastewater in flowsheet environment. Commercial flowsheet simulator programs were investigated: ChemCAD for thermal desalination and WAVE program for membrane separation. The calculation of the developed MSF model was verified based on industrial data. It can be stated that both simulators are capable of reducing saline content from 4.5 V/V% to 0.05 V/V%. The simulation results are in accordance with the expectations: MSF has higher yield, but reverse osmosis is simpler process with lower energy demand. The main additional value of the research lies in the comparison of desalination modelling in widely commercially available computer programs. Furthermore, complex functions are established between the optimized operating parameters of multi-stage flash distillation allowing to review trends in flash steps for complete desalination plants.
Andras Jozsef Toth
added an update
Journal paper
Andras Jozsef Toth, Eniko Haaz, Reka Ladanyi, Botond Szilagyi, Daniel Fozer, Asmaa Selim, Tibor Nagy, Peter Mizsey: Modelling of organophilic and hydrophilic pervaporations for separation of ethyl acetate – water mixture, Computer Aided Chemical Engineering, 48, 2020, pp. 757–762., doi: 10.1016/B978-0-12-823 377-1.50127-0
Do Thi Huyen Trang, Andras Jozsef Toth: Treatment of industrial wastewater by hybrid process: distillation and hydrophilic pervaporation, MASZESZ Hírcsatorna, 2020/3, pp. 40–49.
Andras Jozsef Toth: Modelling and Optimisation of Multi-stage Flash Distillation and Reverse Osmosis for Desalination of Process Wastewater Sources, Membranes, accepted for publication
 
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Do Thi Huyen Trang, Tóth András József: Ipari hulladékvizek kezelése hibrid eljárással: desztilláció és hidrofil pervaporáció, MASZESZ Hírcsatorna, 3, 2020, pp. 40–49. Megállapítható, hogy a finomkémiai iparokban, főként a gyógyszeriparban a gyártástechnológia során nagy mennyiségű folyékony hulladék, illetve ipari hulladékoldószer keletkezik. Ezek kezelése kiemelt kérdés, mert ártalmatlanításuk sokszor az egész technológia költségének a legnagyobb hányadát teszi ki. Így olyan regenerálási eljárások kidolgozására van szükség, amelyek anyagilag kedvezőek a gyár számára és lehetőleg van, a körforgásos gazdaság jegyében, az adott technológiában vagy esetleg máshol újra felhasználni a folyékony hulladékokat. A desztillációs technika sok esetben jó megoldásnak bizonyul, azonban nagy víztartalmú, kevés illékony komponenst tartalmazó elegyek esetén ez az eljárás a nagy gőzfogyasztása miatt sokszor nem kifizetődő, illetve azeotróp elegyek esetében elválasztási korlátokba ütközünk. Jelen munkában a desztilláció és az alternatívájának tekintett membrános eljárás, a pervaporáció kerül bemutatásra alacsony alkoholtartalmú vizes elegyek kezelésén keresztül. Etanol tartalmú technológiai hulladékvizeket vizsgáltunk professzionális folyamatszimulátor környezetben. Megállapítottuk, hogy az etanol és a víz elválasztására alkalmas a desztilláció és a hidrofil pervaporáció kombinálása.
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Presentation
Agnes Szanyi (speaker), Eniko Haaz, Asmaa Selim, Andras Jozsef Toth, Daniel Fozer, Peter Mizsey: Saving Natural Resources with Extractive Heterogeneous-Azeotropic Distillation, 23nd Conference on Process Integration for Energy Saving and Pollution Reduction - PRES'20, Xi’an, China, 17–21. August 2020.
Daniel Fozer (speaker), Andras Jozsef Toth, Petar Sabev Varbanov, Jiří Jaromír Klemeš, Peter Mizsey: Modelling of biomass hydrothermal conversion for methanol production, 23nd Conference on Process Integration for Energy Saving and Pollution Reduction - PRES'20, Xi’an, China, 17–21. August 2020.
Journal paper
Andras Jozsef Toth: Summary of research work in ÚNKP 19-4-BME-416 (2019/2020/2), Circular Economy and Environmental Protection, 4/1, 2020, pp. 18–20.
Agnes Szanyi, Eniko Haaz, Asmaa Selim, Andras Jozsef Toth, Daniel Fozer, Peter Mizsey: Saving Natural Resources with Extractive Heterogeneous-Azeotropic Distillation, Chemical Engineering Transactions, 81, 2020, pp. 1363-1368., doi: 10.3303/CET2081228
 
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Efficient processes save natural resources, e.g. chemicals, energy carriers. The Extractive Heterogeneous Azeotropic Distillation (EHAD) is an efficient, novel process for the separation of highly non-ideal liquid mixtures. On the one hand, it consumes less energy than any other separation process and on the other hand the separated compounds of highly non-ideal mixtures can be reused. The EHAD contributes to the saving of natural resources and sustainability. The efficiency of the EHAD is presented on the separation of three highly non-ideal quaternary mixtures of fine chemistry and printing company origins. In this work, the comparison of the efficiency of different separation technologies are compared based on their energy consumptions. It is concluded that the EHAD based separation technology needs the least energy among the investigated alternatives and also enables the recovery and reuse of precious organic compounds.
Andras Jozsef Toth
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Journal paper
Andras Jozsef Toth, Botond Szilagyi, Daniel Fozer, Eniko Haaz, Asmaa Selim, Milan Szori, Bela Viskolcz, Peter Mizsey: Membrane Flash Index: Powerful and Perspicuous Help for Efficient Separation System Design, ACS Omega, doi: 10.1021/acsomega.0c01063
Anita Andre, Andras Jozsef Toth, Eniko Haaz, Daniel Fozer, Agnes Szanyi, Peter Mizsey: When chemistry and engineering meet: the tetrahydrofuran dewatering case study, ACS Sustainable Chemistry & Engineering, doi: 10.1021/acssuschemeng.0c01691
 
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Presentation
Tóth András József (speaker): Comparison of process wastewater treatment methods: distillation and membrane processes (in Hungarian), BME 2019/2020. academic year online conference of New National Excellence Program, Budapest, Hungary, 27. May 2020., p. 162.
Journal paper
Asmaa Selim*, Andras Jozsef Toth, Eniko Haaz, Daniel Fozer, Peter Mizsey: Comparison of Single and Double-network PVA Pervaporation Performance: Effect of Operating Temperature, Periodica Polytechnica Chemical Engineering, 64/3, 2020, pp. 377–383., doi: 10.3311/PPch.15214
 
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Journal paper
Botond Szilagyi, Do Thi Huyen Trang, Daniel Fozer, Asmaa Selim, Eniko Haaz, Andras Joszef Toth: Modelling of Hybrid Method for VOC Removal from Process Wastewater: Distillation and Hydrophilic Pervaporation, Periodica Polytechnica Chemical Engineering, doi: 10.3311/PPch.15190
 
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The study is motivated by the industrial problem from pharmaceutical industry, which is ethanol and methanol removal from process wastewater. To complete this goal hybrid method is investigated and optimized. Two distillation columns are sufficient for separation of alcohol-water mixture. Suitable water can be purified as bottom product of first column. Ethanol and methanol purification is achieved with combination of second distillation column and pervaporation. The target of this research is to rigorously model and optimize the separation of water-ethanol-methanol ternary mixture in professional flowsheet simulator environment. The minimal sufficient membrane transfers area and number of minimal theoretical stages of the columns are determined. Cost estimation is also investigated according to Douglas methodology. Considering the simulation and economic results it can be determined that, the hybrid configuration is suitable for separation of ternary mixture in 99.5 weight percent purity.
Andras Jozsef Toth
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Presentation
Andras Jozsef Toth (speaker): Wastewater desalination with multistage flash distillation (MSF) (in Hungarian), Hungarian Water- and Wastewater Association Dr. Dulovics Dezső Junior Symposium, Budapest, Hungary, 5 March 2020, p. 2.
Do Thi Huyen Trang (speaker), Andras Jozsef Toth: Process wastewater treatment with combination of distillation and pervaporation techniques (in Hungarian), Hungarian Water- and Wastewater Association Dr. Dulovics Dezső Junior Symposium, Budapest, Hungary, 5 March 2020, p. 2.
 
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https://www.interkonyv.hu/konyvek?konyvek=&ref=toth_hulladekgazdalkodas
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Journal paper
Asmaa Selim, Andras Jozsef Toth, Daniel Fozer, Eniko Haaz, Tibor Nagy, Peter Mizsey: Laponite /PVA Pervaporation membrane for desalinating simulated RO high-salinity by-product, Desalination and Water Treatment, doi: 10.5004/dwt.2020.24912
Greta Sztancs, Lilla Juhasz, Balazs Jozsef Nagy, Aron Nemeth, Asmaa Selim, Anita Andre, Andras Jozsef Toth, Peter Mizsey, Daniel Fozer: Co-Hydrothermal gasification of Chlorella vulgaris and hydrochar: The effects of waste-to-solid biofuel production and blending concentration on biogas generation, Bioresource Technology, doi: 10.1016/j.biortech.2020.122793
Asmaa Selim, Andras Jozsef Toth, Daniel Fozer, Eniko Haaz, Peter Mizsey: Pervaporative desalination of concentrated brine solution employing crosslinked PVA/Silicate nanoclay Membranes, Chemical Engineering Research and Design, doi: 10.1016/j.cherd.2020.01.015
 
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Journal paper
Andras Jozsef Toth*, Botond Szilagyi, Daniel Fozer, Do Thi Huyen Trang, Eniko Haaz: Separation of acetone-butanol-ethanol (ABE) fermentation products by pervaporation, Circular Economy and Environmental Protection, 3/3, 2019, pp. 5–19.
Andras Jozsef Toth*: Summary of research work in ÚNKP 19-4-BME-416 (2019/2020/1), Circular Economy and Environmental Protection, 3/3, 2019, pp. 20–25.
Andras Jozsef Toth: Editorial preface, Circular Economy and Environmental Protection, 3/3, 2019, pp. 4.
Andras Jozsef Toth: 11th Eastern European Young Water Professionals Conference, Circular Economy and Environmental Protection, 3/3, 2019, pp. 26.
Andras Jozsef Toth: Introduction of “Improvements for circular economy: development of new physicochemical process wastewater treatment methods and their evaluation” project (OTKA-FK 131586), Circular Economy and Environmental Protection, 3/4, 2019, pp. 20-21.
Presentation
Botond Szilagyi (speaker), Andras Jozsef Toth: High purity separation of ethyl acetate - water binary heterogeneous azeotropic mixture, 19th PhD Conference of Association of Professors for the European Hungary, Budapest, Hungary, 14 November 2019.
 
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Presentation
Andras Jozsef Toth (speaker), Reka Ladanyi, Botond Szilagyi, Eniko Haaz: Isopropanol removal from pharmaceutical process wastewater with combination of distillation and pervaporation (in English), 11th Eastern European IWA Young Water Professionals Conference, Prague, Czech Republic, 1–5 October 2019.
Asmaa Selim (speaker), Andras Jozsef Toth, Eniko Haaz, Daniel Fozer, Peter Mizsey: Clean water production from high salinity water using pervaporation membranes (in English), 11th Eastern European IWA Young Water Professionals Conference, Prague, Czech Republic, 1–5 October 2019.
Andras Jozsef Toth (speaker): Investigation of tetrahydrofuran removal technology from process wastewater (in English), 11th Eastern European IWA Young Water Professionals Conference, Prague, Czech Republic, 1–5 October 2019.
 
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The work is motivated by an industrial problem, which is tetrahydrofuran removal from pharmaceutical process wastewater with extractive distillation. The goal of the research is to rigorously model and optimize this operation in professional flowsheet simulator environment based on adequate and consistent vapour-liquid equilibrium data. The number of minimal theoretical plates of distillation columns, binary mixture feed stage, solvent feed stage location, optimal reflux ratios and Total Annual Cost (TAC) are determined. Dimethyl sulfoxide (DMSO) is used as extractive agent. Considering the results, it can be concluded that, the extractive distillation process is suitable for separation tetrahydrofuran and water in 99.9 weight percent (m/m%) purity of water and 99.5 m/m% tetrahydrofuran.
The research is motivated by an industrial problem, that is isopropanol (IPA) removal from pharmaceutical process wastewater. To complete the target hybrid treatment is investigated. Isopropanol dehydration with combination of distillation and hydrophilic pervaporation (PV) is used. The goal of this research is to rigorously model and optimize this hybrid treatment in professional flowsheet simulator environment. The number of minimal theoretical stages of distillation column and minimal membrane transfer area are determined. Considering the results, it can be concluded that, the distillation and pervaporation methods are suitable for separation isopropanol and water in min. 99.5 weight percent purity (m/m%).
Andras Jozsef Toth
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Journal paper
Asmaa Selim*, Andras Jozsef Toth, Daniel Fozer, Eniko Haaz, Tibor Nagy, Peter Mizsey: Laponite /PVA Pervaporation membrane for desalinating simulated RO high-salinity by-product, Desalination and Water Treatment, accepted for publication
Presentation
Anita Andre, Asmaa Selim, Anita Sz-K Farkas, Daniel Fozer, Eniko Haaz, Peter Mizsey, Tibor Nagy, Andras Jozsef Toth: The Environmental Process Engineering Group, Szent-Györgyi Albert College Days, Budapest, Hungary, 23–26 September 2019.
 
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Presentation
Asmaa Selim (speaker), Andras Jozsef Toth, Eniko Haaz, Daniel Fozer, Peter Mizsey: Separation of aqueous salt solution using PVA based pervaporation membrane: Effect of nanofiller concentration (in English), PERMEA – International Conference on Membrane Processes, Budapest, Hungary, 26–29 August 2019.
Andras Jozsef Toth (speaker), Eniko Haaz, Tibor Nagy, Daniel Fozer, Anita Andre, Asmaa Selim, Peter Mizsey: Sustainable, hybrid method for VOC removal from pharmaceutical process wastewater: distillation and hydrophilic pervaporation (in English), PERMEA – International Conference on Membrane Processes, Budapest, Hungary, 26–29 August 2019.
Andras Jozsef Toth (speaker), Judit Nagy, Aniko Zseni, Juho Kaljunen: Modelling of gas separation in flowsheet environment: ammonia recovery from wastewater (in English), PERMEA – International Conference on Membrane Processes, Budapest, Hungary, 26–29 August 2019.
Andras Jozsef Toth (speaker): Modelling of process wastewater desalination: reverse osmosis and distillation (in English), PERMEA – International Conference on Membrane Processes, Budapest, Hungary, 26–29 August 2019.
 
Andras Jozsef Toth
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Presentation
Tóth András József (speaker): Investigation of reverse osmosis and distillation for process wastewater desalination (in English), Hungarian Hydrological Society – 37th National Symposium, Pecs, Hungary, 3–5 July 2019., pp. 26.
 
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Journal paper
Asmaa Selim, Andras Jozsef Toth, Eniko Haaz, Daniel Fozer, Peter Mizsey: Pervaporation performance of Ag-PVA nanocomposite membranes: Effect of operating temperature, Periodica Polytechnica Chemical Engineering, accepted for publication
Eniko Haaz, Botond Szilagyi, Daniel Fozer, Andras Jozsef Toth: Combining extractive heterogeneous-azeotropic distillation and hydrophilic pervaporation for enhanced energetic separation of non-ideal ternary mixtures, Frontiers of Chemical Science and Engineering, accepted for publication
Andras Jozsef Toth: Summary of research work in ÚNKP 18-4-BME-209 (2018/2019/2), Circular Economy and Environmental Protection, 3/1, 2019, pp. 25–29.
Presentation
Andras Jozsef Toth (speaker), Daniel Fozer, Tibor Nagy, Eniko Haaz, Judit Nagy, Peter Mizsey: Modelling of extractive heterogeneous-azeotropic distillation in dividing wall column (in English), 29th European Symposium on Computer-Aided Process Engineering (ESCAPE-29), Eindhoven, Netherlands, 16–19. June 2019.
Tibor Nagy (speaker), Gergely Csorja, Eniko Haaz, Daniel Fozer, Andras Jozsef Toth, Peter Mizsey: Flexible and efficient solution for control problems of chemical laboratories (in English), 29th European Symposium on Computer-Aided Process Engineering (ESCAPE-29), Eindhoven, Netherlands, 16–19. June 2019.
 
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Mentioned articles: [1] Eniko Haaz, Daniel Fozer, Tibor Nagy, Nora Valentinyi, Anita Andre, Judit Matyasi, Jozsef Balla, Peter Mizsey, Andras Jozsef Toth: Vacuum evaporation and reverse osmosis treatment of process wastewaters containing surfactant material: COD reduction and water reuse, Clean Technologies and Environmental Policy, 21/4, 2019, pp. 861–870. doi: 10.1007/s10098-019-01673-5 [2] Judit Nagy, Juho Kaljunen, Andras Jozsef Toth: Nitrogen recovery from wastewater and human urine with hydrophobic gas separation membrane: experiments and modelling, Chemical Papers doi: 10.1007/s11696-019-00740-x [3] Andras Jozsef Toth, Botond Szilagyi, Eniko Haaz, Szabolcs Solti, Tibor Nagy, Agnes Szanyi, Judit Nagy, Peter Mizsey: Enhanced separation of maximum boiling azeotropic mixtures with extractive heterogeneous-azeotropic distillation, Chemical Engineering Research and Design, 147, 2019, pp. 55–62. doi: 10.1016/j.cherd.2019.05.002 [4] Andras Jozsef Toth: Comprehensive evaluation and comparison of advanced separation methods on the separation of ethyl acetate-ethanol-water highly non-ideal mixture, Separation and Purification Technology, 224, 2019, pp. 490–508. doi: 10.1016/j.seppur.2019.05.051 [5] Eniko Haaz, Botond Szilagyi, Daniel Fozer, Andras Jozsef Toth: Combining extractive heterogeneous-azeotropic distillation and hydrophilic pervaporation for enhanced energetic separation of non-ideal ternary mixtures, Frontiers of Chemical Science and Engineering, under publication
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In chemical laboratories there are always a permanent need to apply flexible, target oriented and efficient control solutions and data acquisition. Traditional equipment and methods utilized are however either time consuming or relatively expensive causing chemical laboratories often to be either not equipped with proper data acquisition and control systems or the installed setup is not easily reconfigured etc... Our aim is to show a simple and promising example that provides flexible and efficient control solution in chemical laboratories.
The distillation based separation can be extremely complex if highly non-ideal mixtures are to be separated. In spite of different successfully applied unit operations there is always a possible way to improve the distillation technique and widen its toolbar. A novel improvement in this area is the development of the extractive heterogeneous-azeotropic distillation (EHAD). For the sake of the demonstration of the efficient use of EHAD in Dividing wall columns (DWC), two quaternary mixtures are selected for separation: Water – Ethanol – Ethyl acetate – Acetone and Water – Ethanol – Ethyl acetate – Ethylene glycol. There are real waste mixtures from pharmaceutical industry. It must be mentioned, extractive heterogeneous-azeotropic distillation method has never been investigated in dividing wall columns. Conventional distillation column sequences and dividing wall columns are selected for comparison. Rigorous steady-state simulations are carried out using ChemCAD flowsheet simulation software. Number of trays, heat duties and Total Annual Cost (TAC) of the systems are optimized. It can be concluded, the application of the EHAD in DWCs allows also the simplification of the separation schemes and the separation reduces the energy requirements of the distillation and opens new horizons for the separation of non-ideal mixtures saving energy, money and natural resources. Using DWCs the reboiler duties can be reduced with 20% and the appropriate separation can be reached with one less column.
Andras Jozsef Toth
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Journal paper
Andras Jozsef Toth, Botond Szilagyi, Eniko Haaz, Szabolcs Solti, Tibor Nagy, Agnes Szanyi, Judit Nagy, Peter Mizsey: Enhanced separation of maximum boiling azeotropic mixtures with extractive heterogeneous-azeotropic distillation, Chemical Engineering Research and Design, doi: 10.1016/j.cherd.2019.05.002
Andras Jozsef Toth: Comprehensive evaluation and comparison of advanced separation methods on the separation of ethyl acetate-ethanol-water highly non-ideal mixture, Separation and Purification Technology, doi: 10.1016/j.seppur.2019.05.051
Presentation
Asmaa Selim (speaker), Andras Jozsef Toth, Eniko Haaz, Daniel Fozer, Peter Mizsey: Influence of silver nanoparticles on pervaporation performance of PVA membranes (in English), 6th International Scientific Conference on Pervaporation, Vapor Permeation and Membrane Distillation, Torun, Poland, 14–17 May 2019.
 
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In agriculture, the human urine could have been used as a natural fertilizer, although there are some problems with the direct utilization, such as the presence of micropollutants in urine, odour and storage of large volume of urine. Therefore, nutrients , such as nitrogen, can be recovered from urine. Continuous flow laboratory membrane reactor was built to investigate nitrogen recovery from wastewater and from human urine. Membrane gas separation method has not been investigated for ammonia recovery from human urine yet. Nitrogen as ammonia gas was recovered in acid using Zeus Aeos™ ePTFE gas-permeable hydrophobic membrane. Acid flux, operating pH, hydraulic retention time and effective membrane surface were experimentally determined. The aim of this work was to verify wastewater experiments in professional flowsheet environment , rigorously modelled with ChemCAD and optimized by dynamic programming optimization method: the membrane separation. Such nitrogen recovery membrane separation has not been published in this professional flowsheet environment yet. The objective function of the process is the ammonia harvesting efficiency. Eighty-five percentage ammonia harvesting efficiency can be reached with 60 membrane surface area/reactor volume ratio, at 35 °C feed temperature with 350 L/m 2 h acid and in 8 h' hydraulic retention time. It can be stated that this separation method is based on physical phenomena without any biological factors. The focus for nitrogen treatment in a wastewater treatment plant is removal instead of recovery. It can be determined that this system is capable for the nitrogen recovery from wastewater, and it can reduce the ammonia content of human urine too.
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Ethyl acetate and ethanol are important organic solvents in fine chemical industry, which form with water ternary minimum-boiling azeotrope and three binary azeotropes, including heterogeneous-azeotrope. In this article, different distillations and pervaporation methods are studied to separate sharply the ternary mixture. In the case of separation of highly non-ideal mixtures the distillation based separation methods can be extraordinarily complex. The extractive heterogeneous-azeotropic distillation (EHAD) as new improvement can be a promising tool for splitting the ternary mixture. This process contains the preferences of heterogeneous-azeotropic- and extractive distillations in one unit without extra material addition. Four advanced separation methods are compared: Method I (pressure swing distillation (PSD) for ethyl acetate purification with extractive distillation (ED) for ethanol purification), Method II (PSD with distillation-hydrophilic pervaporation (D+HPV) for ethanol purification), Method III (EHAD+PSD with ED) and Method IV (EHAD+PSD with D+HPV). The different alternatives are rigorously modelled in ChemCAD simulator and optimized with the dynamic programming optimization method first in the literature. In the case of distillation operations, heat integration is also considered, the feed is preheated with its bottom stream. Such ternary pervaporation separation with new semi-empirical model has not been published in this professional flowsheet environment yet. The distillation and pervaporation models are experimentally verified. Separation factor values are compared to those of other published membranes in the recent literature and it is found that PERVAP™ 1510 has the highest separation factor value. It can be determined that every method is capable for the separation of ethyl acetate-ethanol-water ternary mixture. The methods are optimized by economic evaluation based on the total annual cost (TAC) and the EHAD+PSD with D+HPV is found the optimum, because it has the lowest heat duties.
Andras Jozsef Toth
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Presentation
Andras Jozsef Toth (speaker), Eniko Haaz, Daniel Fozer, Anita Andre, Tibor Nagy: Comparison of alcohol-water separation techniques (in Hungarian), Conference of Chemical Engineering, Veszprém, Hungary, 16–18 April 2019.
Botond Szilagyi (speaker), Andras Jozsef Toth: Separation of maximal boiling azeotrope mixtures with extractive distillation (in Hungarian), Conference of Chemical Engineering, Veszprém, Hungary, 16–18 April 2019.
 
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Human excreta contains all the macroelements which are important for the soil, for example nitrogen, phosphorus and potassium. Although there are many ways of treating human excreta, composting is often regarded as the best solution because the final result of this treatment is valuable humus. However, human urine contains the most of the nutrients, so it may be more reasonable to apply human urine alone as a fertilizer. Direct utilization of urine emerges a lot of problems, but there are several existing technologies which are able to recover the nutrients from urine. These technologies (stripping, absorption, struvite precipitation and membrane technologies) also capable to recover nutrients from wastewater. Our paper are focusing on the comparison of composting toilet and urine-diversion toilet by analysing the advantages and disadvantages of the two methods.
Andras Jozsef Toth
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Journal paper
Judit Nagy, Juho Kaljunen, Andras Jozsef Toth: Nitrogen recovery from wastewater and human urine with hydrophobic gas separation membrane: experiments and modelling, Chemical Papers, doi: 10.1007/s11696-019-00740-x
Asmaa Selim, Andras Jozsef Toth, Eniko Haaz, Daniel Fozer, Agnes Szanyi, Nora Hegyesi, Peter Mizsey: Preparation and characterization of PVA/GA/Laponite membranes to enhance pervaporation desalination performance, Separation and Purification Technology, doi: 10.1016/j.seppur.2019.03.084
Presentation
Andras Jozsef Toth (speaker): Modell developments for membrane separation of process wastewaters (in Hungarian), Hungarian Water- and Wastewater Association Dr. Dulovics Dezső Junior Symposium, Budapest, Hungary, 6 March 2019, pp. 2.
Judit Nagy (speaker), Aniko Zseni, Andras Jozsef Toth: The utilization of human excreta and human urine in the agriculture as a fertilizer (in English), The International Conference on Architecture, Engineering and Technologies (AET), Cairo, Egypt, 30-31 March 2019.
 
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The problem of process wastewater arises not only in fine chemical industry, but also where water is used for washing. In these cases, surfactant material is given to the water, so its washing capability is enhanced. The used water contains surfactant material and dirt. It has high chemical oxygen demand (COD) resulting in serious environmental problems. Finding a solution is inevitable because of the high wastewater fine which has to be paid by the factories if wastewater is emitted without any treatment. A suitable method had to be found that follows the principles of circular economy, so the industrial cycles can be closed like in nature and the water can be reused. Our designed method focuses on different kinds of wastewater containing special surfactant materials, and it has chemical industry relations. The treatment should have reduced the high COD value below to 1000 mgO2/L, which is the discharge limit. It was also aimed that instead of discharging, the treated water could be recycled and reused. Our new physicochemical treatment process consists of a vacuum evaporation method that reduces COD from c.a. 8400 to 1100 mgO2/L. Both laboratory and pilot experiments were investigated. Since this COD value was not satisfactory, a subsequent reverse osmosis membrane operation was also applied. This two-step method, vacuum evaporator followed by reverse osmosis, was able to reduce the COD in wastewater containing surfactant/washing material below the discharge limit. 100 mgO2/L could be reached with using TriSep™ X201 membrane. Penalty calculation and cost estimation also demonstrate the efficiency of our novel method. Graphical abstract Open image in new window
Andras Jozsef Toth
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Journal paper
Nora Valentinyi, Anita Andre, Eniko Haaz, Daniel Fozer, Andras Jozsef Toth, Tibor Nagy, Peter Mizsey: Experimental investigation and modelling of the separation of ternary mixtures by hydrophilic pervaporation, Separation Science and Technology, doi: 10.1080/01496395.2019.1569692
Eniko Haaz, Daniel Fozer, Tibor Nagy, Nora Valentinyi, Anita Andre, Judit Matyasi, Jozsef Balla, Peter Mizsey, Andras Jozsef Toth: Vacuum evaporation and reverse osmosis treatment of process wastewaters containing surfactant material: COD reduction and water reuse, Clean Technologies and Environmental Policy, doi: 10.1007/s10098-019-01673-5
 
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In the course of the present study, the pervaporative dehydration of two ternary mixtures: ethanol/n-butanol/water and ethanol/ethyl acetate/water were investigated through hydrophilic polymer composite PERVAP 1210 membrane. The effects of temperature and the concentrations of water and organic components on permeation were studied through pervaporation experiments. The influence of Hansen solubility parameters of the components and mixtures on their permeation was also examined. It has been found that changes of organic ratios in the feed solution affect organic permeation due to mutual interactions and flux coupling. This interaction was built in a suggested semi-empirical mass-transport model for ternary mixtures with optional simplifications. The modeled partial fluxes are in good accordance with the measured values.
Andras Jozsef Toth
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The industrial production unavoidably generates waste in many cases but that should be recycled and reused following the principle of circular economy. New waste treatment methods or green technologies with zero waste should be developed in order to solve this problem. Since zero emission technology is a difficult task, it is rather typical that waste treatment process is developed. A typical example can be found in pharmaceutical industries because these plants generate wastewaters with high organic content, so-called process wastewaters. These waters should be definitely treated before discharging, their organic content must be removed and then the process wastewater may be usually allowed into the sewer. Nowadays, the physicochemical methods are increasingly used since they have a smaller footprint compared to that of the biological treatments. On the other hand, the polluting organic substances can be recovered and recycled or reused. In our novel method distillation is applied that is based on relative volatility differences of the individual components. The more volatile organic pollutants of the treated process wastewaters are obtained as the top product of the distillation, preferably in reusable form. The bottom product of distillation, namely the process wastewater should satisfy the discharge limits. Our novel innovative method is developed to remove and reuse the organically bound halogens (AOX) and to reduce the chemical oxygen demand (COD) below the emission limit of process wastewaters. Our method is implemented and this well-planned industrial apparatus meets the requirement of the Sustainable Water Solutions and Circular Economy, and moreover the payback time of the investment is less than two years.
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Journal paper
Judit Nagy, Andras Jozsef Toth: Comparison of nutrient recovery methods from human urine in the spirit of circular economy, Circular Economy and Environmental Protection, 2/4, 2018, pp. 5–21.
Andras Jozsef Toth: Summary of research work in ÚNKP 18-4-BME-209 (2018/2019/1), Circular Economy and Environmental Protection, 2/4, 2018, pp. 29–33.
Andras Jozsef Toth: 10th Eastern European Young Water Professionals Conference, Circular Economy and Environmental Protection, 2/1, 2018, pp. 31.
Andras Jozsef Toth: 28th European Symposium on Computer Aided Process Engineering (ESCAPE28), Circular Economy and Environmental Protection, 2/2, 2018, pp. 35-36.
Andras Jozsef Toth: 11th International Conference on Distillation & Absorption, Circular Economy and Environmental Protection, 2/3, 2018, pp. 17-18.
Andras Jozsef Toth: Editorial preface, Circular Economy and Environmental Protection, 2/4, 2018, pp. 4.
Presentation
Andras Jozsef Toth (speaker): Industrial case studies III: membrane techniques (in Hungarian), BME Zielinski Szilárd College, Budapest, Hungary, 3. December 2018.
 
Andras Jozsef Toth
added 2 research items
Mentioned research articles: [1] Eniko Haaz, Nora Valentinyi, Ariella Janka Tarjani, Daniel Fozer, Anita Andre, Selim Asmaa, Fuad Rahimli, Tibor Nagy, Peter Mizsey, Csaba Deak, Andras Jozsef Toth: Platform molecule removal from aqueous mixture with organophilic pervaporation: experiments and modelling, Periodica Polytechnica Chemical Engineering, 63/1, 2019, pp. 138–146. doi: 10.3311/PPch.12151 [2] Andras Jozsef Toth, Eniko Haaz, Szabolcs Solti, Nora Valentinyi, Anita Andre, Daniel Fozer, Tibor Nagy, Peter Mizsey: Parameter estimation for modelling of organophilic pervaporation, Computer-Aided Chemical Engineering, 43, 2018, pp. 1287–1292. doi: 10.1016/B978-0-444-64235-6.50226-6 [3] Eniko Haaz, Andras Jozsef Toth: Methanol dehydration with pervaporation: experiments and modelling, Separation and Purification Technology, 205, 2018, pp. 121–129. doi: 10.1016/j.seppur.2018.04.088 [4] Andras Jozsef Toth, Eniko Haaz, Tibor Nagy, Ariella Janka Tarjani, Daniel Fozer, Anita Andre, Nora Valentinyi, Szabolcs Solti, Peter Mizsey: Treatment of pharmaceutical process wastewater with hybrid separation method: distillation and hydrophilic pervaporation, Waste Treatment and Recovery, 3, 2018, pp. 8–13. doi: 10.1515/ wtr-2018-0002 [5] Andras Jozsef Toth, Botond Szilagyi, Eniko Haaz, Szabolcs Solti, Tibor Nagy, Ariella Janka Tarjani, Nora Valentinyi, Peter Mizsey: Separation of mixture containing maximum boiling azeotrope with extractive heterogeneous-azeotropic distillation, Chemical Engineering Transactions, 69, 2018, pp. 571-576. doi: 10.3303/CET1869096 [6] Andras Jozsef Toth, Eniko Haaz, Tibor Nagy, Ariella Janka Tarjani, Daniel Fozer, Anita Andre, Nora Valentinyi, Peter Mizsey: Novel method for the removal of organic halogens from process wastewaters enabling water reuse, Desalination and Water Treatment, 130, 2018, pp. 54–62. doi: 10.5004/dwt.2018.22987 [7] Andras Jozsef Toth, Eniko Haaz, Nora Valentinyi, Tibor Nagy, Ariella Janka Tarjani, Daniel Fozer, Anita Andre, Selim Asmaa, Szabolcs Solti, Peter Mizsey: Selection between separation alternatives: Membrane Flash Index (MFLI), Industrial and Engineering Chemistry Research, 57/33, 2018, pp. 11366–11373. doi: 10.1021/acs.iecr.8b00430
There are several methods for removal nutrients from human urine. Among them, the main and successfully applied methods are presented, such as struvite precipitation, absorption and stripping, and membrane oparations. In this paper the advantages and disadvantages of these methods are compared. The main purpose of nutrient removal is to recycle as a natural fertilizer to ensure the supply of raw materials for fertilizer, which will be a major problem in the coming decades.
Andras Jozsef Toth