Richard A. Bourne's research while affiliated with University of Leeds and other places
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Publications (123)
Understanding complex reaction systems is critical in chemistry. While synthetic methods for selective formation of products are sought after, oftentimes it is the full reaction signature, i.e., complete profile of products/side-products, that informs mechanistic rationale and accelerates discovery chemistry. Here, we report a methodology using hig...
Ruthenium nanoparticles stabilised by an amine‐modified Ordered Mesoporous Silica Immobilized Ionic Liquid (OMSIIL) are efficient catalysts for the partial reduction of nitrobenzene to hydrazobenzene with 100% selectivity as well as the complete reduction to aniline. High selectivity for the partial reduction of nitrobenzene to hydrazobenzene was o...
Heterogeneous catalysis is widely exploited by the chemical industry, both in batch reactors and in continuous flow, the latter via the use of packed bed reactors. Unfortunately, the transfer of...
Industry 4.0 has birthed a new era for the chemical manufacturing sector, transforming reactor design and integrating digital twin into process control. To bridge the gap between autonomous chemistry development,...
We present an approach to harnessing the tuneable catalytic properties of complex nanomaterials for continuous flow heterogeneous catalysis by combining them with the scalable and industrially implementable properties of carbon pelleted supports. This approach, in turn, will enable these catalytic materials, which largely currently exist in forms u...
Palladium nanoparticles stabilised by aniline modified polymer immobilised ionic liquid is a remarkably active catalyst for the hydrogenation of CO2 to formate giving a TOF of 500 h-1 which is...
RuNPs stabilised by amino‐decorated imidazolium‐based polymer immobilized ionic liquids catalyse the dimethylamine borane mediated reduction of quinolines to 1,2‐dihydroquinoline (DHQ) and 1,2,3,4‐tetrahydroquinoline (THQ). Partial reduction of 3‐substituted quinolines to the corresponding 1,2‐dihydroquinoline was achieved with 100 % selectivity in...
Understanding complex reaction systems and networks is critical in chemistry. While synthetic methods for the selective formation of products are highly sought after, oftentimes it is the full signature of a specific reaction, i.e. the complete profile of products/side-products, that informs mechanistic rationale and acceler-ates discovery chemistr...
In this study, changes in the adsorbed amount and surface structure of sodium hexametaphosphate (SHMP) were investigated for aluminum-doped TiO2 pigment undergoing milling. Relaxation NMR was utilized as a potential at-line technique to monitor the effect of milling on surface area and surface chemistry, while XPS was used primarily to consider the...
Understanding complex reaction systems and networks is critical in chemistry. While synthetic methods for the selective formation of products are highly sought after, oftentimes it is the full signature of a specific reaction, i.e. the complete profile of products/side-products, that informs mechanistic rationale and acceler-ates discovery chemistr...
From the start of a synthetic chemist's training, experiments are conducted based on recipes from textbooks and manuscripts that achieve clean reaction outcomes, allowing the scientist to develop practical skills and some chemical intuition. This procedure is often kept long into a researcher's career, as new recipes are developed based on similar...
The exploitation of computational techniques to predict the outcome of chemical reactions is becoming commonplace, enabling a reduction in the number of physical experiments required to optimize a reaction. Here, we adapt and combine models for polymerization kinetics and molar mass dispersity as a function of conversion for reversible addition fra...
Automated platforms allow for fast and efficient optimisation of single and multi-objective chemical systems. Herein, we report the application of automated optimisation platforms for the chemical screening of sulfide oxidations...
To aid the advancement of hydrometallurgical reprocessing of used nuclear fuel, this work has explored and optimised the synthesis of DEHiBA in continuous flow, to establish a scalable, cost-effective manufacture route.
The optimization of multistep chemical syntheses is critical for the rapid development of new pharmaceuticals. However, concatenating individually optimized reactions can lead to inefficient multistep syntheses, owing to chemical interdependencies between the steps. Herein, we develop an automated continuous flow platform for the simultaneous optim...
The optimization of multistep chemical syntheses is critical for the rapid development of new pharmaceuticals. However, concatenating individually optimized reactions can lead to inefficient multistep syntheses, owing to chemical interdependencies between the steps. Herein, we develop an automated continuous flow platform for the simultaneous optim...
RuNPs stabilised by a polymer immobilised ionic liquid derived from co-polymerisation of a PEG-substituted imidazolium-based styrene monomer and diphenyl(4-vinylphenyl)phosphine oxide, [email protected]=PPh2-PEGPIILS, (2) is a remarkably efficient and selective catalyst for the hydrazine hydrate-mediated partial reduction of nitroarenes to the corr...
For the discovery of new candidate molecules in the pharmaceutical industry, library synthesis is a critical step, in which library size, diversity, and time to synthesise are fundamental. In this work we propose stopped-flow synthesis as an intermediate alternative to traditional batch and flow chemistry approaches, suited for small molecule pharm...
Ruthenium nanoparticles stabilised by polymer immobilized ionic liquids catalyse the hydrolytic release of hydrogen from sodium borohydride. The composition of the polymer influences performance and ruthenium nanoparticles stabilised by an amine-decorated imidazolium-based polymer immobilised ionic liquid ([email protected]2-PIILS) was the most eff...
The consideration of discrete variables (e.g. catalyst, ligand, solvent) in experimental self-optimisation approaches remains a significant challenge. Herein we report the application of a new mixed variable multi-objective optimisation (MVMOO) algorithm for the self-optimisation of chemical reactions. Coupling of the MVMOO algorithm with an automa...
This study investigates the dynamics of a novel, oscillatory, intensified plug-flow reactor – an agitated tubular reactor (ATR) – designed for efficient flow processing of solid-liquid mixtures. The relative movement of the reactor and agitator bar, and associated effects on fluid mixing were characterised physically with a suite of experimental in...
The development of an integrated multistep flow platform that incorporates high-throughput electrochemical synthesis of metal catalysts and catalysis screening is described. Ligand libraries can be screened through the implementation of an autosampler, and online HPLC analysis facilitates continuous monitoring of the reaction. The equipment is cont...
![Fig. 3 N 1s valence RXPS for 1.0 M [N 4,1,1,0 ][HSO 4 ] in water. (a)...](publication/358656656/figure/fig1/AS:1160515300671489@1653699817378/N-1s-valence-RXPS-for-10-M-N-4-1-1-0-HSO-4-in-water-a-Heat-map-of-photon-energy_Q320.jpg)
Valence electronic structure is crucial for understanding and predicting reactivity. Valence non-resonant X-ray photoelectron spectroscopy (NRXPS) provides a direct method for probing the overall valence electronic structure. However, it is often difficult to separate the varying contributions to NRXPS; for example, contributions of solutes in solv...
Impregnation of phosphine-decorated styrene-based Polymer Immobilized Ionic Liquid (PPh 2 -PIIL) with ruthenium (III) trichloride resulted in facile reduction of the ruthenium to afford Ru(II) impregnated phosphine oxide-decorated PIIL (O=PPh 2 PIIL). The derived...
Application of artificial intelligence and machine learning for polymer discovery offers an opportunity to meet the drastic need for the next generation high performing and sustainable polymer materials. Here, these technologies were employed within a computationally controlled flow reactor which enabled self-optimisation of a range of RAFT polymer...
Although kinetic analysis has traditionally been conducted in a batch vessel, continuous-flow aided kinetic analysis continues to swell in popularity. This can be partly attributed to the favourable characteristics of flow reactors and the growth of flow chemistry in general. However, the development of innovative techniques in recent years to obta...
Multi-objective optimisation algorithms (MOOAs) are, of increasing interest for the efficient optimisation of chemical processes. However, an algorithms performance can vary on a case-by-case basis, depending on the complexity of...
Platinum nanoparticles stabilized by imidazolium‐based phosphine‐decorated Polymer Immobilized Ionic Liquids (PPh2‐PIIL) catalyze the hydrolytic evolution of hydrogen from sodium borohydride with remarkable efficiency, under mild conditions. The composition of the polymer influences efficiency with the catalyst based on a polyethylene glycol modifi...
Due to the heterogenous nature of electrochemical reactions, mass transport is an important consideration during reaction and reactor development. The effect of different flow channel geometries on mass transfer between wall and solution within a continuous electrochemical reactor has been investigated using experimental studies and computational f...
We present a rapid continuous processing methodology to screen for the optimal, selective, liquid-liquid extraction conditions, from a typical post-reaction mixture of amines, using both inline and online analysis to systematically alter the pH, by controlling the acid addition pump. A mixture of 95% α-methyl-benzylamine, 1, and 5% N-benzyl-α-methy...
In many real-world problems there is often the requirement to optimise multiple conflicting objectives in an efficient manner. In such problems there can be the requirement to optimise a mixture of continuous and discrete variables. Herein, we propose a new multi-objective algorithm capable of optimising both continuous and discrete bounded variabl...
We herein report experimental applications of a novel, automated computational approach to chemical reaction network (CRN) identification. This report shows the first chemical applications of an autonomous tool to identify the kinetic model and parameters of a process, when considering both catalytic species and various integer and non-integer orde...
An automated continuous flow reactor system equipped with inline analysis, was developed and applied in the self-optimisation of a nanoparticle catalysed reaction. The system was used to optimise the experimental conditions of a gold nanoparticle catalysed 4-nitrophenol reduction reaction, towards maximum conversion in under 2.5 hours. The data obt...
An on-demand electrochemical synthesis of copper(I) triflate under both batch and continuous flow conditions has been developed. A major benefit of the electrochemical methodology is that the only byproduct of the reaction is hydrogen gas, which obviates the need for workup and purification, and water is not incorporated into the product. Upon comp...
The electrochemical generation of N ‐heterocyclic carbenes (NHCs) offers a mild and selective alternative to traditional synthetic methods that usually rely on strong bases and air‐sensitive materials. The use of electrons as reagents results in an efficient and clean synthesis that enables the direct use of NHCs in various applications. Herein, th...
p>An on-demand electrochemical synthesis of copper(I) triflate under both batch and continuous flow conditions has been developed. A major benefit of the electrochemical methodology is that the only by-product of the reaction is hydrogen gas which obviates the need for work-up and purification, and water is not incorporated into the product. Upon c...
The Corning Advanced-FlowTM Reactor (AFR) whose productivity is ready for scale-up with limited loss of transport properties was implemented in the continuous synthesis of Ag nanoparticles (NPs). To demonstrate the effect of mixing on Ag NPs, the flow pattern and mixing characteristic (mainly on the meso- and macroscale) in AFR were studied by flow...
Implementing statistical training into undergraduate or postgraduate chemistry courses can provide high-impact learning experiences for students. However, the opportunity to reinforce this training with a combined laboratory practical can significantly enhance learning outcomes by providing a practical bolstering of the concepts. This paper outline...
Enzymatic saccharification of lignocellulosic biomass to soluble sugars is vulnerable to microbial contamination. Identification of early stage indicators of contamination could allow for more rapid intervention and improved sugar retention. Here we validate the use of dissolved oxygen (DO) and pH as early-stage indicators, and used to evaluate the...
Synthetic electrochemistry has recently become an exciting technology for chemical synthesis. The majority of reported syntheses use either constant current or constant potential, however a few use nonlinear profiles – mostly alternating polarity – to maintain efficiency throughout the process, such as controlling deposits on electrodes or ensuring...
Recent advances in the latest generation of MEMS (micro-electro-mechanical system) Fabry-Pérot interferometers (FPI) for near infrared (NIR) wavelengths has led to the development of ultra-fast and low cost NIR sensors with potential to be used by the process industry. One of these miniaturised sensors operating from 1350 to 1650 nm, was integrated...
We herein report a novel kinetic modelling methodology whereby identification of the correct reaction model and kinetic parameters is conducted by an autonomous framework combined with transient flow measurements to enable comprehensive process understanding with minimal user input. An automated flow chemistry platform was employed to initially con...
A significantly renewed interest in synthetic electrochemistry is apparent in the increasing number of publications over the last few years. Electrochemical synthesis offers a mild, green and atom efficient route to interesting and useful molecules, thus avoiding harsh chemical oxidising and reducing agents used in traditional synthetic methods. As...
A standardized and versatile electrochemical batch reactor that has wide applicability in both organic and inorganic synthesis and analytical electrochemistry has been developed. A variety of synthetic electrochemical transformations have been performed to showcase the versatility and demonstrate the reactor, including the synthesis of five Cu(I)–N...
PurposeThe current trend for continuous drug product manufacturing requires new, affordable process analytical techniques (PAT) to ensure control of processing. This work evaluates whether property models based on spectral data from recent Fabry–Pérot Interferometer based NIR sensors can generate a high-resolution moisture signal suitable for proce...
Ultrafast RAFT polymerisation is exploited under dispersion polymerisation conditions for the synthesis of poly(dimethylacrylamide)-b-poly(diacetoneacrylamide) (PDMAmx-b-PDAAmy) diblock copolymer nanoparticles. This process is conducted within continuous-flow reactors, which are well suited to fast reactions and can easily dissipate exotherms makin...
Heterogenous hydrogenations of high value chemicals are a widely used class of reaction that potentially benefit from the advantages continuous processing possesses. Trickle bed reactors offer a viable alternative to batch manufacture, however further understanding of the interplay between hydrogen masstransfer and catalytic reaction is required to...
Process analytical technologies (PAT) applied to process monitoring and control generally provide multiple outputs that can come from different sensors or from different model outputs generated from a single multivariate sensor. This paper provides a contribution to current data fusion strategies for the combination of sensor and/or model outputs i...
Downstream purification of products and intermediates is essential for the development of continuous flow processes. Described herein, is a study on the use of a modular and reconfigurable continuous flow platform for the self-optimisation of reactive extractions and multi-step reaction-extraction processes. The selective extraction of one amine fr...
The level of uncertainty during quantification of hazardous elements/properties of waste-derived products is affected by sub-sampling. Understanding sources of variability in sub-sampling can lead to more accurate risk quantification and effective compliance statistics. Here, we investigate a sub-sampling scheme for the characterisation of solid re...
There has been an increasing interest in the use of automated self-optimising continuous flow platforms for the development and manufacture in synthesis in recent years. Such processes include multiple reactive and work-up steps, which need to be efficiently optimised. Here, we report the combination of multi-objective optimisation based on machine...
The first CFD-enabled multi-objective design optimisation methodology for continuous oscillatory baffled reactors (COBRs), used for flow chemistry-based process development, is described, where performance is quantified in terms of two metrics: a mixing efficiency index and the variance of the residence time distribution. The effect of cross-valida...
Guest Editors Richard Bourne, King Kuok (Mimi) Hii and Brandon Reizman introduce this themed collection on progress towards data-driven synthesis and an ‘internet of chemistry’.
Self-optimising chemical systems have experienced a growing momentum in recent years, with the evolution of self-optimising platforms leading to their application for reaction screening and chemical synthesis. With the desire for improved process sustainability, self-optimisation provides a cheaper, faster and greener approach to the chemical devel...
A new hybridized algorithm that combines process optimisation with response surface mapping was developed and applied in an automated continuous flow reaction. Moreover, a photochemical cascade CSTR was developed and characterised by chemical actinometry, showing photon flux density
of ten times greater than previously reported in batch. The succes...
The atomic contributions to valence electronic structure for 37 ionic liquids (ILs) are identified using a combination of variable photon energy XPS, resonant Auger electron spectroscopy (RAES) and a subtraction method. The ILs studied include a diverse range of cationic and anionic structural moieties. We introduce a new parameter for ILs, the ene...
We present the synthesis of metal nanowires in a multiplexed device configuration using single‐walled carbon nanotubes (SWNTs) as nanoscale vector templates. The SWNT templates control the dimensionality of the wires, allowing precise control of their size, shape, and orientation; moreover, a solution‐processable approach enables their linear depos...
Progress reaction profiles are affected by both catalyst activation and deactivation processes occurring alongside the main reaction. These processes complicate the kinetic analysis of reactions, often directing researchers toward incorrect conclusions. We report the application of two kinetic treatments, based on variable time normalization analys...
Currently, rate-based understanding of organic reactions employed in the manufacture of active pharmaceutical ingredients (APIs) is often not obtained. In many cases, the generation of kinetic models is still seen as a specialised and time intensive activity, which can only be justified at certain instances in development. In this Communication, we...
We present the synthesis of metal nanowires in a multiplexed device configuration using single‐walled carbon nanotubes (SWNTs) as nanoscale vector templates. The SWNT templates control the dimensionality of the wires, allowing precise control of their size, shape and orientation; moreover a solution processable approach enables their linear deposit...
Mit der Zeit gehen: Zwei verschiedene kinetische Analysemethoden auf Basis der zeitvarianten Normierungsanalyse (VTNA) werden für die Untersuchung von Reaktionen mit Katalysator‐Desaktivierungsprozessen und ‐Aktivierungsprozessen beschrieben. Die studierten Fälle sind eine von einem supramolekularen Rh‐Komplex katalysierte Hydroformylierung und ein...
Gold nanoparticles stabilized by phosphine-decorated polymer immobilized ionic liquids (AuNP@PPh2-PIILP) is an extremely efficient multi-product selective catalyst for the sodium borohydride-mediated reduction of nitrobenzene giving either N-phenylhydroxylamine, azoxybenzene or aniline as the sole product under mild conditions and a very low cataly...
This paper investigates the characterisation of alumina-doped titania nanoparticles, milled under high-shear over time, in the presence of sodium hexametaphosphate (SHMP) dispersant. Transmission electron microscopy (TEM) indicated that prolonged milling times led to the formation of 10 nm particle fines which were electrostatically attracted to la...
We report the scalable, all-aqueous synthesis of poly(dimethyl acrylamide)-poly(diacetone acrylamide) (PDMAm-PDAAm) diblock copolymer spheres, worms and vesicles by reversible addition-fragmentation chain transfer (RAFT) aqueous dispersion polymerisation in a low-cost continuous-flow (CF) reactor. A transient state kinetic profiling method using a...
The sections in this article are
• Introduction
• Principles of Self‐Optimization and Requirements for Experimental Systems
• Analytical Techniques for Closed‐Loop Optimization
• Decision Algorithms in Closed‐Loop Optimization
• Application Examples of Closed‐Loop Discovery and Optimization
• Conclusions and Future Directions
• Acknowledgments
Automated development of chemical processes requires access to sophisticated algorithms for multi-objective optimization, since single-objective optimization fails to identify the trade-offs between conflicting performance criteria. Herein we report the implementation of a new multi-objective machine learning optimization algorithm for self-optimiz...
Thermal decomposition (TD) products of the ionic liquids (ILs) [CnC1Im][BF4] and [CnC1Im][PF6] ([CnC1Im]+ = 1-alkyl-3-methylimidazolium, [BF4]- = tetrafluoroborate, and [PF6]- = hexafluorophosphate) were prepared, ex situ, by bulk heating experiments in a bespoke setup. The respective products, CnC1(C3N2H2)BF3 and CnC1(C3N2H2)PF5 (1-alkyl-3-methyli...
A combination of X-ray photoelectron spectroscopy and near edge X-ray absorption fine structure spectroscopy has been used to provide an experimental measure of nitrogen atomic charges in nine ionic liquids (ILs). These experimental results are used to validate charges calculated with three computational methods: charges from electrostatic potentia...
This paper demonstrates the influence of surface charge chemistry on the application of nuclear magnetic relaxation measurements (NMR relaxometry) for the in situ determination of particle surface area, in the presence of high electrolyte concentration. Specifically, dispersions of titania, calcite and silica with and without 1 M KCl were investiga...
Palladium nanoparticles stabilized by lightly cross-linked phosphine-decorated polymer immobilized ionic liquids (PIIL) and their PEGylated counterparts (PEGPIIL) are highly effective catalysts for the aqueous phase hydrogenation and sodium borohydride-based reduction of a wide range of nitroaromatic and heteroaromatic compounds under mild conditio...
Reaction optimisation and understanding is fundamental for process development and is achieved using a variety of techniques. This paper explores the use of self-optimisation and experimental design as a tandem approach to reaction optimisation. A Claisen-Schmidt condensation was optimised using a branch and fit minimising algorithm, with the resul...
Experimental near edge X–ray absorption fine structure (NEXAFS) spectra are reported for 12 ionic liquids (ILs) encompassing a range of chemical structures for both the sulfur 1s and nitrogen 1s edges and compared with time–dependent density functional theory (TD–DFT) calculations. The energy scales for the experimental data were carefully calibrat...
The preparation of inorganic nanomaterials with a desired structure and specific properties requires the ability to strictly control their size, shape and composition. A series of chemical reactions with platinum compounds carried out within the 1.5 nm wide channel of single-walled carbon nanotubes (SWNTs) have demonstrated the ability of SWNTs to...
This presentation gives an overview of recent advances in the 1st- and 2nd generation MEMS FPI processes for near- and mid- infrared (NIR-MIR) wavelength sensing applications for automotive and process industry. The measured values for the 1st generation NIR MEMS FPI devices for γ = 1.5 - 2.0 μm show FWHM = 15 nm at the optimization wavelength of 1...
Experimental near edge X-ray absorption fine structure (NEXAFS) spectra, X-ray photoelectron (XP) spectra and Auger electron spectra are reported for sulfur in ionic liquids (ILs) with a range of chemical structures. These values provide experimental measures of the atomic charge in each IL and enable the evaluation of the suitability of NEXAFS spe...
Experimental near edge X-ray absorption fine structure (NEXAFS) spectra, X-ray photoelectron (XP) spectra and Auger electron spectra are reported for sulfur in ionic liquids (ILs) with a range of chemical structures. These values provide experimental measures of the atomic charge in each IL and enable evaluation of the suitability of NEXAFS spectro...
Today, the generation of kinetic models is still seen as a resource intensive and specialised activity. We report an efficient method of generating reaction profiles from transient flows using a state-of-the-art continuous-flow platform. Experimental data for multistep aromatic nucleophilic substitution reactions are collected from an automated lin...
Phosphino-decorated polymer immobilised ionic liquid phase stabilised palladium nanoparticles (PdNP@PPh2-PIILP) and their PEGylated counterparts (PdNP@PPh2-PEGPIILP) are remarkably active and exceptionally selective catalysts for the aqueous phase hydrogenation of α,β-unsaturated aldehydes, ketones, esters and nitriles with PdNP@PPh2-PEGPIILP givin...
Phosphino-decorated polymer immobilised ionic liquid phase stabilised palladium nanoparticles (PdNP@PPh2-PIILP) and their PEGylated counterparts (PdNP@PPh2-PEGPIILP) are remarkably active and exceptionally selective catalysts for the aqueous phase hydrogenation of alpha,beta-unsaturated aldehydes, ketones, esters and nitriles with PdNP@PPh2-PEGPIIL...
Today, the generation of kinetic models is still seen as a resource intensive and specialised activity. We report an efficient method of generating reaction profiles from transient flows using a state-ofthe-art continuous-flow platform. Experimental data for multistep aromatic nucleophilic substitution reactions are collected from an automated line...
Styrene-based peroxotungstate-modified polymer immobilized ionic liquid phase catalysts [PO4{WO(O2)2}4]@ImPIILP (Im = imidazolium) are remarkably efficient systems for the selective oxidation of sulfides under mild conditions both in batch and as a segmented or continuous flow process using ethanol as the solvent and mobile phase, respectively. The...
Self-optimising flow reactors combine online analysis with evolutionary feedback algorithms to rapidly achieve optimum conditions. This technique has been applied to the final bond-forming step in the synthesis of AZD9291, an irreversible epidermal growth factor receptor kinase inhibitor developed by AstraZeneca. A four parameter optimisation of a...
This chapter considers the beneficial combination, and potential impact, of continuous flow methodology with the twelve Principles of Green Chemistry as developed by Anastas. Whilst the application of continuous flow reactions is changing the way medicinal chemists are making and trying to identify lead bioactive compounds, the main impact of flow...
An automated continuous reactor for the synthesis of organic compounds, which uses online mass spectrometry (MS) for reaction monitoring and product quantification, is presented. Quantitative and rapid MS monitoring was developed and calibrated using HPLC. The amidation of methyl nicotinate with aqueous MeNH2 was optimised using design of experimen...
The 2–4 keV energy range provides a rich window into many facets of materials science and chemistry. Within this window, P, S, Cl, K and Ca
K
-edges may be found along with the
L
-edges of industrially important elements from Y through to Sn. Yet, compared with those that cater for energies above
ca.
4–5 keV, there are relatively few resources avai...
In this paper we apply the concept of a kinetic motif as a simple way to represent all the time-dependent behaviour in a single-step or multi-step reaction system. Small-scale continuous-flow reactors offer the potential to rapidly collect large amounts of data while accessing conventionally challenging experimental conditions. The scope of the app...
A highly robust immobilized [Cp*IrCl2]2 precatalyst on Wang resin for transfer hydrogenation, which can be recycled up to 30 times, was studied using a novel combination of X-ray Absorption Spectroscopy (XAS) at Ir L3-edge, Cl K-edge and K K-edge. These culminate in an in situ XAS experiments which links structural changes of the Ir complex with it...
A highly robust immobilized [Cp*IrCl2]2 precatalyst on Wang resin for transfer hydrogenation, which can be recycled up to 30 times, was studied using a novel combination of X-ray absorption spectroscopy (XAS) at Ir L3-edge, Cl K-edge, and K K-edge. These culminate in in situ XAS experiments that link structural changes of the Ir complex with its ca...
n-Butanol (BuOH) often has superior properties as a bio-fuel compared to ethanol (EtOH). However finding a sustainable source of BuOH is proving difficult. In this paper, we compare producing BuOH directly from EtOH over four Cu catalysts, synthesised by us, supported on different solid acids. These catalysts were tested in a continuous flow superc...
Developing cleaner chemical processes often involves sophisticated flow-chemistry equipment that is not available in many economically developing countries. For reactions where it is the data that are important rather than the physical product, the networking of chemists across the internet to allow remote experimentation offers a viable solution t...
This comprehensive book approaches sustainability from two directions, the reduction of pollution and the maintaining of existing resources, both of which are addressed in a thorough examination of the main chemical processes and their impact. Divided into five sections, each introduced by a leading expert in the field, the book takes the reader th...
One nanometre wide carbon nanoreactors are utilised as the reaction vessel for catalytic chemical reactions on a preparative scale. Sub-nanometre ruthenium catalytic particles which are encapsulated solely within single-walled carbon nanotubes offering a unique reaction environment are shown to be active when embedded in a supercritical CO2 continu...
Citations
... eV and that the negative shift of O 1s peaks is likely caused by the presence of non-bridging Bi-O species. [74][75][76][77][78] Thus, the new peak may be caused by surface oxygen species such as Bi-O species generated on BiPO 4 , which possibly react with CH 4 to give HCHO as a primary product. There was no significant difference in the XPS Bi 4f spectra between the fresh and recovered BiPO 4 -DEG catalysts after the CH 4 oxidation under the conditions in Fig. S6, † which suggests that the in situ generated oxygen species observed in the reaction temperature range play an important role in the present CH 4 oxidation. ...
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... The fundamental challenge of RO lies in its expansive search space, which consists of a multitude of categorical (e.g., choice of reagent, base, catalyst, methods) and continuous (e.g., temperature, concentration, reagent equivalent) parameters. Some common approaches [1] to solving such a task are high-throughput experimentation (HTE) [2], one factor at a time (OFAT) [3], design of experiment (DoE) [4], and, more recently, AI-guided optimization [5][6][7]. All approaches share the ultimate goal of identifying one or more optimal solutions within the high-dimensional parameter space. ...
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... The bilinear synthesis routes for the target thioether-containing m-diamine compound (A and B) are shown in Scheme 1 depending on the references and exploration [5,[12][13][14]. The key intermediate, 2-fluoro-3-(N-methylbenzamido)benzoic acid (4), can be smoothly prepared from methyl 2-fluoro-3-nitrobenzoate as the starting material. ...
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... Using 4-nitroacetophenone as the substrate gave a 100 % of conversion after 40 min at the same conditions, while the selectivity to the corresponding N-arylhydroxylamine decreased (74 %) due to the complete reduction to 4-aminoacetophenone, in good agreement with a previous report for this substrate. [13] Previous reports showed that halogen-substituted nitroarenes are not suitable substrates for the synthesis of the corresponding N-arylhydroxylamines due to the dehalogenation. [14] Surprisingly, in our catalytic reaction system the reduction of nitroarenes bearing chloroand bromo-groups at the 2-position achieved 100 % conversions to form the corresponding N-arylhydroxylamines in 97 % and 96 % yields, respectively (entries 2-3), with no observation of any dehalogenation products, which was attributed to the mild reaction conditions used in this work. ...
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... The utilization of data-driven approaches extends beyond model development and has also been used in optimization studies. Bayesian optimization and machine learning have emerged as key tools in autonomous experimentation [16][17][18]. Moreover, the extensive historical archive of organic synthesis literature has inspired research that leverages existing data for the construction of machine learning models, streaming the exploration of optimal conditions across vast parameter spaces [19]. ...
... Given the time-and cost-consuming nature of synthesis, the "M" phase remains the bottleneck of the DMTA cycle 13 . Numerous efforts have been made to expedite the "M" phase, incorporating technologies such as robotic arms [14][15][16] , continuous or stopped ow reactions [17][18][19][20] , and other devices 21 . Focusing on the "M" phase, the key to improving the e ciency of the entire DMTA process lies in intelligently integrating individual techniques from each phase in a compatible and automated manner. ...
... Flow technology is one of the most impactful paradigm changes in the modern history of organic chemistry, offering superior process control, reduced waste generation, and enhanced safety from R&D to production scale. [1][2][3] These advantages, which are obtained through the use of micro/ mesofluidic reactors (MFRs) can be further enhanced with the integration of artificial intelligence, [4,5] process analytical technology (PAT) tools, [6] and automation. [7,8] This makes flow technology particularly adapted to robust and versatile production systems, [9,10] and yet, breaking away from centuries of macroscopic batch synthesis has remained difficult. ...
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... An alternative oscillating intensified plug-flow reactor, which has been designed for better incorporation of solids with reduced fouling, is the agitated tubular reactor (ATR), such as the AM Technology Coflore® reactor (shown schematically in Fig. 8a) which is primarily aimed to optimise multiphase mixing/contact operations in continuous solids catalysed chemical reactions [145]. Similar to an OBR, it decouples lateral shear from plug-flow throughput rates using oscillations, allowing residence times to be increased without compromising mixing. ...
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... The results on KIE for catalysts containing metal active components have mostly been investigated in processes (1) and (2). They have shown that for the hydrolysis of both SBH and AB, a primary isotopic effect (kH/kD > 2) is observed when the reaction takes place in deuterated water, and a secondary KIE is noted with isotope-labeled hydrides [43,46,47]. Our tests of the Co 0 catalyst in heavy water are shown in Figure 2a. ...
... Early evaluation of these metrics under a sampling of recent SDL literaturedetailed in Table 1 leads to several technological indicators that can already affect decision-making in SDL studies. 4,[13][14][15][16][17][18][19][20][21][22][23][24][25][26][27][28] First, of the available technologies, microfluidic platforms have demonstrated unassisted generation of larger data sets and at a higher demonstrated throughput, as shown in Fig. 5. Among liquid handling tools, micro-well plate systems were at the top in performance. ...
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