James Hanley Clark

James Hanley Clark
The University of York · Department of Chemistry

BSc PhD

About

674
Publications
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30,242
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Publications

Publications (674)
Article
Lignin is a natural and renewable aromatic raw material of aromatic chemicals and its depolymerization and downstream products conversion has drawn considerable attention. Herein, a series of Ni loaded metal phosphates (Ni/MP, M = Ti, Zr, Nb, La, or Ce) catalysts were fabricated for the hydrodeoxygenation (HDO) of lignin-derived vanillin (VAN) to p...
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The potential of mitigation actions to limit global warming within 2 °C (ref. ¹) might rely on the abundant supply of biomass for large-scale bioenergy with carbon capture and storage (BECCS) that is assumed to scale up markedly in the future2–5. However, the detrimental effects of climate change on crop yields may reduce the capacity of BECCS and...
Article
This study innovated the concept in designing an efficient and reusable microwave (MW) absorbent through concurrent exploitation of carbon graphitization, oxygen functionalization, and carbothermal iron reduction underpinned by an endothermic co-pyrolysis of wood waste and low-dosage iron. A powerful MW assimilation was accomplished from nanoscale...
Article
Biomass valorization to chemicals is an important application of this renewable resource. This study reports the production of two versatile value-added organic acids, i.e., gluconic acid (GOA) and glucuronic acid (GUA), from biomass-derived glucose via microwave-assisted catalytic oxidation. A series of novel low-cost biochar-supported Cu-based ca...
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Oleaginous yeast, cultured on second-generation lignocellulosic resources, has the potential to be a key part of the future energy sector. However, the multiple unit operations necessary to produce concentrated hydrolysates, with a minimum of fermentation inhibitors, limit the applicability to date. In this study, a simple microwave-assisted hydrot...
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The aza-Michael addition is a versatile reaction for the modification of α,β-unsaturated carbonyl compounds with amines. The reactivity of dimethyl itaconate as a bio-based Michael acceptor is explored in this work. Through its reactions with piperidine and dibutylamine, it was found that the order of reaction can be changed by the choice of cataly...
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Hierarchically porous activated Starbons® derived from starch are found to make excellent adsorbents for methylene blue, even in the presence of other dyes and inorganic salts, highlighting their potential to be used in water purification. The optimal material (S950C90) has a methylene blue adsorption capacity (891 mg g⁻¹) almost nine times higher...
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The current process to purify CBD from C. sativa extract is long and intensive, requiring several steps such as winterification for 48 hours at -45 °C and high-temperature, high vacuum distillation. These processes are capital intensive and generate large amounts of toxic solvent waste. In contrast, the solid phase extraction (SPE) methodology prop...
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Cottonseed protein (CP) was compounded with polycaprolactone (PCL) in different concentrations by melt blending, and then hot-pressed to prepare CP/PCL blend films. A co-continuous phase is formed when the CP/PCL content is 50/50, and the tensile strength, modulus and toughness are 9, 10, and 63 times greater than that of neat CP film. This remarka...
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With mounting concerns over critical element sustainability in future bio-refineries, the conversion of phyto-extracted nickel (from contaminated lands) into an inexpensive and clean catalyst could help to reduce demand for virgin precious metals. Utilizing this green approach, noble metal catalysts, which require substantial downstream processing,...
Article
A considerable amount of food waste generated globally could be upcycled to synthesise platform chemicals to enhance environmental sustainability and help realise a circular economy. This study investigates the catalytic production of the vital platform molecule levulinic acid (LA) from bread waste, a typical stream of starch-rich food waste genera...
Article
Due to the global shortage of phosphate ore, sewage sludge is an important resource for P recovery. This study aims to investigate how P was migrated and transformed during the microwave hydrothermal (MHT) process of sewage sludge. The effects of MHT and hydrothermal (HT) conversion were compared. The results reveals that there were no significant...
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Cyclohexanol is an essential intermediate in the chemical industry for the synthesis of nylon and other materials, but the direct hydrogenation of phenol to produce cyclohexanol is problematic due to excessive energy consumption associated with the harsh reaction conditions. In this regard, the novel composite catalysts (Ru/Nb2O5-nC18PA) coated wit...
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Methylation of acetoin with dimethyl carbonate was performed in a sustainable one-step process, with improved process mass intensity (PMI) and atom economy compared to previously published methods. The resulting product, 3-methoxybutan-2-one (MO) was successfully evaluated as a bio-based solvent, while both Kamlet–Taft solvatochromic parameters and...
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There is ever increasing demand to develop surfactants based on sophorolipids because they are produced by non-pathogenic organisms, biodegradable and less toxic to humans and the environment. Herein, commercially available lactonic sophorolipid was modified via epoxidation of the fatty acid units C[double bond, length as m-dash]C and subsequent ri...
Article
The lignin-first biorefinery strategy could produce bio-based phenols from the extraction and depolymerization of native lignin in lignocellulosic biomass. Herein, we report an effective Lewis acid-promoted delignification and production of monophenolic compounds in birch sawdust assisted by microwave heating without external hydrogen for the first...
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2,2,5,5-tetramethyloxolane (TMO) has recently been identified and demonstrated as a safer solvent to replace toluene, THF, and hydrocarbons in a handful of applications. Herein, several bio-based routes to TMO are presented and assessed for greenness, assisted by the CHEM21 Metrics Toolkit and BioLogicTool plots. Using glucose as a common starting...
Article
This study explores a binary solvent system of bio-based Cyrene and its derivative, Cygnet 0.0, with novel properties for applications in membranes technology and bio-catalysed synthesis of polyesters. Cygnet-Cyrene blends have not been reported prior to this work and could represent viable replacements for toxic polar aprotic solvents. The use of...
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This study explores a binary solvent system of biobased Cyrene and its derivative, Cygnet 0.0, with novel properties for applications in membranes technology and bio‐catalysed synthesis of polyesters. Cygnet‐Cyrene blends have not been reported prior to this work and could represent viable replacements for toxic polar aprotic solvents. The use of a...
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The coating of the beech sawdust using a catalytic amount of graphite (as low as 0.25 wt%) allowed a step improvement in the microwave-assisted thermolysis. Results demonstrated that the pyrolysis performance was linked to an electrical conductivity threshold of the coated samples rather than a gradual increase. With as low as 0.13 mS m−1 of electr...
Article
The methylation of alcohols is of great importance since a broad number of bioactive and pharmaceutical alcohols contain methyl groups. Here, a highly efficient β-methylation of primary and secondary alcohols with methanol has been achieved by using bis-N-heterocyclic carbene iridium (bis-NHC-Ir) complexes. Broad substrate scope and up to quantitat...
Article
Furfural is a promising platform chemical that can be catalyzed from lignocellulose biomass. In this study, a novel micro-mesoporous carbon supported tin oxide catalyst (MC-SnOx) was developed to convert xylose into furfural in a low sodium chloride (NaCl) concentration and acid-free biphasic system. The catalysts synthesized by annealing from 400...
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As China ramped-up coal power capacities rapidly while CO 2 emissions need to decline, these capacities would turn into stranded assets. To deal with this risk, a promising option is to retrofit these capacities to co-fire with biomass and eventually upgrade to CCS operation (BECCS), but the feasibility is debated with respect to negative impacts o...
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A multifunctional Ru/SBA-15 catalyst is prepared via impregnation, and used in the depolymerization of crude waste corn stover enzymatic lignin (CSEL) to produce monophenols and unexpectedly, the industrially important organic siloxanes. In the depolymerization of CSEL over Ru/SBA-15, a high phenolic monomer yield of 13.91 wt. % with a high selecti...
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An oligosaccharide-based masking agent suitable for chrome-free metal tanning was produced from cellulose via a stepwise degradation and oxidation process. Firstly, an AlCl3-NaCl-H2O/γ-valerolactone (GVL) biphasic solvent system was established for cellulose conversion (87.6%), which allowed in situ separation of the oligosaccharides and valuable s...
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Biomass-derived N-doped carbon (BNC) is an important environmental material and widely used in the fields of water purification and soil remediation. However, the toxicant in the commonly used synthesis process of BNC materials have been largely ignored. Herein, we firstly report the presence of a highly toxic by-product (KCN) in the activation pro...
Article
ABSTRACT: This work addresses the management of Brewers’ Spent Grain (BSG) using a state-of-the-art, microwave-assisted, hydrothermal carbonization (MA-HTC) process, for the production of hydrochar, i.e., a renewable solid biomaterial with many industrial applications. For the first time, a detailed relationship has been established between the pro...
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Hesperidin and rutin are two sought-after natural flavonoids, traditionally extracted from abundant natural citrus fruits and tea leaves using large amounts of ethanol or methanol solvents. Recent trends in extractions have focused on minimizing the use of solvents and creating simpler cost-effective processes. This study aims to apply the concept...
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An approach of largely improving the properties of protein-based biopolymers is reported. Cottonseed protein concentrate (CPC) purified from cottonseed protein powder waste, with a protein content of >70% and a plasticizing efficiency of 4.2, was used to produce bioplastic polymer. A prepreg consisting of relatively oriented sisal fiber (SF) was tr...
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Porous organometallic polymers (POMPs) with controllable porosity and enhanced CO2 adsorption capability were fabricated via the direct knitting strategy. Excellent selectivity and activity with a record turnover number (TON=1.58×10⁶) in the N‐formylation reaction with CO2 and H2 to N,N‐dimethylformamide (DMF) were achieved under mild reaction cond...
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The valorization of carbon dioxide (CO2 ) to fine chemicals is one of the most promising approaches for CO2 capture and utilization. Herein we demonstrated a series of porous organometallic polymers could be employed as highly efficient and recyclable catalysts for this purpose. Synergetic effects of specific surface area, iridium content, and CO2...
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Microwaves (MWs) are promising technologies for energy-efficient biorefineries which reduce our dependence on petroleum. Here we present evidence for the first time of important interactions between MW and starch, a major biomass from massive global food wastes, which can be observed under both hydrolytic and pyrolytic conditions. Starch is transfo...
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The cultivation of oleaginous yeast on second-generation feedstocks is an attractive alternative for edible lipid production. Despite many studies in this area addressing single aspects of this bioprocess, one of the major bottlenecks is the integration and optimization of the multiple unit operations while demonstrating this on a larger scale. In...
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Floridoside (2-α-O-D-galactopyranosyl glycerol) is a glycerol glycoside that is biosynthesised by most species of red algae and has been implicated as an intracellular regulator of various homeostatic functions. Here, we report the identification of two unforeseen crystal forms of the ubiquitous natural osmolyte floridoside including a seemingly un...
Article
This study investigated migration and transformation mechanism of P in waste activated sludge (WAS) during anaerobic fermentation (AF) process and the subsequent hydrothermal conversion (HTC) process. Control of pH during the AF processes was found to be significant, whereby the use of acidic (pH = 5.5) or alkaline conditions (pH = 9.5) facilitated...
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The efficient valorization of lignin could dictate the success of the 2 nd generation biorefinery. Lignin, accounting for on average a third of the lignocellulosic biomass, is the most promising candidate for sustainable production of value‐added phenolics. However, the structural alteration induced during the lignin isolation is often depleting hi...
Article
In this study, a facile and eco-friendly method for synthesis of granular fuel and granular activated carbon was developed. The approach needs not to add a harmful binder due to inherent characteristics of sawdust hydrochar and has not been previously reported. Granular fuel was prepared from densification of sawdust hydrochar acquired from hydroth...
Article
Catalytic hydrogenolysis of lignin to obtain value-added phenolic chemicals is a sustainable and cost-effective strategy for the efficient valorization of biomass derived wastes. Herein, an innovative approach by using a single-step microwave assisted depolymerization of lignin from birch sawdust without external hydrogen in the mixture of water-al...
Article
Green Tycoon is a free-of-charge game-based mobile application that embraces a systems thinking approach to introducing students to a biorefining process model within green chemistry. Players adopt the role of a manager in a chemical factory, synthesizing the fictional compound, Yorkanone. Through upgrading the system and engaging with the integrat...
Article
Driven by the worldwide demand for sustainable resources and renewable energy, the synthesis of bio-based platform chemicals has attracted broad interest. The isomerisation of glucose to fructose acts as a critical intermediate step among many chemical synthesis routes. In this study, biochar (BC), graphitic oxide (GIO), and graphene oxide (GO) wer...
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The past decades have seen an increasing interest in developing pathways to produce bio-based chemicals from lignocellulosic biomass and organic waste as renewable resources. Using biomass as a source of chemical building blocks is critical to a future sustainable chemical industry. The successful development of bio-chemicals will also have a profo...
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Deep eutectic solvents (DES) are one of the most promising green technologies to emerge in recent years given their combination of environmentally friendly credentials and useful functionalities. Considering the continued search for new DES – especially those that exemplify the aforementioned characteristics, we report the preparation of DES based...
Article
Energy-saving, chemical-free, and high-efficiency microwave (MW)-assisted water treatment can be greatly facilitated via tailored design of an economical, sustainable, and ‘green’ carbonaceous catalyst. In this study, various biochars (BC) were pyrolyzed from two lignocellulosic waste biomasses, oak (O) and apple tree (A), at high temperature (900...
Article
With the aim to develop optimized biochar with minimal contaminants, it is important significance to broaden the understanding of biochar. Here, we disclose for the first time, a highly toxic substance (metal cyanide, MCN, such as KCN or NaCN) in biochar. The cyanide ion (CN⁻) content in biochar can be up to 85,870 mg/kg, which is determined by the...
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Hydrogen is recognized as one of the cleanest energy carriers, which can be produced from renewable biomass as a promising feedstock to achieve sustainable bioeconomy. Thermochemical technologies (e.g., gasification and pyrolysis) are the main routes for hydrogen production from biomass. Although biomass gasification, including steam gasification a...
Article
The interest in adsorbing toxic gases nowadays is primarily due to their short- and long-term adverse health effects. It is generally accepted that the pore morphology and the surface nature play key roles in the adsorption mechanism of any molecules. The interactions between the adsorbate and adsorbent are affected by their polarity, where nonpola...
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Three dipolar aprotic solvents were designed to possess high dipolarity and low toxicity: N , N , N ’, N ’‐tetrabutylsuccindiamide (TBSA), N , N ’‐diethyl‐ N , N ’‐dibutylsuccindiamide (EBSA), N , N ’‐dimethyl‐ N , N ’‐dibutylsuccindiamide (MBSA). They were synthesized catalytically using a K60 silica catalyst in a solventless system. Their water‐i...
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The development, implementation and social acceptance of resource efficient, circular, bio-based economies require critical understanding of the whole supply chain from feedstock to end-use. Trust, transparency and traceability will be paramount. Though life cycle assessment (LCA) is a universally chosen approach to fulfil this purpose, the nature...
Chapter
This work addresses a novel process for the co-production of lignin and oligosaccharides from rapeseed meal, examining the effects of the temperature (150–210 °C), reaction time (0–60 min) and catalyst amount (1–4 mol/L, CH3COOH) on the process. The yields to gas, liquid and solid varied by 0–18%, 22–64% and 34–74%, respectively. The solid consiste...
Chapter
This work addresses the production of fermentable liquid aqueous solutions by microwave-assisted hydrothermal treatment of cellulose and hemicellulose and alginic acid. A reactivity comparison was established at different temperatures (160–210 °C), reaction times (0 and 5 min) and solid/water ratios (1/20 and 1/10 g/g). The nature of the carbohydra...
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Bio-based solvents were investigated for the biocatalysed amidation reactions of various ester-amine combinations by Pseudomonas stutzeri lipase (PSL). Reactions were undertaken in a range of green and potentially bio-based solvents including terpinolene, p-cymene, limonene, 2-methyl THF, ɣ-valerolactone, propylene carbonate, dimethyl isosorbide, g...
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Increasing demand for chemicals worldwide, depleting resources, consumer pressure, stricter legislation, and the rising cost of waste disposal are placing increasing pressure on chemical and related industries. For any organization to survive in the current arena of growing climate change laws and regulations, and increasing public influence, the i...
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This work addresses a microwave-assisted, NaCl–H2O/γ-valerolactone (GVL) solvent system for the co-production of 5-hydroxymethylfurfural (HMF) and saccharides from cellulose, examining the effects of the solvent system (H2O/GVL), NaCl concentration and reaction time. Oligosaccharides and glucose were completely recovered in the aqueous phase and th...
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Green Machine is a competitive strategy card game facilitating a systems thinking approach to learning recycling processes and green chemistry in accordance with the United Nations Sustainable Development Goals. Players compete to be the first to be able to launch their recycling plant by collecting a series of playing cards. Players must use inter...
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A more sustainable dialysis and water filtration membrane has been developed, by using the new, safer, bio-based solvent Cyrene® in place of N-methyl pyrrolidinone (NMP). The effects of solvent choice, solvent evaporation time, the temperature of casting gel, and coagulation bath together with the additive concentration on porosity and pore size di...
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There is demand for safer and bio-based solvents, brought on by legislation and sustainability objectives. The prediction of physical properties is highly desirable to help design new molecules. Here we present an in silico approach to obtain calculated Kamlet–Abboud–Taft solvatochromic parameters using virtual experiments. The tautomerisation equi...