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Qiao, Li (author), Zhang, Jing (author), Jiang, Yongjian (author), Ma, Bianqin (author), Chen, Haomin (author), Gao, Peng (author), Zhang, Pengfei (author), Wang, Anming (author), Sheldon, R.A. (author)
Effective photolytic regeneration of the NAD(P)H cofactor in enzymatic reductions is an important and elusive goal in biocatalysis. It can, in principle, be achieved using a near-infrared light (NIR) driven artificial photosynthesis system employing H<sub>2</sub>O as the sacrificial reductant. To this end we utilized TiO<sub>2</sub>/reduced...
journal article 2024
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Luo, Zhiyuan (author), Qiao, Li (author), Chen, Haomin (author), Mao, Zhili (author), Wu, Shujiao (author), Ma, Bianqin (author), Xie, Tian (author), Wang, Anming (author), Pei, Xiaolin (author), Sheldon, R.A. (author)
The design and orderly layered co-immobilization of multiple enzymes on resin particles remain challenging. In this study, the SpyTag/SpyCatcher binding pair was fused to the N-terminus of an alcohol dehydrogenase (ADH) and an aldo-keto reductase (AKR), respectively. A non-canonical amino acid (ncAA), p-azido-L-phenylalanine (p-AzF), as the...
journal article 2024
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Qiao, Li (author), Luo, Zhiyuan (author), Wang, Ru (author), Pei, Xiaolin (author), Wu, Shujiao (author), Chen, Haomin (author), Xie, Tian (author), Sheldon, R.A. (author), Wang, Anming (author)
Two non-canonical amino acids (ncAAs) with bio-orthogonal reactive groups, namely, p-azido-l-phenylalanine (p-AzF) and p-propargyloxy-l-phenylalanine (p-PaF), were genetically inserted into an aldo-keto reductase (AKR) and an alcohol dehydrogenase (ADH), respectively, at two preselected sites for each enzyme. The variants were expressed in...
journal article 2023
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Sheldon, R.A. (author), Bode, Moira L. (author), Mathebula, Nompumelelo (author)
The discovery that enzymes could function efficiently in organic solvents revolutionized their use in industry but represented a change from the natural “green” solvent, water, to a host of environmentally undesirable solvents. Considerable effort is being devoted to making such processes greener again. Bio-based solvents, derived from waste...
review 2023
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Sheldon, R.A. (author)
The introduction of the E Factor in 1992 focussed attention on the problem of waste generation, defined as everything but the desired product, in chemicals manufacture and gave rise to a paradigm shift in our concept of efficiency in chemical processes, from one based solely on chemical yield to one that assigns value to eliminating waste....
review 2023
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Qiao, Li (author), Luo, Zhiyuan (author), Chen, Haomin (author), Zhang, Pengfei (author), Wang, Anming (author), Sheldon, R.A. (author)
The use of engineered ketoreductases (KREDS), both as whole microbial cells and isolated enzymes, in the highly enantiospecific reduction of prochiral ketones is reviewed. The homochiral alcohol products are key intermediates in, for example, pharmaceuticals synthesis. The application of sophisticated protein engineering and enzyme...
journal article 2023
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Sheldon, R.A. (author), Bode, Moira L. (author), Akakios, Stephanie G. (author)
The increasingly apparent negative impact of human activities on the environment has heightened the urgency for the chemistry community to adopt greener and more sustainable practices. The E-factor can still be considered a valuable tool in this drive, particularly because of its broad acceptance and familiarity amongst both industrial and...
review 2022
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Pei, Xiaolin (author), Luo, Zhiyuan (author), Qiao, Li (author), Xiao, Qinjie (author), Zhang, Pengfei (author), Wang, Anming (author), Sheldon, R.A. (author)
The covalent immobilisation of enzymes generally involves the use of highly reactive crosslinkers, such as glutaraldehyde, to couple enzyme molecules to each other or to carriers through, for example, the free amino groups of lysine residues, on the enzyme surface. Unfortunately, such methods suffer from a lack of precision. Random formation...
review 2022
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Mathebula, Nompumelelo P. (author), Sheldon, R.A. (author), Bode, Moira L. (author)
Acylated Morita-Baylis-Hillman (MBH) adducts were synthesised and subjected to enzymatic kinetic resolution (EKR) by hydrolysis employing various lipase enzymes: from P. fluorescens, P. cepacia (PCL), C. antarctica A (CAL−A), C. antarctica B (CAL−B) and Novozyme 435. In a number of instances enantiopure Morita-Baylis-Hillman acetates or...
journal article 2022
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Sheldon, R.A. (author), Brady, Dean (author)
In the movement to decarbonize our economy and move away from fossil fuels we will need to harness the waste products of our activities, such as waste lignocellulose, methane, and carbon dioxide. Our wastes need to be integrated into a circular economy where used products are recycled into a manufacturing carbon cycle. Key to this will be the...
review 2022
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Sheldon, R.A. (author)
This perspective reviews the current status and prospects of biocatalysis in ionic liquids. Although they are not strictly speaking ionic liquids, deep eutectic solvents are included because of the close similarities of their properties and potential applications with those of ionic liquids. One consequence of the ongoing transition from an...
journal article 2021
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Roschangar, Frank (author), Li, Jun (author), Zhou, Yanyan (author), Aelterman, Wim (author), Borovika, Alina (author), Colberg, Juan (author), Dickson, David P. (author), Gallou, Fabrice (author), Sheldon, R.A. (author)
The large and steadily growing demand for medicines combined with their inherent resource-intensive manufacturing necessitates a relentless push for their sustainable production. Pharmaceutical companies are constantly seeking to perform reliable life cycle assessments of their medicinal products and assess the true value of their sustainable...
journal article 2021
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Akakios, Stephanie Gina (author), Bode, Moira Leanne (author), Sheldon, R.A. (author)
The greenness and sustainability of three different routes for the synthesis of (3R,3aS,6aR)-hexahydrofuro [2,3-b] furan-3-ol (bis-furan alcohol), an advanced intermediate for a group of HIV protease inhibitors, including the FDA approved darunavir, used in antiretroviral (ARV) therapy, were compared. The method involved a comparison of (i)...
journal article 2021
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Sheldon, R.A. (author), Basso, Alessandra (author), Brady, Dean (author)
This tutorial review focuses on recent advances in technologies for enzyme immobilisation, enabling their cost-effective use in the bio-based economy and continuous processing in general. The application of enzymes, particularly in aqueous media, is generally on a single use, throw-away basis which is neither cost-effective nor compatible...
review 2021
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Sheldon, R.A. (author), Brady, Dean (author), Bode, ML (author)
Enzymes are excellent catalysts that are increasingly being used in industry and academia. This perspectiveis primarily aimed at synthetic organic chemists with limited experience using enzymes and providesa general and practical guide to enzymes and their synthetic potential, with particular focus on recentapplications
review 2020
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Papadogianakis, Georgios (author), Sheldon, R.A. (author), Murzin, Dmitry Yu (author), Wu, Yulong (author)
contribution to periodical 2020
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Sheldon, R.A. (author)
The role of bio- and chemo-catalytic aerobic oxidations in the production of commodity chemicals in a bio-refinery is reviewed. The situation is fundamentally different to that in a petrochemicals refinery where the feedstocks are gaseous or liquid hydrocarbons that are oxidized at elevated temperatures in the vapor or liquid phase under...
review 2020
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Sheldon, R.A. (author), Norton, Michael (author)
The linear economy for plastic packaging, which currently leads to excessive carbon dioxide emissions and leakage into the environment, needs to be reformed to a greener circular model which is resource efficient and environmentally benign. This requires a system-wide redesigning of rules and incentives that apply to the plastics value chain,...
review 2020
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Sheldon, R.A. (author)
Two of the grand societal and technological challenges of the twenty first century are the 'greening' of chemicals manufacture and the ongoing transition to a bio-based economy: that is a sustainable, carbon-neutral economy based on renewable biomass as the raw material. These challenges are motivated by the need to eliminate environmental...
journal article 2019
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Sheldon, R.A. (author)
Biocatalysis has emerged in the last decade as a pre-eminent technology for enabling the envisaged transition to a more sustainable bio-based economy. For industrial viability it is essential that enzymes can be readily recovered and recycled by immobilization as solid, recyclable catalysts. One method to achieve this is via carrier-free...
journal article 2019
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