Article
Engineering, Chemical
Mengya Guo, Fengjuan Gu, Lingding Meng, Qiyong Liao, Zihui Meng, Wenfang Liu
Summary: This study investigates the reduction of CO2 to formaldehyde using a photo-enzyme coupled system. The optimal pH values and electron donors for the reactions are determined. Furthermore, the loading ratio of enzymes and the concentration of cofactors are optimized, and the stability of the system is examined. The results demonstrate the efficiency and stability of the photo-enzyme coupled system in producing formaldehyde from CO2.
SEPARATION AND PURIFICATION TECHNOLOGY
(2022)
Article
Chemistry, Multidisciplinary
Shih-Hao Wang, Rathinam Raja, Chuen-Yo Hsiow, Farheen Khurshid, Hau-Ren Yang, Po-Wen Chung, Yu-Ying Lai, Ru-Jong Jeng, Leeyih Wang
Summary: This work demonstrates the efficient catalytic conversion of CO2 to CO using a fullerene derivative, DTBT-C-60, as a photocatalyst, which exhibits excellent solar absorption and durable catalytic activity.
Review
Chemistry, Physical
Lucy C. Ward, Hannah V. McCue, Andrew J. Carnell
Summary: The review focuses on the potential use of carboxyl methyltransferases (CMTs) in industrial biotechnology, highlighting their ability to generate diverse methyl esters under aqueous conditions. Strategies for regenerating the required cofactor S-adenosylmethionine (SAM) are discussed, which will further improve the industrial applications of CMTs.
Article
Chemistry, Multidisciplinary
David M. Klein, Santiago Rodriguez-Jimenez, Marlene E. Hoefnagel, Andrea Pannwitz, Amrutha Prabhakaran, Maxime A. Siegler, Tia E. Keyes, Erwin Reisner, Albert M. Brouwer, Sylvestre Bonnet
Summary: The length of alkyl tails in lipid bilayers affects the photocatalytic performance of liposomes containing molecular catalysts and photosensitisers. Shorter alkyl chains result in higher CO production due to the presence of more mobile and less buried molecular species in the membrane, leading to enhanced electron transfer kinetics.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Multidisciplinary
Niklas Noll, Tobias Gross, Kazutaka Shoyama, Florian Beuerle, Frank Wuerthner
Summary: We report a series of bipyridine-containing di- to tetranuclear Ru(bda) macrocycles 2C-4C that promote O-O bond formation for photocatalytic water oxidation. Under neutral conditions, all complexes 2C-4C adopt a folded conformation and follow the water nucleophilic attack (WNA) pathway with high turnover frequencies up to 15.5 s(-1) per Ru unit. Crystal structure analysis reveals increased intramolecular pi-pi stacking and preorganization of proximal bases for larger macrocycles. H/D kinetic isotope effect studies and electrochemical data confirm the key role of proximal bipyridines as proton acceptors in lowering the activation barrier for the crucial nucleophilic attack of H2O in the WNA mechanism.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Constantin D. Sahm, Geani M. Ucoski, Souvik Roy, Erwin Reisner
Summary: This study presents a continuous-flow setup for studying photocatalytic CO2 reduction systems, demonstrating the advantages of automation and efficiency. The methodology is shown to be effective in studying photocatalyst systems under various conditions, advancing the understanding of light absorber platforms and molecular co-catalyst hybrids for CO2 reduction.
Article
Chemistry, Physical
Elif Erdem, Lenny Malihan-Yap, Leen Assil-Companioni, Hanna Grimm, Giovanni Davide Barone, Carole Serveau-Avesque, Agnes Amouric, Katia Duquesne, Veronique de Berardinis, Yagut Allahverdiyeva, Veronique Alphand, Robert Kourist
Summary: BVMOXeno is a highly efficient Baeyer-Villiger monooxygenase with higher reaction rates and lower KM value compared to currently known BVMOs, almost completely suppressing unwanted side reactions. The recombinant production of BVMO in cyanobacteria allows more efficient utilization of water and oxygen generated by photosynthesis.
Article
Polymer Science
Xu Han, Yun Tao, Chao Xu, Yicong Deng, Zisen Meng, Zhenhao Dou, Peng Wang, Quan Feng
Summary: The study developed an electrospinning approach to immobilize hemin particulates onto PAN nanofibers and utilized H2O2 as an oxidant to simulate hemin's enzymatic catalysis in organisms. The nanocomposite membranes showed excellent properties in adsorption and degradation, with a significant red shift in light absorption attributed to the molecular interaction between polymer and hemin.
Article
Chemistry, Multidisciplinary
Markus Hobisch, Jelena Spasic, Lenny Malihan-Yap, Giovanni Davide Barone, Kathrin Castiglione, Paula Tamagnini, Selin Kara, Robert Kourist
Summary: This study demonstrates the use of internal illumination to overcome the cell density limitation of cyanobacterial biotransformations, achieving high reaction rates in a scalable photobioreactor.
Article
Engineering, Environmental
Shujie Liang, Xiaohui Zhong, Zuqi Zhong, Bin Han, Weiyi Chen, Kainan Song, Hong Deng, Zhang Lin
Summary: The research presented a biomimetic artificial photosynthesis system based on ZrO2 nanoframes and metalloporphyrin to mimic the morphology of trees. The system achieved high photocatalytic performance, displaying high selectivity for CO production and significant apparent quantum efficiency.
CHEMICAL ENGINEERING JOURNAL
(2021)
Article
Chemistry, Multidisciplinary
Pragya Singh, Rohit Srivastava
Summary: This review highlights the importance of reducing CO2 emissions and utilizing it through enzymatic methods, focusing on converting CO2 into hydrocarbon fuels. Enzymatic approaches are shown to be a green, efficient, and less toxic way of producing useful products from CO2, with potential applications in various industries.
JOURNAL OF CO2 UTILIZATION
(2021)
Article
Multidisciplinary Sciences
Le Zeng, Ling Huang, Wenhai Lin, Lin-Han Jiang, Gang Han
Summary: The authors reported the photoreduction of aryl halides enabled by red light without the need for sacrificial electron donors. They achieved this by introducing a red light-absorbing photosensitizer and using the triplet-triplet annihilation strategy.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Niklas Noll, Frank Wuerthner
Summary: The cyclic dinuclear ruthenium complex with oligo(ethylene glycol)-functionalized axial calix[4]arene ligands showed enhanced catalytic activity in water oxidation compared to the mononuclear reference compound. The kinetic studies revealed a unimolecular water nucleophilic attack mechanism for this novel dinuclear water oxidation catalyst, demonstrating its potential for artificial photosynthesis. The photocatalytic performance of this complex was reported to be the highest among Ru(bda) complexes, indicating its promising application in the field of water oxidation research.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Physical
David M. Klein, Leonardo Passerini, Martina Huber, Sylvestre Bonnet
Summary: Photocatalytic proton reduction is a promising method for producing clean and sustainable dihydrogen. Immobilizing catalysts and photosensitizers on liposomes is an attractive approach for biomimetic solar fuel production. The stability of the catalyst has been a limitation in current systems, but a new cobalt complex immobilized on the lipid bilayer of liposomes has shown improved performance in this study.
Review
Chemistry, Physical
Qian Wang, Zhenhua Pan
Summary: This review provides a comprehensive summary of recent advancements in cocatalysts for photocatalytic CO2 reduction reaction (CO2RR), offering insights and guidance for future research directions and best practices.
Article
Chemistry, Physical
Yunjian Ma, Zongquan Li, Hao Zhang, Vincent Kam Wai Wong, Frank Hollmann, Yonghua Wang
Summary: This study proposes a parallel cascade using aryl alcohol oxidase (PeAAOx) from Pleurotus eryngii and unspecific peroxygenase (AaeUPO) from Agrocybe aegerita to convert aromatic primary alcohols into high-value aromatic aldehydes. Key factors such as enzyme dosage, pH, and temperature were investigated. The study evaluates the universality of PeAAOx coupled with AaeUPO cascade catalysis for the synthesis of aromatic aldehyde flavor compounds.
Article
Chemistry, Multidisciplinary
Xiaomin Xu, Jacob M. A. van Hengst, Yejia Mao, Mireia Martinez, Sergi Roda, Martin Floor, Victor Guallar, Caroline E. Paul, Miguel Alcalde, Frank Hollmann
Summary: A peroxygenase-catalysed hydroxylation of organosilanes has been reported, demonstrating efficient conversion of various silane starting materials and high catalyst performance. Molecular modelling of the enzyme-substrate interaction provides a basis for understanding the selectivity of AaeUPO.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Biochemistry & Molecular Biology
Henrik Terholsen, Kamela Myrtollari, Mirna Larva, Christina Moeller, Andreas Taden, Robert Kourist, Uwe T. Bornscheuer, Daniel Kracher
Summary: Biocatalytic decarboxylation of hydroxycinnamic acids yields phenolic styrenes, which are important precursors for antioxidants, epoxy coatings, adhesives, and other polymeric materials. This study presents two robust and sensitive assays based on photometry and fluorimetry to track decarboxylation reactions with high sensitivity while avoiding product extraction and long analysis times. The optimized assay procedures were used to measure BsPAD activity and determine the kinetic constants of the purified enzyme for different hydroxycinnamic acids, showing substrate inhibition for caffeic acid.
Article
Chemistry, Physical
Yinqi Wu, Caroline E. Paul, Thomas Hilberath, Ewald P. J. Jongkind, Wuyuan Zhang, Miguel Alcalde, Frank Hollmann
Summary: The utilization of fatty acids can be expanded by adding new functionalities to the hydrocarbon part. In this study, a peroxygenase mutant AaeUPO-Fett is demonstrated to selectively oxyfunctionalize fatty acids, leading to the production of ?-1 hydroxy fatty acid (esters). These hydroxy fatty acid (esters) can be further transformed into lactones, alcohols, esters, and amines through multi-enzyme cascades, providing new pathways for fatty acid valorisation.
Article
Chemistry, Physical
Andrea M. Chanique, Nakia Polidori, Lucija Sovic, Daniel Kracher, Leen Assil-Companioni, Philipp Galuska, Loreto P. Parra, Karl Gruber, Robert Kourist
Summary: Cold-active enzymes have optimal activity at low temperatures, making them useful for preserving heat-sensitive compounds. A cold-active flavin-dependent monooxygenase (FMO) was discovered in an Antarctic organism, showing high activity between 5 and 25 degrees C and promiscuity towards NADH and NADPH. The enzyme exhibits high enantioselectivity and has a unique active site structure.
Review
Chemistry, Physical
Veronique Alphand, Willem J. H. van Berkel, Valentina Jurkas, Selin Kara, Robert Kourist, Wolfgang Kroutil, Francesco Mascia, Marc M. Nowaczyk, Caroline E. Paul, Sandy Schmidt, Jelena Spasic, Paula Tamagnini, Christoph K. Winkler
Summary: The recent increase of interest in photocatalysis has expanded to biocatalysis and led to a surge in the development of light-dependent enzyme-mediated or enzyme-coupled processes. Reviewing the progress in photobiocatalysis, we suggest categorizing it into different disciplines and providing guidelines for reporting research results and performing photobiocatalytic reactions. Overall, we believe that this field enhances the diversity of biocatalytic reactions and harnesses the selectivity of enzymes in photocatalysis. We anticipate that the ongoing enthusiasm for light-dependent enzymatic processes will uncover new photobiocatalytic mechanisms, complementing biocatalysis with novel bond-forming reactions and innovative strategies for utilizing light as a sustainable energy source.
Article
Multidisciplinary Sciences
Shun Zhang, Ruizhi Wu, Feng Zhong, Xiaochun Ma, Xiang Wang, Qiang Wu
Summary: The strength of bcc-structured Mg-Li alloy is improved by alloying Zn, with compressive yield strength reaching over 300 MPa due to semi-coherent B2 nanoparticles in cast state Mg-13Li-9Zn alloy. The compressive yield strength immediately increases to 400 MPa in as-quenched state Mg-13Li-15Zn (LZ1315) alloy, thanks to solid solution strengthening of Zn and the spinodal zone. Additionally, as-quenched LZ1315 alloy exhibits natural aging strengthening behavior, with yield strength up to 495 MPa due to precipitation of B2 nanoparticles.
FUNDAMENTAL RESEARCH
(2023)
Article
Chemistry, Physical
Chang Hyun Kim, Jinhyun Kim, Frank Hollmann, Chan Beum Park
Summary: Solar-driven N2 fixation provides a green alternative to the energy-intensive Haber-Bosch process, but the effect of oxidation reaction on N2 reduction has not been investigated in N2-reducing photo-electrochemical (PEC) studies. In this study, a bias-free PEC platform for N2 reduction and H2O oxidation was developed, and valuable chemicals were simultaneously synthesized on both electrodes using N2, H2O, and sunlight. This work represents the first example of a PEC NRR platform coupled with H2O oxidation and H2O2-dependent oxygenation for unbiased chemical synthesis.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Inorganic & Nuclear
Carolin Muegge, Nora Nowak, Martin Strack, Nils Metzler-Nolte, Wolfgang Weigand
Summary: Metal-containing peptide conjugates have potential for bioinorganic and medicinal research. Synthetic strategies and the order of conjugation and complexation are important for successful synthesis. Different linking methods, such as click reactions and amide bond conjugation, can be applied depending on the demands of the metal bioconjugate.
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Physical
Tiantian Li, Hongjing Liang, Bin Wu, Dongming Lan, Yunjian Ma, Frank Hollmann, Yonghua Wang
Summary: In this study, a new peroxygenase (AbvbUPO) was identified and successfully used for the selective oxyfunctionalisation of various organic compounds. The activity of AbvbUPO on fatty acids was also investigated in detail, showing higher activity in cyclohexene epoxidation and sulfonation of sulfide substrates.
MOLECULAR CATALYSIS
(2023)
Article
Chemistry, Physical
Andrea M. Chanique, Nakia Polidori, Lucija Sovic, Daniel Kracher, Leen Assil-Companioni, Philipp Galuska, Loreto P. Parra, Karl Gruber, Robert Kourist
Summary: Cold-active enzymes maintain high activity at low temperatures, making them useful for avoiding side reactions and preserving heat sensitive compounds. Through genome mining, a cold-active enzyme was discovered in an Antarctic organism, showing high activity at temperatures between 5 and 25 degrees C and displaying promiscuity towards NADH and NADPH, as well as a wide range of ketones and thioesters.
Article
Chemistry, Multidisciplinary
Patricia Gomez de Santos, Ivan Mateljak, Manh Dat Hoang, Sarel J. Fleishman, Frank Hollmann, Miguel Alcalde
Summary: In this study, we used the FuncLib algorithm based on phylogenetic and Rosetta calculations to design a diverse repertoire of active, stable, and enantiodivergent fungal perox-ygenases. These designs, which carried 4-5 mutations in the catalytic core, were functionally expressed in yeast and showed remarkable improvements in catalytic efficiency and enantiodivergence compared to the parental enzyme. The functional divergence was attributed to beneficial epistasis among the mutations and extensive reorganization of the heme channel. This work highlights the potential of FuncLib in designing highly functional libraries of enantioselective peroxygenases for biotechnological applications.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Applied
Yunjian Ma, Xuanru Zhong, Bin Wu, Dongming Lan, Hao Zhang, Frank Hollmann, Yonghua Wang
Summary: In this study, a new fatty acid photodecarboxylase (FAP) called McFAP was discovered from the marine organism Micractinium conductrix. Unlike other known FAPs, McFAP shows high catalytic activity towards short and medium fatty acids. The recombinant expression and basic biochemical characterization of this new FAP member are reported.
CHINESE JOURNAL OF CATALYSIS
(2023)
