Molecule-electron-proton transfer in enzyme-photo-coupled catalytic system

doi:10.1016/S1872-2067(22)64154-8

Chinese Journal of Catalysis ›› 2023, Vol. 44: 96-110.DOI: 10.1016/S1872-2067(22)64154-8

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Molecule-electron-proton transfer in enzyme-photo-coupled catalytic system

Shihao Li^a^,^c, Jiafu Shi^b^,^c^,^*(), Shusong Liu^b, Wenping Li^a^,^c, Yu Chen^b, Huiting Shan^a^,^d, Yuqing Cheng^a^,^c, Hong Wu^a^,^c^,^*(), Zhongyi Jiang^a^,^c^,^d^,^*()

^aKey Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China
^bSchool of Environmental Science & Engineering, Tianjin University, Tianjin 300072, China
^cCollaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin 300072, China
^dJoint School of National University of Singapore and Tianjin University, International Campus of Tianjin University, Fuzhou 350207, Fujian, China

Received:2022-05-28 Accepted:2022-07-14 Online:2022-12-10 Published:2022-12-08
Contact: Jiafu Shi, Hong Wu, Zhongyi Jiang
About author:Jiafu Shi (School of Environmental Science & Engineering, Tianjin University) obtained his PhD in Chemical Technology from Tianjin University (China) in 2013. After graduation, he joined the faculty of Tianjin University, and started working at the School of Environmental Science and Engineering. He was a visiting scholar of University of California at Berkeley with Professor Phillip B. Messersmith from 2016 to 2017. He is the winner of National Science Fund for Excellent Young Scholars in China. His research interest encompasses enzyme-catalyzed biomanufacturing processes. He has co-authored over 100 peer-reviewed papers, including in Chemical Society Reviews, Journal of the American Chemical Society, ACS Catalysis, Advanced Functional Materials, Chem, Angewandte Chemie International Edition, Joule, etc.
Hong Wu (School of Chemical Engineering and Technology, Tianjin University) received her PhD in Chemical Engineering from Tianjin University (China). Her research interests include membrane materials and membrane processes as well as enzyme immobilization and enzymatic catalysis. To date, she has co-authored over 300 peer-reviewed papers including in Nature Communications, Chemical Society Reviews, Journal of the American Chemical Society, Angewandte Chemie International Edition, Advanced Materials, Advanced Functional Materials, etc.
Zhongyi Jiang (School of Chemical Engineering and Technology, Tianjin University) obtained a PhD degree from Tianjin University (China) in 1994. He was a visiting scholar of University of Minnesota with Prof. Edward Cussler in 1997 and California Institute of Technology with Prof. David Tirrell in 2009. He is the winner of National Science Fund for Distinguished Young Scholars in China, Cheung Kong Chair Professor, Fellow of the Royal Society of Chemistry. His research interest includes biomimetic and bioinspired membranes and membrane processes, biocatalysis, photocatalysis. To date, he has co-authored over 600 peer-reviewed papers, including in Nature Sustainability, Nature Communications, Chemical Society Reviews, Progress in Polymer Science, Journal of the American Chemical Society, Angewandte Chemie International Edition, Advanced Materials, ACS Catalysis, etc.
Supported by:
National Excellent Youth Science Fund Project of National Natural Science Foundation of China(22122809);National Key R&D Program of China(2020YFA0907902);National Natural Science Funds of China(21621004);Natural Science Fund of Tianjin(19JCYBJC19700);Open Funding Project of the State Key Laboratory of Biochemical Engineering(2020KF-06)

Abstract

Abstract:

Enzyme-Photo-coupled Catalytic System (EPCS) integrates the light absorption capacity of photocatalysts and the high activity/specificity of enzymes, which is becoming an emerging technology platform to mimic natural photosynthesis for harnessing solar energy to generate valuable products, including bulk chemicals, energy chemicals and pharmaceutical chemicals. Cofactors including NAD(P)⁺/NAD(P)H, as "energy currency", are involved in over 80% biocatalytic redox reactions, establishing a bridge of mass/energy exchange between photocatalysis and cofactor-dependent enzyme catalysis. Although numerous efforts have been devoted, the performance of current EPCS is far from the theoretical upper limit. The individual and synergistic intensification of molecule-electron-proton transfer evolves a critical yet challenging issue in EPCS. This Review will focus on the molecule-electron-proton transfer in natural photosynthesis and in EPCS. Future endeavors to intensify all three transfers to construct a more efficient EPCS are suggested as pursuit for a new pattern of modern chemical engineering.

Key words: Enzyme-photo-coupled catalytic system, Molecule-electron-proton transfer, NAD(P)H regeneration, Enzyme catalysis, Photocatalysis

Shihao Li, Jiafu Shi, Shusong Liu, Wenping Li, Yu Chen, Huiting Shan, Yuqing Cheng, Hong Wu, Zhongyi Jiang. Molecule-electron-proton transfer in enzyme-photo-coupled catalytic system[J]. Chinese Journal of Catalysis, 2023, 44: 96-110.

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Figures/Tables 9

Fig. 1. General framework for EPCS.

Fig. 2. (a) Schematic diagram of natural photosynthesis. (b) Partial process of CCM in algal cells. (c) The photosynthetic electron and proton transfer in algal cells. (d) Schematic view of the molecule-electron-proton transfer in algal cells. Reprinted with permission from Ref. [46]. Copyright 2022, Springer Nature.

Fig. 3. Strategies for the intensification of molecule transfer. (a) Fortifying the mixing of the reaction system by a highly reactive agitating impeller. (b) Shortening the molecule transfer distance; (c) Enlarging the pore size. (d) Shortening the channel length. (e) Altering the morphology and dimension of the catalysts.

Fig. 4. Intensification of molecule transfer in EPCS. (a) Intensifying the transfer of TEOA to the photogenerated holes by regulating the thickness of the shell. Reprinted with permission from Ref. [73]. Copyright 2022, American Chemical Society. (b-d) Improving the shuttling of NAD+/NADH molecules between photocatalysts and enzyme catalysts by reducing the mass transfer distance. Reprinted with permission from Ref. [10]. Copyright 2022, John Wiley and Sons, Ref. [71]. Copyright 2022, American Chemical Society and Ref. [74]. Copyright 2022, American Chemical Society.

Fig. 5. Strategies for the intensification of electron transfer. (a) Fine-tuning the electron transfer distance. (b) Optimizing the electron transfer interface. (c) Building electron transfer channel. (d) Introducing electrically conductive template. (e) Introducing electron transfer mediator.

Fig. 6. (a) Improving the electron transfer by introducing electrically conductive module chemically converted graphene (CCG). Reprinted with permission from Ref. [89]. Copyright 2022, American Chemical Society. (b) Together enhancing the electron generation and electron transfer by adding additional photocatalyst (α-Fe302) and optimizing the interface of photocatalyst and building fast electron transfer channel (C, carbon moiety). Reprinted with permission from Ref. [90]. Copyright 2022, American Chemical Society. (c) Coordinating the fast electron transfer and the slow electron utilization by the reaction centers [Cp*Rh(bpydc)H2O]2+ behave as the electron buffer tank and store these electrons in the form of hydrides for subsequent regeneration of NADH. Reprinted with permission from Ref. [91]. Copyright 2022, American Chemical Society.

Fig. 8. (a) The proton gradient formed by the transmembrane migration of protons in NADH subsequently drives the synthesis of ATP for the autonomous self-sustaining production of glucose-6-phosphate. Reprinted with permission from Ref. [110]. Copyright 2022, John Wiley and Sons. (b) Rapid intermolecular proton migration in NADH-mediated photocatalytic hydrogen evolution and enzymatic dehydrogenation of alcohol within the ADH catalytic pocket. Reprinted with permission from Ref. [114]. Copyright 2022, Springer Nature. (c) Intramolecular proton migration process in the Ru-BNAH/TiO2/Cu2O photocathode catalytic CO2 reduction by using BNAH as proton carrier. Reprinted with permission from Ref. [115]. Copyright 2022, Royal Society of Chemistry.

Fig. 9. Synergistic intensification of molecule and electron transfer in EPCS. (a) The electron-mediator was anchored to the nodes of the metal-organic framework to facilitate electron transfer and the shortened distance between photocatalytic and enzymatic systems could promote the shuttling of NAD+/NADH molecules. Reprinted with permission from Ref. [72]. Copyright 2022, American Chemical Society. (b) The conductive amorphous titania (a-TiO2) nanoshell facilitated the transfer of photogenerated electrons from GCN to the a-TiO2 surface, and the diffusion of TEOA from the a-TiO2 surface to GCN for consuming the holes could be enhanced by regulating the thickness of the shell. Reprinted with permission from Ref. [66]. Copyright 2022, American Chemical Society. (c) The Z-scheme photocatalysis module allowed the efficient transfer of electrons flowing along “BP-AM-M”, and the integration of NAD+ and the enzyme between the AM and BP layers enhanced the synergy between the photocatalytic and enzymatic systems. Reprinted with permission from Ref. [70]. Copyright 2022, Royal Society of Chemistry.

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Molecule-electron-proton transfer in enzyme-photo-coupled catalytic system

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