酶-光偶联催化系统中分子-电子-质子传递过程与机制

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

催化学报 ›› 2023, Vol. 44: 96-110.DOI: 10.1016/S1872-2067(22)64154-8

酶-光偶联催化系统中分子-电子-质子传递过程与机制

李诗浩^a^,^c, 石家福^b^,^c^,^*(), 刘书松^b, 李文萍^a^,^c, 陈裕^b, 单慧婷^a^,^d, 程雨晴^a^,^c, 吴洪^a^,^c^,^*(), 姜忠义^a^,^c^,^d^,^*()

^a天津大学化工学院, 天津 300072
^b天津大学环境科学与工程学院, 天津 300072
^c天津化学化工协同创新中心, 天津300072
^d天津大学-新加坡国立大学福州联合学院, 福建福州 350207

收稿日期:2022-05-28 接受日期:2022-07-14 出版日期:2022-12-10 发布日期:2022-12-08
通讯作者: 石家福,吴洪,姜忠义
基金资助:
国家优秀青年科学基金(22122809);国家重点研发计划(2020YFA0907902);国家自然科学基金(21621004);天津市自然科学基金(19JCYBJC19700);生化工程国家重点实验室开放式基金项目(2020KF-06)

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)

摘要/Abstract

摘要：

酶-光偶联催化系统(EPCS)集成了半导体的光吸收能力和酶的高活性/特异性, 可模拟自然界光合作用实现太阳能驱动的有用化学品合成. 作为EPCS中的“能量货币”, 辅因子(如NAD(P)+和NAD(P)H)参与了约80%的酶促氧化还原反应, 且在酶-光间充当物质/能量交换的枢纽. 然而, EPCS涉及光催化和酶催化反应, 涉及分子、电子和质子传递过程, 属于典型的复杂多相反应, 导致其光-化学转化效率与理论值差距较大.

本文从微观尺度对EPCS中分子-电子-质子传递过程进行了理解和剖析, 系统介绍了自然界光合作用和EPCS中的“新三传”现象. 此外, 与传统化工领域通过强化宏观尺度上“三传”(即质量传递、热量传递和动量传递)提升单元操作过程效率的方法类似, 本文总结并提出了通过协调优化“新三传”(即分子传递、电子传递和质子传递)来强化EPCS中物质-能量耦合关系, 进而提升光-化学转化效率的新策略. 其中, 分子传递主要包括电子供体分子从反应液向催化剂传递以及辅因子分子在光催化模块和酶催化模块间穿梭; 电子传递主要包括光生电子从其生成位点到光催化剂表面进而到电子媒介的传递; 质子传递主要包括质子从溶液或催化剂表面向电子媒介的传递. 期望通过“新三传”强化EPCS效率的理念, 打破自然界光合作用的局限, 实现温和条件下多种功能分子的高效合成, 为人工光合与绿色生物制造领域提供新思路.

关键词: 酶-光偶联催化系统, 分子-电子-质子传递, NAD(P)H再生, 酶催化, 光催化

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

李诗浩, 石家福, 刘书松, 李文萍, 陈裕, 单慧婷, 程雨晴, 吴洪, 姜忠义. 酶-光偶联催化系统中分子-电子-质子传递过程与机制[J]. 催化学报, 2023, 44: 96-110.

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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图/表 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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酶-光偶联催化系统中分子-电子-质子传递过程与机制

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

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