材料-生物杂化体的光驱生物催化

doi:10.12211/2096-8280.2021-078

合成生物学 ›› 2022, Vol. 3 ›› Issue (1): 98-115.DOI: 10.12211/2096-8280.2021-078

材料-生物杂化体的光驱生物催化

王雪云¹^,², 杨文君¹^,², 钟超¹^,², 高翔¹^,²

^1.中国科学院深圳先进技术研究院，深圳合成生物学创新研究院，中国科学院定量工程生物学重点实验室，广东深圳 518055
^2.中国科学院深圳先进技术研究院，深圳合成生物学创新研究院，材料合成生物学中心，广东深圳 518055

收稿日期:2021-07-23 修回日期:2021-10-14 出版日期:2022-02-28 发布日期:2022-03-14
通讯作者: 高翔
作者简介:王雪云（1993—），女，博士后。研究方向为半导体材料光驱动合成生物学。E-mail：xy.wang5@siat.ac.cn
杨文君（1986—），女，博士后。研究方向为半导体材料光驱动合成生物学。E-mail：wj.yang@siat.ac.cn
高翔（1987—），男，博士，副研究员。研究方向材料-细菌人工杂合系统的设计与应用。E-mail：gaoxiang@siat.ac.cn
基金资助:
国家自然科学基金面上项目(32171426);深圳先进技术研究院优青基金新引进人才项目(E1G022)

Biohybrid materials for light-driven biocatalysis

Xueyun WANG¹^,², Wenjun YANG¹^,², Chao ZHONG¹^,², Xiang GAO¹^,²

^1.CAS Key Laboratory of Quantitative Engineering Biology，Shenzhen Institute of Synthetic Biology，Shenzhen Institutes of Advanced Technology，Chinese Academy of Sciences，Shenzhen 518055，Guangdong，China
^2.Center for Materials Synthetic Biology，Shenzhen Institute of Synthetic Biology，Shenzhen Institutes of Advanced Technology，Chinese Academy of Sciences，Shenzhen 518055，Guangdong，China

Received:2021-07-23 Revised:2021-10-14 Online:2022-02-28 Published:2022-03-14
Contact: Xiang GAO

摘要/Abstract

摘要：

材料-生物杂化体的光驱生物催化，又称为半人工光合作用，利用高效捕获光能的材料与高选择性的生物催化相结合，从而实现光能到化学能高效、高特异性的转化。天然光合系统光能到化学能的转换效率低，进而发展了光能捕获和转换效率更高的人工光合作用，然而人工光合系统很难实现特异性合成高能量密度、高附加值的多碳化合物。基于材料-生物杂化体构建的半人工光合作用，同时具备材料和生物系统两者的优势，实现优势互补，为光能到化学能的转化提供新的机遇和应用。本文详细介绍了材料-生物杂化体的构建方式，杂化体通过光吸收剂与催化剂进行复合，其复合方式包括以天然光系统作为光吸收剂与纳米催化剂相结合，和以材料作为光吸收剂与酶或微生物全细胞催化剂相结合；分别总结不同复合方式的研究进展、不同系统之间的优缺点以及不同杂化体的应用方向，并对未来发展方向进行了展望。

关键词: 光合作用, 人工光合作用, 材料-生物杂化体

Abstract:

Biohybrid materials for light-driven biocatalysis, also named semi-artificial photosynthesis, are efficient light-harvesting materials that couple with highly specific biocatalysts for solar-to-chemical energy conversion. The natural photosynthesis that converts solar energy to chemical compounds is limited by the low efficiency of light absorption and the limited understanding of complicated cellular metabolism. Artificial photosynthesis, mimic to natural photosynthesis, has the potential for highly efficient solar-to-chemical energy conversion. However, the production of compounds containing two or more carbons with higher value through such a pathway is still challenging. Recent development in synthetic biology enables biological systems to produce more high valued and specifical chemicals. The semi-biological approaches have been developed for complementary advantages in materials science and biology, which gain new opportunities for solar-to-chemical energy conversion. The hybrid systems have been elaborated in a variety of ways, such as biological antenna as a light-harvester for nanoparticle catalysts or materials functioning as a light capturer to couple conversion catalyzed by enzymes and bacterial whole cells. The biological photosensitizer-material hybrids that use photosystems Ⅰ/Ⅱ and photosensitizing proteins to harvest light energy for synthetic materials through catalyzing the reduction reactions have been studied with a focus primarily on hydrogen production. The pure isolated biological photosensitizers are good candidates for exploring the electron transport pathway. However, photosystems Ⅰ/Ⅱ can only maintain activity for a couple of hours, making them difficult for applying to industrial processes, but the material antenna-based biohybrids take the advantage of more stable semiconductors that can be engineered to produce lots of specific chemicals. In this article, advantages and recent processes on the application of the hybrid systems are commented, and their future development is highlighted.

Key words: photosynthesis, artificial photosynthesis, material biohybrids

中图分类号:

王雪云, 杨文君, 钟超, 高翔. 材料-生物杂化体的光驱生物催化[J]. 合成生物学, 2022, 3(1): 98-115.

Xueyun WANG, Wenjun YANG, Chao ZHONG, Xiang GAO. Biohybrid materials for light-driven biocatalysis[J]. Synthetic Biology Journal, 2022, 3(1): 98-115.

图/表 4

图1 天然光合作用和人工光合作用（a）天然光合作用的电子和能量传递示意图，天然光合作用分为光反应（下）和暗反应（上）：光反应通过吸收光能并将能量储存在NADPH和ATP中；暗反应的CBB循环利用NADPH和ATP驱动CO2固定，合成生物质和多碳化合物［3， 10， 15-16］人工光合作用系统包含半导体材料体系和电极体系。（b）利用半导体材料分解水时，材料吸收光能产生电荷分离，e-从价带（V.B.）跃迁到导带（C.B.），在V.B.上留下空穴（h+），水为还原剂消耗h+并释放O2，导带上e-将H+还原成H2［6］。（c）光阳极材料氧化水生成O2并提供e-，并传递到光阴极端，还原H+成H2［3］

Fig. 1 Diagram for natural photosynthesis and artificial photosynthesis(a) Schematic diagram of natural photosynthesis with light reaction (lower) and dark reaction (upper). Photoreaction uses light energy to generate NADPH and ATP, and in the dark reaction, NADPH and ATP are used to drive CO2 fixation through the CBB cycle. (b) The artificial photosynthesis composed of a semiconductor material system and an electrode system [3, 10-12]. The semiconductor material absorbs light and generates electron (e-), e- transitions from the valence band (V.B.) to the conduction band (C.B.) to reduces H+ to H2[6]. The holes (h+) left on V.B. are consumed using water as reducing agent and O2 is released. (c) The photoanode material oxidizes water to generate O2 and provide e-, and the electron is transferred to the photocathode for reducing H+ to H2[3]

图2 基于生物光吸收剂的杂化体示意图H2ase—氢酶；FDHase—甲酸脱氢酶（a） PSⅠ作为光敏剂，吸收光能后发生电子-空穴分离，导带上e-转移给非生物催化剂，最终还原H+成H2［44］；（b） PSⅡ和Ru/SrTiO3：Rh构建Z型方式传递，PSⅡ导带上激发的光电子传递到Ru/SrTiO3：Rh，经过二次激发产生电势较高的电子，用于还原H+成H2［45］；（c） PSⅡ和DPP染料构建Z型电子传递链，与H2ase或FDHase构建半导体-酶杂化体［46］；DPP染料C.B.的光生电子参与酶催化反应将H+还原为H2或将CO2固定为甲酸盐；（d）在PSⅡ和H2ase/FDHase酶构成的对电极中，PSⅡ作为阳极光解水提供电子，阴极的酶则利用电子进行还原反应［3， 47-48］

Fig. 2 Diagram for biological photosensitizer-material hybrids(a) PSⅠ photosensitizer harvests light and generates e-, which is then transferred to non-biological catalyst for reducing H+ to H2[44]. (b) PSⅡ and Ru/SrTiO3:Rh form a Z-scheme structure. Photoelectrons from PSⅡ neutralize h+ on V.B. of Ru/SrTiO3:Rh, leaving electrons with higher reduction potential on C.B. of Ru/SrTiO3:Rh to reduce H+ to H2[45]. (c) PSⅡ and DPP dye form a Z-scheme electron transfer structure, and together with formate dehydrogenase (H2ase) or formate dehydrogenase (FDHase) to build semiconductor-enzyme hybrid. Electrons on C.B. of DPP dye participate in catalytic reaction of enzyme to reduce H+ to H2 or fix carbon dioxide into formate[46]. (d) PSⅡ acts as photoanode to catalyze water splitting to provide electrons, and enzyme at photocathode uses the electrons to drive reduction reaction[3, 47-48]

图3 材料-酶杂化体中的主要组成部分（a）常用光吸收剂主要分为蛋白质光敏剂，染料/高分子为主的有机光敏剂和半导体材料［57］；（b）用于构建的材料-酶杂化体中常用的酶［3］；（c）主要电子供体的结构式，电子供体用于在催化体系中中和空穴，提供电子，使反应顺利连续进行［57］；（d）氧化还原介质的结构式，其中［Cp*Rh（bpy）H2O］2+和NAD（P）H是使用最广泛的介质［57］；PSP—光敏蛋白质［59］

Fig. 3 Diagram for components in materials-enzymes hybrid systems(a) Major photosensitizers including proteins, organic photosensitizers and semiconductor materials[57]. (b) Representative enzymes used in the material-enzyme hybrids[3]. (c) Major electron donors[57]. (d) Redox mediators. [Cp*Rh(bpy)H2O]2+ and NAD(P)H are the most widely used mediators[57]. PSP—Photo-sensitive protein[59]

图4 材料-生物杂化体示意图［在基于半导体或电极构筑的材料-酶杂化体系中，电子的转移方式分为直接电子转移（a）和间接电子转移（b）［3， 57］；在材料-微生物杂化体（c）中，材料可以分布在细胞外，细胞膜上和细胞内部，材料产生的光电子会进入微生物细胞内，为胞内代谢途径提供能量［3］；电极-细菌杂化体（d）分为游离系统和固定化系统［3， 9， 61］］

Fig. 4 Diagram for materials biohybrid systems[In semiconductor/electrode-enzyme hybrid systems, there are two electron transfer routes: direct (a) and indirect electron transfer (b) [3, 57]; In semiconductor-microbial hybrid systems (c), the nanoparticles are distributed at different sites of the cell, including extracellular, surface and intracellular[3]; Electrode-bacteria hybrids (d) include free and immobilized cell systems[3, 9, 61]]

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材料-生物杂化体的光驱生物催化

Biohybrid materials for light-driven biocatalysis

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