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化学进展 2021, Vol. 33 Issue (11): 2103-2115 DOI: 10.7536/PC200877 前一篇   后一篇

• 综述 •

生物杂化体介导的半人工光合作用:机理、进展及展望

胡安东, 周顺桂, 叶捷*()   

  1. 福建农林大学资源与环境学院 福州 350002
  • 收稿日期:2020-08-30 修回日期:2020-11-02 出版日期:2020-12-28 发布日期:2020-12-28
  • 通讯作者: 叶捷
  • 基金资助:
    国家自然科学基金项目(41925028); 国家自然科学基金项目(41977281)
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The Mechanism, Progress and Prospect of Biohybrid Mediated Semi-Artificial Photosynthesis

Andong Hu, Shungui Zhou, Jie Ye()   

  1. College of Resources and Environment, Fujian Agriculture and Forestry University,Fuzhou 350002, China
  • Received:2020-08-30 Revised:2020-11-02 Online:2020-12-28 Published:2020-12-28
  • Contact: Jie Ye
  • Supported by:
    National Natural Science Foundation of China(41925028); National Natural Science Foundation of China(41977281)

半人工光合系统通过利用人工光合系统与自然光合系统关键功能组分的协同效应以实现太阳能-化学能的转化。生物杂化体介导的半人工光合系统(biohybrid mediated semi-artificial photosynthetic system, BMSAPS)创新性地耦合了光敏剂优异的光捕获特性及生物催化剂高效的催化能力,从而利用太阳能高效驱动特定的化学转化过程。强化光敏剂与生物催化剂微界面间电子的产生、传输及利用是提高BMSAPS性能的关键。本文从BMSAPS的基本原理出发,分析了BMSAPS构建的关键科学问题及研究现状,阐述了该系统光生电子传递的相关机制及研究手段,总结了其在可再生能源转化、二氧化碳减排等方面的研究进展,并就未来的研究方向提出展望。本文有助于加深对BMSAPS的认识,从而为进一步优化其在能源生产和环境修复领域的应用提供理论基础和技术支撑。

关键词： 半人工光合作用, 电子传递, 光敏剂, 生物催化剂

Semi-artificial photosynthetic system could realize the solar-to-chemical energy conversion by utilizing the synergistic effects of key functional components of artificial and natural photosynthetic systems. The biohybrid mediated semi-artificial photosynthetic system(BMSAPS) can effectively trigger the specific solar-to-chemical conversion due to the excellent light-harvesting properties of photosensitizers and highly-efficient biological catalytic abilities of biocatalysts. Enhancing the photoelectron generation, transfer and utilization on the micro-interface of photosensitizer-biocatalyst hybrids is considered to be crucial for improving the performance of BMSAPS. This review innovatively concludes the key scientific issues and research status on the BMSAPS construction based on its constituent elements. Meanwhile, the relevant mechanisms and research methods for the photogenerated electron transport in the BMSAPS are also described. In addition, the research progress of the BMSAPS on different fields such as the renewable energy conversion and CO2 emission reduction are summarized, followed by the future research directions. This review is expected to deepen the understanding of the BMSAPS, thereby providing the theoretical foundation and technical support for further optimizing its application in the field of energy production and environmental restoration.

Contents

1 Introduction

2 The basic principles of BMSAPS

3 The BMSAPS construction

3.1 Photosensitizers

3.2 Biocatalysts

4 The typical BMSAPS

4.1 Photoelectrode-biohybrid system

4.2 Inorganic semiconductor-biohybrid system

4.3 Plasmon-biohybrid system

4.4 Research methods for typical biohybrid system

5 The BMSAPS application

5.1 Carbon dioxide fixation

5.2 Nitrogen fixation

5.3 Hydrogen production

6 Outlook

Key words: semi-artificial photosynthesis, electron transport, photosensitizers, biocatalysts
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表1 常见的生物杂化体介导的半人工光合系统(BMSAPS)
Table 1 Common biohybrid mediated semi-artificial photosynthetic system(BMSAPS)
Photosensitizer Biocatalyst Sacrificial electron donor Substrate/Product Quantum yield ref
CdS [FeFe]-hydrogenase I Ascorbic acid H2O/H2 20%(with 405 nm LED) 23
CdS CO dehydrogenases 2-(N-morpholino)
ethanesulfonic acid		 CO2/CO - 39
CNx-TiO2 [NiFeSe]-hydrogenase EDTA H2O/H2 4.8%(with simulated sunlight) 40
CdSe NADP+-reductase Ascorbic acid NADPH 5.8%(with 405 nm LED) 41
CdS MoFe protein Ethyl sulfonic acid N2/NH3 - 34
WO3 Photosynthetic membrane protein - H2O/H2,O2 - 42
g-C3N4 Formate dehydrogenase Triethanolamine(TEOA) CO2/HCOOH - 43
Rutile A. ferrooxidans Ascorbic acid Fe3+/Fe2+ - 44
CdS M. thermoacetica Cysteine CO2/CH3COOH 2.44% ± 0.62%(with simulated sunlight) 24
AglnS2/In2S3 E. coli Cysteine H2O/H2 3.3%(with Xenon lamp) 45
InP S. cerevisiae - 3-Dehydroshikimic acid/Shikimic acid 1.58% ± 0.05%(with cold-while LED) 28
CdS T. denitrificans Cysteine N/N2O 2.0%(with 395 nm LED) 46
CdS M. barkeri Cysteine CO2/CH4 0.34%(with 395 nm LED) 47
CdS NPs R. palustris Cysteine CO2/C2+ 6.73% 48
g-C3N4 R. eutropha Triethanolamine(TEOA) Fructose/PHB - 49
WO3/MoO3/g-C3N4 S. marcescens Propidium iodide HC/Acetic acid - 50
图1 半导体光催化示意图(价带(valence band,VB),导带(conduction band,CB),禁带宽度(band gap))
Fig. 1 Schematic diagram of semiconductor photocatalysis(valence band, VB; conduction band, CB; band gap)
图2 良好生物相容性的光敏剂与生物体结合图像:(a)CdS-M. thermoacetica杂化体系[24];(b)CdS-T. denitrificans杂化体系[46];(c)CdS-M. barkeri杂化体系[47];(d)AglnS2/In2S3-E. coli杂化体系[52];(e)PDI/PFP-M. thermoacetica杂化体系[53];(f)碳点-叶绿体杂化体系[54]
Fig. 2 The images of biocompatible photosensitizers bound to organisms.(a) CdS-M. thermoacetica hybrid system[24];(b) CdS-T. denitrificans hybrid system[46];(c) CdS-M. barkeri hybrid system[47];(d) AglnS2/In2S3-E. coli hybrid system[52];(e) PDI/PFP-M. thermoacetica hybrid system[53];(f) carbon dots-chloroplast hybrid system[54]
图3 部分BMSAPS中光敏剂的简化能带图
Fig. 3 Simplified band diagram of photosensitizer in BMSAPS
图4 常见的生物酶催化剂[51,74]
Fig. 4 Common bio-enzyme catalysts[51,74]
图5 光电极-生物杂化体系电子传递示意图:(a)p型NiO还原CO2的光电化学电池示意图[83];(b)酶串联还原CO2生产甲醇示意图[85];(c)纳米线-细菌光电化学电池系统原理图[87]
Fig. 5 Electron transfer schematic diagram of photelectrode-biohybrid system.(a) Schematic diagram of photoelectrochemical cell for the reduction of CO2 by p-type NiO[83];(b) schematic diagram of the production of methanol from CO2 by enzyme cascade[85];(c) schematics of the close-packed nanowire-bacteria hybrid system[87]
图6 无机半导体-生物杂化体系电子传递示意图:(a)CdS-M. thermoacetica电荷转移示意图[88];(b)CdS-M. thermoacetica电荷转移和CO2固定途径示意图[89]
Fig. 6 Electron transfer mechanism diagram of inorganic semiconductor-biohybrid system.(a) Schematic of CdS-M. thermoacetica charge transfer[88];(b) schematic diagram of CdS-M. thermoacetica charge transfer and CO2 fixation pathway[89]
图7 等离激元电子产生及利用示意图:(a)等离激元金纳米颗粒受激发的电子转移示意图[92];(b)AuNCs-M. thermoacetica电子转移和CO2固定途径示意图[31]
Fig. 7 Schematic diagram of plasma electron generation and utilization.(a) Schematic diagram of electron transfer of excited plasma gold nanoparticles[92];(b) schematic diagram of AuNCs-M. thermoacetica charge transfer and CO2 fixation pathway[31]
表2 BMSAPS研究方法
Table 2 The research methods of BMSAPS
Methods Roles Specific steps ref
Transient absorption(TA)
spectroscopy		 Characterizing the electrons transfer Measuring with an Ultrafast
systems Helios TA system		 88
Time-resolved infrared(TRIR)
spectroscopy		 Characterizing the instantaneous lifetime changes of group Measuring with self-made device 88
NADH/NAD ratio Characterizing intracellular redox potential changes Measuring with MAK037,
Sigma-Aldrich kit		 26
Incident photon-to-current
conversion efficiency(IPCE)		 Characterizing photon-to-current conversion efficiency Measuring with a motorized monochromator(M10; Jasco Corp.) 42
Structure illumination microscopy(SIM) Characterizing intracellular gold nanoclusters Measuring with an ELYRA PS.1 system(Zeiss) 31
Intracellular ROS Characterizing intracellular reactive oxygen species Measuring with fluorometric intracellular ROS assay MAK143 Kit 31
Real-time polymerase chain reaction(PCR) Characterizing of gene expression Using kits to extract and measuring with LightCycler 96 46
Flow cytometry Characterizing of cell total protein, total nucleic acid, etc. Staining with green fluorescent dye and measuring with flow cytometer 47
Scanning electrochemical
microscopy(SECM)		 Characterizing photocurrent of BMSAPS Measuring with a VersaSCAN
SECM instrument(AMETEK Inc., Berwyn, USA)		 47
Fluorescence spectroscopy Characterizing synthesis of cadmium sulfide Measuring with fluorescence spectroscopy(FP-6500, JASCO) 97
Proteomics Characterizing protein expression of BMSAPS Extraction, digestion and quantitative analysis of extracellular proteins 89
Metabolomics Characterizing metabolites of BMSAPS Extracting intracellular metabolites and using LC-MS for quantitative analysis 89
Circular dichroic(CD) spectrum Characterizing secondary structure of protein Measuring with spectrometer(JASCO J-715) 100
图8 BMSAPS分析技术:(a,b)分别为瞬时吸收光谱的原理图及其数据表征图[88,98];(c,d)分别为结构光照明显微镜原理图及其数据表征图[31,99];(e,f)分别为扫描电化学显微镜原理图及其数据表征图[47]
Fig. 8 The analytical techniques for BMSAPS.(a) and(b) respectively represent schematic diagram and data characterization diagram of transient absorption spectroscopy[88,98];(c) and(d) respectively represent schematic diagram and data characterization image of the structure illumination microscopy[31,99];(e) and(f) respectively represent schematic diagram and data characterization images of scanning electrochemical microscopy[47]
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