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化学进展 2022, Vol. 34 Issue (7): 1590-1599 DOI: 10.7536/PC220323 前一篇   后一篇

• 综述 •

人工光合作用

张德善1,2, 佟振合1,2, 吴骊珠1,2,*()   

  1. 1.中国科学院理化技术研究所 光化学转换与功能材料重点实验室 北京 100190
    2.中国科学院大学未来技术学院 北京 100049
  • 收稿日期:2022-03-23 修回日期:2022-04-21 出版日期:2022-07-24 发布日期:2022-06-20
  • 通讯作者: 吴骊珠
  • 基金资助:
    国家自然科学基金项目(22088102); 科技部(2017YFA0206903); 中国科学院战略重点研究项目(XDB17000000); 中国科学院前沿科学重点研究计划(QYZDY-SSW-JSC029)
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Artificial Photosynthesis

Deshan Zhang1,2, Chenho Tung1,2, Lizhu Wu1,2()   

  1. 1. Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences,Beijing 100190, China
    2. School of Future Technology, University of Chinese Academy of Sciences,Beijing 100049, China
  • Received:2022-03-23 Revised:2022-04-21 Online:2022-07-24 Published:2022-06-20
  • Contact: Lizhu Wu
  • Supported by:
    National Natural Science Foundation of China(22088102); Ministry of Science and Technology of China(2017YFA0206903); Strategic Priority Research Program of the Chinese Academy of Science(XDB17000000); Key Research Program of Frontier Sciences of the Chinese Academy of Science(QYZDY-SSW-JSC029)

光合作用将太阳能储存在化学反应中,是绿色高效的能量转换途径。模拟自然光合作用系统活性中心的结构和功能,实现小分子物质(H2O、CO2、N2等)中惰性化学键的活化转化,对于解决能源和环境等问题具有重要意义。本文综述了人工光合作用在水分解、二氧化碳及氮气还原领域取得的重要进展,分析了相关光化学转换体系的设计思路和工作原理,并对人工光合作用面临的挑战和未来发展方向进行讨论。

关键词： 太阳能, 人工光合作用, 分解水, 二氧化碳还原, 固氮

Photosynthesis in nature stores solar energy in chemical bonds through a green and efficient way. Mimicking the structure and function of the active center of natural photosynthesis, inert chemical bonds of small molecules (H2O, CO2 and N2 etc.) can be activated and converted for energy conversion. Herein, we summarize the important progress of artificial photosynthesis in water splitting into oxygen and hydrogen, carbon dioxide and nitrogen reduction. Meanwhile, we analyze the design ideas and working principles of related photochemical conversion systems, and discuss the challenges and future development of artificial photosynthesis.

Contents

1 Introduction

2 Artificial photosynthesis

2.1 Water oxidation

2.2 Proton reduction of water

2.3 Carbon dioxide reduction

2.4 Nitrogen reduction

3 Conclusion and outlook

Key words: solar energy, artificial photosynthesis, water splitting, carbon dioxide reduction, nitrogen fixation
()
图1 自然界光合作用示意图
Fig. 1 The natural photosynthesis
图2 (a) 天然OEC结构; (b) 人工合成的Mn4CaO4结构[25]
Fig. 2 (a) Native OEC structure; (b) artificial complex Mn4CaO4 structure[25]
图3 单体Ru(bda) (N-OTEG)和氧桥连绿色二聚体[30]
Fig. 3 Monomer catalyst Ru(bda) (N-OTEG) and oxo-bridged green dimer[30]. Copyright 2020, Elsevier
图4 多金属氧酸盐分子催化剂光催化水氧化[38]
Fig. 4 Polyoxometalate molecular catalyst for photocatalytic water oxidation[38]
图5 天然[FeFe]氢化酶活性中心结构
Fig. 5 The active site of natural [FeFe]-hydrogenase
图6 PAA-g-Fe2S2的光催化析氢过程[47]
Fig. 6 PAA-g-Fe2S2 for the photocatalytic H2 production[47]
图7 (a) 含钴肟配合物的CdSe/ZnS核壳量子点光还原质子产氢; (b) 光催化剂能级图[52]
Fig. 7 (a) CdSe/ZnS core/shell QDs with cobaloxime reduce protons to produce hydrogen; (b) energetic diagram of CdSe/ZnS core/shell QDs and cobaloxime hybrid[52]. Copyright 2012, American Chemical Society
图8 (a) CdSe/CdS量子点/Pt纳米颗粒光催化产氢示意图; (b) 组装及分离体系的产氢性能对比[54]
Fig. 8 (a) Schematic illustration of the assembly of CdSe/CdS QDs/Pt nanoparticles and the corresponding solar H2 evolution process; (b) photocatalytic H2 evolution of CdSe/CdS QDs/Pt nanoparticle assembly and individually separated system using MPA-stabilized counterparts[54]. Copyright 2017, American Chemical Society
图9 一氧化碳脱氢酶修饰的TiO2纳米颗粒光还原C O 2[58]
Fig. 9 Carbon monoxide dehydrogenase-modified TiO2 nanoparticles for photocatalytic reduction of C O 2[58]. Copyright 2010, American Chemical Society
图10 切换配合物的金属中心选择性生成CO和HCOOH[60]
Fig. 10 Selective production of CO vs HCOOH by switching of the metal center[60]. Copyright 2015, American Chemical Society
图11 (a) DOR结构材料ZnSe/CdS的电荷转移过程; (b) 导带电子和价带空穴的径向分布函数[69]
Fig. 11 (a) Charge transfer process of DOR structured ZnSe/CdS; (b) conduction band (CB) electrons (red traces) and valence band (VB) holes (green lines) in ZnSe/CdS DORs[69]. Copyright 2021, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
图12 光还原CO2和有机转换结合[70]
Fig. 12 Efficient and selective CO2 reduction integrated with organic synthesis by solar energy[70]
图13 Fe掺杂SrMoO4光还原N2机理图[76]
Fig. 13 Mechanism illustration of Fe doped SrMoO4 for photocatalytic nitrogen reduction[76]
图14 TiO2表面氧空位光催化氮气还原[85]
Fig. 14 Photocatalytic reduction of nitrogen on surface oxygen vacancies of Ti O 2[85]. Copyright 2017, American Chemical Society
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摘要

人工光合作用