过渡金属-氮活性位点在二氧化碳电化学还原反应中的应用

doi:10.1016/S1872-2067(18)63161-4

催化学报 ›› 2019, Vol. 40 ›› Issue (1): 23-37.DOI: 10.1016/S1872-2067(18)63161-4

过渡金属-氮活性位点在二氧化碳电化学还原反应中的应用

阎程程^a,b, 林龙^a,b, 汪国雄^a,c, 包信和^a,c

a 中国科学院大连化学物理研究所催化基础国家重点实验室, 中国科学院纳米科学卓越创新中心, 辽宁大连 116023;
b 中国科学院大学, 北京 100049;
c 中国科学院大连化学物理研究所洁净能源国家实验室(筹), 辽宁大连 116023

收稿日期:2018-09-04 修回日期:2018-09-19 出版日期:2019-01-18 发布日期:2018-11-09
通讯作者: 汪国雄, 包信和
基金资助:
国家重点研发计划（2017YFA0700102）；国家自然科学基金（21573222，91545202）；大连杰出青年人才计划（2017RJ03）；中国科学院大连化学物理研究所DMTO项目（DICP DMTO201702）；中国科学院战略性先导科技专项（XDB17020200）；中国科学院青年创新促进会（2015145）.

Transition metal-nitrogen sites for electrochemical carbon dioxide reduction reaction

Chengcheng Yan^a,b, Long Lin^a,b, Guoxiong Wang^a,c, Xinhe Bao^a,c

a State Key Laboratory of Catalysis, CAS Center for Excellence in Nanoscience, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China;
b University of Chinese Academy of Sciences, Beijing 100049, China;
c Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China

Received:2018-09-04 Revised:2018-09-19 Online:2019-01-18 Published:2018-11-09
Contact: 10.1016/S1872-2067(18)63161-4
Supported by:
This work was supported by the National Key R&D Program of China (2017YFA0700102), the National Natural Science Foundation of China (21573222 and 91545202), the Outstanding Youth Talent Project of Dalian (2017RJ03), the DMTO Project of Dalian Institute of Chemical Physics, CAS (DICP DMTO201702), the Strategic Priority Research Program of the Chinese Academy of Sciences (XDB17020200), and the Youth Innovation Promotion Association, CAS (2015145).

摘要/Abstract

摘要：

大气中过高的CO₂浓度严重影响自然界的碳循环平衡，对全球气候和生态环境提出了严峻挑战.但同时CO₂作为一种潜在的碳资源，可通过催化转化生成高附加值的化学品.CO₂电化学还原反应（CO₂RR）可利用太阳能、风能等可再生能源产生的电能将CO₂直接转化生成高附加值化学品和燃料，有助于构建"碳中性"的能源循环利用网络，具有极具潜力的应用前景.然而，活化稳定的CO₂分子需克服一定的过电势，且由于反应在水相中进行，CO₂RR与析氢反应互相竞争，因此开发高效、廉价、稳定的催化剂一直是CO₂RR研究的难点.研究表明，含有金属-氮（M-N_x）活性位的催化材料如卟啉、酞菁等大环配合物、金属有机骨架材料以及通过热解法制备的金属-氮-碳（M-N-C）材料具有优异的CO₂RR性能.本文从实验和理论两方面综述了近年来该类材料领域的相关进展，重点介绍了金属位点种类、配体结构、载体选择对催化剂本征活性的影响，并讨论了反应条件优化对CO₂RR性能提升的作用.结合原位表征和理论计算结果探讨了含M-N_x材料反应条件下活性位的结构及反应路径，为合理设计和优化CO₂RR催化剂体系提供了新思路.

关键词: 二氧化碳电化学还原反应, 金属-氮位点, 含金属-氮位点的大环化合物, 金属有机骨架, 沸石咪唑骨架, 金属-氮掺杂碳材料

Abstract:

Electrochemical CO₂ reduction reaction (CO₂RR) powered by renewable electricity has emerged as the most promising technique for CO₂ conversion, making it possible to realize a carbon-neutral cycle. Highly efficient, robust, and cost-effective catalysts are highly demanded for the near-future practical applications of CO₂RR. Previous studies on atomically dispersed metal-nitrogen (M-N_x) sites constituted of earth abundant elements with maximum atom-utilization efficiency have demonstrated their performance towards CO₂RR. This review summarizes recent advances on a variety of M-N_x sites-containing transition metal-centered macrocyclic complexes, metal organic frameworks, and M-N_x-doped carbon materials for efficient CO₂RR, including both experimental and theoretical studies. The roles of metal centers, coordinated ligands, and conductive supports on the intrinsic activity and selectivity, together with the importance of reaction conditions for improved performance are discussed. The mechanisms of CO₂RR over these M-N_x-containing materials are presented to provide useful guidance for the rational design of efficient catalysts towards CO₂RR.

Key words: Electrochemical carbon dioxide reduction reaction, Metal-nitrogen sites, Metal-nitrogen containing macrocyclic complexes, Metal organic frameworks, Zeolitic imidazolate frameworks, Carbon material doped with metal-nitrogen sites

阎程程, 林龙, 汪国雄, 包信和. 过渡金属-氮活性位点在二氧化碳电化学还原反应中的应用[J]. 催化学报, 2019, 40(1): 23-37.

Chengcheng Yan, Long Lin, Guoxiong Wang, Xinhe Bao. Transition metal-nitrogen sites for electrochemical carbon dioxide reduction reaction[J]. Chinese Journal of Catalysis, 2019, 40(1): 23-37.

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过渡金属-氮活性位点在二氧化碳电化学还原反应中的应用

Transition metal-nitrogen sites for electrochemical carbon dioxide reduction reaction

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