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（英文）
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摘要
大气中过高的CO_2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CO_2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. CO_2电化学还原反应(CO_2RR)可利用太阳能、风能等可再生能源产生的电能将CO_2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CO_2分子需克服一定的过电势,且由于反应在水相中进行, CO_2RR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CO_2RR研究的难点.研究表明,含有金属-氮(M-Nx)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CO_2RR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CO_2RR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-Nx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CO_2RR催化剂体系提供了新思路.
Electrochemical CO_2 reduction reaction(CO_2 RR) powered by renewable electricity has emerged as the most promising technique for CO_2 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 CO_2 RR. Previous studies on atomically dispersed metal-nitrogen(M-Nx)sites constituted of earth abundant elements with maximum atom-utilization efficiency have demonstrated their performance towards CO_2 RR. This review summarizes recent advances on a variety of M-Nx sites-containing transition metal-centered macrocyclic complexes, metal organic frameworks, and M-Nx-doped carbon materials for efficient CO_2 RR, 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 CO_2 RR over these M-Nx-containing materials are presented to provide useful guidance for the rational design of efficient catalysts towards CO_2 RR.
Electrochemical CO_2 reduction reaction(CO_2 RR) powered by renewable electricity has emerged as the most promising technique for CO_2 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 CO_2 RR. Previous studies on atomically dispersed metal-nitrogen(M-Nx)sites constituted of earth abundant elements with maximum atom-utilization efficiency have demonstrated their performance towards CO_2 RR. This review summarizes recent advances on a variety of M-Nx sites-containing transition metal-centered macrocyclic complexes, metal organic frameworks, and M-Nx-doped carbon materials for efficient CO_2 RR, 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 CO_2 RR over these M-Nx-containing materials are presented to provide useful guidance for the rational design of efficient catalysts towards CO_2 RR.
引文
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