CO2电还原用氮掺杂碳基过渡金属单原子催化剂

N-Doped Porous Carbon Supported Transition Metal Single Atomic Catalysts for CO2 Electroreduction Reaction

温和条件下将CO2电催化还原(CO2RR)为高能量密度燃料和高附加值碳产品是降低大气中CO2浓度、储存间歇性可再生能源、实现碳中和的重要途径之一。设计和开发对电催化CO2RR兼具高活性、高选择性、高稳定性、且对析氢反应(HER)具有显著抑制作用的高性能廉价催化剂是CO2RR研究的关键。单原子催化剂(SACs)由于其独特的电子结构和几何结构对许多重要化学反应(如CO氧化反应、加氢反应、析氧反应、氧还原反应、析氢反应等)显示出优异的催化活性而广受关注。近年来,N掺杂多孔碳载体过渡金属单原子催化材料(M-N-C)显示出对电化学二氧化碳还原的广阔前景、并有望成为在水相电解质中还原CO2的贵金属(Au,Ag)催化剂的替代品。本文从单原子催化材料M-N-C的制备、影响电催化性能的因素及MNx活性基团三个方向介绍了单原子催化剂M-N-C电催化CO2RR的研究现状和进展。最后,就目前该方向研究中尚待解决的问题进行了总结、并对下一步的研究进行了展望。

Electrocatalytic reduction of CO2 reduction reaction(CO2RR) to high energy density fuel and high value-added carbon products under mild conditions is an extremely promising way for reduction of the CO2 concentration in atmosphere and storage of the intermittent renewable energy, as well as for carbon neutralization. The design and development of low-cost high-performance catalysts with high activity, high selectivity, high stability and significant suppress of hydrogen evolution reaction(HER) is the key to the CO2RR research. On the other hand, single atomic catalysts (SACs), due to their unique electronic and geometric structures, exhibit unusual catalytic activity for many important chemical reactions, such as CO oxidation, hydrogenation, OER, ORR, HER, etc., and have attracted extensive attention. Inspired by the profound progress, very recently, Ndoped porous carbon support transition metal single atomic materials(M-N-C) have been employed in CO2RR research. The results manifest that M-N-C catalytic materials have exciting prospects for CO2RR, and are expected to be a substitute for precious metal(Au, Ag) catalysts for CO2 reduction in electrolyte aqueous media. This review is focused on fabrications, electrocatalytic performance and MNx active sites of M-N-C SACs used in electrochemical CO2RR. Finally, the problems remaining to be solved are summarized, and future research aspects and new ideas are prospected.