反钙钛矿代表了一类新兴的功能材料,具有明确的立方晶格晶体结构,为研究多相催化中的构效关系提供了一个很好的实体.在此,合成了 In基反钙钛矿氮化物InNNi3,并首次探讨了其在电催化二氧化碳(CO2RR)还原中的催化性能.研究发现:将Se引入InNNi3中可以取代部分正八面体Ni3N中的N的位点,因为较大的离子半径的差距造成晶格结构被破环,从而暴露出更多In活性位点,显著提高催化剂电化学活性;InNNi3/Se=2∶1催化剂在-1.1 V vs.RHE的电位下电流密度高达180 mA/cm2,在-0.754 V vs.RHE电位下法拉第效率高达91.3％.这项工作首次探讨了 InNNi3/Se在CO2RR中超高的导电性和选择性,为In基反钙钛矿氮化物材料作为电催化CO2还原催化剂提供了可行的策略.
Se-Doped Anti-Perovskite InNNi3 Catalysts for Efficient Electrocatalytic CO2 Reduction Reaction
Anti-perovskite is a new type of functional material with a well-defined cubic lattice structure,mak-ing it ideal for studying conformational relationships in multiphase catalysis.In this study,we synthesized In-based anti-perovskite nitride,InNNi3,and investigated its performance in electrocatalytic carbon dioxide reduc-tion(CO2RR)for the first time.Our findings revealed that introducing selenium(Se)into InNNi3 can replace some nitrogen(N)atoms in the ortho-octahedral Ni3N structure.This substitution leads to lattice disruptions due to the larger ionic radii of Se,which in turn exposes more active In sites and significantly enhances the elec-trochemical activity of the catalyst.Specifically,the InNNi3/Se catalyst with a ratio of 2∶1 achieved a high cur-rent density of 180 mA/cm2 at a potential of-1.1 V vs.RHE.Additionally,it exhibited a Faraday efficiency of up to 91.3％at a potential of-0.754 V vs.RHE.This work demonstrates the ultra-high conductivity and se-lectivity of InNNi3/Se in CO2RR,offering a promising strategy for using In-based anti-perovskite nitride mate-rials as electrocatalytic CO2 reduction catalysts.
anti-perovskite nitrideSe-dopedelectrocatalytic CO2 reductionformic acid
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