文献类型：期刊文献

英文题名：Boosting C=O Bond Scissoring Over a Pyridinic Nitrogen-Modified Cu-MoC Interface for High-Efficiency CO2 Hydrogenation to CO

作者：Liao, Haiquan[1] Wang, Caikang[1] Pan, Xueyuan[1] Sun, Hao[1] Liao, Yanlin[2,3] Ma, Mingzhe[1] Zhan, Guowu[4] Fan, Mengmeng[5] Ding, Linfei[5] Xu, Jingcheng[5] Wang, Yali[1] Sun, Kang[1] Yuan, Xiangzhou[2,3] Jiang, Jianchun[1]

第一作者：Liao, Haiquan

通信作者：Sun, H[1];Sun, K[1];Yuan, XZ[2];Yuan, XZ[3]

机构：[1]Chinese Acad Forestry, Inst Chem Ind Forest Prod, State Key Lab Dev & Utilizat Forest Food Resources, Nanjing, Peoples R China;[2]Southeast Univ, Sch Energy & Environm, Key Lab Energy Thermal Convers & Control, Minist Educ, Nanjing, Peoples R China;[3]Southeast Univ, Sch Energy & Environm, Key Lab Funct Polymers Sustainabil Jiangsu, Nanjing, Peoples R China;[4]Huaqiao Univ, Acad Adv Carbon Convers Technol, Coll Chem Engn, Xiamen, Fujian, Peoples R China;[5]Nanjing Forestry Univ, Int Innovat Ctr Forest Chem & Mat, Nanjing, Peoples R China

年份：2026

外文期刊名：CARBON ENERGY

收录：;EI(收录号：20260219865505);Scopus(收录号：2-s2.0-105026607273);WOS:【SCI-EXPANDED(收录号:WOS:001653295200001)】；

基金：National Natural Science Foundation of China, Grant/Award Number: 42377249, 52476183; National Key Research and Development Program of China, Grant/Award Number: 2023YFD2201605

语种：英文

外文关键词：circular carbon economy; Cu clusters; interfacial electron transfer; nitrogen doped; alpha-MoC nanoislands

摘要：Reverse water-gas shift (RWGS) reaction-aided sustainable CO2 conversion has emerged as one promising and effective approach for simultaneously mitigating climate change and solidifying energy security. Molybdenum carbide-based catalysts demonstrate excellent selectivity for sustainably transforming CO2 into CO product, but harsh carburization syntheses and insufficient catalytic activity and stability significantly hinder their related commercial applications. Herein, a facile "inside-out" synthesis strategy was proposed to fabricate dispersed Cu clusters on sub-2 nm alpha-MoC nanoislands confined in pyridinic nitrogen-doped carbon (Cu-MoC/NC). This catalyst achieves the highest CO2 conversion rate of 2583.4 mmolCO2 gcat -1 h-1 compared to those of all reported Mo-based catalysts, and maintains excellent catalytic stability for 500 h under a low H2 partial pressure. Combined with X-ray absorption spectroscopy (XAS) and density functional theory (DFT) calculations, the electronegativity of pyridinic nitrogen intensifies the electron deficiency of alpha-MoC and strengthens the chemisorption of Cu clusters on alpha-MoC nanoislands surface, facilitating the electronic interaction and stability of Cu-MoC interface. This pyridinic nitrogen-modified Cu-MoC interface promotes the CO2 bridged adsorption at the interface and thus boosts C=O bond scissoring, inducing the transition of rate-limiting step and energy barrier reduction of the key intermediates. This interfacial engineering provides a sustainable and efficient strategy for improving both catalytic activity and stability of RWGS reaction to transform CO2 into value-added fuels and chemicals.