文献类型：期刊文献

英文题名：Space-Confined Molecular Catalysis toward Electrocatalytic CO2 Reduction on Metal Phthalocyanine@Nitrogen-Doped Carbon Nanosheet

作者：Zheng, Hongbing[1];Wu, Haoran[2];Qiu, Liming[1];Yu, Mingyao[1];Zhou, Jiajun[1];Xu, Hui[1];Lv, Chunmei[1];Tian, Pengfei[3];Wang, Jitong[1,4];Ling, Licheng[1]

机构：[1]East China Univ Sci & Technol, Sch Chem Engn, Key Lab Green Chem Engn & Ind Catalysis, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Sch Mech & Power Engn, Key Lab Pressure Syst & Safety, Minist Educ, Shanghai 200237, Peoples R China;[4]Guangxi Univ, Guangxi Key Lab Petrochem, Resource Proc & Proc Intensificat Tech, Sch Chem & Chem Engn, Nanning 530004, Peoples R China

年份：2024

卷号：7

期号：23

起止页码：27275

外文期刊名：ACS APPLIED NANO MATERIALS

收录：;EI(收录号：20244817416001);WOS:【SCI-EXPANDED(收录号:WOS:001361780400001)】；

基金：This work is financially supported by the National Natural Science Foundation of China (Nos. U21A2060, 22178116 and No. 22308095), the Natural Science Foundation of Shanghai (No. 22ZR1417400), and the Fundamental Research Funds for the Central Universities (222201817001, 50321041918013, JKA01221601, and JKD01241701).

语种：英文

外文关键词：CO2RR; multilayer mesoporous carbon; molecular scale dispersion; phthalocyanine; space-confined; nitrogen-doped

摘要：Phthalocyanines have emerged as attractive materials for electrocatalytic carbon dioxide reduction. However, the challenge of finding a support that is stable while maintaining catalytic activity and loading remains elusive. Porous carbon materials are considered reliable substrates for supporting molecular catalysts. Herein, a nitrogen-rich carbon nanosheet (NiPc/NMCN) with multilayer and mesoporous structure is synthesized based on a kinetically controlled self-assembly strategy and used for phthalocyanine loading. The multilayer composite structure of NMCN guides the molecular-scale dispersion of phthalocyanine and plays a crucial role in its catalytic process. Moreover, the phthalocyanine molecules retain their metal-N4 structure after impregnation. Therefore, the remarkable CO2 electroreduction properties of phthalocyanine are fully demonstrated. At -0.73 V vs. RHE, NiPc/NMCN achieves the highest CO faradaic efficiency (FECO) of 96.0%. Meanwhile, current densities in membrane electrode module electrolyzers can reach industrial amperage levels, while the FEco remains at 60% at 880 mA cm-2. Density functional theory (DFT) indicates that the high performance of NiPc/NMCN is attributed to the significant reduction of the CO2RR energy barrier. Phthalocyanines restricted by the porous carbon could produce the intermediate *COOH more rapidly, determining high CO2RR selectivity, which is confirmed by in situ (FTIR) spectroscopy. Consequently, the strategy of constructing confined multilayer mesoporous carbon structures provides an avenue for the design of efficient CO2 reduction molecular catalysts.