文献类型：期刊文献

英文题名：Isolation of Highly Reactive Cobalt Phthalocyanine via Electrochemical Activation for Enhanced CO2 Reduction Reaction

作者：Wu, Xuefeng[1];Zhao, Jia Yue[1];Sun, Ji Wei[1];Li, Wen Jing[1];Yuan, Hai Yang[1];Liu, Peng Fei[1];Dai, Sheng[2];Yang, Hua Gui[1]

机构：[1]East China Univ Sci & Technol, Shanghai Engn Res Ctr Hierarch Nanomat, Sch Mat Sci & Engn, Key Lab Ultrafine Mat,Minist Educ, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Inst Fine Chem, Key Lab Adv Mat & Feringa Nobel Prize Scientist Jo, Sch Chem & Mol Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China

年份：2023

卷号：19

期号：23

外文期刊名：SMALL

收录：;EI(收录号：20231213761749);WOS:【SCI-EXPANDED(收录号:WOS:000943881200001)】；

基金：This work was financially supported by the Science and Technology Commission of Shanghai Municipality (21DZ1207101, 22ZR1416400, and 22ZR1415700), the Key Program of National Natural Science Foundation of China (22239001), the International (Regional) Cooperation and Exchange Projects of the National Natural Science Foundation of China (51920105003), the National Natural Science Funds for Distinguished Young Scholars (51725201), the Innovation Program of Shanghai Municipal Education Commission (E00014), the Shanghai Engineering Research Center of Hierarchical Nanomaterials (18DZ2252400), Shanghai Rising-star Program (20QA1402400), the Fundamental Research Funds for the Central Universities, and the Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning. Additional support was provided by the Feringa Nobel Prize Scientist Joint Research Center. The authors also thank the Frontiers Science Center for Materiobiology and Dynamic Chemistry.

语种：英文

外文关键词：CO2-to-CO conversion; cobalt phthalocyanine; electrochemical activation; molecularly migration

摘要：Electrochemical CO2-to-CO conversion offers an attractive and efficient route to recycle CO2 greenhouse gas. Molecular catalysts, like CoPc, are proved to be possible replacement for precious metal-based catalysts. These molecules, a combination of metal center and organic ligand molecule, may evolve into single atom structure for enhanced performance; besides, the manipulation of molecules' behavior also plays an important role in mechanism research. Here, in this work, the structure evolution of CoPc molecules is investigated via electrochemical-induced activation process. After numbers of cyclic voltammetry scanning, CoPc molecular crystals become cracked and crumbled, meanwhile the released CoPc molecules migrate to the conductive substrate. Atomic-scale HAADF-STEM proves the migration of CoPc molecules, which is the main reason for the enhancement in CO2-to-CO performance. The as-activated CoPc exhibits a maximum FECO of 99% in an H-type cell and affords a long-term durability at 100 mA cm(-2) for 29.3 h in a membrane electrode assembly reactor. Density-functional theory (DFT) calculation also demonstrates a favorable CO2 activation energy with such an activated CoPc structure. This work provides a different perspective for understanding molecular catalysts as well as a reliable and universal method for practical utilization.