Bioinspired iron porphyrins with appended poly-pyridine/amine units for boosted electrocatalytic CO_(2) reduction reaction
作者机构:Key Laboratory of Applied Surface and Colloid ChemistryMinistry of EducationSchool of Chemistry and Chemical EngineeringShaanxi Normal UniversityXi'an710119China Ruhr-Universität BochumFakultät für Chemie und BiochemieAnorganische Chemie I Universitätsstrasse 15044801BochumGermany Fraunhofer UMSICHTDepartment for Electrosynthesis46047OberhausenGermany
出 版 物:《eScience》 (电化学与能源科学(英文))
年 卷 期:2022年第2卷第6期
页 面:623-631页
基 金:We are grateful for support from National Natural Science Foundation of China(21773146,22003036 and 22171176) Fok Ying-Tong Education Foundation for Outstanding Young Teachers in University,Fundamental Research Funds for the Central Universities(GK202103045 and GK202103033) Research Funds of Shaanxi Normal University,and the open fund of State Key Laboratory of Structural Chemistry.U.-P.A.thanks for the support by the Fraunhofer Internal Programs under Grant No.Attract 097-602175 and the DFG under Germany's Excellence Strategy-EXC-2033-Projektnummer 390677874“RESOLV”
主 题:CO_(2)reduction reaction Fe porphyrin Molecular electrocatalysis Structural effect Water network
摘 要:Developing highly efficient electrocatalysts for the CO_(2) reduction reaction(CO_(2)RR)has attracted increasing interest in the past ***,we report on the design and synthesis of Fe porphyrin 1 with an appended N,N-di(2-picolyl)ethylenediamine(DPEN)unit that boosts electrocatalytic activity for CO_(2)-to-CO conversion in acetonitrile with water as the proton *** mimicking carbon monoxide dehydrogenase(CODH),1 has poly-pyridine/amine units located at the active site to form hydrogen-bonded water-containing networks that enable fast proton *** protonated and positively charged DPEN unit can also stabilize CO_(2) reduction intermediates through electrostatic and hydrogen-bonding *** factors make 1 a highly active electrocatalyst for the CO_(2)RR by achieving a TOFmax of 5.0×10^(4)s^(−1) with water providing the *** critical roles of the DPEN unit in the CO_(2)RR are further supported by theoretical *** work is significant to highlight the benefits of using molecular catalysts to elucidate structural effects.