期刊
CHEMSUSCHEM
卷 13, 期 16, 页码 4111-4120出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cssc.202001143
关键词
catalytic mechanism; CO(2)reduction; iron complexes; molecular electrocatalysis; Schiff base
资金
- Fondazione Cariparo
- Department of Chemical Sciences at University of Padova (Project PHOETRY, P-DiSC) [10BIRD2018-UNIPD]
- Institut Universitaire de France (IUF)
- Italian MIUR [2017PBXPN4]
- Erasmus internship program of the University of Padova
Iron complexes with a N2O2-typeN,N '-bis(salicylaldehyde)-1,2-phenylenediaminesalophen ligand catalyze the electrochemical reduction of CO(2)to CO in acetonitrile with phenol as the proton donor, giving rise to 90-99 % selectivity, faradaic efficiency up to 58 %, and turnover frequency up to 10(3) s(-1)at an overpotential of 0.65 V. This novel class of molecular catalyst for CO(2)reduction operate through a mononuclear Fe(I)intermediate, with phenol being involved in the process with first-order kinetics. The molecular nature of the catalyst and the low cost, easy synthesis and functionalization of the salophen ligand paves the way for catalyst engineering and optimization. Competitive electrodeposition of the coordination complex at the electrode surface results in the formation of iron-based nanoparticles, which are active towards heterogeneous electrocatalytic processes mainly leading to proton reduction to hydrogen (faradaic efficiency up to 80 %) but also to the direct reduction of CO(2)to methane with a faradaic efficiency of 1-2 %.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据