电催化剂
共价键
密度泛函理论
共价有机骨架
催化作用
选择性
化学
法拉第效率
化学工程
纳米技术
材料科学
电化学
物理化学
有机化学
计算化学
电极
工程类
作者
Meng Lu,Mi Zhang,Chunguang Liu,Jiang Liu,Lin‐Jie Shang,Min Wang,Jia‐Nan Chang,Shun-Li Li,Ya‐Qian Lan
标识
DOI:10.1002/anie.202011722
摘要
Abstract In this work, we rationally designed a series of crystalline and stable dioxin‐linked metallophthalocyanine covalent organic frameworks (COFs; MPc‐TFPN COF, M=Ni, Co, Zn) under the guidance of reticular chemistry. As a novel single‐site catalysts (SSCs), NiPc/CoPc‐TFPN COF exhibited outstanding activity and selectivity for electrocatalytic CO 2 reduction (ECR; Faradaic efficiency of CO (FE CO )=99.8(±1.24) %/ 96.1(±1.25) % for NiPc/CoPc‐TFPN COF). More importantly, when coupled with light, the FE CO and current density ( j CO ) were further improved across the applied potential range (−0.6 to −1.2 V vs. RHE) compared to the dark environment for NiPc‐TFPN COF ( j CO increased from 14.1 to 17.5 A g −1 at −0.9 V; FE CO reached up to ca. 100 % at −0.8 to −0.9 V). Furthermore, an in‐depth mechanism study was established by density functional theory (DFT) simulation and experimental characterization. For the first time, this work explored the application of COFs as photo‐coupled electrocatalysts to improve ECR efficiency, which showed the potential of using light‐sensitive COFs in the field of electrocatalysis.
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