Covalent triazine framework modified with coordinatively-unsaturated Co or Ni atoms for CO2 electrochemical reduction

Chemical Science
Panpan SuShuji Nakanishi

Abstract

The electrochemical reduction of carbon dioxide (CO2) has attracted considerable attention as a means of maintaining the carbon cycle. This process still suffers from poor performance, including low faradaic efficiencies and high overpotential. Herein, we attempted to use coordination number as a control parameter to improve the electrocatalytic performance of metal species that have previously been thought to have no CO2 reduction activity. Covalent triazine frameworks (CTF) modified with coordinatively-unsaturated 3d metal atoms (Co, Ni or Cu) were developed for efficient electroreduction of CO2. Co-CTF and Ni-CTF materials effectively reduced CO2 to CO from -0.5 V versus RHE. The faradaic efficiency of the Ni-CTF during CO formation reached 90% at -0.8 V versus RHE. The performance of Ni-CTF is much higher than that of the corresponding metal-porphyrin (using tetraphenylporphyrin; TPP). First principles calculations demonstrated that the intermediate species (adsorbed COOH) was stabilized on the metal atoms in the CTF due to the low-coordination structure of this support. Thus, the free energy barriers for the formation of adsorbed COOH on the metal atoms in the CTF supports were lower than those on the TPP supports.

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Citations

Nov 1, 2018·Angewandte Chemie·Jiafang XieJiannian Yao
Jan 22, 2020·ChemSusChem·Laurent DelafontainePlamen Atanassov
Apr 9, 2020·Chemical Communications : Chem Comm·Yiju LvHongbing Ji
Apr 22, 2021·Chemical Society Reviews·Xiaojia ZhaoArne Thomas
Nov 30, 2018·ACS Applied Materials & Interfaces·Xiang ZhuSheng Dai
Nov 3, 2020·Chemical Reviews·Yuxuan WangChao Wang
Jan 8, 2021·Journal of the American Chemical Society·Haesol KimChang Hyuck Choi
Jan 23, 2020·Chemical Reviews·Keyu GengDonglin Jiang
Oct 5, 2021·Chemistry, an Asian Journal·Jing DuBien Tan
Oct 22, 2021·Chemistry : a European Journal·Mahnaz NajafiMehrorang Ghaedi

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Methods Mentioned

BETA
X-ray
transmission
nuclear magnetic resonance
NMR

Software Mentioned

OpenMX
Athena
FEFF6L
ARTEMIS

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