Introducing La into a Customized Dual Cu Covalent Organic Framework to Steer CO₂ Electroreduction Selectivity from C₂H₄ to CH₄

TY - JOUR

T1 - Introducing La into a Customized Dual Cu Covalent Organic Framework to Steer CO2 Electroreduction Selectivity from C2H4 to CH4

AU - Dong, Xiao Yu

AU - Chen, Hong

AU - Wang, Shan

AU - Zou, Ru Yi

AU - Zang, Shuang Quan

AU - Cai, Jinmeng

N1 - Publisher Copyright: © 2024 Wiley-VCH GmbH.

PY - 2025/2/12

Y1 - 2025/2/12

N2 - Customizing multi-metal site catalysts for achieving controllable CO2 reduction reaction (CO2RR) product tuning holds immense promise yet poses formidable challenges. The traditional synthesis method of multi-metal sites is the pyrolysis of metal-containing precursors, which is inherently uncontrollable. Herein, a bottom-up strategy is employed to customize and synthesize multi-metal sites in covalent organic frameworks (COFs), aiming to controllably switch the CO2 reduction selectivity by regulating the electronic structure of active sites. Briefly, La element provides chances for manipulating and finetuning the electronic structure of the customized dual Cu sites, and converts the main catalytic product of CO2RR from ethylene to methane. Density functional theory calculations show that the introduction of La alters the electronic structure around Cu, enhances CO2 and H2O activation, and changes the formation of energy barriers of key intermediates. To the best of the author's knowledge, this study constructed the first example of customized multi-metal site COF catalysts and provided new ideas for controllable modulation of products.

AB - Customizing multi-metal site catalysts for achieving controllable CO2 reduction reaction (CO2RR) product tuning holds immense promise yet poses formidable challenges. The traditional synthesis method of multi-metal sites is the pyrolysis of metal-containing precursors, which is inherently uncontrollable. Herein, a bottom-up strategy is employed to customize and synthesize multi-metal sites in covalent organic frameworks (COFs), aiming to controllably switch the CO2 reduction selectivity by regulating the electronic structure of active sites. Briefly, La element provides chances for manipulating and finetuning the electronic structure of the customized dual Cu sites, and converts the main catalytic product of CO2RR from ethylene to methane. Density functional theory calculations show that the introduction of La alters the electronic structure around Cu, enhances CO2 and H2O activation, and changes the formation of energy barriers of key intermediates. To the best of the author's knowledge, this study constructed the first example of customized multi-metal site COF catalysts and provided new ideas for controllable modulation of products.

KW - CO reduction

KW - covalent organic framework

KW - customization

KW - multivariate metal sites

KW - product regulation

UR - https://www.scopus.com/pages/publications/85212274678

U2 - 10.1002/adma.202413710

DO - 10.1002/adma.202413710

M3 - Article

C2 - 39690887

AN - SCOPUS:85212274678

SN - 0935-9648

VL - 37

JO - Advanced Materials

JF - Advanced Materials

IS - 6

M1 - 2413710

ER -