Unravelling intrinsic descriptors based on a two-stage activity regulation of bimetallic 2D c-MOFs for CO2RR

The bimetallic 2D conductive MOFs of M1Pc–M2–O, possessing dual metal sites to realize flexible molecular-level structural modification, are brilliant catalysts for electrochemical CO2 reduction. However, the bimetallic centers bring about the complex regulatory mechanism of catalytic activity and o...

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Veröffentlicht in:Nanoscale 2023-03, Vol.15 (10), p.4991-5000
Hauptverfasser: Zhang, Qi, Ping-Ao Hu, Zhi-Yuan, Xu, Tang, Bei-Bei, Hui-Ru, Zhang, Yu-Hong, Xiao, Yu-Cheng, Wu
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container_end_page 5000
container_issue 10
container_start_page 4991
container_title Nanoscale
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creator Zhang, Qi
Ping-Ao Hu
Zhi-Yuan, Xu
Tang, Bei-Bei
Hui-Ru, Zhang
Yu-Hong, Xiao
Yu-Cheng, Wu
description The bimetallic 2D conductive MOFs of M1Pc–M2–O, possessing dual metal sites to realize flexible molecular-level structural modification, are brilliant catalysts for electrochemical CO2 reduction. However, the bimetallic centers bring about the complex regulatory mechanism of catalytic activity and obscure principles for catalyst design. Herein, systematical theoretical investigation unravels intrinsic descriptors to design favorable M1Pc–M2–O catalysts based on the discovered coarse-fine two-stage activity regulation mechanism. The reaction site controls the M–COOH distance of the key intermediate and therefore affects the reaction kinetics for the first stage of coarse regulation. The other metal site influents the d-band center of the reaction site and thus constitutes the second stage of fine regulation. The coarse and fine regulation are related to the valence electrons (V), electronegativity (E), and bond length (LM–N/O) between the metal and coordination atoms. The intrinsic descriptor φ = (4 × VM1 × (EM1 + EN/O)/EN/O + VM2 × (EM2 + EN/O)/EN/O) × LM1–N/O (with a coefficient ratio of 4 : 1) was eventually established and correlated well with the reported experiments. On this basis, the favorable catalysts CoPc–Zn–O and CoPc–Co–O were located. The research results could contribute to the diversity of bimetallic 2D c-MOFs in CO2RR.
doi_str_mv 10.1039/d2nr07301c
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However, the bimetallic centers bring about the complex regulatory mechanism of catalytic activity and obscure principles for catalyst design. Herein, systematical theoretical investigation unravels intrinsic descriptors to design favorable M1Pc–M2–O catalysts based on the discovered coarse-fine two-stage activity regulation mechanism. The reaction site controls the M–COOH distance of the key intermediate and therefore affects the reaction kinetics for the first stage of coarse regulation. The other metal site influents the d-band center of the reaction site and thus constitutes the second stage of fine regulation. The coarse and fine regulation are related to the valence electrons (V), electronegativity (E), and bond length (LM–N/O) between the metal and coordination atoms. The intrinsic descriptor φ = (4 × VM1 × (EM1 + EN/O)/EN/O + VM2 × (EM2 + EN/O)/EN/O) × LM1–N/O (with a coefficient ratio of 4 : 1) was eventually established and correlated well with the reported experiments. 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On this basis, the favorable catalysts CoPc–Zn–O and CoPc–Co–O were located. The research results could contribute to the diversity of bimetallic 2D c-MOFs in CO2RR.</abstract><cop>Cambridge</cop><pub>Royal Society of Chemistry</pub><doi>10.1039/d2nr07301c</doi><tpages>10</tpages></addata></record>
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subjects Bimetals
Catalysts
Catalytic activity
Electronegativity
Influents
Metal-organic frameworks
Reaction kinetics
Regulatory mechanisms (biology)
title Unravelling intrinsic descriptors based on a two-stage activity regulation of bimetallic 2D c-MOFs for CO2RR
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