Organic frameworks confined Cu single atoms and nanoclusters for tandem electrocatalytic CO2 reduction to methane

Zhao, Qinglan1; Wang, Yian1; Li, Meng2; Zhu, Shangqian1; Li, Tiehuai1; Yang, Jixiang1; Lin, Ting1; Delmo, Ernest P.1; Wang, Yinuo1; Jang, Juhee1; Gu, Meng3; Shao, Minhua1,4

2022-03-01

10.1002/smm2.1098

SMARTMAT   Impact Factor & Quartile

2766-8525

2688-819X

The electrochemical reduction reaction of carbon dioxide (CO2RR) is considered to be an effective way to realize carbon neutrality. As a type of intensively studied materials, covalent organic frameworks (COFs) with a tunable pore structure and various functional groups are promising catalysts for CO2RR. Herein, COF synthesized by 2,6-diaminoanthraquinone and 2,4,6-triformylphloroglucinol is employed to assist the synthesis of electrocatalysts from Cu single atoms (SAs) to nanoclusters by controlling the electrodeposition. A tandem catalyst for CO2-to-CH4 conversion is thus achieved by the Cu nanoclusters dispersed among the isolated Cu SAs in the COF network. It is proposed that CO2 is first reduced to CO over the atomically isolated Cu SAs, followed by diffusion onto the neighboring Cu nanoclusters for further reduction into CH4. In addition, mechanistic analysis suggests that the coordinated K+ ions on the COF network promote the activation of CO2 and the adsorption of reaction intermediates, thus realizing the suppressed hydrogen evolution reaction and selective production of CH4. This study presents a new insight of COFs for the confined synthesis of a tunable SA to nanocluster electrocatalysts, disclosing the great potential of COFs in electrocatalysis.

carbon neutrality CO2 reduction reaction covalent organic framework nanocluster single atom

ESCI

English

Others

Innovation and Technology Commission of the Hong Kong Special Administrative Region[ITC-CNERC14EG03] ; University Grants Committee["16309418","26206115","HKUST PDFS2021-4S12","HKUST PDFS2021-6S08"]

Chemistry ; Materials Science

Chemistry, Multidisciplinary ; Materials Science, Multidisciplinary

WOS:000844493100015

WILEY

Web of Science

1.Hong Kong Univ Sci & Technol, Dept Chem & Biol Engn, Hong Kong, Peoples R China
2.Jinan Univ, Coll Life Sci & Technol, Guangdong Prov Res Ctr Environm Pollut Control &, Guangzhou, Peoples R China
3.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen, Peoples R China
4.Hong Kong Univ Sci & Technol, Chinese Natl Engn Res Ctr Control & Treatment Hea, Energy Inst, Hong Kong, Peoples R China

Zhao, Qinglan,Wang, Yian,Li, Meng,et al. Organic frameworks confined Cu single atoms and nanoclusters for tandem electrocatalytic CO2 reduction to methane[J]. SMARTMAT,2022,3(1).

Zhao, Qinglan.,Wang, Yian.,Li, Meng.,Zhu, Shangqian.,Li, Tiehuai.,...&Shao, Minhua.(2022).Organic frameworks confined Cu single atoms and nanoclusters for tandem electrocatalytic CO2 reduction to methane.SMARTMAT,3(1).

Zhao, Qinglan,et al."Organic frameworks confined Cu single atoms and nanoclusters for tandem electrocatalytic CO2 reduction to methane".SMARTMAT 3.1(2022).