Enhancing C Product Selectivity in CO Electroreduction by Enriching Intermediates over Carbon-based Nanoreactors

Overview

Journal Chem Sci

Publisher Royal Society of Chemistry

Specialty Chemistry

Date 2024 Jun 7

PMID 38846399

Authors

Min Wang

Chunjun Chen

Shuaiqiang Jia

Shitao Han

Xue Dong

Dawei Zhou

Ting Yao

Minghui Fang

Mingyuan He

Wei Xia

Haihong Wu

Buxing Han

Affiliations

Soon will be listed here.

Abstract

Electrochemical CO reduction reaction (CORR) to multicarbon (C) products faces challenges of unsatisfactory selectivity and stability. Guided by finite element method (FEM) simulation, a nanoreactor with cavity structure can facilitate C-C coupling by enriching *CO intermediates, thus enhancing the selectivity of C products. We designed a stable carbon-based nanoreactor with cavity structure and Cu active sites. The unique geometric structure endows the carbon-based nanoreactor with a remarkable C product faradaic efficiency (80.5%) and C-to-C selectivity (8.1) during the CO electroreduction. Furthermore, it shows that the carbon shell could efficiently stabilize and highly disperse the Cu active sites for above 20 hours of testing. A remarkable C partial current density of-323 mA cm was also achieved in a flow cell device. Raman spectra and density functional theory (DFT) calculation studies validated that the *CO intermediates are concentrated in the nanoreactor, which reduces the free energy of C-C coupling. This work unveiled a simple catalyst design strategy that would be applied to improve C product selectivity and stability by rationalizing the geometric structures and components of catalysts.

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