Dual-site synergy via interfacial engineering for enhanced CO₂ electroreduction to methanol.

Authors

Junpeng Huang, Wenbo Wang, Hongyang Zhou, Yujie Tao, Bin Liu, Guoxing Zhu, Xiaomeng Lv

Published in

Journal of colloid and interface science. Volume 724. Issue Pt 1. Pages 140992. Jun 26, 2026. Epub Jun 26, 2026.

Abstract

Electrocatalytic CO₂-to-methanol (MeOH) is hindered by the low efficiency of single-site catalysts, primarily due to insufficient local concentration of the key ^⁎CO intermediate. This work aims to construct a dual-site catalyst to synergistically boost ^⁎CO generation and its subsequent hydrogenation, thereby enhancing methanol production. Herein, a cooperative interface was designed by integrating single atoms Ni (SAs Ni) for CO₂-to-CO conversion and amino-functionalized cobalt phthalocyanine (CoPc-NH₂) for methanol formation on N-doped carbon nanotubes ((SAs Ni + CoPc-NH₂)/N-CNT). The dual-site catalyst achieves a remarkable methanol Faradaic efficiency (FE_MeOH) of 48.7% and a total current density of 45.6 mA cm^-2 at -1.05 V vs. RHE, outperforming single-component CoPc-NH₂/N-CNT (FE_max = 28.4%) and physically mixed SAs Ni/N-CNT + CoPc-NH₂/N-CNT (FE_max = 30.6%) in an H-cell. A peak FE_MeOH of 51.9% and a methanol partial current density of 103.8 mA cm^-2 are achieved in a flow cell. When tested in a membrane electrode assembly (MEA) electrolyzer fed with simulated flue gas (10% CO₂), the catalyst delivers a current density of 500 mA cm^-2, while maintaining a FE_MeOH of 67.1%. In situ attenuated total reflectance-surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) confirms the enhanced surface coverage of ^⁎CO and the emergence of the ^⁎CHO intermediate exclusively on the dual-site interface, revealing a synergistic mechanism wherein SAs Ni sites enrich the local ^⁎CO concentration and adjacent CoPc-NH₂ sites facilitate its selective hydrogenation to methanol. This work provides a catalyst design paradigm for efficient CO₂-to-methanol conversion and offers fundamental insights into constructing cooperative interfaces for multistep electrocatalytic reactions.

PMID:
42372335
Bibliographic data and abstract were imported from PubMed on 30 Jun 2026.

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