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Tailoring the Cu Local Microenvironment to Create Formate Conversion-Desorption Equilibrium for Industrial Level
Peiyuan Mao1, Huizhu Cai2, Hongting Ma1
1State Key Laboratory of Fine Chemicals, School of Chemistry, Dalian University of Technology, Dalian, China.
Angewandte Chemie (International Ed. in English)
|June 18, 2026
Summary
Copper electrocatalysts deactivate due to formate buildup, not oxidation. Engineering the electronic environment with silver (Ag) weakens formate adsorption, enabling stable, high-current formaldehyde oxidation catalysis.
Area of Science:
- Electrochemistry
- Materials Science
- Catalysis
Background:
- Copper-based electrocatalysts show high initial activity for formaldehyde oxidation but degrade rapidly at high current densities.
- Instability is often attributed to copper oxidation, but the primary cause of performance decay is debated.
Purpose of the Study:
- To identify the fundamental origin of performance decay in copper electrocatalysts for formaldehyde oxidation.
- To develop a strategy for enhancing catalyst stability and activity through electronic microenvironment engineering.
Main Methods:
- Fabrication of silver-copper (AgCu) microsphere catalysts (AgCu-MSs/CF) with controlled silver loading (4.1 wt.%).
- Electrochemical characterization including cyclic voltammetry and chronoamperometry.
- In situ spectroscopy (e.g., X-ray photoelectron spectroscopy) and density functional theory (DFT) calculations.
- Testing of a bipolar formaldehyde oxidation (FOR)||hydrogen evolution reaction (HER) electrolyzer.
Main Results:
- Persistent accumulation of formate intermediates, not copper oxidation, was identified as the primary deactivation pathway.
- The AgCu-MSs/CF catalyst achieved a current density of 1068 mA cm⁻² at 1.0 V versus RHE and stable operation up to 1.3 V versus RHE.
- Ag incorporation induced electron transfer from Ag to Cu, downshifting the Cu d-band center and weakening formate adsorption.
- The bipolar FOR||HER electrolyzer demonstrated stable operation for over 312 hours.
Conclusions:
- Engineering the dynamic equilibrium between intermediate formation and removal is a generalizable strategy to prevent poisoning in copper-based catalysts.
- Optimizing the electronic microenvironment of copper electrocatalysts can overcome performance limitations in complex oxidation reactions.
- The developed AgCu catalyst design offers a promising approach for efficient and stable formaldehyde oxidation catalysis.
