Work

Defect-mediated electron pumping at heterointerfaces boosts CO2-to-fuels conversion

Year: 2025

Type: article

Abstract: Developing CO 2 electroreduction (CO 2 RR) catalysts that exhibit high activity, selectivity, and long-term stability is a crucial challenge in the pursuit of carbon-neutral energy systems. In this work, we had engineered a Ruddlesden-Popper (RP) perovskite/CuO heterostructure catalyst with remarkable CO 2 RR performance. By strategically modulating the valence of the A-site, the performances of the catalyst were optimized through tailored surface/interface oxygen vacancies (Ovs). The optimized La 1.9 CuO 4 /CuO catalyst achieved a CO Faradaic efficiency (FE CO ) of 97.54 % at −0.8 V vs. RHE and demonstrated stability for over 48 h during continuous testing. Mechanism research combining experimental analysis and density functional theory (DFT) calculations revealed that the heterojunction directionally accumulated electrons to the copper oxide domains, forming a distinctive "electron pumping" that promoted CO 2 activation and lowered the Gibbs free energy barrier for carboxyl intermediate formation, thereby enhancing its binding capability in the CO 2 RR. Concurrently, Ovs enhanced CO 2 activation kinetics and stabilized the ∗CO intermediate.

Source: Materials Today Chemistry

DOI: 10.1016/j.mtchem.2025.103242

Authors: Meng Shi, Ying-Ying Chao, Meng-Qi Zhang, Ke-Xin Du, Feng-Cui Shen

Institution: Anhui Polytechnic University

Language: English

Topic: CO2 Reduction Techniques and Catalysts

Subfield: Renewable Energy, Sustainability and the Environment

Field: Energy

Domain: Physical Sciences

SDGs: Affordable and clean energy, Climate action

Open Access status: hybrid

Estimated APC paid: $3,500