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Electronic Structure Tailoring of Copper by Oxygen-Enriched Carbon Dots Enables Nitrate-to-Ammonia Electrosynthesis via *NO2 Decoupling.

Created on 17 Jul 2026

Authors

Yunliang Liu, Ruixi Dong, Yixian Liu, Jingwen Yu, Zhiquan Lang, Yaxi Li, Yuanyuan Cheng, Yi Yang, Fan Gao, Hao Li, Naiyun Liu, Hui Huang, Zhenhui Kang, Haitao Li

Published in

Inorganic chemistry. Jul 17, 2026. Epub Jul 17, 2026.

Abstract

The electrochemical nitrate reduction reaction (NITRR) represents a sustainable strategy for ambient ammonia synthesis. However, copper-based catalysts often suffer from excessive adsorption of the *NO2 intermediate due to the high electron density on the Cu surface, resulting in active-site poisoning and sluggish reaction kinetics. Achieving an optimal balance between *NO2 adsorption and activation remains a major challenge for efficient nitrate reduction. Herein, we design a NITRR electrocatalyst consisting of oxygen-enriched carbon dots (CDs) and a carbon layer encapsulating copper nanoparticles (CuCECDs). Benefiting from the optimized decoupling of *NO2, the catalyst achieves an outstanding ammonia yield rate of 2.5 mol. gcat-1 h-1 with a Faradaic efficiency (FE) of 85% at -0.5 V versus RHE. Combined experimental and theoretical studies demonstrate that the oxygen-enriched carbon dots effectively regulate the electronic structure of Cu, weakening the excessive adsorption of *NO2 while confining its subsequent conversion within the carbon layer, thereby promoting efficient *NO2 transformation (*NO2 decoupling). Moreover, the carbon shell induces lattice strain in the Cu nanoparticles (Cu NPs), facilitating water dissociation and hydrogen generation, which further enhances ammonia electrosynthesis performance.

PMID:
42467471
Bibliographic data and abstract were imported from PubMed on 17 Jul 2026.

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