On-Demand Hydrogen Supply Over Co-Cu Bimetallic Sulfide Nanoflowers for Efficient Electrocatalytic Nitrate Reduction to Ammonia.

IF 3.6 2区化学 Q2 CHEMISTRY, MULTIDISCIPLINARY

Chemistry - A European Journal Pub Date : 2026-09-03 DOI:10.1002/chem.71663

Cheng Song, Tinghui Liu, Xiaohui Yang, Xingzu Wang, Hong Liu

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引用次数: 0

Abstract

Electrocatalytic nitrate (NO₃ ^-) reduction offers a sustainable route for simultaneous NO₃ ^- remediation and ammonia (NH₃) production, yet its efficiency is limited by the competing hydrogen evolution reaction (HER) and the imbalance between NO₃ ^- activation and hydrogen supply. Herein, Co-Cu bimetallic sulfide nanoflowers were synthesized via a one-step hydrothermal method and optimized for NO₃ ^- to NH₃ conversion. The Co_0.9Cu_0.1S nanoflowers, assembled from two-dimensional nanosheets, delivered 97.83% ± 1.71% nitrate conversion, nearly complete NH₄ ⁺-N selectivity, and a Faradaic efficiency of 98.52% ± 0.83% at -0.75 V vs. RHE. Systematic Co/Cu-ratio studies, electrochemical kinetics, Bode analysis, hydrogen adsorption/desorption behavior, and XPS results reveal that Cu promotes NO₃ ^- activation and electronically modulates Co sites, while Co facilitates reactive hydrogen generation and utilization. This synergy enables on-demand hydrogen supply, directing hydrogen toward NO₃ ^- hydrogenation rather than HER. pH-dependent tests further identify a neutral electrolyte as favorable for balancing proton supply and competitive HER.

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在Co-Cu双金属硫化物纳米花上按需供氢，用于高效电催化硝酸还原为氨。

电催化硝酸还原（NO3 -）为同时修复NO3 -和生成氨（NH3）提供了一条可持续的途径，但其效率受到析氢反应（HER）的竞争和NO3 -活化与供氢之间的不平衡的限制。本文采用一步水热法合成了Co-Cu双金属硫化物纳米花，并对NO3 -转化为NH3进行了优化。由二维纳米片组装而成的Co0.9Cu0.1S纳米花在-0.75 V下的硝酸盐转化率为97.83%±1.71%，NH4 +-N选择性接近完全，法拉第效率为98.52%±0.83%。系统的Co/Cu比研究、电化学动力学、Bode分析、氢吸附/解吸行为和XPS结果表明，Cu促进NO3 -活化并电子调节Co位点，而Co促进反应氢的生成和利用。这种协同作用使按需氢供应成为可能，将氢导向NO3 -氢化而不是HER。ph依赖性测试进一步确定中性电解质有利于平衡质子供应和竞争性HER。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Chemistry - A European Journal 化学-化学综合

CiteScore

7.90

自引率

4.70%

发文量

1808

审稿时长

1.8 months

期刊介绍： Chemistry—A European Journal is a truly international journal with top quality contributions (2018 ISI Impact Factor: 5.16). It publishes a wide range of outstanding Reviews, Minireviews, Concepts, Full Papers, and Communications from all areas of chemistry and related fields. Based in Europe Chemistry—A European Journal provides an excellent platform for increasing the visibility of European chemistry as well as for featuring the best research from authors from around the world. All manuscripts are peer-reviewed, and electronic processing ensures accurate reproduction of text and data, plus short publication times. The Concepts section provides nonspecialist readers with a useful conceptual guide to unfamiliar areas and experts with new angles on familiar problems. Chemistry—A European Journal is published on behalf of ChemPubSoc Europe, a group of 16 national chemical societies from within Europe, and supported by the Asian Chemical Editorial Societies. The ChemPubSoc Europe family comprises: Angewandte Chemie, Chemistry—A European Journal, European Journal of Organic Chemistry, European Journal of Inorganic Chemistry, ChemPhysChem, ChemBioChem, ChemMedChem, ChemCatChem, ChemSusChem, ChemPlusChem, ChemElectroChem, and ChemistryOpen.