Oxygen vacancy-assisted CuCo tandem catalyst boosts efficient electrocatalytic neutral ultralow-concentration nitrate to ammonia

IF 13.2 1区工程技术 Q1 ENGINEERING, CHEMICAL

Chemical Engineering Journal Pub Date : 2025-09-03 DOI:10.1016/j.cej.2025.168046

Xing Fan, Cui Lai, Lei Qin, Mingming Zhang, Huchuan Yan, Shiyu Liu, Dengsheng Ma, Qianting Liu, Lin Tang

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引用次数: 0

Abstract

The electrochemical nitrate reduction reaction (NO₃RR) is a promising approach as a zero‑carbon route. Notable progress has been made in the high-concentration NO₃⁻ field, but the high-efficiency transformation of neutral low-concentration NO₃⁻ to ammonia (NH₃) still faces a huge challenge because of the slow reaction kinetics of NO₃RR and the strong competitive reaction of hydrogen evolution reaction (HER). To overcome the dilemma, we design the oxygen vacancy (Ov) assisted traditional CuCo tandem catalyst. CuCo tandem catalyst greatly improves the reaction kinetics of NO₃RR. Electrochemical measures and theoretical calculations show that Ov promotes water dissociation and the hydrogenation of NO₃⁻ and intermediates, thereby inhibiting the competitive HER. At −0.6 V vs RHE, a high NH₃ yield rate (1615 μg h⁻¹ cm⁻²) and Faradaic efficiency (FE) of 95.6 % were obtained during the treatment of 5 mM nitrate wastewater via electronic structure regulation and tandem catalytic synergetic mechanism. In addition, the development of an integrated system coupling simultaneous NO₃RR and ammonia recovery facilitates synergistic pollutant removal and resource recovery. This work contributes a novel insight into the promotion of efficient conversion of neutral ultralow-concentration NO₃⁻ and establishes a fresh guideline for broadening the application of tandem electrocatalysts.

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氧空位辅助CuCo串联催化剂提高了中性超低浓度硝酸盐对氨的高效电催化

电化学硝酸还原反应（NO3RR）是一种很有前途的零碳途径。高浓度NO3−领域已取得显著进展，但中性低浓度NO3−高效转化为氨（NH3）仍面临巨大挑战，原因是NO3RR反应动力学缓慢，析氢反应（HER）竞争反应强。为了克服这一难题，我们设计了氧空位（Ov）辅助的传统CuCo串联催化剂。CuCo串联催化剂极大地改善了NO3RR的反应动力学。电化学测量和理论计算表明，Ov促进了水的解离和NO3−和中间体的加氢，从而抑制了竞争性HER。在−0.6 V vs RHE条件下，通过电子结构调控和串联催化协同机制处理5 mM硝酸废水，获得了较高的NH3产率（1615 μg h−1 cm−2）和95.6% %的法拉第效率。此外，开发NO3RR和氨回收同时耦合的集成系统，促进污染物的协同去除和资源的回收。本研究为促进中性超低浓度NO3−的高效转化提供了新的思路，并为拓展串联电催化剂的应用开辟了新的思路。

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来源期刊

Chemical Engineering Journal 工程技术-工程：化工

CiteScore

21.70

自引率

9.30%

发文量

6781

审稿时长

2.4 months

期刊介绍： The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.