Boosting Electrocatalytic Nitrate Reduction to Ammonia on a Hierarchical Nanoporous Ag,Ni-Codoped Cu Catalyst via Trimetallic Synergistic and Nanopore Enrichment Effects

IF 9.1 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nano Letters Pub Date : 2025-01-01 DOI:10.1021/acs.nanolett.4c05376

Yuhuan Cui, Changning Sun, Yuexuan He, Zixuan Feng, Guopeng Ding, Qingqing Dai, Tonghui Wang, Zhili Wang, Qing Jiang

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Abstract

The electrochemical nitrate (NO₃^–) reduction reaction (NO₃^–RR) offers a promising route for NO₃^– wastewater treatment and sustainable ammonia (NH₃) synthesis. However, the reaction still faces the challenges of unsatisfactory productivity and selectivity. Herein, we report a hierarchical nanoporous Ag,Ni-codoped Cu (np Ag,Ni-Cu) catalyst that exhibits a high NH₃ Faradaic efficiency of 98.5% with an attractive NH₃ yield rate of 41.1 mg h^–1 mg_cat^–1 at −0.2 V vs RHE for the NO₃^–RR. Density functional theory calculations and molecular dynamics simulations suggest that the excellent performance of np Ag,Ni-Cu results from a trimetallic synergistic effect and nanopore enrichment/confinement effect, in which the codoping of Ni and Ag into Cu can enhance NO₃^– adsorption, prevent *NO₂ desorption, and suppress the hydrogen evolution reaction, while nanopores can promote NO₃^– accumulation on the internal surface of nanopores and confine the reaction intermediates within the nanopores for a deeper NO₃^– electroreduction.

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基于三金属协同效应和纳米孔富集效应的分级纳米孔银、镍共掺杂铜催化剂电催化硝酸还原制氨

电化学硝酸（NO3 -）还原反应（NO3 - rr）为NO3 -废水处理和氨（NH3）的可持续合成提供了一条有前景的途径。然而，该反应仍然面临着生产率和选择性不理想的挑战。本文报道了一种分层纳米孔Ag、ni共掺杂Cu （np Ag,Ni-Cu）催化剂，在- 0.2 V / RHE条件下，NO3-RR的NH3产率为41.1 mg h-1 mgcat-1， NH3法拉第效率高达98.5%。密度泛函理论计算和分子动力学模拟表明，np Ag、Ni-Cu的优异性能源于三金属协同效应和纳米孔富集/约束效应，其中Ni和Ag共掺杂Cu可以增强NO3 -吸附，阻止*NO2解吸，抑制析氢反应。而纳米孔可以促进NO3 -在纳米孔内表面的积累，并将反应中间体限制在纳米孔内，从而实现更深层次的NO3 -电还原。

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

Nano Letters 工程技术-材料科学：综合

CiteScore

16.80

自引率

2.80%

发文量

1182

审稿时长

1.4 months

期刊介绍： Nano Letters serves as a dynamic platform for promptly disseminating original results in fundamental, applied, and emerging research across all facets of nanoscience and nanotechnology. A pivotal criterion for inclusion within Nano Letters is the convergence of at least two different areas or disciplines, ensuring a rich interdisciplinary scope. The journal is dedicated to fostering exploration in diverse areas, including: - Experimental and theoretical findings on physical, chemical, and biological phenomena at the nanoscale - Synthesis, characterization, and processing of organic, inorganic, polymer, and hybrid nanomaterials through physical, chemical, and biological methodologies - Modeling and simulation of synthetic, assembly, and interaction processes - Realization of integrated nanostructures and nano-engineered devices exhibiting advanced performance - Applications of nanoscale materials in living and environmental systems Nano Letters is committed to advancing and showcasing groundbreaking research that intersects various domains, fostering innovation and collaboration in the ever-evolving field of nanoscience and nanotechnology.