Curvature-programmed nitrate electroreduction via single-atom protrusions on quantum dots

IF 12.5 1区综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES

Science Advances Pub Date : 2026-05-08

Dong Chen, Shaoce Zhang, Dongchang He, Haifan Li, Xinru Yang, Di Yin, Mengxue Chen, Quan Quan, Yuxuan Zhang, Boxiang Gao, Yi Shen, Weijun Wang, Zenghui Wu, You Meng, SenPo Yip, Chun-Yuen Wong, Chunyi Zhi, Johnny C. Ho

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Abstract

Local geometric constraints have a substantial influence on electronic structure renormalization, offering a promising approach to enhance single-atom catalysts (SACs) beyond traditional limits. Conventional SACs typically feature planar-confined sites, but three-dimensional configurations remain underexplored. This study introduces a “curvature-programming” strategy to drive electrochemical nitrate reduction by assembling FeCu dual single-atom protrusions on molybdenum carbide quantum dots (FeCu/MoC_x-5 QDs). The high-curvature QDs and protruding geometries mimic active vertex sites, enhancing electric fields to polarize N─O bonds. This delivers nearly 100% NH₃ Faradaic efficiency over a wide potential window (−0.1 to −0.4 V versus reversible hydrogen electrode), with an ultralow overpotential (300 mV) and energy consumption (7.52 Wh g_NH3⁻¹ mg_cat⁻¹). FeCu/MoC_x-5 effectively reduces nitrate levels in wastewater, producing scalable (NH₄)₂SO₄, thus integrating environmental remediation with renewable energy storage. This work provides a promising strategy for developing SACs for broader energy applications.

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量子点上单原子突起的曲率编程硝酸电还原

局部几何约束对电子结构重整化有重大影响，为提高单原子催化剂（SACs）的性能提供了一种超越传统限制的有前途的方法。传统的sac通常具有平面受限的位置，但三维结构仍未得到充分探索。本研究引入了一种“曲率规划”策略，通过在碳化钼量子点（FeCu/ mox -5量子点）上组装FeCu双单原子突起来驱动电化学还原硝酸盐。高曲率量子点和突出的几何形状模拟了活跃的顶点位置，增强了电场，使N─O键极化。这在宽电位窗口（−0.1至−0.4 V相对可逆氢电极）内提供了接近100%的NH3法拉第效率，具有超低过电位（300 mV）和能量消耗（7.52 Wh gNH3−1 mgcat−1）。FeCu/ mox -5有效降低了废水中的硝酸盐水平，产生可扩展的（NH4）2SO4，从而将环境修复与可再生能源储存结合起来。这项工作为开发更广泛的能源应用的sac提供了一个有希望的策略。

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来源期刊

Science Advances 综合性期刊-综合性期刊

CiteScore

21.40

自引率

1.50%

发文量

1937

审稿时长

29 weeks

期刊介绍： Science Advances, an open-access journal by AAAS, publishes impactful research in diverse scientific areas. It aims for fair, fast, and expert peer review, providing freely accessible research to readers. Led by distinguished scientists, the journal supports AAAS's mission by extending Science magazine's capacity to identify and promote significant advances. Evolving digital publishing technologies play a crucial role in advancing AAAS's global mission for science communication and benefitting humankind.