Boosting the Volmer step by synergistic coupling of dilute CuRu nanoalloy with Cu/Ru dual single atoms for efficient and CO-tolerant alkaline hydrogen oxidation

IF 15.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis Pub Date : 2025-05-01 DOI:10.1016/S1872-2067(25)64670-5

Yi Liu , Shuqing Zhou , Chenggong Niu , Tayirjan Taylor Isimjan , Yongfa Zhu , Dingsheng Wang , Xiulin Yang , Jieshan Qiu , Bin Wu

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引用次数: 0

Abstract

Active and poisoning-resistant Ru-based electrocatalysts for the hydrogen oxidation reaction (HOR) are designed and fabricated by integrating Cu/Ru dual single atoms and alloy CuRu nanoparticles (N-(CuRu)_NP+SA@NC) through a strategy involving weak chemical reduction and ammonia-assisted gas-phase nitridation. The resultant N-(CuRu)_NP+SA@NC electrocatalysts feature nitrogen atoms coordinated to both Cu and Ru metal atoms via strong N-metal interactions. Density functional theory calculations revealed that alloyed CuRu nanoparticles and monodispersed Cu atoms are vital for altering the electronic configuration of the host Ru elements. This finely tuned structure enhanced the adsorption of H and OH and promoted CO oxidation over the N-(CuRu)_NP+SA@NC electrocatalyst, resulting in high alkaline HOR activity, as evidenced by the higher exchange current density of 3.74 mA cm^–2 and high mass activity of 3.28 mA μg_Ru^–1, which are far superior to those of most Ru-based catalysts reported to date. Moreover, the N-(CuRu)_NP+SA@NC electrocatalysts are resistant to CO poisoning and can be used at a high concentration of 1000 ppm CO with no distinct decay in the activity, in stark contrast to the commercial Pt/C catalyst under the same conditions.

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稀cuu纳米合金与Cu/Ru双单原子的协同耦合提高了Volmer步长，实现了高效耐co的碱性氢氧化

通过弱化学还原和氨辅助气相氮化的策略，将Cu/Ru双单原子和合金CuRu纳米颗粒（N-(CuRu)NP+SA@NC）集成在一起，设计并制备了用于氢氧化反应（HOR）的活性和耐毒性Ru基电催化剂。合成的N-(CuRu)NP+SA@NC电催化剂的特征是氮原子通过强N-金属相互作用与Cu和Ru金属原子配位。密度泛函理论计算表明，合金cuu纳米颗粒和单分散的Cu原子对于改变宿主Ru元素的电子构型至关重要。该结构增强了N-(CuRu)NP+SA@NC电催化剂对H和OH的吸附，促进了CO的氧化，从而获得了较高的碱性HOR活性，其交换电流密度高达3.74 mA cm-2，质量活性高达3.28 mA μ gr - 1，远远优于目前报道的大多数ru基催化剂。此外，N-(CuRu)NP+SA@NC电催化剂具有抗CO中毒能力，可在1000ppm的CO浓度下使用，活性无明显衰减，与相同条件下的商用Pt/C催化剂形成鲜明对比。

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

Chinese Journal of Catalysis 工程技术-工程：化工

CiteScore

25.80

自引率

10.30%

发文量

235

审稿时长

1.2 months

期刊介绍： The journal covers a broad scope, encompassing new trends in catalysis for applications in energy production, environmental protection, and the preparation of materials, petroleum chemicals, and fine chemicals. It explores the scientific foundation for preparing and activating catalysts of commercial interest, emphasizing representative models.The focus includes spectroscopic methods for structural characterization, especially in situ techniques, as well as new theoretical methods with practical impact in catalysis and catalytic reactions.The journal delves into the relationship between homogeneous and heterogeneous catalysis and includes theoretical studies on the structure and reactivity of catalysts.Additionally, contributions on photocatalysis, biocatalysis, surface science, and catalysis-related chemical kinetics are welcomed.