Interstitial Cobalt in Pt Shell of Pd@Pt Mesoporous Core-Shell Nanospheres with Strong d-d Orbital Hybridization for Enhanced Electrocatalytic Ammonia Oxidation.

IF 26.8 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Advanced Materials Pub Date : 2025-09-09 DOI:10.1002/adma.202511476

Cuiping Lin,Shanghai Yu,Yuxin Zhang,Chenchen Wang,Bo Ouyang,Ziqi Dong,Baotao Kang,Cuncheng Li,Yiqiang Sun,Kun Xu

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引用次数: 0

Abstract

Ammonia oxidation reaction (AOR) is critical for efficient ammonia utilization as a hydrogen carrier, yet state-of-the-art Pt-based catalysts suffer significant activity loss due to strong *NOx species (*NO, *NO2) adsorption. Herein, Pd@Pt mesoporous core-shell nanospheres with interstitial Co in Pt shell (Pd@Pt-Co MCSN) are demonstrated as an excellent AOR electrocatalyst, which achieves a mass activity of 293.6 A g-1 at 0.7 V versus RHE, 4.8-fold higher than commercial Pt/C. The interstitial Co dopant tunes the d-d orbital hybridization state, optimizes the Pt d-band center position, and facilitates electron transfer from Co to Pt, which effectively weakens the adsorption of toxic *NOx and lowers the energy barrier for N-N coupling. When integrated into a Zn-NH3 battery, the catalyst enables efficient NH3-to-H2 conversion with a Faradaic efficiency of 96.8% and stable operation for 30 hours at 12 mA cm-2. The work may provide a new design concept to develop advanced electrocatalysts for AOR.

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具有强d-d轨道杂化的Pd@Pt介孔核-壳纳米球Pt壳上的间隙钴增强电催化氨氧化。

氨氧化反应（AOR）作为氢载体对氨的高效利用至关重要，但最先进的pt基催化剂由于对NOx （*NO, *NO2）的强吸附而遭受显著的活性损失。研究结果表明，Pd@Pt介孔核壳纳米球（Pd@Pt-Co MCSN）是一种优异的AOR电催化剂，在0.7 V时，其质量活性达到293.6 a g-1，比商用Pt/C高4.8倍。间隙Co掺杂调整了d-d轨道杂化态，优化了Pt d带中心位置，促进了Co向Pt的电子转移，有效地减弱了有毒*NOx的吸附，降低了N-N耦合的能垒。当集成到Zn-NH3电池中时，该催化剂可实现nh3到h2的高效转化，法拉第效率为96.8%，并在12 mA cm-2下稳定运行30小时。本研究为开发先进的AOR电催化剂提供了一种新的设计思路。

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

Advanced Materials 工程技术-材料科学：综合

CiteScore

43.00

自引率

4.10%

发文量

2182

审稿时长

2 months

期刊介绍： Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.