C15‐Phase Platinum‐Lanthanide Intermetallics for Efficient Hydrogen Evolution: Identifying Lanthanide's Enhanced Mechanism

IF 27.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Wei Yan, Yimin Mou, Meng Li, Kaiyue Ma, Zhiwen Xu, Tingyu Lu, Han Du, Caikang Wang, Huamei Sun, Lei Chen, Yawen Tang, Yu Wang, Gengtao Fu
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Abstract

Platinum‐Lanthanide (Pt‐Ln) intermetallic compounds (IMCs) are a promising new class of electrocatalytic materials, yet their synthesis remains a significant challenge, and the role of ordered Ln sites in enhancing catalytic performance is not fully understood. Herein, an effective and rapid avenue for synthesizing carbon‐supported C15‐phase Pt2Ln IMCs (Ln: Sm, Eu, Gd, and Tb) through Joule heating technology is proposed. The JH‐Pt2Ln/C IMCs exhibit excellent electrocatalytic performance toward alkaline hydrogen evolution reaction (HER), in which JH‐Pt2Tb/C presents the lowest overpotential of 17 mV at 10 mA cm−2. The ordered Pt2Tb structure offers favorable Pt2 dimer sites for the desorption of H* intermediates, in contrast to the Pt3 trimer sites in disordered Pt2Tb and pure Pt. The ordered Tb sites play a bifunctional role in HER: i) The oxophilic Tb atoms are in favor of the H2O adsorption and dissociation through Tb‐4f‐OH binding; ii) The strong Tb 4f‐Pt 5d orbital hybridization leads to form negatively charged Pt sites, which promotes the desorption of H* intermediates. Furthermore, the anion exchange membrane water electrolyzer equipped with JH‐Pt2Tb/C delivers a low voltage of only 1.79 Vcell to reach 1 A cm−2 and maintains the stable operation at 1 A cm−2 for over 100 h.
高效析氢的C15 -相铂-镧系金属间化合物:确定镧系元素的增强机制
铂-镧系(Pt - Ln)金属间化合物(IMCs)是一类很有前途的新型电催化材料,但它们的合成仍然是一个重大挑战,并且有序的Ln位点在提高催化性能方面的作用尚未完全了解。本文提出了一种利用焦耳加热技术快速合成碳负载C15相Pt2Ln IMCs (Ln: Sm, Eu, Gd和Tb)的有效途径。JH‐Pt2Ln/C IMCs对碱性析氢反应(HER)表现出优异的电催化性能,其中JH‐Pt2Tb/C在10 mA cm−2下的过电位最低,为17 mV。与无序Pt2Tb和纯Pt中的Pt3三聚体位点相比,有序Pt2Tb结构为H*中间体的解吸提供了有利的Pt2二聚体位点。有序Tb位点在HER中起双重功能作用:i)亲氧Tb原子通过Tb‐4f‐OH结合有利于H2O的吸附和解离;ii)强烈的Tb 4f - Pt 5d轨道杂化导致形成带负电荷的Pt位,促进H*中间体的解吸。此外,配备JH - Pt2Tb/C的阴离子交换膜水电解槽电压仅为1.79 Vcell,达到1 a cm - 2,并能在1 a cm - 2下稳定运行100小时以上。
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来源期刊
Advanced Materials
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.
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