L1₀-PtCo and L1₂-Pt₃Co Intermetallics for Oxygen Reduction Reaction: The Influence of Composition and Structure on Properties.

IF 3 4区化学 Q2 CHEMISTRY, MULTIDISCIPLINARY ChemPlusChem Pub Date : 2024-10-04 DOI:10.1002/cplu.202400322

Mingwang Lu, Yuekun Hu, Guanhua Zhang, Xiaowei Zhao, Xiaojing Yang, Xiaofei Yu, Xinghua Zhang, Zunming Lu, Yan Liu, Lanlan Li

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Abstract

Pt-based intermetallics are regarded as highly efficient electrocatalysts for oxygen reduction reaction (ORR). However, Pt-based intermetallics with different Pt: M atomic ratios have different atomic arrangements and crystal structures, which will change the electronic structure and coordination environment of Pt, thus affecting the electrocatalytic activity. In this work, we prepared L1₂-Pt₃Co and L1₀-PtCo intermetallic catalysts by modulating the molar ratio of Pt and Co precursors using a thermal annealing method. The mass activity (MA) of L1₀-PtCo is 0.52 A mg^-1 _Pt at 0.9 V, which is 1.44 times larger than that of L1₂-Pt₃Co (0.36 A mg^-1 _Pt). In addition, the MA of L1₀-PtCo decreases by 17.31 % after 10,000 CV cycles, which is smaller than that of L1₂-Pt₃Co (25.00 % loss in MA), showing excellent structural stability. Theoretical calculations reveal that compared to L1₂-Pt₃Co, L1₀-PtCo has more electrons transferred to the Pt sites, which further optimizes the electronic structure of Pt and reduces the d-band center, leading to the increase of the electrocatalytic performance. This work provides new insights into the study of Pt-based intermetallics with different Pt: M ratios, which is helpful for the screening and preparation of high-performance Pt-based intermetallics.

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用于氧还原反应的 L10-PtCo 和 L12-Pt3Co 金属间化合物：成分和结构对性能的影响。

铂基金属间化合物被认为是氧气还原反应（ORR）的高效电催化剂。然而，具有不同 Pt：M原子比的铂基金属间化合物具有不同的原子排列和晶体结构，这将改变铂的电子结构和配位环境，从而影响其电催化活性。本研究采用热退火方法，通过调节铂和钴前驱体的摩尔比，制备了 L12-Pt3Co 和 L10-PtCo 金属间化合物催化剂。在 0.9 V 下，L10-PtCo 的质量活度（MA）为 0.52 A mg-1Pt，是 L12-Pt3Co （0.36 A mg-1Pt）的 1.44 倍。此外，在 10,000 次 CV 循环后，L10-铂钴的 MA 下降了 17.31%，小于 L12-Pt3Co 的 MA 下降率（25.00%），显示出优异的结构稳定性。理论计算表明，与 L12-Pt3Co 相比，L10-PtCo 有更多的电子转移到铂位点，从而进一步优化了铂的电子结构，降低了 d 带中心，从而提高了电催化性能。这项工作为研究不同 Pt：M比的铂基金属间化合物的研究提供了新的见解，有助于筛选和制备高性能的铂基金属间化合物。

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

ChemPlusChem CHEMISTRY, MULTIDISCIPLINARY-

CiteScore

5.90

自引率

0.00%

发文量

200

审稿时长

1 months

期刊介绍： ChemPlusChem is a peer-reviewed, general chemistry journal that brings readers the very best in multidisciplinary research centering on chemistry. It is published on behalf of Chemistry Europe, an association of 16 European chemical societies. Fully comprehensive in its scope, ChemPlusChem publishes articles covering new results from at least two different aspects (subfields) of chemistry or one of chemistry and one of another scientific discipline (one chemistry topic plus another one, hence the title ChemPlusChem). All suitable submissions undergo balanced peer review by experts in the field to ensure the highest quality, originality, relevance, significance, and validity.