Generalized chalcogenation for boosting the electrocatalytic alcohol oxidation of Pd nanoflowers

IF 2.6 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY
CrystEngComm Pub Date : 2025-09-05 DOI:10.1039/D5CE00688K
Zuoran Li, Lijie Zhu, Li Liu, Zhiwei He, JingYi Jiang, Hongyi Chen and Jiafu Zhong
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引用次数: 0

Abstract

The electrocatalytic alcohol oxidation reaction (AOR) is a crucial process in fuel cells; however, conventional electrocatalysts underperform owing to their limited electrocatalytic activity and poor stability, and achieving the dissociation of C–C bonds in alcohols is one of the biggest challenges in improving AOR efficiency. Herein, we propose a generalized chalcogenation strategy for significantly promoting the electrocatalytic AOR performance of Pd nanoflowers. Surprisingly, the mass activity and specific activity of the ethylene glycol oxidation reaction (EGOR) based on the optimized Pd8Te1 nanocatalyst remarkably enhanced by 1.72 and 1.25 times, respectively. In addition to the EGOR, the as-obtained PdTe electrocatalysts were demonstrated to be highly active toward the ethanol oxidation reaction (EOR) and glycerol oxidation reaction (GOR). Detailed investigations reveal that their superior electrocatalytic activity and durability are attributed to the effect of chalcogenation, which could induce modification of the electronic structure of Pd to not only boost electron transfer but also significantly decrease the activation energy. More significantly, the chalcogenation strategy is general and thus can be extended to construct other efficient AOR electrocatalysts with enhanced performance. Considering the high electrocatalytic properties and facile synthesis method, we suggest that this generalized chalcogenation strategy will open a new avenue for the production of advanced electrocatalysts and boost the development of fuel cells.

Abstract Image

广义硫代作用促进钯纳米花电催化醇氧化
电催化醇氧化反应(AOR)是燃料电池中的一个关键过程。然而,传统的电催化剂由于其有限的电催化活性和较差的稳定性而表现不佳,实现醇中C-C键的解离是提高AOR效率的最大挑战之一。在此,我们提出了一种通用的硫代化策略,以显著提高钯纳米花的电催化AOR性能。令人惊讶的是,优化后的Pd8Te1纳米催化剂的乙二醇氧化反应(EGOR)的质量活性和比活性分别提高了1.72倍和1.25倍。除EGOR外,所制备的PdTe电催化剂对乙醇氧化反应(EOR)和甘油氧化反应(GOR)也有较高的催化活性。详细的研究表明,它们优异的电催化活性和耐久性归因于硫代作用的影响,硫代作用可以诱导Pd的电子结构发生修饰,从而促进电子转移,同时显著降低活化能。更重要的是,该加硫策略是通用的,因此可以扩展到构建其他性能更高的高效AOR电催化剂。考虑到其高电催化性能和简便的合成方法,我们认为这种通用的硫代化策略将为先进电催化剂的生产开辟新的途径,促进燃料电池的发展。
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来源期刊
CrystEngComm
CrystEngComm 化学-化学综合
CiteScore
5.50
自引率
9.70%
发文量
747
审稿时长
1.7 months
期刊介绍: Design and understanding of solid-state and crystalline materials
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