Pb–Pd alloy catalysts with intercalated Pb atoms: optimized electronic and lattice structures for enhanced electrochemical ethanol oxidation†

IF 3.5 3区 化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR
Yonghui Ye, Yu Zhang, Xintong Yan, Gong Ning and Shi Hu
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Abstract

A facile one-step method is employed to synthesize carbon-supported Pd–Pb binary metal catalysts for the ethanol oxidation reaction (EOR) in alkaline electrolytes. A variety of characterization techniques have demonstrated that the alloying of Pd with Pb alters the electronic structure and induces lattice expansion. Electrochemical tests for the EOR in alkaline electrolytes demonstrated that the Pd3Pb/C catalyst exhibited the highest mass activity (3.59 A mgPd−1) and specific activity (17.97 mA cm−2), which are 4.6 and 4.7 times those of the Pd/C catalyst prepared by the same method, respectively. The intercalation of lead atoms has altered both the lattice and the electronic structure of palladium, leading to opposing shifts in the d-band center that collectively optimize the adsorption strength of CO* and OH*, key intermediates of the EOR. Consequently, the Pd3Pb/C electrocatalyst exhibits significant EOR catalytic activity. This study provides a viable implementation plan and analytical strategy for optimizing palladium-based catalysts with non-noble metals by integrating electronic transfer, bifunctional effects, and d-band center adjustments for bimetallic catalysts.

具有夹杂铅原子的铅钯合金催化剂:优化电子和晶格结构以增强乙醇的电化学氧化作用
采用简便的一步法合成了碱性电解液中乙醇氧化反应用碳负载钯-铅二元金属催化剂。多种表征技术表明,Pd与Pb的合金化改变了电子结构并诱发了晶格膨胀。碱性电解环境下提高采收率的电化学实验表明,Pd3Pb/C催化剂具有最高的质量活性(3.59 A·mgPd-1)和比活性(17.97 mA·cm- 2),分别是相同方法制备的Pd/C催化剂的4.6倍和4.7倍。铅原子的插入改变了钯的晶格和电子结构,导致d带中心的相反位移,共同优化了CO*和OH*的吸附强度,这是提高采收率的关键中间体。因此,Pd3Pb/C电催化剂表现出显著的EOR催化活性。本研究通过整合双金属催化剂的电子转移、双功能效应和d带中心调整的解释,为优化非贵金属钯基催化剂提供了可行的实施计划和分析策略。
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
Dalton Transactions
Dalton Transactions 化学-无机化学与核化学
CiteScore
6.60
自引率
7.50%
发文量
1832
审稿时长
1.5 months
期刊介绍: Dalton Transactions is a journal for all areas of inorganic chemistry, which encompasses the organometallic, bioinorganic and materials chemistry of the elements, with applications including synthesis, catalysis, energy conversion/storage, electrical devices and medicine. Dalton Transactions welcomes high-quality, original submissions in all of these areas and more, where the advancement of knowledge in inorganic chemistry is significant.
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