氢化钯中掺入铋用于增强 CO 耐受性的电催化乙醇氧化,ACS Applied Materials & Interfaces

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氢化钯中掺入铋用于增强 CO 耐受性的电催化乙醇氧化
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2023-08-22 , DOI: 10.1021/acsami.3c08885
Xianlong Yang _{1,

2} , Xinghao Li _{1,

2} , Shu Bu ₁ , Tingting Wan _{1,

2} , Dong Xiang ₁ , Lina Ye ₁ , Zhenjie Sun ₁ , Kun Wang ₁ , Manzhou Zhu _{1,

2} , Peng Li _{1,

2}

Affiliation

将非金属和亲氧金属引入钯（Pd）基催化剂有利于增强电催化性能，特别是在提高质量活性（MA）和CO耐受性方面。在此，通过一种简单的一步法成功地制备了稳定的铋掺杂氢化钯（Bi/PdH）网络。间隙H原子的嵌入扩大了Pd的晶格，亲氧金属Bi的掺杂抑制了有毒中间体在Pd表面的吸附，从而提高了所制备的催化剂在乙醇氧化反应（EOR）中的活性和耐久性。）。所获得的Bi/PdH网络表现出显着的MA为8.51 A·mg _Pd^–1，比商业Pd/C（0.76 A·mg _Pd^–1）高11.18倍。CO 剥离分析结果表明，Bi 掺杂可以显着抑制 Bi/PdH 网络表面的 CO 吸附。密度泛函理论 (DFT) 计算还表明，Bi 掺杂增强了催化剂表面的 OH* 吸附，并减轻了 Pd 和 CO* 中间体之间的相互作用，从而为增强 EOR 活性和 CO 耐受性的起源提供了更深入的见解。这项工作描述了生产高性能和耐用的 PdH 纳米催化剂的有效途径。

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Bismuth Incorporation in Palladium Hydride for the Electrocatalytic Ethanol Oxidation with Enhanced CO Tolerance

Introducing nonmetal and oxophilic metal into palladium (Pd)-based catalysts is beneficial for boosting electrocatalysis, especially regarding the improvement of mass activity (MA) and CO tolerance. Herein, the stable bismuth-doped palladium hydride (Bi/PdH) networks have been successfully fabricated through a simple one-step method. The intercalation of interstitial H atoms expands the lattice of Pd, and the doping of oxophilic metal Bi restrains the adsorption of poisonous intermediates on the surface of Pd, thereby improving the activity and durability of the as-prepared catalysts in the ethanol oxidation reaction (EOR). The obtained Bi/PdH networks manifest a remarkable MA of 8.51 A·mg_Pd^–1, which is 11.18 times higher than that of commercial Pd/C (0.76 A·mg_Pd^–1). The CO-stripping analysis results indicate that Bi doping can significantly prohibit CO adsorption on the surface of the Bi/PdH networks. The density functional theory (DFT) calculations also reveal that Bi doping enhances the OH* adsorption on the catalyst surface and mitigates the interaction between Pd and CO* intermediates, providing deeper insights into the origin of the enhanced EOR activity and CO tolerance. This work describes an impactful path for producing high-performance and durable PdH-based nanocatalysts.

更新日期：2023-08-22

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