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通过掺入磷来诱导富电子催化界面,增强 Pd-Ir 纳米合金的电催化甲醇氧化。

Enhancing electrocatalytic methanol oxidation of Pd-Ir nanoalloy through electron-rich catalytic interface induced by incorporating phosphorus.

机构信息

State Key Laboratory of Applied Organic Chemistry (SKLAOC), College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000, China.

Inner Mongolia Key Laboratory of Photoelectric Functional Materials, College of Chemistry and Life Sciences, Chifeng University, Chifeng 024000, China.

出版信息

J Colloid Interface Sci. 2023 Oct;647:438-445. doi: 10.1016/j.jcis.2023.05.174. Epub 2023 May 29.

Abstract

Incorporating less expensive nonmetal phosphorus (P) into noble metal-based catalysts has become a developing strategy to enhance the catalytic performance of electrocatalysts for methanol electrooxidation reaction (MOR), attributing to the electronic and synergistic structure alteration mechanism. In the work, three-dimensional nitrogen-doped graphene anchoring ternary Pd-Ir-P nanoalloy catalyst (PdIrP/NG) was prepared by co-reduction strategy. As a multi-electron system, elemental P adjusts the outer electron structure of Pd and diminishes the particle size of nanocomposites, which heightens the electrocatalytic activity effectively and accelerate MOR kinetics in alkaline medium. The study reveals that the electron effect and ligand effect induced by P atoms on the hydrophilic and electron-rich surface of PdIr/NG and PdIrP/NG samples can reduce the initial oxidation potential and peak potential of CO, showing significantly enhanced the anti-poisoning ability compared with commercial Pd/C as the benchmark. Meanwhile, the stability of PdIrP/NG is significantly higher than that of commercial Pd/C. The facile synthetic approach provides an economic option and a new vision for the development of electrocatalysts in MOR.

摘要

将较便宜的非金属磷 (P) 纳入贵金属基催化剂中,已成为提高甲醇氧化反应 (MOR) 电催化剂催化性能的一种发展策略,这归因于电子和协同结构改变机制。在这项工作中,采用共还原策略制备了三维氮掺杂石墨烯锚定三元 Pd-Ir-P 纳米合金催化剂 (PdIrP/NG)。作为多电子体系,元素 P 调整了 Pd 的外层电子结构并减小了纳米复合材料的粒径,这有效地提高了电催化活性并加速了碱性介质中的 MOR 动力学。研究表明,P 原子在亲水性和富电子的 PdIr/NG 和 PdIrP/NG 样品表面引起的电子效应和配体效应对 CO 的初始氧化电位和峰电位有降低作用,与商业 Pd/C 相比,表现出明显增强的抗中毒能力,后者被用作基准。同时,PdIrP/NG 的稳定性明显高于商业 Pd/C。这种简便的合成方法为 MOR 中电催化剂的发展提供了一种经济选择和新视角。

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