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不同尺寸的钯银纳米粒子:简便的一步合成法及其对甲酸氧化的高电催化活性

PdAg Nanoparticles with Different Sizes: Facile One-Step Synthesis and High Electrocatalytic Activity for Formic Acid Oxidation.

作者信息

Yang Lei, Wang Yawen, Feng Hetian, Zeng Huajie, Tan Changhui, Yao Junjie, Zhang Junchang, Jiang Lin, Sun Yinghui

机构信息

College of Chemistry and Chemical Engineering, Henan Polytechnic University, Jiaozuo, 454003, P. R. China.

Institute of Functional Nano & Soft Materials Laboratory (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Suzhou, 215123, P. R. China.

出版信息

Chem Asian J. 2021 Jan 4;16(1):34-38. doi: 10.1002/asia.202001253. Epub 2020 Dec 7.

Abstract

Recently, direct formic acid fuel cells (DFAFCs) which possess superior advantages such as a low operating temperature, light environmental pollution and high energy density, have been considered as one of the power generation technologies with a bright prospect. Herein, bimetallic PdAg nanoparticles (NPs) with different particle sizes were successfully produced via an easy one-pot solvothermal co-reduction synthetic route and their electrocatalytic performance for formic acid oxidation (FAO) were further investigated. In our strategy, the size of PdAg NPs can be easily controlled by only varying the concentration of precursors. The larger sized PdAg alloy (9.5 nm, noted as PdAg-L) was obtained at a low concentration of precursors, while the smaller PdAg alloy (3.7 nm, named as PdAg-S) was separated from the reaction system with higher solubility by centrifugation. The electrocatalytic activity and stability of the obtained PdAg NPs could be well optimized when incorporated with carbon (C), which is owing to a synergetic effect. The PdAg-S/C exhibits the highest mass activity with around 1.6 times that of PdAg-L/C and 2 times that of commercial Pd/C, which can be attributed to its larger ECSA and lower adsorption energy of the intermediate to facilitate the direct oxidation of HCOOH molecule.

摘要

最近,直接甲酸燃料电池(DFAFCs)因其具有诸如低工作温度、轻度环境污染和高能量密度等优越优势,被视为具有光明前景的发电技术之一。在此,通过简便的一锅溶剂热共还原合成路线成功制备了具有不同粒径的双金属钯银纳米颗粒(NPs),并进一步研究了它们对甲酸氧化(FAO)的电催化性能。在我们的策略中,仅通过改变前驱体的浓度就可以轻松控制钯银纳米颗粒的尺寸。在前驱体浓度较低时获得了较大尺寸的钯银合金(9.5 nm,记为PdAg-L),而较小尺寸的钯银合金(3.7 nm,命名为PdAg-S)通过离心从具有较高溶解度的反应体系中分离出来。当与碳(C)结合时,所获得的钯银纳米颗粒的电催化活性和稳定性可以得到很好的优化,这归因于协同效应。PdAg-S/C表现出最高的质量活性,约为PdAg-L/C的1.6倍和商业Pd/C的2倍,这可归因于其更大的电化学活性表面积(ECSA)和中间体较低的吸附能,有利于HCOOH分子的直接氧化。

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