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Solvent Engineering of Highly Conductive and Porous Fullerene Ammonium Iodide for Immobilizing Pd Nanoparticles with Enhanced Electrocatalytic Activity Toward Ethanol Oxidation
Electrocatalysis ( IF 3.1 ) Pub Date : 2019-05-18 , DOI: 10.1007/s12678-019-00535-4
Zhouchen Lin , Huanhuan Wang , Ming Lei

So far, the application of fullerene derivative support in electrocatalysis has been limited by fullerene’s low electronic conductivity and the difficulty in film morphology control. Although highly conductive (1.5 s m−1) fullerene ammonium iodide (PCBANI) had been demonstrated to be a potential support, the solid self-assembled film is not of benefit for metallic nanoparticle (NP) to exhibit catalytic activity. In this work, we found solvent engineering of pristine PCBANI aggregate could maintain stacked short-range assembly structure and porous morphology. Moreover, PCBANI film fabricated from the optimized DMSO/methanol could immobilize Pd NPs with a uniform size of around 4.8 ± 1.7 nm which was characterized by SEM, TEM, and SAED. The resulting Pd/PCBANI-1-coated electrode exhibits a mass-specific activity for Pd of 3361.0 mA mg−1 at a scan rate of 50 mV s−1 and good stability toward alcohol electrooxidation, which are both significantly higher than that of the Pd/PCBANI-2 fabricated from PCBANI’s acetic acid/methanol dispersion and commercial Pd/C (active carbon). To the best of our knowledge, Pd/PCBANI-1 exhibits almost the highest catalytic activity among the existing fullerene-based Pd nanocatalysts. The high performance of the as-fabricated catalyst is attributed to highly conductive and porous PCBANI support, good dispersibility of Pd NPs on support, and favorable mass transfer.

Open image in new windowGraphical Abstract
Graphical Abstract

Highly conductive and porous fullerene ammonium iodide film fabricated from the optimized DMSO/methanol dispersion could be used as a synergistic support to immobilize Pd nanoparticle electrocatalyst which exhibits a highly mass-specific activity for Pd of 3361.0 A g−1.



中文翻译:

高导电性和多孔性富勒烯碘化铵的溶剂工程,用于固定具有增强的乙醇氧化电催化活性的Pd纳米颗粒

迄今为止,由于富勒烯的低电子电导率和膜形态控制的困难,限制了富勒烯衍生物载体在电催化中的应用。虽然导电性高(1.5 s m -1)富勒烯碘化铵(PCBANI)已被证明是潜在的载体,固体自组装膜不利于金属纳米颗粒(NP)表现出催化活性。在这项工作中,我们发现原始PCBANI聚集体的溶剂工程可以保持堆叠的短程组装结构和多孔形态。此外,由优化的DMSO /甲醇制备的PCBANI膜可以固定4.8 1.7 nm左右大小的Pd NP,通过SEM,TEM和SAED对其进行表征。将所得的Pd / PCBANI -1-涂覆的电极显示出对3361.0毫安毫克的钯特定的质量活性-1以50毫伏s的扫描速率-1以及对醇电氧化的良好稳定性,均明显高于由PCBANI的乙酸/甲醇分散体和市售Pd / C(活性炭)制成的Pd / PCBANI-2。据我们所知,Pd / PCBANI-1在现有的基于富勒烯的Pd纳米催化剂中几乎表现出最高的催化活性。制成的催化剂的高性能归因于高导电性和多孔性的PCBANI载体,Pd NP在载体上的良好分散性以及良好的传质性。

在新窗口中打开图像图形概要
图形概要

由优化的DMSO /甲醇分散体制成的高导电性和多孔性富勒烯碘化铵薄膜可以用作固定化Pd纳米粒子电催化剂的协同载体,该催化剂对Pd的质量比活性很高,为3361.0 A g -1

更新日期:2019-05-18
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