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在聚多巴胺还原氧化石墨烯载体上电催化增强铂和钯金属对醇氧化的作用。

Electrocatalytic enhancement of platinum and palladium metal on polydopamine reduced graphene oxide support for alcohol oxidation.

机构信息

Department of Chemistry, Faculty of Science, Chiang Mai University, Chiang Mai 50200, Thailand; Graduate School, Chiang Mai University, Chiang Mai 50200, Thailand.

Department of Chemistry, Faculty of Science, Chiang Mai University, Chiang Mai 50200, Thailand; Materials Science Research Center, Faculty of Science, Chiang Mai University, Chiang Mai 50200, Thailand.

出版信息

J Colloid Interface Sci. 2018 Nov 15;530:98-112. doi: 10.1016/j.jcis.2018.06.072. Epub 2018 Jun 25.

Abstract

The objective of our work is to improve low-temperature fuel cell catalysts by increasing the surface area to augment the efficiency of catalytic reactions. Reduced graphene oxide (rGO) supports were prepared by adding N-containing derivatives of polydopamine (PDA) and loading of Pt and Pt-based metal alloy nanoparticles were accomplished for catalyst preparation. To study the effects of surface modification on catalyst activity, the GO surfaces modified by addition of PDA (PDA-rGO) were richer in oxygen- and nitrogen-containing functional groups, which reduced the number of graphene defects. Reduction of metals (M = Pt, Pd, PtPd where x and y = 1-3) by NaBH produced M/GO (metal on GO) and M/PDA-rGO (metal on PDA-rGO) catalysts. Examination of morphology and chemical composition confirmed that the existence of particle size on M/PDA-rGO catalysts was smaller than that on M/GO catalysts in agreement with calculated electrochemically active surface areas (ECSA). Electrochemical analysis was conducted to evaluate the catalyst activity and stability. The prepared catalysts had significantly greater surface areas as a result of association between the metal nanoparticles and the oxygen and nitrogen functional groups on the rGO supports. The catalysts also exhibited lower onset potentials and greater current intensities, I/I values, and long-term stabilities for methanol and ethanol oxidation compared with those of commercial PtRu/C. Moreover, the diameter of the Nyquist plot of the catalysts on PDA-rGO were smaller than that of the catalysts M/GO. The results suggest that variation of the PtPd atomic ratio on carbon nanocomposites is an encouraging means of enhancing electrocatalytic performance in direct alcohol fuel cell applications.

摘要

我们的工作目标是通过增加表面积来提高低温燃料电池催化剂的效率,从而提高催化反应的效率。通过添加含氮的聚多巴胺(PDA)衍生物制备还原氧化石墨烯(rGO)载体,并完成负载 Pt 和 Pt 基金属合金纳米粒子以制备催化剂。为了研究表面修饰对催化剂活性的影响,通过添加 PDA(PDA-rGO)对 GO 表面进行修饰,使氧和氮含量丰富的官能团增多,减少了石墨烯缺陷的数量。通过 NaBH 还原金属(M=Pt、Pd、PtPd,其中 x 和 y=1-3),得到 M/GO(金属在 GO 上)和 M/PDA-rGO(金属在 PDA-rGO 上)催化剂。形貌和化学组成的检查证实,M/PDA-rGO 催化剂上的颗粒尺寸小于 M/GO 催化剂上的颗粒尺寸,与计算得出的电化学有效表面积(ECSA)一致。进行了电化学分析以评估催化剂的活性和稳定性。由于金属纳米粒子与 rGO 载体上的氧和氮官能团之间的相互作用,制备的催化剂具有更大的表面积。与商业 PtRu/C 相比,这些催化剂在甲醇和乙醇氧化中具有更低的起始电位和更大的电流强度 I/I 值以及更长的稳定性。此外,催化剂在 PDA-rGO 上的奈奎斯特图的直径小于在 M/GO 上的催化剂的直径。结果表明,改变碳纳米复合材料中 PtPd 原子比是提高直接醇燃料电池应用中电催化性能的一种有希望的方法。

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