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通过在金纳米晶上沉积层状 Pt(2+)的转化化学来制备具有增强的甲酸氧化电催化活性的负载型 AuPt 合金纳米晶。

Fabrication of Supported AuPt Alloy Nanocrystals with Enhanced Electrocatalytic Activity for Formic Acid Oxidation through Conversion Chemistry of Layer-Deposited Pt(2+) on Au Nanocrystals.

机构信息

Department of Chemistry, Pohang University of Science and Technology (POSTECH), Pohang, Gyeongbuk, 790-784, Korea.

Department of Chemistry, Chungbuk National University, Cheongju, Chungbuk, 362-763, Korea.

出版信息

Small. 2015 Oct 7;11(37):4884-93. doi: 10.1002/smll.201500947. Epub 2015 Jul 1.

DOI:10.1002/smll.201500947
PMID:26136254
Abstract

The exploitation of nanoconfined conversion of Au- and Pt-containing binary nanocrystals for developing a controllable synthesis of surfactant-free AuPt nanocrystals with enhanced formic acid oxidation (FAO) activity is reported, which can be stably and evenly immobilized on various support materials to diversify and optimize their electrocatalytic performance. In this study, an atomic layer of Pt(2+) species is discovered to be spontaneously deposited in situ on the Au nanocrystal generated from a reverse-microemulsion solution. The resulting Au/Pt(2+) nanocrystal thermally transforms into a reduced AuPt alloy nanocrystal during the subsequent solid-state conversion process within the SiO2 nanosphere. The alloy nanocrystals can be isolated from SiO2 in a surfactant-free form and then dispersedly loaded on the carbon sphere surface, allowing for the production of a supported electrocatalyst that exhibits much higher FAO activity than commercial Pt/C catalysts. Furthermore, by involving Fe3O4 nanocrystals in the conversion process, the AuPt alloy nanocrystals can be grown on the oxide surface, improving the durability of supported metal catalysts, and then uniformly loaded on a reduced graphene oxide (RGO) layer with high electroconductivity. This produces electrocatalytic AuPt/Fe3O4/RGO nanocomposites whose catalyst-oxide-graphene triple-junction structure provides improved electrocatalytic properties in terms of both activity and durability in catalyzing FAO.

摘要

本文报道了利用金和铂二元纳米晶体的纳米受限转化来开发可控合成无表面活性剂的 AuPt 纳米晶体的方法,这种方法可以稳定均匀地固定在各种载体材料上,从而多样化和优化其电催化性能。在这项研究中,发现在 Au 纳米晶体生成的反胶束溶液中,原子层的 Pt(2+) 物种可以自发地原位沉积。所得的 Au/Pt(2+) 纳米晶体在随后的 SiO2 纳米球内的固态转化过程中热转化为还原的 AuPt 合金纳米晶体。可以将无表面活性剂的合金纳米晶体从 SiO2 中分离出来,然后分散地负载在碳球表面上,从而制备出负载型电催化剂,其甲酸氧化(FAO)活性比商业 Pt/C 催化剂高得多。此外,通过将 Fe3O4 纳米晶体引入转化过程中,可以在氧化物表面上生长 AuPt 合金纳米晶体,提高负载型金属催化剂的耐久性,然后均匀地负载在具有高导电性的还原氧化石墨烯(RGO)层上。这产生了电催化 AuPt/Fe3O4/RGO 纳米复合材料,其催化剂-氧化物-石墨烯三结合结构在催化 FAO 方面提供了活性和耐久性方面的改进的电催化性能。

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