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还原氧化石墨烯负载铂钯作为用于高活性和稳定析氢及甲醇氧化反应的双功能电催化剂。

Platinum-palladium-on-reduced graphene oxide as bifunctional electrocatalysts for highly active and stable hydrogen evolution and methanol oxidation reaction.

作者信息

Feng Yingliang, Zhu Lihua, Pei An, Zhang Sifan, Liu Kunming, Wu Fengshun, Li Wenqi

机构信息

Jiangxi Provincial Key Laboratory of Functional Molecular Materials Chemistry, College of Chemistry and Chemical engineering, Faculty of Materials Metallurgy and Chemistry, Jiangxi University of Science and Technology, Ganzhou 341000, Jiang Xi, China.

出版信息

Nanoscale. 2023 Nov 2;15(42):16904-16913. doi: 10.1039/d3nr04014c.

DOI:10.1039/d3nr04014c
PMID:37853801
Abstract

In the context of the gradual depletion of global fossil fuel resources, it is increasingly necessary to explore new alternative energy. Hydrogen energy has attracted great interest from researchers because of its green and pollution-free characteristics. Moreover, the methanol oxidation reaction (MOR) can combine the hydrogen evolution reaction (HER), replacing the anode reaction (oxygen evolution reaction-OER) in overall water splitting and efficiently producing hydrogen. In this study, platinum-palladium nanoparticles on reduced graphene oxide (PtPd/rGO) were successfully synthesized as HER and MOR bifunctional electrocatalysts under alkaline conditions by the stepwise loading of Pt and Pd bimetallic nanoparticles on rGO using a simple liquid-phase reduction method. PtPd/rGO-2 with 0.99 wt% Pt and 2.86 wt% Pd in the HER has the lowest overpotential (87.16 mV at 100 mA cm), with the smallest Tafel slope (18.9 mV dec). The exceptional mass activity of PtPd/rGO-2 in the MOR reaches 10.75 A mg, which is 18.22 and 53.75 times greater than that of commercial Pt/C (Pt/C) and commercial Pd/C (Pd/C), respectively. PtPd/rGO-2 is 0.935 V lower in the coupling reaction of HER and MOR (MOR ∥ HER) compared to the overall water splitting (OER ∥ HER) without methanol (10 mA cm). This is probably because appropriate Pt and Pd loading exposes many more catalytic sites, and the synergistic interaction between Pt, Pd, and Pt-Pd enhances the catalytic performance. This strategy can be used for the synthesis of novel bifunctional electrocatalysts.

摘要

在全球化石燃料资源逐渐枯竭的背景下,探索新的替代能源变得越来越必要。氢能因其绿色无污染的特性而引起了研究人员的极大兴趣。此外,甲醇氧化反应(MOR)可以与析氢反应(HER)相结合,取代全水解中的阳极反应(析氧反应 - OER)并高效制氢。在本研究中,通过简单的液相还原法将铂和钯双金属纳米颗粒逐步负载在还原氧化石墨烯(rGO)上,成功合成了还原氧化石墨烯负载的铂钯纳米颗粒(PtPd/rGO)作为碱性条件下的HER和MOR双功能电催化剂。在HER中,Pt含量为0.99 wt%且Pd含量为2.86 wt%的PtPd/rGO - 2具有最低的过电位(100 mA cm²时为87.16 mV),塔菲尔斜率最小(18.9 mV dec⁻¹)。PtPd/rGO - 2在MOR中的优异质量活性达到10.75 A mg⁻¹,分别是商业Pt/C(Pt/C)和商业Pd/C(Pd/C)的18.22倍和53.75倍。与无甲醇的全水解(OER ∥ HER,10 mA cm²)相比,PtPd/rGO - 2在HER和MOR的耦合反应(MOR ∥ HER)中的电位低0.935 V。这可能是因为适当的Pt和Pd负载量暴露出更多的催化位点,并且Pt、Pd和Pt - Pd之间的协同相互作用增强了催化性能。该策略可用于合成新型双功能电催化剂。

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