Zhu Zhiqiang, Liu Feng, Fan Jinchen, Li Qiaoxia, Min Yulin, Xu Qunjie
Shanghai Key Laboratory of Materials Protection and Advanced Materials in Electric Power, College of Environmental and Chemical Engineering Shanghai University of Electric Power, Yangpu District, 2588 Changyang Road, Shanghai 200090, China.
Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200090, China.
ACS Appl Mater Interfaces. 2020 Nov 25;12(47):52731-52740. doi: 10.1021/acsami.0c16215. Epub 2020 Nov 10.
The exploration of ternary Pt-based catalysts represents a new trend for the application of electrocatalysts in fuel cells. In the present study, intermetallic PtPbBi hexagonal nanoplates (HNPs) with a hexagonal close-packed structure have been successfully synthesized via a facile solvothermal synthesis approach. The optimized PtPbBi HNPs exhibited excellent mass activity in the ethanol oxidation reaction (8870 mA mg) in an alkaline ethanol solution, which is 12.7 times higher than that of JM Pt/C. Meanwhile, the mass activity of PtPbBi HNPs in an ethylene glycol solution (10,225 mA mg) is 1.85 times higher than that of JM Pt/C. In particular, its catalytic activity is better than that of most reported Pt-based catalysts. In addition, the optimized PtPbBi HNPs also show a better operational durability than commercial Pt/C. For the ethylene glycol oxidation reaction, a mass activity of 42.7% was retained even after a chronoamperometric test for 3600 s, which is rare among the reported Pt-based catalysts. By combining X-ray photoelectron spectroscopy and electrochemical characterization, we reveal the electron transfer between Pt, Pb, and Bi; this would lead to weakened CO adsorption and enhanced OH adsorption, thereby promoting the removal of toxic intermediates and ensuring that PtPbBi HNP samples have high activity and excellent stability. This work can inspire the design and synthesis of Pt-based nanocatalysts.
探索基于铂的三元催化剂代表了电催化剂在燃料电池中应用的新趋势。在本研究中，通过简便的溶剂热合成方法成功合成了具有六方密堆积结构的金属间化合物PtPbBi六角纳米片（HNPs）。优化后的PtPbBi HNPs在碱性乙醇溶液中的乙醇氧化反应中表现出优异的质量活性（8870 mA mg），比JM Pt/C高12.7倍。同时，PtPbBi HNPs在乙二醇溶液中的质量活性（10225 mA mg）比JM Pt/C高1.85倍。特别是，其催化活性优于大多数已报道的基于铂的催化剂。此外，优化后的PtPbBi HNPs还表现出比商业Pt/C更好的操作耐久性。对于乙二醇氧化反应，即使在进行3600 s的计时电流测试后，仍保留了42.7%的质量活性，这在已报道的基于铂的催化剂中是罕见的。通过结合X射线光电子能谱和电化学表征，我们揭示了Pt、Pb和Bi之间的电子转移；这将导致CO吸附减弱和OH吸附增强，从而促进有毒中间体的去除，并确保PtPbBi HNP样品具有高活性和优异的稳定性。这项工作可以启发基于铂的纳米催化剂的设计和合成。
