Yang Likang, Li Ze, Chen Chen, Wang Jiasheng, Yin Qizhi, Zhang Yuxiang, Guo Peizhi
Institute of Materials for Energy and Environment, College of Materials Science and Engineering, Qingdao University, Qingdao 266071, P. R. China.
Inorg Chem. 2023 Sep 18;62(37):15320-15328. doi: 10.1021/acs.inorgchem.3c02558. Epub 2023 Sep 5.
Direct alcohol fuel cells are popular due to their high energy density, abundant sources, and ease of transportation and storage. Palladium-based nanosheet self-assembled materials have emerged as an effective catalyst for alcohol oxidation reactions. In this work, nanosheets were synthesized with the same feeding ratio assembly of alloyed PdM (M = Ag, Cu, and Sn). The introduction of the second element was able to enhance the catalytic response of the catalysts to alcohol electrooxidation. Among them, the PdCu alloy exhibited the best performance in terms of catalytic activity, toxicity resistance, and stability to ethanol oxidation reaction (EOR) and methanol oxidation reaction (MOR). The catalytic current densities for EOR can reach 2226, 2518, and 1598 mA mg for PdAg, PdCu, and PdSn nanosheet assemblies, respectively. These are mainly attributed to better electronic effects, altered atomic distances within the cell for the -band centers of Pd, and a larger electrochemical active surface area (ECSA). The optimized -band center is beneficial to promote the catalytic performance of EOR and MOR. Experimental data also demonstrated that higher electrocatalytic temperature, higher pH, and higher alcohol concentration can accelerate the rate of alcohol electrooxidation. These results have the potential to be extended to Pd-M (M = other metals) nanosheets and help for a wider range of catalytic applications.
直接醇类燃料电池因其高能量密度、来源丰富以及易于运输和储存而受到欢迎。钯基纳米片自组装材料已成为醇氧化反应的有效催化剂。在这项工作中，通过合金化的PdM（M = Ag、Cu和Sn）以相同的进料比组装合成了纳米片。第二种元素的引入能够增强催化剂对醇电氧化的催化响应。其中，PdCu合金在催化活性、抗毒性以及对乙醇氧化反应（EOR）和甲醇氧化反应（MOR）的稳定性方面表现出最佳性能。对于PdAg、PdCu和PdSn纳米片组装体，EOR的催化电流密度分别可达2226、2518和1598 mA mg。这些主要归因于更好的电子效应、电池内Pd的能带中心原子间距的改变以及更大的电化学活性表面积（ECSA）。优化后的能带中心有利于促进EOR和MOR的催化性能。实验数据还表明，较高的电催化温度、较高的pH值和较高的醇浓度可以加速醇电氧化的速率。这些结果有可能扩展到Pd-M（M =其他金属）纳米片，并有助于更广泛的催化应用。
