Pang Mingyuan, Yang Min, Yan Jie, Zhang Ben, Zang Lei, Fu Aiping, Guo Peizhi
Institute of Materials for Energy and Environment, College of Materials Science and Engineering, Qingdao University, Qingdao 266071, P. R. China.
College of Chemical Science and Engineering, Qingdao University, Qingdao 266071, P. R. China.
Langmuir. 2022 Apr 12;38(14):4287-4294. doi: 10.1021/acs.langmuir.1c03466. Epub 2022 Apr 1.
Two-dimensional (2D) nanostructured catalysts have attracted great attention in many important fields, including energy applications and chemical industry. In this study, PdCu nanosheet assemblies (NSAs) have been synthesized and investigated as electrocatalysts for direct ethanol fuel cells in an alkaline medium. A great number of active sites on the nanosheets of PdCu NSAs for ethanol electro-oxidation are exposed, where the electron structures are optimized combined with the second element copper. Electrochemical measurements show that PdCu NSA1 exhibits excellent catalytic activity (2536 mA mg) and cyclic stability compared to PdCu NSA2 (1700 mA mg) and PdCu NSA3 (1436 mA mg), much higher than commercial Pd/C. Kinetics studies on the electrolysis of ethanol suggest that PdCu NSAs should be more favorable at higher catalytic temperatures, higher concentrations of ethanol, and low pH value environments. The unique composition and structures PdCu NSA1 would result in the lowest energy barrier in the rate-controlling step of the ethanol oxidation reaction (EOR), confirmed by density functional theory (DFT). The formation mechanism of PdCu NSAs and their excellent electrocatalytic activity toward EOR have been discussed and analyzed.
二维（2D）纳米结构催化剂在包括能源应用和化学工业在内的许多重要领域都引起了极大关注。在本研究中，已合成并研究了钯铜纳米片组装体（NSAs）作为碱性介质中直接乙醇燃料电池的电催化剂。钯铜NSAs纳米片上大量用于乙醇电氧化的活性位点被暴露出来，其中电子结构与第二元素铜结合得到优化。电化学测量表明，与钯铜NSA2（1700 mA mg）和钯铜NSA3（1436 mA mg）相比，钯铜NSA1表现出优异的催化活性（2536 mA mg）和循环稳定性，远高于商业钯碳催化剂。乙醇电解的动力学研究表明，钯铜NSAs在较高催化温度、较高乙醇浓度和低pH值环境下应更具优势。密度泛函理论（DFT）证实，独特的组成和结构的钯铜NSA1在乙醇氧化反应（EOR）的速率控制步骤中会导致最低的能垒。已对钯铜NSAs的形成机理及其对EOR的优异电催化活性进行了讨论和分析。
