Hu Jinwu, Fang Caihong, Jiang Xiaomin, Zhang Deliang, Cui Zhiqing
College of Chemistry and Materials Science, the Key Laboratory of Functional Molecular Solids, Ministry of Education, Anhui Laboratory of Molecular-Based Materials, Center for Nano Science and Technology, Key Laboratory of Electrochemical Clean Energy of Anhui Higher Education Institutes, Anhui Normal University, Wuhu 241000, China.
Inorg Chem. 2022 Jun 20;61(24):9352-9363. doi: 10.1021/acs.inorgchem.2c01257. Epub 2022 Jun 8.
We precisely synthesized two-dimensional (2D) PtPdCu nanostructures with the morphology varying from porous circular nanodisks (CNDs) and triangular nanoplates (TNPs) to triangular nanoboomerangs (TNBs) by tuning the molar ratios of metal precursors. The PtPdCu trimetallic nanoalloys exhibit superior electrocatalytic performances to alcohol oxidation reactions due to their unique structural features and the synergistic effect. Impressively, PtPdCu TNBs exhibit a high mass activity of 3.42 mg and 1.06 A·mg for ethanol and methanol oxidation compared to PtPd, PtCu, and pure Pt, which is 3.93 and 4.07 times that of commercial Pt/C catalysts, respectively. Moreover, 2D PtPdCu TNPs and PtPdCu CNDs also show a highly improved electrocatalytic activity. Furthermore, as all-in-one electrocatalysts, PtPdCu nanoalloys display excellent electrocatalytic activity and stability toward the oxidation of other alcohol molecules, such as isopropyl alcohol, glycerol, and ethylene glycol. The enhanced mechanism was well proposed to be the abundant active sites and upshifted -band center based on density functional theory calculations.
通过调节金属前驱体的摩尔比,我们精确合成了二维(2D)PtPdCu纳米结构,其形态从多孔圆形纳米盘(CND)、三角形纳米板(TNP)到三角形纳米回飞镖(TNB)不等。PtPdCu三金属纳米合金由于其独特的结构特征和协同效应,对醇氧化反应表现出优异的电催化性能。令人印象深刻的是,与PtPd、PtCu和纯Pt相比,PtPdCu TNB对乙醇和甲醇氧化的质量活性分别为3.42 mg和1.06 A·mg,分别是商业Pt/C催化剂的3.93倍和4.07倍。此外,二维PtPdCu TNP和PtPdCu CND也表现出高度提高的电催化活性。此外,作为一体化电催化剂,PtPdCu纳米合金对其他醇分子如异丙醇、甘油和乙二醇的氧化表现出优异的电催化活性和稳定性。基于密度泛函理论计算,提出增强机制是丰富的活性位点和上移的能带中心。