Modulating the intrinsic properties of platinum-cobalt nanowires for enhanced electrocatalysis of the oxygen reduction reaction

被引:8
作者
Chang, Fangfang [1 ]
Liu, Yongpeng [1 ]
Yang, Lin [1 ]
Zhang, Qing [1 ]
Wei, Juncai [1 ]
Wang, Xiaolei [2 ]
Bai, Zhengyu [1 ]
机构
[1] Henan Normal Univ, Collaborat Innovat Ctr Henan Prov Green Mfg Fine, Sch Chem & Chem Engn, Key Lab Green Chem Media & React,Minist Educ, Xinxiang 453007, Henan, Peoples R China
[2] Univ Alberta, Dept Chem & Mat Engn, Edmonton, AB T6G 1H9, Canada
基金
美国国家科学基金会;
关键词
ALLOY NANOWIRES; CATALYSTS; SYNERGY; FACETS; STRAIN;
D O I
10.1039/d2nj01146h
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The ability to improve the intrinsic activity of nanoalloy electrocatalysts is essential for designing highly efficient electrocatalysts by optimizing the basic physical properties of the nanoalloy. This report describes that the electrocatalytic performance of ultrathin PtnCo100-n alloy nanowires (PtnCo100-n NWs) toward the oxygen reduction reaction (ORR) is enhanced by regulating the lattice strain, highly active facets, and the electronic structure of the alloy, which can be achieved by optimizing the ratio of platinum-to-cobalt in alloys. The catalyst of PtnCo100-n nanoalloy NWs features subtle lattice strain and (111) facets. The electrochemical results show excellent activity and durability toward ORR at a Pt : Co ratio of similar to 70 : 30, which suggests compressively-strained single-phase alloy state revealed by X-ray diffraction (XRD) results. The correlation of facets, lattice strain, electronic structure, and activity is evaluated by the theoretical model based on the density functional theory (DFT) calculations of nanoalloy clusters, which show electron transfer from the PtCo alloy to oxygen. There is a relatively low energy difference between the HOMO of the PtCo nanoalloy and the LUMO of oxygen as the Pt : Co atom ratio is 70 : 30. By analyzing the adsorption of OH, O, and OOH intermediates on the surface of PtCo(111) facets of different compositions, it is observed that the adsorption energy of the Pt2Co8 cluster (Pt : Co20 : 80) is the strongest, resulting in low activity. Interestingly, the adsorption energy of the Pt7Co3 cluster is between that of the Pt6Co4 and Pt-10 cluster, which is thought to be related to the highest catalytic activity of the nanoalloy when the Pt : Co atom ratio is similar to 70 : 30. This finding will provide a new strategy for studying the relationship between the structure and the catalytic activity of nanocatalysts.
引用
收藏
页码:8122 / 8130
页数:9
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