化学
杂原子
催化作用
锌
煅烧
碳纤维
化学工程
聚合物
无机化学
阴极
硫脲
有机化学
复合数
材料科学
物理化学
复合材料
戒指(化学)
工程类
作者
Liying Yang,Jianyang Gao,Min Yuan,Hongdong Li,Yuting Chen,Yunmei Du,Zhenyu Xiao,Kang Liu,Lei Wang
标识
DOI:10.1021/acs.inorgchem.4c00859
摘要
Heteroatom doping and heterostructure construction are the key methods to improve the performance of electrocatalysts. However, developing such catalysts remains a challenging task. Herein, we designed two comparable polymers, phytic acid/thiourea polymer (PATP) and phytic acid/urea polymer (PAUP), as precursors, which contain C, N, S/O, and P by microwave heating. To pinpoint how the introduction of sulfur would affect the electronic structure and catalytic activity, these two polymers were physically blended with CoCo-Prussian blue analogue (CoCo-PBA) and further calcination, respectively. The highly dispersed CoP/Co2P-rich interfacial catalysts anchored on the N,S-codoped or N-doped carbon support were successfully prepared (CoP/Co2P@CNS and CoP/Co2P@CN). The prepared CoP/Co2P@CNS catalyst showed good ORR properties (E1/2 = 0.856 V vs RHE) and OER properties (Ej10 = 1.54 V vs RHE), which were superior to the commercial Pt/C and RuO2 catalysts. The reversible oxygen electrode index (ΔE = Ej10 – E1/2) can reach ∼0.684 V. Meanwhile, the rechargeable zinc–air battery assembled with a CoP/Co2P@CNS catalyst as the air cathode also showed excellent performance, with a charge–discharge cycle stability of up to 900 h. DFT calculations further confirm that the introduction of S atoms can affect the electronic structure and enhance the catalytic activity of C and N atoms on carbon support.
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