Atomically Dispersed CoN3C1-TeN1C3 Diatomic Sites Anchored in N-Doped Carbon as Efficient Bifunctional Catalyst for Synergistic Electrocatalytic Hydrogen Evolution and Oxygen Reduction

被引:0
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作者
Wang, Minmin [1 ]
Zheng, Xiuhui [1 ]
Li, Min [1 ]
Sun, Kaian [2 ]
Liu, Chuhao [2 ]
Cheong, Weng-Chon [2 ]
Liu, Zhi [1 ]
Chen, Yanju [1 ]
Liu, Shoujie [2 ]
Wang, Bin [3 ]
Li, Yanpeng [1 ]
Liu, Yunqi [1 ]
Liu, Chenguang [1 ]
Feng, Xiang [1 ]
Yang, Chaohe [1 ]
Pan, Yuan [1 ]
Chen, Chen [2 ]
机构
[1] China Univ Petr East China, State Key Lab Heavy Oil Proc, Qingdao 266580, Peoples R China
[2] Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
[3] Shaanxi Normal Univ, Sch Chem & Chem Engn, Xian 710119, Peoples R China
关键词
bifunctional catalysts; diatomic active sites; electrochemistry; encapsulation-adsorption-pyrolysis strategy; extended X-ray absorption fine structure (EXAFS);
D O I
暂无
中图分类号
P9 [自然地理学]; K9 [地理];
学科分类号
0705 ; 070501 ;
摘要
A encapsulation-adsorption-pyrolysis strategy for the construction of atomically dispersed Co-Te diatomic sites (DASs) that are anchored in N-doped carbon is reported as an efficient bifunctional catalyst for electrocatalytic hydrogen evolution reaction (HER) and oxygen reduction reaction (ORR). The as-constructed catalyst shows the stable CoN3C1-TeN1C3 coordination structure before and after HER and ORR. The *OOH/*H intermediate species are captured by in situ Raman and in situ attenuated total reflectance-surface enhanced infrared absorption spectroscopy, indicating that the reactant O-2/H2O molecule has a strong interaction with the Co site, revealing that Co delta+ is an effective active site. Theoretical calculations show that the Co delta+ has adsorption-activation function and the neighboring Te delta+ acts as an electron donor adjusting the electronic structure of Co delta+, promoting the dissociation of H2O molecules and the adsorption of H and oxygen-containing intermediates in HER and ORR. In the meanwhile, the nearest C atom around Co also profoundly affects the adsorption of H atoms. This results in the weakening of the OH adsorption and enhancement of H adsorption, as well as the more stable water molecule dissociation transition state, thus significantly boosting ORR and HER performance.
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页数:12
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