期刊
APPLIED SURFACE SCIENCE
卷 596, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apsusc.2022.153574
关键词
Janus-MXenes; Bifunctional atom; Double empty orbitals; First-principles
类别
资金
- Research Grants Council of Hong Kong (CityU) [11306517, 11305919, 11308620]
- NSFC/RGC Joint Research Scheme [N_CityU104/19]
- Hong Kong Research Grant Council Collaborative Research Fund [C6021-19EF]
In this study, high-activity ORR/OER bifunctional catalysts were screened using first-principles calculations. By adjusting the electronic properties of MXenes-based catalysts, the catalytic performance of the catalysts was improved. Additionally, catalysts with ultra-low overpotential for ORR, OER, and ORR/OER reactions were identified, which preferentially adsorb O2 instead of hydrogen.
Developing high-activity and low-cost oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) bifunctional catalysts is strategic to metal-air batteries. Herein, based on the idea that functionalized atoms can adjust the electronic properties of MXenes-based catalysts, we have screened some catalysts with high catalytic activity for ORR/OER using first-principles calculations. Specifically, we firstly explored the stability of Pt doped Ti2CNL ((N = F, Cl, Br and I, L = O, S and Se)) and Ti2CN(L)2 though calculating the vacancy formation energy and binding energy. Moreover, compared the overpotential of Pt doped Ti2CN(L)2 and Ti2CNL for ORR and OER, the Janus-MXenes configurations can tune the d-band center, work-function, density of state (DOS) and charge distribution of the catalysts, and then improve the catalytic performance of catalysts. Pt-VS-Ti2CSBr, Pt-VI-Ti2COI and Pt-VS-Ti2CSBr as ORR, OER and ORR/OER bifunctional catalysts were revealed due to their ultra-low overpotential of 0.35, 0.34 and 0.79 V, respectively. Additionally, compared to H ions, the catalyst preferentially adsorbs O2, thus ensuring the ORR advantage to proceed rather than hydrogen evolution reaction (HER). Even so, Pt-VO-Ti2COI, Pt-VS-Ti2CSI and Pt-VSe-Ti2CSeI have high activity for HER. Our work not only screened out catalysts with encouraging catalytic performance but also guided the design of high-performance catalysts.
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