Cooperatively interface role of surface atoms and aqueous media on single atom catalytic property for H 2 O 2 synthesis

• Published in: Journal of colloid and interface science 2022-07, Vol.617, p.752
• Main Authors: Fang, Qiao-Jun, Pan, Jin-Kong, Zhang, Wei, Sun, Fu-Li, Chen, Wen-Xian, Yu, Yi-Fan, Hu, An-Fu, Zhuang, Gui-Lin
• Format: Article
• Language: English
• Subjects: Catalysis; Hydrogen Bonding; Hydrogen Peroxide - chemistry
• ISSN: 1095-7103

Direct electrosynthesis of hydrogen peroxide (H O ) from H and O is a promising alternative to currently industrial Riedl-Pfleiderer route. Utilizing a combination of density functional theory (DFT) and ab-initio-molecular dynamic simulation (AIMD), we presented an effective computational framework to identify the cooperative role of surface atoms(e.g. O, N and S) and aqueous media on catalytic performance of single-atom catalysts (SACs) supported Nb C MXenes. Computational results shown that both Ni/Nb CN and Co/Nb CS have low overpotentials of 0.17 V and 0.20 V, and the barrier of 0.89 eV and 0.67 eV for 2e ORR under gas phase, respectively, while in aqueous phase, hydrogen bond framework on the surface promotes the transfer of proton, resulting in the lower 2e ORR overpotential (0.05 V) in Co/Nb CS and lower barrier (almost 0.01 eV) for rate-determining step (RDS) in Ni/Nb CN . Electronically, we found that the less-electronegativity N and S relative to O more benefit to mediate the activation degree of O on SACs and thereby improve catalytic selectivity. Thus, it is concluded that both surface atom and aqueous medium synergistically promote catalytic property for H O synthesis.