催化作用
过电位
化学
水溶液
电负性
密度泛函理论
过氧化氢
双水相体系
Atom(片上系统)
选择性
物理化学
计算化学
有机化学
电化学
嵌入式系统
电极
计算机科学
作者
Qiaojun Fang,Jin-kong Pan,Wei Zhang,Fu-li Sun,Wenxian Chen,Yingda Yu,Anfu Hu,Guilin Zhuang
标识
DOI:10.1016/j.jcis.2022.03.052
摘要
Direct electrosynthesis of hydrogen peroxide (H2O2) from H2 and O2 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 Nb2C MXenes. Computational results shown that both Ni/Nb2CN2 and Co/Nb2CS2 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/Nb2CS2 and lower barrier (almost 0.01 eV) for rate-determining step (RDS) in Ni/Nb2CN2. Electronically, we found that the less-electronegativity N and S relative to O more benefit to mediate the activation degree of O2 on SACs and thereby improve catalytic selectivity. Thus, it is concluded that both surface atom and aqueous medium synergistically promote catalytic property for H2O2 synthesis.
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