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A Density Functional Theory Study of the Two-Dimensional Bis(iminothiolato)metal Monolayers as Efficient Electrocatalysts for Oxygen Reduction Reaction
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2020-03-27 , DOI: 10.1021/acs.jpcc.9b11890 Guanru Xing 1, 2 , Lin Cheng 1 , Kai Li 2 , Yan Gao 3 , Hao Tang 3 , Ying Wang 2 , Zhijian Wu 2
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2020-03-27 , DOI: 10.1021/acs.jpcc.9b11890 Guanru Xing 1, 2 , Lin Cheng 1 , Kai Li 2 , Yan Gao 3 , Hao Tang 3 , Ying Wang 2 , Zhijian Wu 2
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In recent years, two-dimensional metal–organic frameworks (MOF)-derived heteroatom-doped carbon-based electrocatalysts have drawn extensive attention due to the superior catalytic activity for oxygen reduction reaction (ORR). In this work, the ORR catalytic activity of a series of bis(iminothiolato)metal (TMIT) (TM = Mn, Fe, Co, Ni, Cu, Ru, Rh, Pd, Ir, and Pt) monolayers has been investigated by using the density functional method. The scaling relations are obtained between the Gibbs adsorption free energies of the oxygenated intermediates. The volcano plot of the ORR activity between ΔG*OH and overpotential is established. The results reveal that FeIT possesses the best ORR activity. The predicted overpotential is 0.52 V for FeIT, close to 0.45 V for pure Pt. The migration of an O atom from the S site to the Fe top site is the rate-determining step with an energy barrier of 0.59 eV, smaller than 0.80 eV for pure Pt. This work may provide an effective method for the design of high-performance ORR catalysts by using the two-dimensional MOFs.
中文翻译：
二维双亚氨基硫基金属单分子层作为高效氧还原反应电催化剂的密度泛函理论研究
近年来，二维金属有机骨架（MOF）衍生的杂原子掺杂碳基电催化剂因其对氧还原反应（ORR）的优异催化活性而受到广泛关注。在这项工作中，已经研究了一系列双（亚氨基硫基）金属（TMIT）（TM = Mn，Fe，Co，Ni，Cu，Ru，Rh，Pd，Ir和Pt）单层的ORR催化活性密度泛函法。在氧化中间体的吉布斯吸附自由能之间获得了比例关系。ΔG * OH之间的ORR活性的火山图并建立了超电势。结果表明，FeIT具有最佳的ORR活性。FeIT的预测过电势为0.52 V，纯Pt接近0.45V。O原子从S位向Fe顶端位的迁移是决定速率的步骤，其能垒为0.59 eV，小于纯Pt的0.80 eV。这项工作可以为使用二维MOF设计高性能ORR催化剂提供一种有效的方法。
更新日期：2020-03-27
中文翻译：
二维双亚氨基硫基金属单分子层作为高效氧还原反应电催化剂的密度泛函理论研究
近年来，二维金属有机骨架（MOF）衍生的杂原子掺杂碳基电催化剂因其对氧还原反应（ORR）的优异催化活性而受到广泛关注。在这项工作中，已经研究了一系列双（亚氨基硫基）金属（TMIT）（TM = Mn，Fe，Co，Ni，Cu，Ru，Rh，Pd，Ir和Pt）单层的ORR催化活性密度泛函法。在氧化中间体的吉布斯吸附自由能之间获得了比例关系。ΔG * OH之间的ORR活性的火山图并建立了超电势。结果表明，FeIT具有最佳的ORR活性。FeIT的预测过电势为0.52 V，纯Pt接近0.45V。O原子从S位向Fe顶端位的迁移是决定速率的步骤，其能垒为0.59 eV，小于纯Pt的0.80 eV。这项工作可以为使用二维MOF设计高性能ORR催化剂提供一种有效的方法。
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