Highly Active and Stable Metal Single-Atom Catalysts Achieved by Strong Electronic Metal-Support Interactions,Journal of the American Chemical Society

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Highly Active and Stable Metal Single-Atom Catalysts Achieved by Strong Electronic Metal-Support Interactions
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2019-09-02 , DOI: 10.1021/jacs.9b06482
Junjie Li _{1,

2} , Qiaoqiao Guan _{1,

2} , Hong Wu ₃ , Wei Liu ₄ , Yue Lin ₁ , Zhihu Sun ₄ , Xuxu Ye ₃ , Xusheng Zheng ₄ , Haibin Pan ₄ , Junfa Zhu ₄ , Si Chen ₃ , Wenhua Zhang _{1,

3,

5} , Shiqiang Wei ₄ , Junling Lu _{1,

2,

3}

Affiliation

Developing an active and stable metal single-atom catalyst (SAC) is challenging due to the high surface free energy of metal atoms. In this work, we report that tailoring of the 5d state of Pt1 single atoms on Co3O4 through strong electronic metal-support interactions (EMSI) boosts an activity up to 68-fold higher than those on other supports in dehydrogenation of ammonia borane for room-temperature hydrogen generation. More importantly, this catalyst also exhibit excellent stability against sintering and leaching, in sharp contrast to the rapid deactivation observed on other Pt single-atom and nanoparticle catalysts. Detailed spectroscopic characterization and theoretical calculations revealed that EMSI tailors the unoccupied 5d state of Pt1 single atoms, which modulates the adsorption of ammonia borane and facilities hydrogen desorption, thus greatly leading to the high activity. Such extraordinary electronic promotion was further demonstrated on Pd1/Co3O4, providing a new promising way to design of advanced SACs with high activity and stability.

中文翻译：

通过强电子金属-载体相互作用实现高活性和稳定的金属单原子催化剂

由于金属原子的高表面自由能，开发活性稳定的金属单原子催化剂 (SAC) 具有挑战性。在这项工作中，我们报告说，通过强电子金属-载体相互作用（EMSI）在 Co3O4 上定制 Pt1 单原子的 5d 态，在氨硼烷脱氢中的活性比其他载体高 68 倍。温度制氢。更重要的是，该催化剂还表现出优异的烧结和浸出稳定性，与在其他 Pt 单原子和纳米颗粒催化剂上观察到的快速失活形成鲜明对比。详细的光谱表征和理论计算表明，EMSI 可以调整 Pt1 单原子的未占据 5d 状态，从而调节氨硼烷的吸附并促进氢解吸，从而极大地导致高活性。这种非凡的电子促进在 Pd1/Co3O4 上得到进一步证明，为设计具有高活性和稳定性的先进 SAC 提供了一种新的有前途的方法。

更新日期：2019-09-02

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