当前位置: X-MOL 学术Adv. Sci. › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
Atomically Dispersed Platinum Modulated by Sulfide as an Efficient Electrocatalyst for Hydrogen Evolution Reaction
Advanced Science ( IF 14.3 ) Pub Date : 2021-05-13 , DOI: 10.1002/advs.202100347
Kai Ling Zhou 1 , Chang Bao Han 1 , Zelin Wang 1 , Xiaoxing Ke 1 , Changhao Wang 1 , Yuhong Jin 1 , Qianqian Zhang 1 , Jingbing Liu 1 , Hao Wang 1 , Hui Yan 1
Affiliation  

Catalytically active metals atomically dispersed on supports presents the ultimate atom utilization efficiency and cost-effective pathway for electrocatalyst design. Optimizing the coordination nature of metal atoms represents the advanced strategy for enhancing the catalytic activity and the selectivity of single-atom catalysts (SACs). Here, we designed a transition-metal based sulfide-Ni3S2 with abundant exposed Ni vacancies created by the interaction between chloride ions and the functional groups on the surface of Ni3S2 for the anchoring of atomically dispersed Pt (PtSA-Ni3S2). The theoretical calculation reveals that unique Pt-Ni3S2 support interaction increases the d orbital electron occupation at the Fermi level and leads to a shift-down of the d -band center, which energetically enhances H2O adsorption and provides the optimum H binding sites. Introducing Pt into Ni position in Ni3S2 system can efficiently enhance electronic field distribution and construct a metallic-state feature on the Pt sites by the orbital hybridization between S-3p and Pt-5d for improved reaction kinetics. Finally, the fabricated PtSA-Ni3S2 SAC is supported by Ag nanowires network to construct a seamless conductive three-dimensional (3D) nanostructure (PtSA-Ni3S2@Ag NWs), and the developed catalyst shows an extremely great mass activity of 7.6 A mg−1 with 27-time higher than the commercial Pt/C HER catalyst.

中文翻译:

硫化物调制的原子分散铂作为析氢反应的高效电催化剂

以原子方式分散在载体上的催化活性金属为电催化剂设计提供了最终的原子利用效率和经济高效的途径。优化金属原子的配位性质代表了提高单原子催化剂(SAC)催化活性和选择性的先进策略。在这里,我们设计了一种过渡金属基硫化物-Ni 3 S 2,其具有丰富的暴露的Ni空位,这些空位是由氯离子与Ni3S2表面上的官能团之间的相互作用产生的,用于锚定原子分散的Pt(Pt SA -Ni 3 S 2)。理论计算表明,独特的Pt-Ni 3 S 2支撑相互作用增加了费米能级的d轨道电子占据,导致d带中心下移,从而有力地增强了H 2 O吸附并提供了最佳的H结合位点。将Pt引入Ni 3 S 2体系中的Ni位置可以有效增强电场分布,并通过S-3p和Pt-5d之间的轨道杂化在Pt位点上构建金属态特征,从而改善反应动力学。最后,所制备的Pt SA -Ni 3 S 2 SAC由Ag纳米线网络支撑,构建了无缝导电三维(3D)纳米结构(Pt SA -Ni 3 S 2 @Ag NWs),并且所开发的催化剂表现出极高的催化性能。质量活性高达 7.6 A mg -1,比商用 Pt/C HER 催化剂高 27 倍。
更新日期:2021-06-24
down
wechat
bug