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Tweaking Nickel with Minimal Silver in a Heterogeneous Alloy of Decahedral Geometry to Deliver Platinum-like Hydrogen Evolution Activity.
Angewandte Chemie International Edition ( IF 16.6 ) Pub Date : 2020-01-09 , DOI: 10.1002/anie.201913704
Rahul Majee 1 , Arun Kumar 1 , Tisita Das 2 , Sudip Chakraborty 3 , Sayan Bhattacharyya 1
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Five-fold intertwined Agx Ni1-x (x=0.01-0.25) heterogeneous alloy nanocrystal (NC) catalysts, prepared through unique reagent combinations, are presented. With only ca. 5 at % Ag (AgNi-5), Pt-like activity has been achieved at pH 14. To reach a current density of 10 mA cm-2 the extremely stable AgNi-5 requires an overpotential of 24.0±1.2 mV as compared to 20.1±0.8 mV for 20 % Pt/C, both with equal catalyst loading of 1.32 mg cm-2 . The turnover frequency (TOF) is as high as 2.1 H2  s-1 at 50 mV (vs. RHE). Site-specific elemental analyses show the Ag:Ni compositional variation, where the apex and edges of the decahedra are Ag-rich, thereby exposing Ni onto the faces to achieve maximum charge transport for an exceptional pH universal HER activity. DFT calculations elucidate the relative H-atom adsorption capability of the Ni centers as a function of their proximity to Ag atom.

中文翻译:

在十面体几何形状的异相合金中用最少的银微调镍,以提供类似铂的氢析出活性。

介绍了通过独特的试剂组合制备的五倍缠绕的Agx Ni1-x(x = 0.01-0.25)多相合金纳米晶体(NC)催化剂。仅约。Ag(AgNi-5)含量为5 at%时,在pH 14时获得了类似Pt的活性。要达到10 mA cm-2的电流密度,极其稳定的AgNi-5需要24.0±1.2 mV的过电势(相比于20.1)对于20%Pt / C为±0.8 mV,两者均以1.32 mg cm-2的相等催化剂负载。在50 mV(vs. RHE)下,周转频率(TOF)高达2.1 H2 s-1。特定位置的元素分析表明,Ag:Ni的组成变化很大,十足点的顶点和边缘富含Ag,从而将Ni暴露在脸上以实现最大的电荷传输,从而具有出色的pH通用HER活性。
更新日期:2020-01-10
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