Lithiation-induced amorphization of Pd3P2S8 for highly efficient hydrogen evolution
Lithiation-induced amorphization of Pd3P2S8 for highly efficient hydrogen evolution
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Pd3P2S8 的锂化诱导非晶化可实现高效析氢
DOI：
10.1038/s41929-018-0072-y
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发表时间：
2018-06
期刊：
影响因子：
37.8
通讯作者：
Zhang H.
中科院分区：
文献类型：
--
作者：
Zhang X.;Luo Z.;Yu P.;Cai Y.;Du Y.;Wu D.;Gao S.;Tan C.;Li Z.;Ren M.;Osipowicz T.;Chen S.;Jiang Z.;Li J.;Huang Y.;Yang J.;Chen Y.;Ang C.Y.;Zhao Y.;Wang P.;Song L.;Wu X.;Liu Z.;Borgna A.;Zhang H.
在原子水平上设计材料结构是调整材料的物理化学性质和优化其在各种潜在应用中性能的一种很有前途的方法。在这里，我们表明，锂诱导的非晶层状晶体Pd3P2S8激活了这种原本具有电化学惰性的材料，作为一种高效的析氢催化剂。层状Pd3P2S8晶体的电化学锂化合成了含有大量空位的非晶态锂掺杂的Pd3P2S8磷化钯纳米点。详细研究了锂离子诱导非晶化过程中的结构变化。非晶态锂掺杂的硫化钯纳米点对析氢反应表现出良好的电催化活性，其起始电位为−52 mV，塔菲尔斜率为29 mV dec−1，并具有良好的长期稳定性。实验和理论研究表明，Pd3P2S8的形貌和结构的调节(如降维、结晶度损失、空位形成和锂掺入)有助于激活其固有的惰性电催化性能。这项工作为材料的结构调整提供了一种独特的途径，可以有效地操纵其催化性能和功能。对非活性材料进行结构修饰以有效地设计活性催化剂是非常有吸引力的。在这里，层状晶体Pd3P2S8通过电化学锂化转变为无定形的锂掺杂纳米点。这一过程将惰性母体材料转化为高度活性和稳定的放氢催化剂。
Engineering material structures at the atomic level is a promising way to tune the physicochemical properties of materials and optimize their performance in various potential applications. Here, we show that the lithiation-induced amorphization of layered crystalline Pd3P2S8 activates this otherwise electrochemically inert material as a highly efficient hydrogen evolution catalyst. Electrochemical lithiation of the layered Pd3P2S8 crystal results in the formation of amorphous lithium-incorporated palladium phosphosulfide nanodots with abundant vacancies. The structure change during the lithiation-induced amorphization process is investigated in detail. The amorphous lithium-incorporated palladium phosphosulfide nanodots exhibit excellent electrocatalytic activity towards the hydrogen evolution reaction with an onset potential of −52 mV, a Tafel slope of 29 mV dec−1 and outstanding long-term stability. Experimental and theoretical investigations reveal that the tuning of morphology and structure of Pd3P2S8 (for example, dimension decrease, crystallinity loss, vacancy formation and lithium incorporation) contribute to the activation of its intrinsically inert electrocatalytic property. This work provides a unique way for structure tuning of a material to effectively manipulate its catalytic properties and functionalities.The structural modification of inactive materials to effectively engineer active catalysts is very attractive. Here, layered crystalline Pd3P2S8 is transformed by electrochemical lithiation into amorphous Li-incorporated nanodots. This process turns the inert parent material into a highly active and stable hydrogen-evolving catalyst.
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影响因子：
10.4
作者：
Wetherell A
通讯作者：
Wetherell A
影响因子：
3
作者：
Grimme, Stefan
通讯作者：
Grimme, Stefan
DOI：
10.1007/978-1-4419-6533-2
发表时间：
1998
期刊：
--
影响因子：
--
作者：
E. Kirkland
通讯作者：
E. Kirkland
影响因子：
3.7
作者：
Kresse, G;Furthmuller, J
通讯作者：
Furthmuller, J
DOI：
10.1016/s0168-583x(03)01003-6
发表时间：
2003-09
影响因子：
1.3
作者：
F. Watt;J. A. Kan;I. Rajta;A. Bettiol;T. F. Choo;M. Breese;T. Osipowicz
通讯作者：
F. Watt;J. A. Kan;I. Rajta;A. Bettiol;T. F. Choo;M. Breese;T. Osipowicz