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.
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This work was supported by MOE under Academic Research Fund Tier 2 (ARC 19/15; numbers MOE2014-T2-2-093, MOE2015-T2-2-057, MOE2016-T2-2-103 and MOE2017-T2-1-162) and Academic Research Fund Tier 1 (2016-T1-001-147, 2016-T1-002-051, 2017-T1-001-150 and 2017-T1-002-119), and NTU under Start-Up Grant M4081296.070.500000 in Singapore. X.W. acknowledges funding support from the NSFC (21421063 and 21573204) and MOST (2016YFA0200602) of China. P. W. would like to acknowledge funding support from the NSFC (11474147) of China. The authors acknowledge the Facility for Analysis, Characterization, Testing and Simulation, Nanyang Technological University, Singapore for use of electron microscopy (and/or X-ray) facilities.
The authors declare no competing interests.
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Zhang, X., Luo, Z., Yu, P. et al. Lithiation-induced amorphization of Pd3P2S8 for highly efficient hydrogen evolution. Nat Catal 1, 460–468 (2018). https://doi.org/10.1038/s41929-018-0072-y
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