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通过辐射技术调控非晶态硫化钼/炭黑纳米复合材料的组成与结构以实现高效析氢

Tuning the Composition and Structure of Amorphous Molybdenum Sulfide/Carbon Black Nanocomposites by Radiation Technique for Highly Efficient Hydrogen Evolution.

作者信息

Cao Pengfei, Peng Jing, Liu Siqi, Cui Yu, Hu Yang, Chen Bo, Li Jiuqiang, Zhai Maolin

机构信息

Beijing National Laboratory for Molecular Sciences, Radiochemistry and Radiation Chemistry Key Laboratory of Fundamental Science, the Key Laboratory of Polymer Chemistry and Physics of the Ministry of Education, College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, China.

出版信息

Sci Rep. 2017 Nov 22;7(1):16048. doi: 10.1038/s41598-017-16015-y.

Abstract

Amorphous molybdenum sulfide/carbon black (MoS/C) nanocomposites are synthesized by a facile one-step γ-ray radiation induced reduction process. Amorphous MoS shows better intrinsic activity than crystalline MoS. And the composition and amorphous structure of MoS could be expediently tuned by absorbed dose for excellent catalytic activity. Meanwhile, the addition of carbon black leads to a significant decrease of charge transfer resistance and increase of active sites of MoS/C composite. Consequently, MoS/C nanocomposite shows Pt-like catalytic activity towards hydrogen evolution reaction (HER), which requires an onset over potential of 40 mV and over potential of 76 mV to achieve a current density of 10 mA cm, and the corresponding Tafel slope is 48 mV decade. After 6000 CV cycles, the catalytic activity of MoS/C shows no obvious decrease. However, when platinum (Pt) foil is used as counter electrode, MoS/C composite show better catalytic activity abnormally after long-term cycling tests. The dissolution of Pt was observed in HER and the Pt dissolution mechanism is elucidated by further analyzing the surface composition of after-cycling electrodes, which offers highly valuable guidelines for using Pt electrode in HER.

摘要

通过简便的一步γ射线辐射诱导还原过程合成了非晶态硫化钼/炭黑(MoS/C)纳米复合材料。非晶态MoS表现出比晶态MoS更好的本征活性。并且MoS的组成和非晶态结构可以通过吸收剂量方便地调节以获得优异的催化活性。同时,炭黑的加入导致MoS/C复合材料的电荷转移电阻显著降低且活性位点增加。因此,MoS/C纳米复合材料对析氢反应(HER)表现出类铂催化活性,达到10 mA cm的电流密度需要40 mV的起始过电位和76 mV的过电位,相应的塔菲尔斜率为48 mV/decade。经过6000次循环伏安(CV)循环后,MoS/C的催化活性没有明显下降。然而,当使用铂(Pt)箔作为对电极时,MoS/C复合材料在长期循环测试后异常地表现出更好的催化活性。在HER中观察到了Pt的溶解,并通过进一步分析循环后电极的表面组成阐明了Pt的溶解机制,这为在HER中使用Pt电极提供了非常有价值的指导。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c30a/5700052/f87e552f9658/41598_2017_16015_Fig1_HTML.jpg

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