Insight into the influence of doped oxygen on active sites of molybdenum sulfide materials in hydrogen evolution reaction

Insight into the influence of doped oxygen on active sites of molybdenum sulfide materials in hydrogen evolution reaction
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探究掺杂氧对硫化钼材料析氢反应活性位点的影响

DOI:
10.1016/j.ijhydene.2021.01.019
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发表时间:
2021-01
影响因子:
7.2
通讯作者:
Chen Zheng
Chen Zheng
中科院分区:
工程技术2区
文献类型:
--
作者:
Wu Qikang;Zhu Yuqin;Guo Jiahui;Wang Songrui;Feng Xueqing;Chen Zheng

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二硫化钼作为一种很有前途的电催化析氢反应非贵金属催化剂,受到了广泛的关注。晶态二硫化钼的有限边产生的活性中心是制约其性能的关键。采用有效的合成策略,通过杂原子掺杂来增加二硫化钼的活性中心,已成为活性改进的重点。本文以硫脲和钼酸钠为原料,采用一种简便、高效的方法合成了掺氧硫化钼催化剂。研究发现,通过控制硫脲和钼酸钠的用量比可以调节活性中心的数量。掺杂的氧和丰富的S赋予硫化钼大量的晶格无序或缺陷,从而提供了足够的活性中心。当硫脲和钼酸钠的最佳摩尔比为40:1时,掺氧硫化钼的双层电荷值达到34.14mF/cm~2(玻碳电极上的质量负载量为0.142 mg/cm~2),与电化学活性面积成正比。拉曼光谱和X射线光电子能谱证实了Mo-O键和桥联S22−键的存在,使硫化钼具有大量的晶格无序或缺陷,从而提供了丰富的活性中心。
Molybdenum disulfide has received great attention as a promising non-noble catalyst for electro-catalyzed hydrogen evolution reaction. The active sites originated from the limited edge of crystalline molybdenum disulfide is the key to restrict its HER performance. To increase the active sites of molybdenum disulfide through the heteroatom doping with effective synthetic strategy has become the focus of activity improvement. Herein, a facile and efficient strategy was adopted to synthesize oxygen-doped molybdenum sulfide catalyst by utilizing thiourea and sodium molybdate as precursors. It was found that the number of active sites could be regulated by controlling the dosage ratio of thiourea to sodium molybdate. The doped oxygen and abundant S endows molybdenum sulfide a great deal of lattice disorder or defects, thus providing adequate active sites. When the optimized ratio of thiourea to sodium molybdate (40:1), the double layer value of oxygen-doped molybdenum sulfide reached 34.14 mF/cm2(mass loading on glassy carbon electrode was 0.142 mg/cm2) which is considered to be proportional to the electrochemical active area. Raman spectroscopy and X-ray photoelectron spectroscopy confirmed the presence of Mo–O bond and bridging S22−bonds which endows molybdenum sulfide with a great deal of lattice disorder or defects, thus providing plentiful active sites.
DOI: 10.1039/c9nr09023a
发表时间: 2019-12
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期刊: Applied Catalysis B: Environmental
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