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In Situ Phase Transformation on Nickel-Based Selenides for Enhanced Hydrogen Evolution Reaction in Alkaline Medium
ACS Energy Letters ( IF 19.3 ) Pub Date : 2020-07-01 , DOI: 10.1021/acsenergylett.0c01385 Lingling Zhai 1 , Tsz Woon Benedict Lo 2 , Zheng-Long Xu 1, 3 , Jonathan Potter 4 , Jiaying Mo 5 , Xuyun Guo 1 , Chiu Chung Tang 4 , Shik Chi Edman Tsang 5 , Shu Ping Lau 1
ACS Energy Letters ( IF 19.3 ) Pub Date : 2020-07-01 , DOI: 10.1021/acsenergylett.0c01385 Lingling Zhai 1 , Tsz Woon Benedict Lo 2 , Zheng-Long Xu 1, 3 , Jonathan Potter 4 , Jiaying Mo 5 , Xuyun Guo 1 , Chiu Chung Tang 4 , Shik Chi Edman Tsang 5 , Shu Ping Lau 1
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Identification of the active species in electrocatalysts toward hydrogen evolution reaction (HER) is of great significance for the development of the catalytic industry; however, it is still the subject of considerable controversy. Herein, we applied operando synchrotron X-ray powder diffraction (SXRD) in the NiSe2 electrocatalyst system, and an in situ phase transformation from cubic NiSe2 to hexagonal NiSe was revealed. The NiSe phase showed an enhanced catalytic activity. Operando Raman spectroscopy verified the decomposition of NiSe2 during HER. Theoretical calculations suggested that the charge transfers from the Se site to Ni site during this evolution process, leading to an increased conductivity and a shifting up of d-band center, which is attributed to the enhanced activity. The generated NiSe phase acts as the “real” active species. Our work unravels the underlying phase transition of the electrocatalyst on reductive conditions in alkaline medium and highlights the significance of identifying the intrinsic active sites under realistic reaction conditions.
中文翻译：
镍基硒化物的原位相变增强碱性介质中的氢释放反应
鉴定电催化剂中发生氢析出反应（HER）的活性物质对于催化工业的发展具有重要意义。但是，它仍然是一个有争议的话题。在本文中，我们在NiSe 2电催化剂体系中应用了操作同步X射线粉末衍射（SXRD），并揭示了从立方NiSe 2到六角形NiSe的原位相变。NiSe相显示出增强的催化活性。Operando拉曼光谱证实了NiSe 2的分解在HER期间。理论计算表明，在此演化过程中，电荷从Se位置转移到Ni位置，导致电导率增加和d谱带中心上移，这归因于活性增强。生成的NiSe相充当“真实”活性物质。我们的工作揭示了碱性介质中还原条件下电催化剂的基本相变，并强调了在实际反应条件下鉴定内在活性位的重要性。
更新日期：2020-08-14
中文翻译：
镍基硒化物的原位相变增强碱性介质中的氢释放反应
鉴定电催化剂中发生氢析出反应（HER）的活性物质对于催化工业的发展具有重要意义。但是，它仍然是一个有争议的话题。在本文中，我们在NiSe 2电催化剂体系中应用了操作同步X射线粉末衍射（SXRD），并揭示了从立方NiSe 2到六角形NiSe的原位相变。NiSe相显示出增强的催化活性。Operando拉曼光谱证实了NiSe 2的分解在HER期间。理论计算表明，在此演化过程中，电荷从Se位置转移到Ni位置，导致电导率增加和d谱带中心上移，这归因于活性增强。生成的NiSe相充当“真实”活性物质。我们的工作揭示了碱性介质中还原条件下电催化剂的基本相变，并强调了在实际反应条件下鉴定内在活性位的重要性。
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