Abstract
Morphological and structural control of amorphous nanomaterials is challenging due to the long-range disordered atomic arrangements. Herein, we firstly propose a controllable self-hydrolyzing etching-precipitating (SHEP) method to fabricate the regular-shaped amorphous Cu2MoS4 nanocages (a-Cu2MoS4 NCs) with hollow porous structures under ambient conditions. Benefitting from the hollow porous structures and the amorphous characteristics with copious sulfur vacancies, the a-Cu2MoS4 NCs possess more enhanced activity toward hydrogen evolution reaction (HER) than their crystalline counterparts. The octahedral a-Cu2MoS4 NCs with a shell thickness of 20 nm, which balance the appropriate surface porosity and good structural stability, exhibit the best HER activity with a low overpotential of 96 mV at 10 mA cm−2 and a small tafel slope of 61 mV decade−1 in alkaline environment. Moreover, this method is very versatile and can be extended to synthesize other ternary nanocages. Our current work may shed light on the precise controllable synthesis of various ternary nanocages and open a new frontier for developing highly active amorphous catalysts.
摘要
非晶纳米材料因长程无序的原子排列, 其形貌和结构的调控极具挑战性. 本文首次报道了一种可控自水解蚀刻-沉淀(SHEP)法, 在常温常压下即可合成出空心多孔且形貌规则的非晶Cu2MoS4纳米笼(a-Cu2MoS4). 得益于其空心多孔结构和非晶的丰富硫缺陷, a-Cu2MoS4表现出比晶体相对物更强的析氢反应(HER)活性. 其中, 壳厚度为20 nm的八面体a-Cu2MoS4表现出最好的HER活性: 在 10 mA cm−2电流密度下, 过电位仅为96 mV, 塔菲尔斜率低至61 mV decade−1; 这主要是因为a-Cu2MoS4合适的厚度既保证了其表面的多孔性, 又确保了其结构的稳定性. 本文提出的合成方法具有普适性, 可扩展到更多的三元纳米笼材料的合成, 为各种三元纳米笼的精确可控制备提供了新视角, 并为开发高活性非晶催化剂开辟了新的途径.
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This work was financially supported by the National Natural Science Foundation of China (51532001).
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Jian Yu received his BSc and MSc degrees from the School of Environmental and Chemical Engineering, Nanchang Hangkong University in 2012 and 2015, respectively. Now, he is a PhD candidate under the supervision of Prof. Lin Guo in the School of Chemistry, Beihang University. His research interest focuses on the synthesis of hollow porous nanomaterials and their applications in catalysis and energy.
Lin Guo received his PhD degree in Beijing University of Institute of Technology in 1997. Currently, he is a professor in the School of Chemistry, Beihang University. His research interests focus on the development of new methods for the synthesis of nano-structured materials and the characterization of their unique properties with high potential for future applications. He is a member of the Chinese Chemical Society, as well as the vice-dean of the School of Chemistry, Beihang University.
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Morphological and structural engineering in amorphous Cu2MoS4 nanocages for remarkable electrocatalytic hydrogen evolution
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Yu, J., Li, A., Li, L. et al. Morphological and structural engineering in amorphous Cu2MoS4 nanocages for remarkable electrocatalytic hydrogen evolution. Sci. China Mater. 62, 1275–1284 (2019). https://doi.org/10.1007/s40843-019-9431-4
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DOI: https://doi.org/10.1007/s40843-019-9431-4