Self-assembled pearl-bracelet-like CoSe2–SnSe2/ CNT hollow architecture as highly efficient electrocatalysts for hydrogen evolution reaction

Self-assembled pearl-bracelet-like CoSe2–SnSe2/ CNT hollow architecture as highly efficient electrocatalysts for hydrogen evolution reaction
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自组装珍珠手链状 CoSe2·SnSe2/ CNT 中空结构作为析氢反应的高效电催化剂

DOI:
10.1039/c7ta08955d
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发表时间:
2017
影响因子:
11.9
通讯作者:
Yuanfu Chen
Yuanfu Chen
中科院分区:
材料科学2区
文献类型:
--
作者:
Bo Yu;Fei Qi;Binjie Zheng;Wenqiang Hou;Wanli Zhang;Yanrong Li;Yuanfu Chen

文献摘要

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首次采用简单的水相反应和硒化工艺合成了一种新型的非贵金属析氢电催化剂--自组装珍珠手镯状CoSe 2-SnSe 2/CNT空心纳米盒(CSCB)。与裸CoSe 2-SnSe 2纳米盒(CSB)相比,CSCB杂化物表现出更快的动力学和更好的HER性能:CSCB的HER机制被改进为Volmer-Tafel组合,而不是Volmer-Heyrovsky组合(如公务员事务局); CSCB的Tafel斜率从74.5 mV dec-1(CSB)急剧下降到32.4 mV dec-1,接近商业Pt/C电催化剂; CSCB混合电路在−250 mV(相对于RHE)下提供35 mA cm−2的超大电流密度,是CSB(0.4 mA cm−2)的85倍以上。此外,CSCB甚至在1500次循环后显示出优异的长期电催化稳定性。CSCB的上级HER性能可归因于其精心设计的具有高电导率和丰富孔隙率的珍珠手镯状中空结构:具有良好机械强度和高电导率的CNT链构建了用于HER期间快速电荷传输的高导电网络;具有大内部空隙和丰富的纳米/介孔的中空CoSe 2-SnSe 2纳米盒提供了丰富的催化活性位点并促进离子扩散。该研究为HER的高效、稳定的非贵过渡金属硫属化合物基电催化剂的合理设计和低成本合成提供了见解。
For the first time, self-assembled pearl-bracelet-like CoSe2–SnSe2/CNT hollow nanoboxes (CSCB), as a novel non-precious electrocatalyst for hydrogen evolution reaction (HER), have been synthesized by a facile aqueous reaction and selenization processes. Compared to bare CoSe2–SnSe2 nanoboxes (CSB), the CSCB hybrid shows much faster kinetics and far better HER performance: the HER mechanism of CSCB is improved to be a Volmer–Tafel combination, instead of Volmer–Heyrovsky combination (as in case of CSB); the Tafel slope of CSCB dramatically decreases from 74.5 mV dec−1 (for CSB) to 32.4 mV dec−1, which nearly approaches to that of the commercial Pt/C electrocatalyst; the CSCB hybrid delivers a very large current density of 35 mA cm−2 at −250 mV vs. RHE, over 85 times larger than that of CSB (0.4 mA cm−2). Furthermore, CSCB shows an excellent long-term electrocatalytic stability even after 1500 cycles. The superior HER performances of CSCB can be attributed to its well-designed pearl-bracelet-like hollow architecture with high conductivity and rich porosity: the CNT chains with a good mechanical strength and high conductivity construct a highly conductive network for fast charge transportation during HER; the hollow CoSe2–SnSe2 nanoboxes with large internal voids and rich nano-/mesopores provide abundant catalytic active sites and facilitate ion-diffusion. This study provides insight into a rational design and low-cost synthesis of the non-precious transition-metal chalcogenide-based electrocatalysts with high efficiency and stability for HER.