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Tailoring the thickness of MoSe2 layer of the hierarchical double-shelled N-doped carbon@MoSe2 hollow nanoboxes for efficient and stable hydrogen evolution reaction
Journal of Catalysis ( IF 6.5 ) Pub Date : 2019-12-05 00:00:00 , DOI: 10.1016/j.jcat.2019.11.013
Weiheng Chen , Ru Qiao , Changsheng Song , Leihong Zhao , Zhong-Jie Jiang , Thandavarayan Maiyalagan , Zhongqing Jiang

Large-scale production of H2 through water electrolysis is limited by the lack of efficient and crust-abundant low-cost electrocatalysts. Here, MoSe2 and N-doped carbon (NC) is successfully constructed into a double-shelled hierarchical hollow nanobox. The obtained NC@MoSe2 is demonstrated to be an active catalyst for hydrogen evolution reaction (HER). The NC@MoSe2 delicately combine the structural and functional advantages of two-dimensional layered transition metal dichalcogenides (TMDs) and NC, which yield the striking synergistic effect to endow them with extremely enhanced electrochemical activity to efficiently catalyze the evolution of H2. Remarkably, the NC@MoSe2 with the optimum thickness of MoSe2 shell can exhibit a fairly low onset potential of 61 mV, an extremely small overpotential of 164 mV vs. RHE at 10 mA cm−2, a greatly reduced Tafel slope of 55 mV dec−1, and a higher exchange current density of 0.102 mA cm−2. Specifically, this is mainly beneficial from the abundant exposed active edges from the edge-terminated ultrathin MoSe2 nanosheets with small size, the overall hierarchical hollow architecture and strong electronic coupling between MoSe2 and NC layer. Density functional theory (DFT) calculation results have well supported the experimental observations, revealing the strong synergistic effect between NC and MoSe2, thus the increased carrier density around the Fermi level and reduced hydrogen adsorption free energy (ΔGH*) for MoSe2 composited with NC.



中文翻译:

量身定制分层双壳N掺杂碳@ MoSe2空心纳米盒的MoSe2层的厚度,以实现高效,稳定的氢生成反应

通过水电解的大规模生产H 2受到缺乏有效且富含壳的低成本电催化剂的限制。在这里,成功地将MoSe 2和N掺杂碳(NC)构造成双壳分层空心纳米盒。已证明所获得的NC @ MoSe 2是用于氢释放反应(HER)的活性催化剂。NC @ MoSe 2巧妙地结合了二维层状过渡金属二硫代双氰胺(TMDs)和NC的结构和功能优势,产生了显着的协同作用,赋予了它们极大的电化学活性,可以有效地催化H 2的释放。值得注意的是,NC @ MoSe 2与MOSE的最佳厚度2外壳可表现出在10mA厘米61 mV的相当低的开始电位,一个非常小的过电压164 mV对RHE的-2,55毫伏分解的大大减小的塔菲尔斜率-1,和一个更高的交换电流密度为0.102 mA cm -2。具体而言,这主要得益于边缘端接的超薄MoSe 2纳米片的小尺寸,整体分层的中空结构以及MoSe 2和NC层之间的强电子耦合,从而获得了大量暴露的有源边缘。密度泛函理论(DFT)的计算结果很好地支持了实验观察,揭示了NC和MoSe 2之间的强大协同作用,从而增加了费米能级附近的载流子密度,并降低了与NC复合的MoSe 2的氢吸附自由能(ΔGH *)。

更新日期:2019-12-05
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