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In situ construction MoS2-Pt nanosheets on 3D MOF-derived S, N-doped carbon substrate for highly efficient alkaline hydrogen evolution reaction
Chemical Engineering Journal ( IF 15.1 ) Pub Date : 2020-10-29 , DOI: 10.1016/j.cej.2020.127556
Jian Rong , Guoliang Zhu , W. Ryan Osterloh , Yuanyuan Fang , Zhongping Ou , Fengxian Qiu , Karl M. Kadish

Integrating the synergistic effect of multiple components is desirable to optimize catalytic performance of composite electrocatalysts for energy conversion and storage. Herein, the electrocatalytic hydrogen evolution reaction (HER) of a three-dimensional (3D) CuSNC@MoS2-Pt featuring Pt-doped MoS2 nanosheets grown in-situ on S, N-doped carbon substrate (CuSNC) derived from rose-like structured Cu-TCPP MOF (TCPP = 5, 10, 15, 20-tetrakis(4-carboxyphenyl)porphyrin) is investigated. Compared with single MoS2, the synergistic effects of Pt-doping, S, N-doped carbon substrate and 3D open porous structural advantages allow CuSNC@MoS2-Pt to achieve optimum alkaline HER activity with small overpotentials of 102.6, 165.6 and 199.0 mV at current densites of 10, 50 and 100 mA cm−2 respectively, and a small Tafel slope of 55.7 mV dec−1. Spectroscopic techniques and density functional theory calculations reveal that pairing of Pt-doping and S, N-doped carbon substrates in CuSNC@MoS2-Pt effectively reduce the kinetic energy barrier of water dissociation and hydrogen generation, thus improving HER activity. In addition, good hydrophilicity of CuSNC@MoS2-Pt is conducive to achieving rapid mass transport. This work provides a facile strategy for simultaneously integrating structural advantages, electrical conductivity and electronic engineering to construct advanced alkaline HER electrocatalysts.



中文翻译:

在3D MOF衍生的S,N掺杂的碳基质上原位构建MoS 2 -Pt纳米片,以进行高效的碱性氢释放反应

整合多种组分的协同作用对于优化复合电催化剂的能量转化和存储的催化性能是理想的。本文中,三维(3D)CuSNC @ MoS 2 -Pt的电催化氢析出反应(HER),其特征在于原位生长S,N掺杂碳衬底(CuSNC)上的Pt掺杂MoS 2纳米片材,其衍生自玫瑰-类似于结构化的Cu-TCPP MOF(TCPP = 5,10,15,20-四(4-羧基苯基)卟啉)。与单一MoS 2相比,Pt掺杂,S,N掺杂碳衬底和3D开放式多孔结构的协同效应使CuSNC @ MoS 2-Pt分别在10、50和100 mA cm -2的电流密度下实现102.6、165.6和199.0 mV的小过电位,以实现最佳的碱性HER活性,而Tafel斜率在dec -1的小值为55.7 mV 。光谱技术和密度泛函理论计算表明,CuSNC @ MoS 2 -Pt中的Pt掺杂和S,N掺杂碳底物配对有效地减少了水离解和氢生成的动能垒,从而提高了HER活性。另外,CuSNC @ MoS 2具有良好的亲水性-Pt有利于实现快速的大众运输。这项工作为同时整合结构优势,导电性和电子工程技术以构建高级碱性HER电催化剂提供了一种简便的策略。

更新日期:2020-10-29
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