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Vertically Aligned MoS2/Mo2C hybrid Nanosheets Grown on Carbon Paper for Efficient Electrocatalytic Hydrogen Evolution
ACS Catalysis ( IF 11.3 ) Pub Date : 2017-09-26 00:00:00 , DOI: 10.1021/acscatal.7b02885 Zhenhuan Zhao 1 , Fan Qin , Sashank Kasiraju , Lixin Xie , Md Kamrul Alam , Shuo Chen , Dezhi Wang , Zhifeng Ren , Zhiming Wang 1 , Lars C. Grabow , Jiming Bao 1
ACS Catalysis ( IF 11.3 ) Pub Date : 2017-09-26 00:00:00 , DOI: 10.1021/acscatal.7b02885 Zhenhuan Zhao 1 , Fan Qin , Sashank Kasiraju , Lixin Xie , Md Kamrul Alam , Shuo Chen , Dezhi Wang , Zhifeng Ren , Zhiming Wang 1 , Lars C. Grabow , Jiming Bao 1
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Maximizing and creating active sites has been a general strategy to increase the performance of a catalyst. Because of the high electrocatalytic hydrogen evolution reactivity (HER) of ultrafine Mo2C nanocrystals and edges of two-dimensional MoS2, an electrode with a synergistic integration of these two nanomaterials is expected to show a better HER performance. Here we report this hybrid nanostructure of vertically aligned MoS2/Mo2C nanosheets on conductive carbon paper. It was revealed that the original structure of MoS2 nanosheets remains intact after the carburization, but the surfaces are incorporated with either Mo2C nanodomains or a heteroatomic mixture of S and C. The hybrid catalyst exhibits a much lower HER overpotential in comparison to those of the corresponding Mo2C and MoS2 alone. Its high activity is congruent with DFT calculations, which show that multiple S and C coordinated Mo sites with near zero Gibbs free energy of hydrogen adsorption exist. Thus, the low overpotential of this binder-free hybrid catalyst is a result of active sites of Mo–S–C and highly dispersed Mo2C nanodomains on the original edges and basal planes of MoS2. Our prediction and realization of active HER sites with this hybrid two-dimensional nanostructure opens up a route toward the development of more active HER catalysts.
中文翻译：
在碳纸上生长的垂直排列的MoS 2 / Mo 2 C杂化纳米片用于高效电催化氢释放
最大化和创建活性位点一直是提高催化剂性能的一般策略。由于超细的Mo 2 C纳米晶体和二维MoS 2的边缘具有很高的电催化放氢反应性（HER），因此有望将具有这两种纳米材料的协同集成的电极显示出更好的HER性能。在这里，我们报告了在导电碳纸上垂直排列的MoS 2 / Mo 2 C纳米片的这种杂化纳米结构。结果表明，MoS 2纳米片的原始结构在渗碳后仍保持完整，但表面均与Mo 2结合在一起。C纳米域或S和C的杂原子混合物。与单独的相应Mo 2 C和MoS 2相比，杂化催化剂表现出低得多的HER超电势。其高活性与DFT计算一致，表明存在多个S和C配位的Mo位，氢吸附的吉布斯自由能接近零。因此，这种无粘合剂的杂化催化剂的低超电势是Mo–S–C的活性位点和MoS 2原始边缘和基面上高度分散的Mo 2 C纳米域的结果。我们对具有这种混合二维纳米结构的活性HER位点的预测和实现为开发更具活性的HER催化剂开辟了一条道路。
更新日期：2017-09-26
中文翻译：
在碳纸上生长的垂直排列的MoS 2 / Mo 2 C杂化纳米片用于高效电催化氢释放
最大化和创建活性位点一直是提高催化剂性能的一般策略。由于超细的Mo 2 C纳米晶体和二维MoS 2的边缘具有很高的电催化放氢反应性（HER），因此有望将具有这两种纳米材料的协同集成的电极显示出更好的HER性能。在这里，我们报告了在导电碳纸上垂直排列的MoS 2 / Mo 2 C纳米片的这种杂化纳米结构。结果表明，MoS 2纳米片的原始结构在渗碳后仍保持完整，但表面均与Mo 2结合在一起。C纳米域或S和C的杂原子混合物。与单独的相应Mo 2 C和MoS 2相比，杂化催化剂表现出低得多的HER超电势。其高活性与DFT计算一致，表明存在多个S和C配位的Mo位，氢吸附的吉布斯自由能接近零。因此，这种无粘合剂的杂化催化剂的低超电势是Mo–S–C的活性位点和MoS 2原始边缘和基面上高度分散的Mo 2 C纳米域的结果。我们对具有这种混合二维纳米结构的活性HER位点的预测和实现为开发更具活性的HER催化剂开辟了一条道路。
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