对质子还原具有增强的电催化活性的3D-2D碳nanohorn-MoS2异质结构的受控化学官能化
Controlled chemical functionalization toward 3D-2D carbon nanohorn-MoS2 heterostructures with enhanced electrocatalytic activity for protons reduction
摘要：
从纳米材料的组合产生的新型异质结构的实现是一种有效的方式来修改其物理化学和电催化性能，使他们增强的特性源于他们的个别成分。碳纳米角（CNH）具有高的孔隙率、大的比表面积和良好的导电性，而MoS 2具有多个电催化活性位点，但缺乏显著的导电性、强的相互作用和有效的结构，这可能是一种促进质子电催化还原为分子氢的策略。在本文中，我们以逐步的方法在CNH的圆锥尖端和侧壁以及MoS 2的基面处共价引入互补官能团，从而构建3D-2D CNH-MoS 2异质结构。增加的MoS 2负载到CNH上，改善和促进邻近CNH中的电荷离域和转移，以及过多的活性位点，导致与商业Pt/C相同的优异的质子还原电催化活性。该异质结构的析氢过电位为0.029 V，Tafel斜率为71 mV/dec，电荷转移电阻为34.5 Ω，具有很小的电催化活性。此外，3D-2D CNH-MoS 2异质结构的稳定性在进行10，000次持续电催化循环后得到验证。
英文摘要：
The realization of novel heterostructures arising from the combination of nanomaterials is an effective way to modify their physicochemical and electrocatalytic properties, giving them enhanced characteristics stemming from their individual constituents. Interfacing carbon nanohorns (CNHs) possessing high porosity, large specific surface area and good electrical conductivity, with MoS2 owning multiple electrocatalytic active sites but lacking significant conductivity, robust interactions and effective structure, can be a strategy to boost the electrocatalytic reduction of protons to molecular hydrogen. Herein, we covalently introduce, in a stepwise approach, complementary functional groups at the conical tips and sidewalls of CNHs, along with the basal plane of MoS2, en route the construction of 3D-2D CNH-MoS2 heterostructures. The increased MoS2 loading onto CNHs, improving and facilitating charge delocalization and transfer in neighboring CNHs, along with the plethora of active sites, results in excellent electrocatalytic activity for protons reduction same to that of commercial Pt/C. We have registered minute overpotential, low Tafel slope and small charge-transfer resistance for electrocatalyzing the evolution of hydrogen from the newly prepared heterostructure of 0.029 V, 71 mV/dec and 34.5 Ω, respectively. Furthermore, the stability of the 3D-2D CNH-MoS2 heterostructure was validated after performing 10,000 ongoing electrocatalytic cycles.
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