Ruthenium Ion-Complexed Graphitic Carbon Nitride Nanosheets Supported on Reduced Graphene Oxide as High-Performance Catalysts for Electrochemical Hydrogen Evolution
Ruthenium Ion-Complexed Graphitic Carbon Nitride Nanosheets Supported on Reduced Graphene Oxide as High-Performance Catalysts for Electrochemical Hydrogen Evolution
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DOI：
10.1002/cssc.201701880
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发表时间：
2018-01-10
期刊：
影响因子：
8.4
通讯作者：
Chen, Shaowei
中科院分区：
文献类型：
--
作者：
Peng, Yi;Pan, Wanzhang;Chen, Shaowei
碳基材料是一种有前途的低成本析氢电催化剂，但其催化性能有待进一步提高。在本研究中，钌离子被引入到石墨化氮化碳/还原氧化石墨烯（rGO）杂化物中，通过Ru-N配位键形成Ru-C3 N4/rGO复合材料。Ru离子的掺入量为1.93at.%，与C3 N4、C3 N4/rGO和Ru-C3 N4相比，其导致材料内的电子重新分布并显著增强HER性能，其中仅-80mV的过电位达到10 mAcm（-2），Tafel斜率为55 mVdec（-1），交换电流密度为0.462mAcm（-2）。这种性能与Pt/C的性能相当，并且归因于复合材料的导带的正位移，其中电荷载流子密度比C3 N4增加约250倍，导致析氢的较低能量势垒。结果表明，在设计和工程的功能性纳米复合材料的有效HER电催化，通过嵌入选择的金属离子到碳基分子骨架的新策略。
Carbon-based materials are promising, low-cost electrocatalysts toward hydrogen evolution reaction (HER), although the catalytic performance needs to be further improved before commercialization. In this study, ruthenium ions are incorporated into graphitic carbon nitride/reduced graphene oxide (rGO) hybrids to form Ru-C3N4/rGO composites through Ru-N coordination bonds. The incorporation of Ru ions, at a loading of 1.93at.%, leads to electron redistribution within the materials and dramatically enhances the HER performance over those of C3N4, C3N4/rGO, and Ru-C3N4, with an overpotential of only -80mV to reach a current density of 10mAcm(-2), a Tafel slope of 55mVdec(-1), and an exchange current density of 0.462mAcm(-2). This performance is comparable to that of Pt/C, and ascribed to the positive shift of the conduction band of the composite, where the charge carrier density increases by a factor of about 250 over that of C3N4, leading to a lower energy barrier for hydrogen evolution. The results suggest a new strategy in the design and engineering of functional nanocomposites for effective HER electrocatalysis by embedding select metal ions into carbon-based molecular skeletons.