催化作用
电催化剂
钴
无机化学
电导率
钼
电解质
材料科学
氧化钴
过渡金属
吉布斯自由能
化学工程
氢燃料
氢
氧化物
纳米颗粒
化学
电化学
纳米技术
电极
物理化学
冶金
热力学
生物化学
物理
有机化学
工程类
作者
Yue Zhang,Wenzhe Zhou,Shanzheng Du,Qi Zhang,Lianwen Deng,Xiaohui Gao,Fangping Ouyang
摘要
The high efficiency of hydrogen evolution reaction (HER) catalysts depends on their electronic structure, conductivity, and intrinsic catalytic activity. Transition-metal oxides (TMO) present a great potential to replace platinum-based catalysts, but further improvements in intrinsic catalytic activity are limited to the materials' conductivity. Herein, theoretical calculations disclosed that the adjusted density of states around the Fermi level caused by Ag introduction increased the conductivity of Co2Mo3O8-Ag, optimizing the water adsorption energy (ΔEad) and Gibbs free energy of hydrogen adsorption (ΔGH*). This can be rationalized through the synergistic effect between electron-rich Co and Mo sites in Co2Mo3O8-Ag. Inspired by this, Ag nanoparticles loaded on Co2Mo3O8 nanosheets (CMO-Ag) as a pH-universal HER catalyst were successfully constructed. As expected, the prepared CMO-Ag catalyst exhibited excellent HER activity with overpotentials of 55.5, 63.2, and 68.2 mV at a current density of 10 mA cm−2 in alkaline, neutral, and acidic electrolyte, respectively, superior to most reported results from molybdenum/cobalt-based electrocatalyst. Meanwhile, the CMO-Ag also presented exceptional stability with negligible change after 20 h of stability tests and 1000 cycles of CV measurements. This work provides a valuable strategy for optimizing catalytic activity sites and improving conductivity through combining metal nanoparticles and TMO, which can be applied for other TMO-based HER pH-universal catalyst.
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