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Amorphous MoS2 nanosheets on MoO2 films/Mo foil as free-standing electrode for synergetic electrocatalytic hydrogen evolution reaction
Affiliation:1. School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang 212013, China;2. School of Pharmacy, Jiangsu University, Zhenjiang 212013, China;1. CAS Key Laboratory of Design and Assembly of Functional Nanostructures, Fujian Provincial Key Laboratory of Nanomaterials, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, 350002, China;2. University of Chinese Academy of Sciences, Beijing, 100049, China;3. Fujian Provincial Key Laboratory of Nanomaterials, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, 350002, China;1. Key Laboratory of Low Dimensional Materials and Application Technology of Ministry of Education, School of Materials Science and Engineering, Xiangtan University, Xiangtan, Hunan, 411105, China;2. School of Management Science and Engineering, Anhui University of Finance & Economics, Bengbu, Anhui, 233030, China;3. Shenzhen Key Laboratory of Nanobiomechanics, Shenzhen Institutes of Advanced Technology, Chinese Academy of Sciences, Shenzhen, 518055, Guangdong, China;4. Department of Materials Science and Engineering, Southern University of Science and Technology, Shenzhen, 518055, Guangdong, China;1. School of Chemistry and Life Science, Advanced Institute of Materials Science, Changchun University of Technology, Changchun 130012, People’s Republic of China;2. State Key Laboratory of Electroanalytical Chemistry, Jilin Province Key Laboratory of Low Carbon Chemical Power, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences 5625 Renmin Street, Changchun, 130022, People’s Republic of China;1. College of Chemistry and Materials Science, The Key Laboratory of Functional Molecular Solids, Ministry of Education, Anhui Normal University, Wuhu 241002, China;2. Center of Single-Atom, Clusters, and Nanomaterials, Anhui Normal University, Wuhu 241002, China;3. Department of Physics and Chemistry, Faculty of Science and Technology, University of Macau, Macao, China;4. School of Chemistry and Chemical Engineering, Anhui University of Technology, Maanshan 243002, China
Abstract:A facile oxidation-sulfidation strategy is proposed to fabricate the vertically aligned amorphous MoS2 nanosheets on MoO2 films/Mo foil (MF) as free-standing electrode, which features as the integration of three merits (high conductivity, abundant exposures of active sites, and enhanced mass transfer) into one electrode for hydrogen evolution reaction (HER). Density functional theory (DFT) calculations reveal the strong interaction between MoS2 and MoO2, which can enhance the intrinsic conductivity with narrow bandgap, and decreases hydrogen adsorption free energy (ΔGH1 = ~0.06 eV) to facilitate the HER process. Benefiting from the unique hierarchical structure with amorphous MoS2 nanosheets on conductive MoO2 films/MF to facilitate the electron/mass transfer by eliminate contact resistance, controllable number of stacking layers and size of MoS2 slabs to expose more edge sites, the optimal MoS2/MoO2/MF exhibits outstanding activity with overpotential of 154 mV at the current density of 10 mA cm?2, Tafel slope of 52.1 mV dec?1, and robust stability. Furthermore, the intrinsic HER activity (vs. ECSA) on MoS2/MoO2/MF is significantly enhanced, which shows 4.5 and 18.6 times higher than those of MoS2/MF and MoO2/MF at overpotential of 200 mV, respectively.
Keywords:Self-supported electrode  Hydrogen evolution reaction  Density functional theory
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