Journal
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
Volume 6, Issue 9, Pages 11502-11510Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.8b01614
Keywords
Hydrogen evolution reaction; Supercritical fluid; Molybdenum dichalcogenides; Solid-solution; Graphene
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Funding
- JSPS KAKENHI [25630353, 15J051979]
- Inter-Graduate School Doctoral Degree Program on Science for Global Safety
- Tohoku University Division for Interdisciplinary Advanced Research and Education
- Research Program for Dynamic Alliance for Open Innovation Bridging Human, Environment and Materials in Network Joint Research Center for Materials and Devices
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The electrocatalytic hydrogen evolution reaction (HER) is known to be an important technique for efficient hydrogen production, and the development of a highly active electrocatalyst with lower overpotential is a key issue. In this study, we demonstrated the rapid, one-pot synthesis of highly active molybdenum dichalcogenide/reduced graphene oxide (Mo(S,Se)/rGO) electrocatalysts from cost-effective and environmentally friendly substances using reductive supercritical conditions. We found that edge-rich MoS2 is synthesized under a high-density ethanol condition and successfully controlled the composition of molybdenum dichalcogenide (MoS2-xSex) nanoflowers at the atomic level by varying the ratio of chalcogen sources. The electrocatalytic HER activity increased with the formation of an edges-rich structure and a solid solution of MoS2 and MoSe2, and by complexing with graphene. The synthesized MoS0.9Se1.1/graphene showed excellent HER properties that can be categorized into the highest-activity group of the previously reported molybdenum dichalcogenide and its composite. Such high electrocatalytic HER performance should be the result of optimizing the hydrogen adsorption free energy of MoS2-xSex and effectively forming conductive paths between MoS0.9Se1.1 and graphene. This rapid one-pot process using supercritical ethanol will be suitable for the mass production of highly active molybdenum dichalcogenide electrocatalysts.
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