Unraveling the role of phase engineering in tuning photocatalytic hydrogen evolution activity and stability |
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| Institution: | 1. College of Environmental Science and Engineering, Yangzhou University, Yangzhou 225127, China;2. School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou 225127, China;3. Institute for Energy Research, Jiangsu University, Zhenjiang 212013, China;4. School of Environmental and Chemical Engineering, Jiangsu University of Science and Technology, Zhenjiang 212003, China;5. Joint International Research Laboratory of Agriculture and Agri-Product Safety of Ministry of Education of China, Yangzhou University, Yangzhou 225127, China;6. Jiangsu Collaborative Innovation Center for Solid Organic Waste Resource Utilization, Nanjing 210095, China |
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| Abstract: | In this work, taking NiSe2 as a prototype to be used as cocatalyst in photocatalytic hydrogen evolution, we demonstrate that the crystal phase of NiSe2 plays a vital role in determining the catalytic stability, rather than activity. Theoretical and experimental results indicate that the phase structure shows negligible influence to the charge transport and hydrogen adsorption capacity. When integrating with carbon nitride (CN) photocatalyst forming hybrids (m-NiSe2/CN and p-NiSe2/CN), the hybrids show comparable photocatalytic hydrogen evolution rates (3.26 μmol/h and 3.75 μmol/h). Unlike the comparable catalytic activity, we found that phase-engineered NiSe2 exhibits distinct stability, i.e., m-NiSe2 can evolve H2 steadily, but p-NiSe2 shows a significant decrease in catalytic process (∼57.1% decrease in 25 h). The factor leading to different catalytic stability can be ascribed to the different surface conversion behavior during photocatalytic process, i.e., chemical structure of m-NiSe2 can be well preserved in catalytic process, but partial p-NiSe2 tends to be converted to NiOOH. |
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