Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 13, Issue 30, Pages 35818-35827Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c09651
Keywords
bicrystalline 1T/2H-MoS2; water splitting; electronic interaction; Z-scheme heterojunction; H2O reactant adsorption
Funding
- National Natural Science Foundation of China [21876078, 21707066]
- Major Science and Technology Program for Water Pollution Control and Treatment [2017ZX07204004]
- Scientific Research Foundation of Graduate School of Nanjing University [2018CL01]
- Australia Research Council [DE210100253]
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By developing an innovative hybrid photocatalyst, this study has achieved high charge separation efficiency and superior hydrogen evolution rate through optimal structure and phase engineering. The design provides a new approach for solar energy conversion.
Developing all-solid-state Z-scheme systems with highly active photocatalysts are of huge interest in realizing long-term solar-to-fuel conversion. Here we reported an innovative hybrid of {110}oriented CeO2 nanorods with edge-enriched bicrystalline 1T/2H-MoS2 coupling as efficient photocatalysts for water splitting. In the composites, the metallic 1T phase acts as an excellent solid state electron mediator in the Z-scheme, while the 2H phase and CeO2 are the adsorption sites of the photosensitizer and reactant (H2O), respectively. Through optimal structure and phase engineering, 1T/2H-MoS2@CeO2 heterojunctions simultaneously achieve high charge separation efficiency, proliferated density of exposed active sites, and excellent affinity to reactant molecules, reaching a superior hydrogen evolution rate of 73.1 mu mol/h with an apparent quantum yield of 8.2% at 420 nm. Furthermore, density functional theory calculations show that 1T/2H-MoS2@CeO2 possesses the advantages of intensive electronic interaction from the built-in electric field (negative MoS2 and positive charged CeO2) and reduced H2O adsorption/dissociation energies. This work sheds light on the design of on-demand noble-metal-free Z-scheme heterostructures for solar energy conversion.
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