Dual Charge-Transfer Channels Harmonize Carrier Separation for Efficient U(VI) Photoreduction.
Pan He, Ling Zhang, Shunhong Xiao, Wenyi Jiang, Yiquan Wu, Chenhui Yan, Xiaoan Li, Zhengguo Chen, Linzhen Wu, Tao Duan
Author Information
Pan He: State Key Laboratory of Environment-friendly Energy Materials, National Co-innovation Center for Nuclear Waste Disposal and Environmental Safety, Southwest University of Science and Technology, Mianyang, Sichuan 621010, China.
Ling Zhang: State Key Laboratory of Environment-friendly Energy Materials, National Co-innovation Center for Nuclear Waste Disposal and Environmental Safety, Southwest University of Science and Technology, Mianyang, Sichuan 621010, China.
Shunhong Xiao: State Key Laboratory of Environment-friendly Energy Materials, National Co-innovation Center for Nuclear Waste Disposal and Environmental Safety, Southwest University of Science and Technology, Mianyang, Sichuan 621010, China.
Wenyi Jiang: State Key Laboratory of Environment-friendly Energy Materials, National Co-innovation Center for Nuclear Waste Disposal and Environmental Safety, Southwest University of Science and Technology, Mianyang, Sichuan 621010, China.
Yiquan Wu: State Key Laboratory of Environment-friendly Energy Materials, National Co-innovation Center for Nuclear Waste Disposal and Environmental Safety, Southwest University of Science and Technology, Mianyang, Sichuan 621010, China.
Chenhui Yan: State Key Laboratory of Environment-friendly Energy Materials, National Co-innovation Center for Nuclear Waste Disposal and Environmental Safety, Southwest University of Science and Technology, Mianyang, Sichuan 621010, China.
Xiaoan Li: NHC Key Laboratory of Nuclear Technology Medical Transformation, Mianyang Central Hospital, Mianyang, Sichuan 621099, China.
Zhengguo Chen: NHC Key Laboratory of Nuclear Technology Medical Transformation, Mianyang Central Hospital, Mianyang, Sichuan 621099, China.
Linzhen Wu: State Key Laboratory of Environment-friendly Energy Materials, National Co-innovation Center for Nuclear Waste Disposal and Environmental Safety, Southwest University of Science and Technology, Mianyang, Sichuan 621010, China.
Tao Duan: State Key Laboratory of Environment-friendly Energy Materials, National Co-innovation Center for Nuclear Waste Disposal and Environmental Safety, Southwest University of Science and Technology, Mianyang, Sichuan 621010, China. ORCID
The low efficient transfer of photogenerated electrons to an active catalytic site is a pivotal problem for the photoreduction of highly soluble hexavalent uranium [U(VI)] to low soluble tetravalent uranium [U(IV)]. Herein, we successfully synthesized a TiO/1T-MoS/reduced graphene oxide heterojunction (TTMR) with dual charge-transfer channels by exploiting the difference in Fermi levels between the heterojunction interfaces, which induced multilevel separation of photogenerated carriers. Theoretical and experimental results demonstrate that the presence of the electron buffer layer promoted the efficient migration of photogenerated electrons between the dual charge-transfer channels, which achieved effective separation of photogenerated carriers in physical/spatial dimensions and significantly extended the lifetime of photogenerated electrons. The migration of photogenerated electrons to the active catalytic site after multilevel spatial separation enabled the TTMR dual co-photocatalyst to remove 97.4% of the high concentration of U(VI) from the liquid-phase system within 80 min. This work provides a practical reference for utilizing multiple co-catalysts to accomplish directed spatial separation of photogenerated carriers.
