A hierarchical heterostructure of CdS QDs confined on 3D ZnIn 2 S 4 with boosted charge transfer for photocatalytic CO 2
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of Nano-Tech and Nano-Bionics, Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), School of Chemistry and Materials Science, and National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230026, China 2 Hefei National Laboratory for Physical Sciences at the Microscale, Synergetic Innovation Center of Quantum Information and Quantum Physics, Department of Chemical Physics, University of Science and Technology of China, Hefei 230026, China 3 Division of Advanced Nanomaterials, Suzhou Institute of Nano-tech and Nano-bionics, Chinese Academy of Sciences, Suzhou 215123, China 4 Center for Micro and Nanoscale Research and Fabrication, University of Science and Technology of China, Hefei 230026, China § Zezhou Zhu and Xiaoxia Li contributed equally to this work. © Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2020 Received: 9 July 2020 / Revised: 3 August 2020 / Accepted: 7 August 2020
ABSTRACT Metal sulfide based materials as photocatalysts for energy conversion are essential to produce value-added chemical fuels, but their intrinsically slow carrier dynamics and low activity are yet to be resolved. Herein, we developed a unique heterogeneously nanostructured ZnIn2S4-CdS heterostructure that involves zero-dimensional (0D) CdS quantum dots uniformly confined on three-dimensional (3D) ZnIn2S4 nanoflowers, which achieves an excellent catalytic performance of CO2 photoconversion under visible-light irradiation. The obtained hierarchical heterostructure can significantly enhance the light harvesting, shorten the migration distance of carriers, and obviously accelerate the transport of electrons. As evidenced by the ultrafast transient absorption spectroscopy, the formed interface can effectively facilitate charge separation and transport. This work opens up a new avenue to carefully design the elaborate heterostructures for achieving optimal charge separation efficiency by lowering interfacial kinetic barriers and energy losses at the interface.
KEYWORDS photocatalysis, CO2 reduction, charge transfer, hierarchical heterostructure
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Introduction
The overreliance on non-renewable fossil fuels has caused a fast increase in the concentration of carbon dioxide (CO2) in the atmosphere. Given the widely concerned energy crisis and environmental pollution issues, numerous efforts have been made to address this challenge [1–3]. Driven by natural solar energy, photocatalytic conversion CO2 into value-added chemicals/fuels such as CH4, CO and CH3OH could be a promising approach [4–9]. In previous reports, the typical semiconductor-based catalytic materials such as metal oxides TiO2 [10–13], metal sulfides CdS [14–17], and polymers C3N4 [18–22] have been extensively utilized in photoreduction CO2 applications. Despite extensive researches in this field, the CO2 photoreduction still suffers from the poor carrier kinetics and the high photogenerated charge recombination a
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