Photocatalytic CO2 reduction (CO2RR) is particularly attractive due to its ability to directly harvest solar energy, representing a promising and sustainable route toward carbon neutrality. All-inorganic halide perovskite nanocrystals, such as CsPbBr3, have emerged as highly promising photocatalysts owing to their exceptional electronic and optical properties. In this work, Cu-atom-doped CsPbBr3 perovskite nanocrystals (Cu-CsPbBr3 PNCs) were successfully developed, and the role of the Cu single atom in CsPbBr3 PNCs for modulating their photocatalytic CO2RR was elucidated. Comprehensive structural characterizations, including X-ray diffraction (XRD), high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), and X-ray absorption spectroscopy (XAS), collectively confirm that the Cu element is atomically distributed as single atoms uniformly within the nanocrystal lattice rather than undergoing phase segregation into clusters or long-range-ordered Cu phases. A slight red shift of the Cu K-edge XANES under illumination was found, indicating a partial reduction of Cu2+ in Cu-CsPbBr3 PNCs. The results represented the occurrence of photoexcited electron transfer from CsPbBr3 to the doped Cu sites during the CO2RR. Moreover, photocatalytic CO2RR revealed that an optimal Cu-doping concentration in Cu-CsPbBr3 PNCs achieves a significantly enhanced CO production rate of 2.80 μmol g-1 h-1, outperforming pristine CsPbBr3 (1.47 μmol g-1 h-1). Time-resolved photoluminescence (TRPL) measurements show a substantial decrease in carrier lifetime from 3.17 ns (pristine CsPbBr3 PNCs) to 0.72 ns (optimal Cu-CsPbBr3 PNCs), evidencing efficient electron trapping by single Cu single atoms. Transient absorption (TA) spectra further reveal modified hot-carrier dynamics and pronounced carrier-trapping behavior. Overall, the enhanced photocatalytic activity of Cu-CsPbBr3 PNCs toward CO2 reduction is attributed to efficient nonradiative charge transfer from photoexcited CsPbBr3 PNCs to the dopant Cu atoms. This design strategy opens a general avenue for the development of metal-atom-doped perovskite-based photocatalysts with improved efficiency for the CO2 reduction reaction.
Building similarity graph...
Analyzing shared references across papers
Loading...
Kuan‐Chang Wu
Yu‐Dian Chen
Yi-Chia Chen
The Journal of Physical Chemistry Letters
Indian Institute of Technology Roorkee
Academia Sinica
Taipei Medical University
Building similarity graph...
Analyzing shared references across papers
Loading...
Wu et al. (Sat,) studied this question.
www.synapsesocial.com/papers/69e7138bcb99343efc98d014 — DOI: https://doi.org/10.1021/acs.jpclett.6c00748