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Anchoring palladium nanoparticles on CsPbBr3 perovskite nanocrystals for enhanced photocatalytic CO2 reduction

通过锚定钯纳米颗粒在CsPbBr3钙钛矿纳米晶体上从而增强光催化CO2还原

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Abstract

Recently, all-inorganic cesium lead halide (CsPbX3 (X = Cl, Br, and I) perovskite nanocrystals (NCs) have been extensively investigated for photocatalytic carbon dioxide (CO2) reduction reaction (CO2RR). However, because the pristine CsPbX3 NCs suffer from severe radiative recombination, it is imperative to elaborately design heterostructures to separate electron-hole pairs for achieving efficient CO2RR. Herein, palladium (Pd) nanoparticles (NPs) are anchored on CsPbBr3 NCs by a photo-assisted approach for the first time. The as-prepared CsPbBr3@Pd NCs not only build Schottky junctions at the CsPbBr3/Pd interfaces that promote the carrier separation and suppress the radiative recombination, but also exhibit lower energy barriers for photocatalytic CO2RR than pristine CsPbBr3 NCs according to the density functional theory calculations. The electron consumption rate reaches a striking peak of 46.2 µmol g−1 h−1 by using CsPbBr3@Pd NCs as photocatalysts for CO2RR, which is 4.8-fold of the counterpart of pristine CsPbBr3 NCs. This work not only presents a photo-assisted strategy for anchoring Pd NPs on CsPbBr3 NCs, but also demonstrates the great potential of using CsPbBr3@Pd NCs for photocatalytic CO2RR.

摘要

最近, 全无机铯铅溴(CsPbX3 (X = Cl, Br, I))钙钛矿纳米晶体被广泛应用于光催化CO2还原(CO2RR)领域. 但是, 由于纯CsPbX3纳米晶体内部载流子辐射复合严重, 所以精心设计基于CsPbX3纳米晶体的异质结构对于分离载流子和实现高效的CO2RR是非常重要的. 本文中, 我们介绍了利用光辅助的方法将Pd纳米颗粒锚定在CsPbX3纳米晶体上. 利用此方法所制备的CsPbBr3@Pd纳米晶体通过在CsPbBr3/Pd界面处构建肖特基结从而促进了载流子的分离并抑制了辐射复合. 第一性原理计算表明: 在CO2RR过程中, CsPbBr3@Pd纳米晶体比纯CsPbX3纳米晶体具有更低的能量势垒. 当CsPbBr3@Pd纳米晶体被用作CO2RR催化剂时, 电子消耗速率高达46.2 µmol g−1 h−1, 是纯CsPbX3纳米晶体作为光催化剂时电子消耗速率的4.8倍. 这项工作不仅介绍了一种利用光辅助将钯纳米颗粒锚定在CsPbX3纳米晶体上的方法, 而且还证明了CsPbBr3@Pd纳米晶体在光催化CO2还原领域的巨大潜能.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (61904023 and 11974063) and the Natural Science Foundation of Chongqing (cstc2019jcyj-bshX0078).

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Authors and Affiliations

  1. Key Laboratory of Optoelectronic Technology & Systems (Ministry of Education), Chongqing University, Chongqing, 400044, China

    Hongbin Xiao  (肖红彬), Qingkai Qian  (钱庆凯) & Zhigang Zang  (臧志刚)

  2. School of Chemistry and Chemical Engineering, Chongqing University, Chongqing, 400044, China

    Hongbin Xiao  (肖红彬)

Authors
  1. Hongbin Xiao  (肖红彬)
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  2. Qingkai Qian  (钱庆凯)
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  3. Zhigang Zang  (臧志刚)
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Contributions

Qian Q and Zang Z supervised the project. Xiao H conceived the idea, designed and completed the experiments. Qian Q performed the simulation calculation and analysis. All authors contributed to reviewing and writing the paper.

Corresponding authors

Correspondence to Qingkai Qian  (钱庆凯) or Zhigang Zang  (臧志刚).

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The authors declare that they have no conflict of interest.

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Supporting data are available in the online version of the paper.

Hongbin Xiao received his PhD degree from The University of Tokyo in 2020. He joined the School of Chemistry and Chemical Engineering, Chongqing University as an assistant researcher in 2020. His research interests mainly focus on the syntheses of perovskites materials and their applications in photodetection, photocatalytic CO2 reduction and lasing.

Qingkai Qian received his PhD degree from Hong Kong University of Science and Technology in 2018. He joined the School of Optoelectronic Engineering, Chongqing University as an associate professor in 2021. His research interests mainly focus on photodetectors, perovskites semiconductor materials and their applications in transistors, solar cells and light-emitting diodes.

Zhigang Zang received his PhD degree from Kyushu University in 2011. He joined the School of Optoelectronic Engineering, Chongqing University as a professor in 2014. His research interests mainly focus on the synthesis of perovskite-based semiconductor materials and their applications in solar cells and light-emitting diodes.

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Xiao, H., Qian, Q. & Zang, Z. Anchoring palladium nanoparticles on CsPbBr3 perovskite nanocrystals for enhanced photocatalytic CO2 reduction. Sci. China Mater. 66, 1810–1819 (2023). https://doi.org/10.1007/s40843-022-2304-2

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