Single-atom modified graphene cocatalyst for enhanced photocatalytic CO2 reduction on halide perovskite

doi:10.1016/S1872-2067(24)60081-1

Abstract

Abstract:

Metal halide perovskite (MHP) has become one of the most promising materials for photocatalytic CO₂ reduction owing to the wide light absorption range, negative conduction band position and high reduction ability. However, photoreduction of CO₂ by MHP remains a challenge because of the slow charge separation and transfer. Herein, a cobalt single-atom modified nitrogen-doped graphene (Co-NG) cocatalyst is prepared for enhanced photocatalytic CO₂ reduction of bismuth-based MHP Cs₃Bi₂Br₉. The optimal Cs₃Bi₂Br₉/Co-NG composite exhibits the CO production rate of 123.16 μmol g^-1 h^-1, which is 17.3 times higher than that of Cs₃Bi₂Br₉. Moreover, the Cs₃Bi₂Br₉/Co-NG composite photocatalyst exhibits nearly 100% CO selectivity as well as impressive long-term stability. Charge carrier dynamic characterizations such as Kelvin probe force microscopy (KPFM), single-particle PL microscope and transient absorption (TA) spectroscopy demonstrate the vital role of Co-NG cocatalyst in accelerating the transfer and separation of photogenerated charges and improving photocatalytic performance. The reaction mechanism has been demonstrated by in situ diffuse reflectance infrared Fourier-transform spectroscopy measurement. In addition, in situ X-ray photoelectron spectroscopy test and theoretical calculation reveal the reaction reactive sites and reaction energy barriers, demonstrating that the introduction of Co-NG promotes the formation of *COOH intermediate, providing sufficient evidence for the highly selective generation of CO. This work provides an effective single-atom-based cocatalyst modification strategy for photocatalytic CO₂ reduction and is expected to shed light on other photocatalytic applications.

Key words: Bismuth-based perovskite, Photocatalysis, CO₂ reduction, Single-atom cocatalyst, Charge separation

Hui Fu, Jin Tian, Qianqian Zhang, Zhaoke Zheng, Hefeng Cheng, Yuanyuan Liu, Baibiao Huang, Peng Wang. Single-atom modified graphene cocatalyst for enhanced photocatalytic CO₂ reduction on halide perovskite[J]. Chinese Journal of Catalysis, 2024, 64: 143-151.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(24)60081-1

https://www.cjcatal.com/EN/Y2024/V64/I9/143

Figures/Tables 6

Fig. 1. (a) Schematic illustration of the synthetic process of Co-NG. SEM (b), TEM (c) and STEM-HAADF (d,e) images of Co-NG. Co XANES K-edge spectra (f) and FT-EXAFS spectra (g) of Co-NG with respect to the reference samples.

Fig. 2. SEM (a) and HRTEM (b) images of Cs3Bi2Br9. SEM (c), HRTEM (d), STEM (e) and EDS elemental mapping (f) images of Cs3Bi2Br9/Co-NG.

Fig. 3. XRD patterns (a) and UV-vis absorption spectra (b) of Cs3Bi2Br9, Co-NG and Cs3Bi2Br9/Co-NG. XPS spectra of Cs 3d (c), Bi 4f (d) and Br 3d (e) of Cs3Bi2Br9 and Cs3Bi2Br9/Co-NG. (f) XPS spectra of Co 2p of Co-NG and Cs3Bi2Br9/Co-NG.

Fig. 4. (a) Photocatalytic CO2 reduction performance of Cs3Bi2Br9 and Co-NG under different reaction conditions (with or without light, catalyst and CO2 atmosphere). (b) CO production rate of Cs3Bi2Br9 and Cs3Bi2Br9/xCo-NG (x = 1, 3, 5 and 7). (c) Photocatalytic CO2 reduction performance of Cs3Bi2Br9/5Co-NG during 10 consecutive cycles of experiments. Each cycle is 4 h. (d) XRD patterns of Cs3Bi2Br9/5Co-NG before and after photocatalytic cycling measurements.

Fig. 5. Surface scan KPFM image (a), surface photovoltage mapping image (b) and surface potential curve (c) of Cs3Bi2Br9/Co-NG. Single-particle PL images of Cs3Bi2Br9 (d) and Cs3Bi2Br9/Co-NG (e). PL spectra (f) and TRPL spectra (g) of Cs3Bi2Br9 and Cs3Bi2Br9/Co-NG. TA spectra of Cs3Bi2Br9 (h) and Cs3Bi2Br9/Co-NG (i). (j) Transient photocurrent response curves of Cs3Bi2Br9 and Cs3Bi2Br9/Co-NG.

Fig. 6. (a,b) In situ DRIFTS measurement for CO2 reduction of Cs3Bi2Br9/Co-NG under dark and light irradiation. In-situ XPS spectra of Bi 4f (c), N 1s (d) and Co 2p (e) of Cs3Bi2Br9/Co-NG under dark and light conditions. (f) Gibbs free energy diagrams of intermediates generated during CO2-to-CO catalysis over Cs3Bi2Br9 and Cs3Bi2Br9/Co-NG. (g) The possible photocatalytic CO2 reduction mechanism in the Cs3Bi2Br9/Co-NG photocatalytic system.

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Single-atom modified graphene cocatalyst for enhanced photocatalytic CO₂ reduction on halide perovskite

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