Dipole moment regulation by Ni doping ultrathin Bi4O5Br2 for enhancing internal electric field toward efficient photocatalytic conversion of CO2 to CO

doi:10.1016/S1872-2067(24)60120-8

Abstract

Abstract:

The low efficiency of photogenerated carrier separation, and the poor adsorption and activation ability of CO₂ on the surface of photocatalyst were the key problems to limit the efficiency of photocatalytic CO₂ reduction. Hence, maximally accelerating the immigration of photogenerated charges d increasing the number of active sites are critical points to boost the overall performance of photocatalytic CO₂ reduction. However, it is still huge challenge. In this work, the Ni-doped ultrathin Bi₄O₅Br₂ nanosheets, which was successfully prepared by hydrothermal and ultrasonic chemical stripping methods, exhibited efficient photocatalytic conversion of CO₂ to CO. The results of experiments and theoretical calculations indicated that the doped Ni²⁺ significantly increased the crystal dipole moment of Bi₄O₅Br₂ in y direction (from 0 to 0.096 eÅ), which enhanced the polarized electric field strength inside Bi₄O₅Br₂, and further promoted the immigration of photogenerated carriers. Meanwhile, the ultrathin structure and doped Ni²⁺ synergistically increased the number of active sites, thereby promoting the adsorption and activation of CO₂ molecules, as evidenced by experimental and theoretical results collectively. As result, The CO yield was as high as 26.57 μmol g^-1 h^-1 for the prepared Ni-doped ultrathin Bi₄O₅Br₂ nanosheets under full spectrum light irradiation, which was 9.48 times that of Bi₄O₅Br₂. Therefore, it is of great scientific significance in this study to explore strategies to promote the separation of photogenerated carriers and enhance the adsorption and activation ability of CO₂ on the surface.

Key words: Ni-doped Bi₄O₅Br₂, Ultra-thin nanomaterial, Dipole moment, Polarized electric field, Photocatalytic CO₂ reduction

Xiaotian Wang, Bo Hu, Yuan Li, Zhixiong Yang, Gaoke Zhang. Dipole moment regulation by Ni doping ultrathin Bi₄O₅Br₂ for enhancing internal electric field toward efficient photocatalytic conversion of CO₂ to CO[J]. Chinese Journal of Catalysis, 2024, 66: 257-267.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(24)60120-8

https://www.cjcatal.com/EN/Y2024/V66/I11/257

Figures/Tables 7

Fig. 1. The XRD patterns of BOB and Nix-BOB samples (a) and the enlarged XRD patterns (b). (c) Raman spectra of BOB, Ni1.0-BOB, UN BOB and UN Ni1.0-BOB. (d,e) AFM images of UN Ni1.0-BOB.

Fig. 2. (a) TEM image. (b) HRTEM images. (c) SAED images. (d) HADDF images. EDS element mapping of Bi (e), O (f), Br (g) and Ni (h) for UN Ni1.0-BOB samples.

Fig. 3. XPS spectra of Bi 4f (a), Br 3d (b), O 1s (c), and Ni 2p (d). (e,f) The charge density distribution of the BOB and UN Ni1.0-BOB.

Fig. 4. (a) UV-vis-NIR DRS of the BOB, Nix-BOB, UN BOB and UN Nix-BOB (insert: Kubelka-Munk function vs. the energy of incident light plots). (b-e) Mott-Schottky (M-S) plot of BOB, Ni1.0-BOB, UN BOB and UN Ni1.0-BOB. (f) XPS valence band spectra of BOB and UN Ni1.0-BOB.

Fig. 5. (a) CO2 reduction rate of all samples. (b) CO2 photoreduction under various reaction conditions over UN Ni1.0-BOB. (c) MS spectrum of photocatalytic reduction of 13CO2. (d) Photoreduction CO2 cycle experiment by UN Ni1.0-BOB. XRD patterns (e) and TEM image (f) of the UN Ni1.0-BOB after reaction.

Fig. 6. (a) Theoretical dipole moments for BOB and UN Ni1.0-BOB. (b) The calculated total DOS of UN Ni1.0-BOB. (c) PL spectra of BOB, Ni1.0-BOB, UN BOB and UN Ni1.0-BOB. Transient photocurrent response (d) and electrochemical impedance spectra (e) of the as-prepared samples. (f) CO2-TPD spectra of BOB, UN BOB and UN Ni1.0-BOB.

Fig. 7. The adsorption energy of CO2 adsorbed on different material surfaces. (a) BOB; (b) UN Ni1.0-BOB. (c) The charge density difference of CO2 adsorbed on UN Ni1.0-BOB. In-situ DRIFTS measurements for CO2 and H2O interaction with BOB and UN Ni1.0-BOB. (d,e) At dark. (f,g) Under full spectral light irradiation.

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Dipole moment regulation by Ni doping ultrathin Bi₄O₅Br₂ for enhancing internal electric field toward efficient photocatalytic conversion of CO₂ to CO

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