Identification of origin of insulating polymer maneuvered photoredox catalysis

doi:10.1016/S1872-2067(24)60070-7

Abstract

Abstract:

Solid non-conjugated polymers have long been regarded as insulators due to deficiency of delocalized π electrons along the molecular chain framework. Up to date, origin of insulating polymer regulated charge transfer has not yet been uncovered. In this work, we unleash the root origin of charge transport capability of insulating polymer in photocatalysis. We ascertain that insulating polymer plays crucial roles in fine tuning of electronic structure of transition metal chalcogenides (TMCs), which mainly include altering surface electron density of TMCs for accelerating charge transport kinetics, triggering the generation of defect over TMCs for prolonging carrier lifetime, and acting as hole-trapping mediator for retarding charge recombination. These synergistic roles contribute to the charge transfer of insulating polymer. Our work opens a new vista of utilizing solid insulating polymers for maneuvering charge transfer toward solar energy conversion.

Key words: Insulating polymer, Charge transfer, Photoredox catalysis, Polyelectrolyte, Self-assembly

Qiao-Ling Mo, Rui Xiong, Jun-Hao Dong, Bai-Sheng Sa, Jing-Ying Zheng, Qing Chen, Yue Wu, Fang-Xing Xiao. Identification of origin of insulating polymer maneuvered photoredox catalysis[J]. Chinese Journal of Catalysis, 2024, 63: 109-123.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(24)60070-7

https://www.cjcatal.com/EN/Y2024/V63/I8/109

Figures/Tables 4

Fig. 1. (a) Schematic illustration of electrostatic self-assembly of bPEI/ZIS nanocomposites. (b) XRD patterns of ZIS and 15bPEI/ZIS. (c) DRS results of ZIS and 15bPEI/ZIS with corresponding transformed plots calculated by the Kubelka-Munk function vs. photon energy (inset). High-resolution Zn 2p (d), In 3d (e), S 2p (f) and N 1s (g) spectra of ZIS and 15bPEI/ZIS. AFM analysis with height profiles in the inset (h), TEM (i) and HRTEM (j) images of 15bPEI/ZIS with SAED pattern in the inset. (k) TEM-EDS mapping result of 15bPEI/ZIS nanocomposite for Zn, In, S, N, and C elements.

Fig. 2. (a) Photoactivities of ZIS and 15bPEI/ZIS toward anaerobic photocatalytic reduction of a series of aromatic nitro compounds including 2-NA, 3-NA, 4-NA, 2-NP, 3-NP, 4-NP, NB, 4-nitrotoluene, 4-nitroanisole and 4-nitroacetophenone with adding ammonium formate as hole scavenger under visible light irradiation (λ > 420 nm). (b) Photoactivities of ZIS, 15PAH/ZIS, 15LPEI/ZIS and ZIS@amine-containing organic molecules (Ethylenediamine, N,N-Dimethylenediamine, N,N,N,N-Tetramethylenediamine and Triethylamine) toward photoreduction of 4-NA under the same conditions with corresponding molecular structures clearly displayed. (c) Photoactivities of CIS and 15bPEI/CIS (25 min), In2S3 and 15bPEI/In2S3 (25 min), and CdS and 15bPEI/CdS (10 min) toward photoreduction of 4-NA. (d) Photoactivities of ZIS, ZIS@xSiO2, and ZIS@xSiO2-15bPEI (x = 1, 2, 3 mL TEOS) with different SiO2 coating thickness, ZIS@3SiO2-Exh (x = 1, 2, 4 h), ZIS@3SiO2-Exh-15bPEI with different etching time, and the optimal 15bPEI/ZIS toward photoreduction of 4-NA. HRTEM images of SiO2-coated ZIS without etching and with etching for different time including ZIS@3SiO2 (e), ZIS@3SiO2-E1h (f), ZIS@3SiO2-E2h (g), and ZIS@3SiO2-E4h (h) with corresponding schematic models displayed in the insets. (i) High angle annular dark-field (HAADF) TEM images of ZIS@3SiO2-E4h nanocomposite with elemental mapping results.

Fig. 3. Characterizations of photoexcited charge separation efficiency. Ultrafast TA kinetics at a probe wavelength of 600 nm for 15bPEI/ZIS (a) and ZIS (b). The TA signal (i.e., differential absorbance, ΔA) is given in mOD, where OD stands for the optical density. (c) Time-resolved transient PL decay curves of ZIS and 15bPEI/ZIS under an excitation wavelength of 540 nm. (d) Room-temperature PL spectra of ZIS and 15bPEI/ZIS. Transient photocurrent responses (e) and anodic transient dynamics (f) of ZIS and 15bPEI/ZIS under visible light irradiation (λ > 420 nm, inset: on-off I-t results). (g) Open-circuit-potential decay curves of ZIS and 15bPEI/ZIS. (h) Nyquist plots of EIS results for ZIS and 15bPEI/ZIS under visible light irradiation (λ > 420 nm). (i) Schematic illustration of the PEC water dissociation mechanism.

Fig. 4. Plot of charge density difference (violet: charge depletion, skyblue: charge accumulation) for the most energy favorable model of H2O (a) and 4-NA (b) molecular absorbed on the ZIS@bPEI monolayer surface. (c) EPR spectra of ZIS and 15bPEI/ZIS. (d) Zn K-edge XANES spectra of Zn foil, ZIS and 15bPEI/ZIS. (e) k3-weighted Fourier transform (FT) χ(k) function of the EXAFS spectra for Zn foil, ZIS and 15bPEI/ZIS. (f) CV curves of bPEI with different concentrations (15, 30, 60 mg mL?1) in CH2Cl2 with 0.1 mol L?1 tetrabutylammonium tetrafluoroborate for scanning profile of ?1.5?1.5 V. (g) Schematic illustration of the photocatalytic mechanism of bPEI/ZIS nanocomposite.

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