Engineering the coordination structure of Cu for enhanced photocatalytic production of C1 chemicals from glucose

doi:10.1016/S1872-2067(24)60098-7

Abstract

Abstract:

Photocatalytic decomposition of sugars is a promising way of providing H₂, CO, and HCOOH as sustainable energy vectors. However, the production of C₁ chemicals requires the cleavage of robust C-C bonds in sugars with concurrent production of H₂, which remains challenging. Here, the photocatalytic activity for glucose decomposition to HCOOH, CO (C₁ chemicals), and H₂ on Cu/TiO₂ was enhanced by nitrogen doping. Owing to nitrogen doping, atomically dispersed and stable Cu sites resistant to light irradiation are formed on Cu/TiO₂. The electronic interaction between Cu and nitrogen ions originates valence band structure and defect levels composed of N 2p orbit, distinct from undoped Cu/TiO₂. Therefore, the lifetime of charge carriers is prolonged, resulting in the production of C₁ chemicals and H₂ with productivities 1.7 and 2.1 folds that of Cu/TiO₂. This work provides a strategy to design coordinatively stable Cu ions for photocatalytic biomass conversion.

Key words: Cu photocatalyst, Coordination structure, Biomass, C-C bond, C₁ chemicals

Lulu Sun, Shiyang Liu, Taifeng Liu, Dongqiang Lei, Nengchao Luo, Feng Wang. Engineering the coordination structure of Cu for enhanced photocatalytic production of C₁ chemicals from glucose[J]. Chinese Journal of Catalysis, 2024, 63: 234-243.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(24)60098-7

https://www.cjcatal.com/EN/Y2024/V63/I8/234

Figures/Tables 4

Fig. 1. Characterization of Cu/N-TiO2 catalyst in comparison to Cu/TiO2 and N-TiO2. (a) Representative XRD patterns of Cu/TiO2 and Cu/N-TiO2. (b) Representative TEM image of Cu/N-TiO2. (c) FTIR spectra of CO adsorbed on Cu/TiO2 and Cu/N-TiO2 before and after irradiation. (d) N 1s XPS spectra of N-TiO2 and Cu/N-TiO2. (e) X-band EPR spectra of Cu/TiO2 and Cu/N-TiO2 were recorded in the dark and under irradiation in Ar and at ?196 °C.

Fig. 2. Schematic diagram and time profiles of photocatalytic glucose decomposition to H2 and C1 chemicals. (a) Schematic diagram of photocatalytic decomposition of glucose. H2, C1 chemical and intermediates production over Cu/TiO2 (b) and Cu/N-TiO2 (c). (d) Performance of photocatalytic sugars and polyols decomposition to H2 and C1 chemicals over Cu/N-TiO2. Reaction conditions: 0.1 mmol of substrate, 0.1 mmol of water, 5 mg of photocatalyst, 1 mL of MeCN, 5 W LEDs (365 ± 5 nm), Ar.

Fig. 3. DOS and the contours of CBM and VBM of Cu1/TiO2 and Cu1/N-TiO2. The DOS of Cu1/TiO2 (a) and Cu1/N-TiO2 (b). The contours of CBM and VBM of Cu1/TiO2 (c) and Cu1/N-TiO2 (d). The contours in yellow around the atoms represent partial charge density.

Fig. 4. Influence of N on the photophysical properties of Cu/TiO2. Photocurrent density (a) and steady-state PL spectra (b) of Cu/N-TiO2 in contrast to TiO2, N-TiO2 and Cu/TiO2. (c) Schematic band diagram Cu/TiO2 and Cu/N-TiO2. Time-resolved PL kinetics recorded at an emission wavelength of 400 (d), 440 (e), and 550 nm (f).

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Engineering the coordination structure of Cu for enhanced photocatalytic production of C₁ chemicals from glucose

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