Metal-organic framework derived multi-functionalized and co-doped TiO2/C nanocomposites for excellent visible-light photocatalysis

doi:10.1016/j.jmst.2021.05.052

Abstract

Abstract:

Multi-functionalized and co-doped TiO₂/C nanocomposites were derived from the pyrolysis of Ti-MOFs at 800 °C under different gaseous atmospheres and their photocatalytic performance were investigated. The gaseous atmosphere during pyrolysis plays a critical role in determining the structural, textural, optical and physicochemical properties of the derived TiO₂/C composites due to the synergistic effect of nitrogen-containing species, carboxylate and sulfur functionalized porous carbon as well as N/S co-doped TiO₂ nanoparticles. All the Ti-MOFs derived TiO₂/C composites exclusively possess homogeneously distributed TiO₂ nanoparticles in a functionalized disc-like porous carbon matrix and demonstrate much enhanced adsorption and photodegradation performance than commercial TiO₂ under the same conditions. The adsorption of methylene blue (MB) in dark on these TiO₂/C composites are dominated with pseudo second-order kinetic model and the high adsorption capacity of MB in dark on composite TiO₂/C derived from MIL-125(Ti) in argon is due to its high surface area with predominant mesoporous carbon matrix in the composite. The composite N-O-TiO₂/C derived from NH₂-MIL-125(Ti) in water vapor exhibited the highest photodegradation activity with 99.7% MB removal in 3 hours under visible light due to the optimal anatase/rutile phasejunction, together with the formation of photoactive oxygen-rich N-O like interstitial/intraband states above the valence band of TiO₂, as well as the presence of N-containing species and -OH/-COOH multi-functional groups with superhydrophilic nature of the composite. This simple one-step and easily modifiable approach can be further employed to modulate homogeneously dispersed multi-functionalized and co-doped metal oxide/carbon nanocomposites for various environment and energy-related applications.

Key words: Nanocomposite, MOF derivative, TiO₂, Porous carbon, Photocatalysis

Mian Zahid Hussain, Zhuxian Yang, Ahmed M.E. Khalil, Shahzad Hussain, Saif Ullah Awan, Quanli Jia, Roland A. Fischer, Yanqiu Zhu, Yongde Xia. Metal-organic framework derived multi-functionalized and co-doped TiO₂/C nanocomposites for excellent visible-light photocatalysis[J]. J. Mater. Sci. Technol., 2022, 101: 49-59.

Figures/Tables 8

Fig. 1. (a) PXRD patterns with Rietveld refinements and (b) highlighted anatase (101) and rutile (110) peaks of TiO2/C (gray), N-TiO2/C (red), N-S-TiO2/C (green) and N-O-TiO2/C (blue).

Fig. 2. (a) Raman spectra of TiO2/C (gray), N-TiO2/C (red), N-S-TiO2/C (green) and N-O-TiO2/C (blue) (b). N2 sorption isotherms of samples TiO2/C, N-TiO2/C, N-S-TiO2/C and N-O-TiO2/C. The filled and empty symbols represent the adsorption and desorption branch of isotherm respectively.

Fig. 3. XPS spectra of (a) elemental survey (b) Ti 2p (c) O 1s (d) N 1s (e) C 1s and (f) S 2p of samples TiO2/C, N-TiO2/C N-S-TiO2/C and N-O-TiO2/C.

Fig. 4. HRTEM images of (a) TiO2/C (b) N-TiO2/C (c) N-S-TiO2/C and (d) N-O-TiO2/C. Inset images show the selected area electron diffraction (SAED) patterns of the respective samples. (e) EDX elemental mappings of Ti, O, C and N of a selected sample N-O-TiO2/C.

Fig. 5. (a) XPS valance band edge spectra and (b) UV-Vis absorption spectra of samples TiO2/C, N-TiO2/C, N-S-TiO2/C and N-O-TiO2/C. Inset in b shows the Tauc plots of the samples.

Fig. 6. (a) Adsorption of MB in dark for samples TiO2/C (gray star), N-TiO2/C (red square), N-S-TiO2/C (green downward triangle), N-O-TiO2/C (blue upward triangle), pure MB (navy blue tetragonal) and comm. TiO2 (orange hexagonal). Fitting with (b) pseudo first-order, (c) pseudo second-order, (d) Elovich kinetic model and (e) intraparticle diffusion model for the studied composite samples TiO2/C, N-TiO2/C, N-S-TiO2/C and N-O-TiO2/C. (The adsorption measurement conditions: MB concentration: 20 mg L-1, catalyst dosage: 200 mg L-1, and measured at room temperature)

Fig. 7. Photodegradation of MB under (a) visible light conditions for samples TiO2/C, N-TiO2/C, N-S-TiO2/C, N-O-TiO2/C, only pure MB and Comm. TiO2; (b) Recyclability test of the best-performed sample N-O-TiO2/C and (c) the active species trapping experiment quantify the contribution of the photogenerated holes (h+) and hydroxyl radicals (•OH) in photocatalytic oxidation reactions. (The measurement conditions: MB concentration: 20 mg L-1; catalyst dosage: 200 mg L-1; Light source: 380 < λ < 700 nm.)

Fig. 8. A proposed schematic diagram of the photocatalytic degradation of MB by Ti-MOF derived composites.

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Metal-organic framework derived multi-functionalized and co-doped TiO₂/C nanocomposites for excellent visible-light photocatalysis

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