Sustainable engineering of TiO2-based advanced oxidation technologies: From photocatalyst to application devices

doi:10.1016/j.jmst.2020.10.061

Abstract

Abstract:

In recent years, photocatalysis (PC) and photoelectrocatalysis (PEC) technologies have shown great promise as low-cost, environmentally friendly, and sustainable strategies in addressing the issues of energy shortages and environmental pollution, which has become a research hotspot. Titanium dioxide (TiO2)-based PC and PEC are the most promising sustainable technologies for advanced oxidation applications. Due to its inherent characteristics, including high oxidation ability, low price, and stability, TiO2 photocatalyst has been widely studied and used in different scales for numerous decades. For practical applications in these areas, the engineering of the photocatalysts and the design of the PC and PEC devices must be both environmentally and economically sustainable. On the one hand, for the engineering of the photocatalysts, the photocatalyst shall be able to deliver the following characteristics, including large specific surface area, high absorption of light, rapid and low-cost separation and regeneration, and high stability. On the other hand, the design of the PC and PEC devices shall facilitate high in energy utilization and catalytic efficiency, and low in building and operational cost. This work covers the reaction mechanism of TiO2-based PC and PEC technologies, sustainable design, and preparation of TiO2 photocatalysts as well as sustainable design in PC and PEC devices for wastewater treatment, sensing, and water splitting. Finally, we provide some critical perspectives on the future development of TiO2-based PC and PEC technology.

Key words: Photocatalysis, Photoelectrocatalysis, TiO₂, Bandgap, Morphology engineering, Sustainable design

Meng Zu, Xiaosong Zhou, Shengsen Zhang, Shangshu Qian, Dong-Sheng Li, Xianhu Liu, Shanqing Zhang. Sustainable engineering of TiO₂-based advanced oxidation technologies: From photocatalyst to application devices[J]. J. Mater. Sci. Technol., 2021, 78: 202-222.

Figures/Tables 22

Fig. 1. Sustainable engineering of TiO2-based PC and PEC technologies: photocatalyst engineering (morphology fabrication, band-gap engineering, and co-catalysts) and device engineering (irradiation source, reactor structure, and applied potential bias), which are utilized for applications for wastewater treatment, sensing, and water splitting.

Fig. 2. Electron-hole generation and separation by the electron acceptor (A) and the electron donor (D) under illumination in n-type semiconductor TiO2 in a PC process.

Fig. 3. Crystalline structures of titanium dioxide (a) anatase, (b) rutile, and (c) brookite.

Fig. 4. Schematic description and corresponding SEM/TEM images of (a-c) TiO2 nanorods, (d-f) TiO2 nanorod arrays, (g-i) branched TiO2 nanorod arrays and (j-l) TiO2 nanorod@nanobowls. (e,h) represent the cross-sectional view, (b,f,i,l) represents the top view. (k) SEM images of TiO2 nanobowls. (Derived from Ref. [[74], [75], [76], [77]]).

Fig. 5. (a) Schematic illustration of the preparation process of TiO2 nanotubes and MoS2 nanosheets@TiO2 nanotubes. The top view and the cross-sectional view of the SEM images of (b,c) TiO2 nanotubes and (d,e) MoS2 nanosheets@TiO2 nanotubes. (Derived from Ref. [93]).

Fig. 6. Top view and a corresponding cross-sectional view (inserted) SEM images of different pore sizes of (a) TiO2 nanorod photonic crystals (216), (b) TiO2 nanorod photonic crystals (292), and (c) disordered TiO2 bi-layer. (d) UV-vis diffused reflectance spectra of the three TiO2 films on the FTO substrate. Scale bars of all inserts in (a), (b), and (c) are 2mm [105].

Fig. 7. Schematic picture of heterostructures of (a) conventional charge-carrier transfer, (b) dye-sensitized transfer, and (c) SPR metal transfer for TiO2-based photocatalyst.

Table 1 The TiO2-based PC/PEC application with different heterostructure formation.

Photocatalyst	Heterostructure formation	PC/PEC application	Performance	Ref.
Ag₃PO₄/TiO₂	conventional	MO degradation, visible light (λ>500nm)	MO degradation rate: 95.5 % after 60min	[136]
porous ZrO₂@TiO₂	conventional	HER, UV light	H₂ evolution rate: 39.7mmol/h/g	[137]
TiO₂/ZnFe₂O₄	Z-scheme	N₂ photofixation, visible light	ammonia generation rate: 1.48μmol/L/min	[138]
TiO₂/CdS	Z-scheme	HER, UV light	H₂ evolution rate: 51.4μmol/h	[139]
E-TiO₂/Au/TiO₂	SPR	HER, visible light	H₂ evolution rate: 26.25μmol/h/g	[140]
Ag-loaded TiO₂ nanotube arrays	SPR	CO₂ reduction, visible light	CH₄ production rate: 48mmol/h/m²	[141]

Fig. 8. Scheme of self-driven dye-sensitized tandem PC cell for water splitting [129].

Fig. 9. Schematic procedure for fabricating the five different samples: (a) TiO2 nanotubes, TiO2 nanotubes-Al2O3, TiO2 nanotubes-Au, TiO2 nanotubes-Au-Al2O3, and TiO2 nanotubes-Al2O3-Au; (b) the simplified schematic structures of (a1) TiO2 nanotubes-Au, (b1) TiO2 nanotubes-Al2O3-Au, and (c1) TiO2 nanotubes-Au-Al2O3 and (a2-c2) the finite difference time domain (FDTD) simulation of the corresponding spatial distribution of electric field density (| E |) on the y-plane for the three structures under 570nm incident light irradiation [135].

Fig. 10. Scheme for a possible influence of electronic band structure at doped TiO2; (a) standard band-gap in pristine TiO2, (b) insertion of local states within the band-gap in a doped TiO2, (c) band-gap narrowing in a doped TiO2.

Table 2 The TiO2-based PC/PEC application with different doping elements.

Photocatalyst	Doping elements	PC/PEC application	Performance	Ref.
Pt-TiO₂	metal	HER, near-UV light	H₂ evolution rate: 0.116μmol/h/cm³	[194]
Fe-TiO₂	metal	MB degradation, visible light	MB degradation rate: 75 % after 90 min	[195]
Cu-TiO₂	metal	antimicrobial, visible light	E-coli degradation rate: 99.9999% after 30 min	[196]
N-TiO₂	non-metal	MO degradation, visible light	MO degradation rate: 65 % after 60 min	[197]
S-TiO₂	non-metal	Acetaldehyde degradation, visible light	Acetaldehyde degradation rate: 75 % after 300 min	[198]
black C-TiO₂	non-metal	MB degradation, UV and visible light	MB degradation rate: 97 % after 120min under UV light; 74 % after 120min under visible light	[45]
Pd-H-TiO₂ nanofibers	self-doping & metal	HER, UV light	H₂ evolution rate: 17mmol/h/g under UV-A irradiation; ∼25.6mmol/h/g under UV-B irradiation	[199]
H-TiO₂/MoS₂	self-doping	HER, visible light	H₂ evolution rate: 1840mmol/h/m²	[200]

Fig. 11. (a) The DOS calculation results of the metal-doped TiO2 (Ti1-xAxO2: A=V, Cr, Mn, Fe, Co, or Ni). Gray solid lines: total DOS; solid black lines: dopant's DOS; (b) scheme of the electronic band structure of doped TiO2 from DOS results [159]; (c) SEM images of i. TiO2, ii. Fe-TiO2, iii. Mn-TiO2 and ix. Co-TiO2 nanorod arrays on FTO substrates. Inserts are the corresponding digital pictures, respectively. All scale bars represent 1mm. Photocurrent densities vs. time of the Fe-doped TiO2, Mn-doped TiO2, Co-doped TiO2, and TiO2 nanorods measured at 0.5V vs. RHE under 100mW cm-2 solar illumination; (d) photocurrent density profile of as-prepared photocatalysts [160].

Fig. 12. The design of electrode back-illumination (a), thin-layer (b), and cylindrical PC reactors (c) to address light absorption from aqueous solution and slow mass transport problems in PC degradation.

Table 3 The TiO2-based electrodes for sustainable PC and PEC water treatment.

Photocatalyst	Irradiation source	Pollutants degradation	Time for degradation of 50 % pollutants (/min)	Ref.
Pt(Au,Ag)/TiO₂	6×6W fluorescent lamps (λmax=365nm)	MO	70	[233]
Mesoporous TiO₂	15W 365nm UV lamp	Rhodamine B	100	[234]
TiO₂@C	Sunlight	Rhodamine B	2	[235]
Y-TiO₂ film	30W UV lamp	MO and Cr(VI) ions	130	[236]
BiOI/TiO₂ NBAs	Visible light 150mW cm^-2	Methyl orange	3.5	[237]
TiO₂/rGO	15W UV-C lamp	Rhodamine B	60	[238]
MnFe2O4@rGO@TiO₂	Solar simulator (1000W/m²)	Ofloxacin	50	[16]
Nano TiO₂ meshes	30W low-pressure Hg vapor UV-C lamp emitting at 254 nm	Real water sample	50	[239]
Graphene/Cu₂O /TiO₂ mesh	Solar light 150W Xe lamp	Bisphenol A	25	[240]
Au/TiO₂ NTAs	Visible light 350W Xe lamp	Methyl orange	230	[241]

Fig. 13. (a) Schematic design of the PC reactor incorporated with an economically friendly UV-LED array and a PeCOD detector, (b) the image of the microfluidic thin-layer PC system with low building and operating cost. [242,245].

Fig. 14. Photocurrent profile of a blank solution and a sample after injecting organic compounds in a PEC thin-layer cell [247].

Fig. 15. (a) General view of three-electrode PEC bulk cell; (b) Schematic diagram of PEC bulk cell. [76].

Fig. 16. The photocurrent for different biosensors (a) PDA platform-Ab2 label, (b) the Au nanoclusters/PDA platform-Ab2 label, (c) the Au nanoclusters/PDA platform-Ab2-SiO2@G-quadruplex label, and (d) the Au nanoclusters/PDA platform-Ab2-SiO2@G-quadruplex-hemin label under the condition of 4-CN and H2O2. (e) The photocurrentof biosensor with different concentrations of MC-LR, (f) the calibration curve, (g) the interference of other chemical compounds. (Derived from Ref. [276]or).

Table 4 Modified TiO2 photocatalysts for sustainable water splitting.

Photocatalysts	Light intensity	Modification method	Electrolyte	Photocurrent Density	Hydrogen Production Rate (mmol/h/cm²)	Ref.
TiO₂ NTAs	UV light 70mW/cm²	-	1M KOH	112μA/cm²	7.1	[281]
H/TiO₂ NWs	UV light 100mW/cm²	doping	1M NaOH	2.7mA/cm²	5.6	[191]
Pt/TiO₂ NTAs	UV light 30mW/cm²	co-catalysis	0.1M Na₂SO₄ and 1M ethylene glycol	45.7μA/cm²	135	[282]
Pd/TiO₂ NTAs	Solar light 320mW/cm²	co-catalysis	2 M Na₂CO₃ and 0.5M ethylene glycol	26.8mA/cm²	592	[283]
Cu/TiO₂ NTAs	Visible light 300W Xe lamp	co-catalysis	5% ethylene glycol	0.193mA/cm²	0.003	[284]
Cu₂O/TiO₂ NTAs	Visible light 300W Xe lamp	heterostructure	5% ethylene glycol (pH=7.40)	1mA/cm²	0.003	[285]
Graphite/ TiO₂ NWs	Solar light 150mW/cm²	heterostructure	30 % methanol	20μA/cm²	4.87	[286]
CdS/TiO₂ NR/NTA	Solar light 320mW/cm²	heterostructure	0.25M Na₂S and 0.35M Na₂SO₃	2.41mA/cm²	24.74	[287]
SrTiO₃/TiO₂ NWA	Solar light 320mW/cm²	heterostructure	0.5M KOH and 0.5M ethylene glycol	1.91mA/cm²	314.9	[288]
TiO₂@BiVO₄ NRAs	Solar light 100mW/cm²	heterostructure	0.1M Na₂SO₃ (pH=7.0)	1.3mA/cm²	16.4	[289]
Graphene/CdS/TiO₂ NTA	Solar light 300mW/cm²	multi-modification	0.1M Na₂S and 0.1M Na₂SO₃	--	10	[290]
CdS,CdSe/TiO₂ NRA	Solar light 100mW/cm²	multi-modification	10 % ethylene glycol and 0.1M Na₂S	0.5mA/cm²	457	[291]

Fig. 17. (a) Photo of UCA-WS device; (b) schematic diagram of UCA-ES device; (c) image of a UCA-WS prototype under white-light illumination. (Derived from Ref. [279]).

Fig. 18. (a) The preparation procedure of photoelectrodes and assemble process in the PEC-PV device; (b) front view of the module; (c) top view and bottom view of the module assembled with four multi-PE windows; (d) detailed view of the counter-electrode support; (e) detailed view of the double-layer reflective shield (PTFE-aluminium). (Derived from Ref. [280]).

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Sustainable engineering of TiO₂-based advanced oxidation technologies: From photocatalyst to application devices

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