Recent advances in metal titanate-based piezocatalysts: Enhancing catalytic performance through improved piezoelectric properties and regulated carrier transport

doi:10.1016/S1872-2067(23)64635-2

Abstract

Abstract:

Piezocatalysis, as an emerging technology, holds the promise for providing sustainable solutions to environmental remediation and energy management through mechanical energy utilization. Metal titanates (MTs) are well-known for their outstanding piezoelectric response, positioning them as the primary candidates for catalysts in this field. Moreover, their eco-friendly and cost-effective attributes have made them the focus of considerable attention among researchers. However, the insufficient piezocatalytic activity continues to constrain the practical application of MTs. Confronted with suboptimal energy conversion efficiency, enhancing the response to mechanical energy and reducing the subsequent conversion losses are pivotal for improving the piezocatalytic performance. This review commences with the classification and introduction of various MTs relevant to the field of piezocatalysis. Subsequently, the main methods for preparing MTs are presented. Particularly, the design strategies of MTs with excellent piezocatalytic properties are discussed from the perspectives of improving piezoelectric properties and regulating carrier transport, including construction of morphotropic phase boundary, strain engineering, Curie point control, external field-induced polarization, oriented crystal growth, co-catalyst loading, carbon modification, and semiconductor heterostructure construction. Finally, comprehensive challenges to the development of piezocatalytic technology are presented to promote the rational design and practical application of piezocatalysts.

Key words: Piezocatalysis, Metal titanates, Enhanced strategy, Piezoelectric response, Carrier transport

Kaiqi Wang, Yiming He. Recent advances in metal titanate-based piezocatalysts: Enhancing catalytic performance through improved piezoelectric properties and regulated carrier transport[J]. Chinese Journal of Catalysis, 2024, 61: 111-134.

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Figures/Tables 18

Fig. 1. (a) Several milestone research works in the field of piezocatalysis. (b) A schematic representation of the piezocatalytic mechanism.

Table 1 Some representative works of piezocatalysis based on different stress sources.

Material	Stress source	Catalytic application	Ref.
ZnO/TiO₂	thermal stress	degradation of MO and MB	[33]
CdS	water stirring	H₂O₂ evolution	[34]
ZnO	mechanical brush/sliding	degradation of MB	[35]
(Ba,Ca)TiO₃	water flushing	degradation of congo red	[36]
Bi₄NbO₈X (X = Cl, Br)	ultrasonic vibration	production of reactive oxygen species	[37]

Fig. 2. (a) Crystallographic structure of R3c ZnSnO3. Reprinted with permission from Ref. [38]. Copyright 2019, John Wiley and Sons. (b) Structure of Pca21 Bi2WO6 unit cell and the spontaneous polarization along different axes. Reprinted with permission from Ref. [39]. Copyright 2021, the Royal Society of Chemistry. (c) Crystal structure of BiO(IO3) and net macroscopic polarization direction towards the c-axis. Reprinted with permission from Ref. [40]. Copyright 2011, American Chemical Society. (d) Crystallographic structure of wurtzite ZnS and schematics of the piezoelectric effect. Reprinted with permission from Ref. [41]. Copyright 2015, American Chemical Society.

Fig. 3. (a) Deviations in the TiO6 crystal structure. (b) Piezoelectric potential of Bi4Ti3O12 simulated by applying an ultrasonic stress of 10 MPa along with the x-, y-, and z-axes. Reprinted with permission from Ref. [42]. Copyright 2023, Elsevier. (c) Publications on piezocatalysis of MTs from 2013 to 2023. (d) Comparison of the publication numbers for different types of piezocatalysts. All dates were collected from the Web of Science using the key words “piezocatalysis” and “Corresponding chemical formulas”.

Fig. 4. A schematic diagram of strategies for enhancing piezocatalytic performance of MTs.

Fig. 5. (a) Cubic structure of BaTiO3 and tetragonal structure of BaTiO3 with spontaneous polarization along [001]. Reprinted with permission from Ref. [56]. Copyright 2020, American Chemical Society. (b) Structure evolution of PbTiO3 with enhanced tetragonality. Reprinted with permission from Ref. [57]. Copyright 2020, John Wiley and Sons.

Fig. 7. SEM images of BaTiO3 nanofibers calcined at different temperatures: (a) 550, (b) 600, (c) 650, (d) 700, (e) 800, and (f) 900 °C. Reprinted with permission from Ref. [98]. Copyright 2021, Elsevier.

Fig. 8. (a) STEM image of the 10 nm BaTiO3 with multiphase coexistence. (b) Landau free energy profiles for the simultaneous coexistence of three ferroelectric phases and (c) it’s 2D projection. Reprinted with permission from Ref. [108]. Copyright 2019, John Wiley and Sons. (d) PFM phase hysteresis loop and displacement butterfly curves of BNKT samples. (e) The piezocatalytic performance of BNKT samples for RhB degradation and (f) the corresponding kinetic rate constants. (g) H2 evolution rates over BNKT samples of various compositions under 40 kHz ultrasonic vibration. Reprinted with permission from Ref. [110]. Copyright 2023, the Royal Society of Chemistry.

Fig. 9. Variation of TiO6 octahedron structures before (a) and after (b and c) Cr3+ and Nb5+ doping. Reprinted with permission from Ref. [113]. Copyright 2022, Elsevier. (d) H2 and O2 evolution rates of the blank sample, BaTiO3, and b-BaTiO3 under 40 kHz ultrasonic vibration, respectively. (e) The recycling piezocatalytic H2 and O2 evolution tests of b-BaTiO3. (f) TEM image of b-BaTiO3. Scale bar = 200 nm. (g) Geometric phase analysis of out-plane strain εyy covering a pore structure. (h) The distribution of potential in a b-BaTiO3 nanoparticle based on COMSOL simulation. Scale bar = 200 nm. Reprinted with permission from Ref. [117]. Copyright 2021, John Wiley and Sons.

Fig. 10. The hysteresis loop of BTS nanoparticles at temperature of 25 °C (a), 35 °C (b) and 45 °C (c). (d) Schematic diagram of spontaneous polarization versus temperature. Piezocatalytic activities of BTS nanoparticles for the removal of RhB (e) and MO (f) under different conditions. Reprinted with permission from Ref. [127]. Copyright 2021, Elsevier.

Fig. 11. (a) The schematic of piezocatalysis induced by electric poling treatment. (b) Decomposition ratios and (c) the corresponding kinetic rate constants of NBT poled with different poling fields. Reprinted with permission from Ref. [130]. Copyright 2021, Elsevier. (d) ESR spectra of ·OH and ·O2? over different piezocatalysts. Reprinted with permission from Ref. [131]. Copyright 2020, Springer Nature.

Fig. 12. (a) Orbital projected electronic band structure and projected density of states of BCTZ. The red color corresponds to O 2p states, while the green color represents Ti 3d states. VBM and CBM orbital arrangements are illustrated. (b) Schematic diagram illustrating the band structure of BCTZ. Reprinted with permission from Ref. [139]. Copyright 2023, John Wiley and Sons. (c) Schematic diagram of domain motion with and without OVs. (d) Calculated d33 at different OVs concentrations. Reprinted with permission from Ref. [140]. Copyright 2022, Elsevier.

Fig. 13. (a) Mechanism of the Ag/BaTiO3 hybrid piezocatalyst during CH3SH removal. Reprinted with permission from Ref. [144]. Copyright 2022, American Chemical Society. (b) Schematic diagram of the modulated Schottky barrier between Pt and PbTiO3 by the directional piezoelectric field. Reprinted with permission from Ref. [145]. Copyright 2023, the Royal Society of Chemistry. (c) The schematics of major radical-involved reactions occurring on BaTiO3-Ag surfaces. Reprinted with permission from Ref. [150]. Copyright 2020, Elsevier. (d) piezo-photocatalytic performance of AuCu/PbTiO3/MnOx and reference samples (① none, ② PbTiO3, ③ PbTiO3/AuCu, ④ PbTiO3/MnOx, ⑤ AuCu/PbTiO3/MnOx, ⑥ PbTiO3/AuCu-MnOx) in (d) CO production and (e) O2 evolution. Free-energy diagrams for (f) the reduction of CO2 to CO on PbTiO3{001} and AuCu(111) surfaces, and (g) the oxidation of H2O to O2 on PbTiO3{001} and MnOx surfaces. (h) The charge separation mechanism of AuCu/PbTiO3/MnOx. Reprinted with permission from Ref. [151]. Copyright 2023, American Chemical Society.

Fig. 14. (a) Reaction kinetics rate constants in the removal of CBZ by different systems. (b) Cycle tests of CBZ removal in CNTs/BaTiO3-PMS system. Reprinted with permission from Ref. [158]. Copyright 2022, Elsevier. (c) Piezocatalytic efficiency of Cu-EDTA over 180 min under different piezocatalytic conditions. (d) The surface potential of different samples under 1 nN stress. Reprinted with permission from Ref. [159]. Copyright 2019, American Chemical Society.

Fig. 15. (a) Schematic diagram of piezo-photocatalysis for the PbTiO3/CdS composite. Reprinted with permission from Ref. [166]. Copyright 2020, Elsevier. (b) Magnified XRD patterns of the NBT/NBT4 composite. (c) Piezocatalytic H2 evolution of NBT/NBT4 composite in different waters. (d) First-principles DFT simulations of band structure of NBT/NBT4 heterojunction. Reprinted with permission from Ref. [68]. Copyright 2023, Elsevier.

Table 2 Summary of promoting effect of different strategies.

Material	Synthetic method	Morphology	Strategy	Reaction condition	Catalytic performance	Increase multiple	Ref.
Pollutant removal
(Na_0.8K_0.2)_0.5Bi_0.5TiO₃	hydrothermal	nanoparticles	MPB	400 W ultrasound	MB, 0.01695 min^‒1	3.51	[60]
Bi_0.5(Na₁₋_xK_x)_0.5TiO₃	hydrothermal	nanoparticles	MPB	80 W ultrasound	RhB, 0.065 min^‒1	3.7	[110]
Ba_0.5Sr_0.5TiO₃	hydrothermal	nanoparticles	strain engineering	100 W ultrasound	CBZ, 0.106 min^‒1	1.86	[169]
V-doped SrTiO₃	electrospinning	nanofibers	strain engineering	150 W ultrasound	bisphenol A, 0.1758 min^‒1	2.74	[170]
OVs-SrBi₄Ti₄O₁₅	molten salt	nanoflakes	strain engineering	300 W Xe lamp, 100 W ultrasound	tetracycline, 0.058 min^‒1	7.25	[121]
BaTi_0.89Sn_0.11O₃	hydrothermal	nanoparticles	T_c operation	120 W ultrasound	RhB, 0.21423 min^‒1; MO, 0.03797 min^‒1	1.48; 1.39	[127]
BaZr_0.02Ti_0.98O₃	solid-state	nanoparticles	electric polarization	70 W ultrasound	RhB, 0.00535 min^‒1; MO, 0.00407 min^‒1	7.15; 6.30	[171]
BaTiO₃	hydrothermal	nanoparticles	electric polarization	80 W ultrasound	indigo carmine, 0.059 min^‒1; RhB, 0.0075 min^‒1	29.5; 7.23	[131]
Na_0.5Bi_0.5TiO₃	solid-state	micronparticles	electric polarization	150 W ultrasound	RhB, 0.00556 min^‒1	8.18	[130]
CoO_x/Bi₄Ti₃O₁₂	molten salt	nanosheets	co-catalyst loading	120 W ultrasound	MO, 0.01817 min^‒1	2.4	[147]
NiO/BaTiO₃	hydrothermal	prismatic blocks	co-catalyst loading	120 W ultrasound	RhB, 0.04017 min^‒1	6.3	[146]
SrBi₄Ti₄O₁₅/Ag₂O	molten salt	nanosheets	co-catalyst loading	300 W Xe lamp, 180 W ultrasound	RhB, 0.5492 min^‒1	7.7	[172]
Ag/BaTiO₃	hydrothermal	nanocubes	co-catalyst loading	120 W ultrasound	bisphenol A, 0.0091 min^‒1	6.5	[150]
RuO₂/BaTiO₃/Pt	hydrothermal	nanoparticles	co-catalyst loading	110 W ultrasound	tricyclazole, 0.032 min^-1	3.11	[148]
Ag/BaTiO₃/Co₃O₄	molten salt	polyhedrons	co-catalyst loading	120 W ultrasound	MO, 0.0539 min^‒1	4.94	[152]
BaTiO₃/C	hydrothermal	nanofibers	carbon modification	150 W ultrasound	RhB, 0.04901 min^‒1	2.52	[155]
CNTs/BaTiO₃	hydrothermal	nanoparticles	carbon modification	1000 rpm stirring	CBZ, 0.02071 min^‒1	6.7	[158]
BaTiO₃@Gr	hydrothermal	nanofibers	carbon modification	200 W ultrasound	Cu-EDTA, 100% for 180 min	—	[159]
BaTiO₃/g-C₃N₄	hydrothermal	nanofibers	heterostructures	120 W ultrasound	RhB, 82.0% for 210 min	1.44	[167]
BaTiO₃/SrTiO₃	electrospinning	nanofibers	heterostructures	30 W UV lamp, 300 W ultrasound	RhB, 97.4% for 30 min	2.2	[173]
H₂ production
10 nm-size BaTiO₃	hydrothermal	nanoparticles	MPB	ultrasound	655 µmol g^‒1 h^‒1	—	[108]
Cr³⁺-Nb⁵⁺ doped Bi₄Ti₃O₁₂	molten salt	nanosheets	strain engineering	300 W Xe lamp, ultrasound	696 µmol g^‒1 h^‒1	3.7	[113]
Porous BaTiO₃	hydrothermal	nanoparticles	strain engineering	ultrasound	159 µmol g^‒1 h^‒1	130	[117]
Pt/PbTiO₃	hydrothermal	nanoplates	co-catalyst loading	100 W ultrasound	360 µmol g^‒1 h^‒1	1.6	[145]
PbTiO₃/CdS	hydrothermal	nanoplates	heterostructures	300 W Xe lamp, 100 W ultrasound	849 µmol g^‒1 h^‒1	2.2	[166]
Na_0.5Bi_0.5TiO₃/ Na_0.5Bi_4.5Ti₄O₁₅	hydrothermal	nanoparticles	heterostructures	400 W ultrasound	128 µmol g^‒1 h^‒1	—	[68]
Other energy synthesis
0.5Ba(Zr_0.2Ti_0.8)O₃- 0.5(Ba_0.7Ca_0.3)TiO₃	solid-state	nanoparticles	MPB	180 W ultrasound	H₂O₂, 692 µmol g^‒1 h^‒1	8.7	[107]
OVs-BaTiO₃	hydrothermal	nanoparticles	strain engineering	300 W Xe lamp, 200 W ultrasound	NH₃, 106.7 µmol g^‒1 h^‒1	4.39	[119]
AuCu/PbTiO₃/MnO_x	hydrothermal	nanoplates	co-catalyst loading	300 W Xe lamp, 120 W ultrasound	CO, 23.9 µmol g^‒1 h^‒1; O₂, 2.6 µmol g^‒1 h^‒1	4.6; 6.3	[151]

Table 2 Summary of promoting effect of different strategies.

Material	Synthetic method	Morphology	Strategy	Reaction condition	Catalytic performance	Increase multiple	Ref.
Pollutant removal
(Na_0.8K_0.2)_0.5Bi_0.5TiO₃	hydrothermal	nanoparticles	MPB	400 W ultrasound	MB, 0.01695 min^‒1	3.51	[60]
Bi_0.5(Na₁₋_xK_x)_0.5TiO₃	hydrothermal	nanoparticles	MPB	80 W ultrasound	RhB, 0.065 min^‒1	3.7	[110]
Ba_0.5Sr_0.5TiO₃	hydrothermal	nanoparticles	strain engineering	100 W ultrasound	CBZ, 0.106 min^‒1	1.86	[169]
V-doped SrTiO₃	electrospinning	nanofibers	strain engineering	150 W ultrasound	bisphenol A, 0.1758 min^‒1	2.74	[170]
OVs-SrBi₄Ti₄O₁₅	molten salt	nanoflakes	strain engineering	300 W Xe lamp, 100 W ultrasound	tetracycline, 0.058 min^‒1	7.25	[121]
BaTi_0.89Sn_0.11O₃	hydrothermal	nanoparticles	T_c operation	120 W ultrasound	RhB, 0.21423 min^‒1; MO, 0.03797 min^‒1	1.48; 1.39	[127]
BaZr_0.02Ti_0.98O₃	solid-state	nanoparticles	electric polarization	70 W ultrasound	RhB, 0.00535 min^‒1; MO, 0.00407 min^‒1	7.15; 6.30	[171]
BaTiO₃	hydrothermal	nanoparticles	electric polarization	80 W ultrasound	indigo carmine, 0.059 min^‒1; RhB, 0.0075 min^‒1	29.5; 7.23	[131]
Na_0.5Bi_0.5TiO₃	solid-state	micronparticles	electric polarization	150 W ultrasound	RhB, 0.00556 min^‒1	8.18	[130]
CoO_x/Bi₄Ti₃O₁₂	molten salt	nanosheets	co-catalyst loading	120 W ultrasound	MO, 0.01817 min^‒1	2.4	[147]
NiO/BaTiO₃	hydrothermal	prismatic blocks	co-catalyst loading	120 W ultrasound	RhB, 0.04017 min^‒1	6.3	[146]
SrBi₄Ti₄O₁₅/Ag₂O	molten salt	nanosheets	co-catalyst loading	300 W Xe lamp, 180 W ultrasound	RhB, 0.5492 min^‒1	7.7	[172]
Ag/BaTiO₃	hydrothermal	nanocubes	co-catalyst loading	120 W ultrasound	bisphenol A, 0.0091 min^‒1	6.5	[150]
RuO₂/BaTiO₃/Pt	hydrothermal	nanoparticles	co-catalyst loading	110 W ultrasound	tricyclazole, 0.032 min^-1	3.11	[148]
Ag/BaTiO₃/Co₃O₄	molten salt	polyhedrons	co-catalyst loading	120 W ultrasound	MO, 0.0539 min^‒1	4.94	[152]
BaTiO₃/C	hydrothermal	nanofibers	carbon modification	150 W ultrasound	RhB, 0.04901 min^‒1	2.52	[155]
CNTs/BaTiO₃	hydrothermal	nanoparticles	carbon modification	1000 rpm stirring	CBZ, 0.02071 min^‒1	6.7	[158]
BaTiO₃@Gr	hydrothermal	nanofibers	carbon modification	200 W ultrasound	Cu-EDTA, 100% for 180 min	—	[159]
BaTiO₃/g-C₃N₄	hydrothermal	nanofibers	heterostructures	120 W ultrasound	RhB, 82.0% for 210 min	1.44	[167]
BaTiO₃/SrTiO₃	electrospinning	nanofibers	heterostructures	30 W UV lamp, 300 W ultrasound	RhB, 97.4% for 30 min	2.2	[173]
H₂ production
10 nm-size BaTiO₃	hydrothermal	nanoparticles	MPB	ultrasound	655 µmol g^‒1 h^‒1	—	[108]
Cr³⁺-Nb⁵⁺ doped Bi₄Ti₃O₁₂	molten salt	nanosheets	strain engineering	300 W Xe lamp, ultrasound	696 µmol g^‒1 h^‒1	3.7	[113]
Porous BaTiO₃	hydrothermal	nanoparticles	strain engineering	ultrasound	159 µmol g^‒1 h^‒1	130	[117]
Pt/PbTiO₃	hydrothermal	nanoplates	co-catalyst loading	100 W ultrasound	360 µmol g^‒1 h^‒1	1.6	[145]
PbTiO₃/CdS	hydrothermal	nanoplates	heterostructures	300 W Xe lamp, 100 W ultrasound	849 µmol g^‒1 h^‒1	2.2	[166]
Na_0.5Bi_0.5TiO₃/ Na_0.5Bi_4.5Ti₄O₁₅	hydrothermal	nanoparticles	heterostructures	400 W ultrasound	128 µmol g^‒1 h^‒1	—	[68]
Other energy synthesis
0.5Ba(Zr_0.2Ti_0.8)O₃- 0.5(Ba_0.7Ca_0.3)TiO₃	solid-state	nanoparticles	MPB	180 W ultrasound	H₂O₂, 692 µmol g^‒1 h^‒1	8.7	[107]
OVs-BaTiO₃	hydrothermal	nanoparticles	strain engineering	300 W Xe lamp, 200 W ultrasound	NH₃, 106.7 µmol g^‒1 h^‒1	4.39	[119]
AuCu/PbTiO₃/MnO_x	hydrothermal	nanoplates	co-catalyst loading	300 W Xe lamp, 120 W ultrasound	CO, 23.9 µmol g^‒1 h^‒1; O₂, 2.6 µmol g^‒1 h^‒1	4.6; 6.3	[151]

Fig. 16. Schematic illustration representing the timeline of recent progress toward MTs-based piezocatalysts.

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