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Defect Engineering in Titanium-Based Oxides for Electrochemical Energy Storage Devices

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Abstract

Defect engineering involves the manipulation of the type, concentration, mobility or spatial distribution of defects within crystalline structures and can play a pivotal role in transition metal oxides in terms of optimizing electronic structure, conductivity, surface properties and mass ion transport behaviors. And of the various transition metal oxides, titanium-based oxides have been keenly investigated due to their extensive application in electrochemical storage devices in which the atomic-scale modification of titanium-based oxides involving defect engineering has become increasingly sophisticated in recent years through the manipulation of the type, concentration, spatial distribution and mobility of defects. As a result, this review will present recent advancements in defect-engineered titanium-based oxides, including defect formation mechanisms, fabrication strategies, characterization techniques, density functional theory calculations and applications in energy conversion and storage devices. In addition, this review will highlight trends and challenges to guide the future research into more efficient electrochemical storage devices.

Graphic Abstract

This work reviews the recent advances in defect-engineered Ti-based oxides, including the mechanism of defect formation, fabrication strategies, the characterization techniques, density functional theory calculations and the applications in energy conversion and storage.

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Fig. 1
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Reprinted with permission from Ref. [63], copyright (2014) Springer Nature. b Ball and stick models for F-doped anatase TiO2. The left panel: a Ti3+ cation directly neighboring a F dopant. The right panel: a Ti3+ cation at ~ 7 Å distance from a F dopant. Reprinted with permission from Ref. [49], copyright (2008) American Chemical Society

Fig. 4

Reprinted with permission from Ref. [71], copyright (2013) Royal Society of Chemistry

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Reprinted with permission from Ref. [81], copyright (2013) American Chemical Society

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Reprinted with permission from Ref. [83], copyright (2013) John Wiley and Sons

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Reprinted with permission from Ref. [89], copyright (2005) American Chemical Society

Fig. 9

Reprinted with permission from Ref. [93], copyright 2015, Chemical Society of Japan(CSJ). b Picture of white TiO2 turning to yellowish brown after microwave treatment. Reprinted with permission from Ref. [91], copyright 2013, Elsevier

Fig. 10

Reprinted with permission from Ref. [52], copyright (2015) American Chemical Society. c Transformation from octahedral to tetrahedral-coordinated Ti4+ in Fe–TiO2 and d high-resolution TEM image of 10% Fe/TiO2 after annealing in air. Reprinted with permission from Ref. [74], copyright (2012) American Chemical Society

Fig. 11

Reprinted with permissions from Ref. [107] under Creative Commons

Fig. 12

Reprinted with permission from Ref. [42], copyright (2012) American Chemical Society. c Photographs of pristine TiO2 and H-TiO2 nanowires annealed in hydrogen at various temperatures from 300 to 550 °C. d Gradual changes in the color of TiO2 from blue to gray at different annealing temperatures and annealing times in a hydrogen atmosphere. Reprinted with permission from Ref. [44], copyright (2013) American Chemical Society

Fig. 13

Reprinted with permission from Ref. [75], copyright (2011) American Association for the Advancement of Science. e XRD spectra of blue and white TiO2 along with corresponding photographs. Reprinted with permission from Ref. [113], copyright (2014) American Chemical Society. f, g SEM images of pristine and blue H-LTO. Reprinted with permission from Ref. [110], copyright (2014) Royal Society of Chemistry. h Photographs and i UV–Vis spectra of P25 treated at different hydrogenation times (35 bar, H2) at room temperature. Reprinted with permission from Ref. [114], copyright (2014) Royal Society of Chemistry

Fig. 14

Reprinted with permission from Ref. [115], copyright (2015) American Chemical Society. b UV–Vis spectra of obtained samples and c band gap energy at different temperatures. Reprinted with permission from Ref. [116], copyright (2015) American Chemical Society. d Color change of TiO2 nanocrystals calcined at various temperatures for 2 h under different atmospheres of air, nitrogen and a hydrogen/nitrogen mixture. Reprinted with permission from Ref. [117], copyright (2016) Elsevier. e TiO2 nanotubes annealed in air, Ar/H2 or high pressure H2. Reprinted with permission from Ref. [118], copyright (2014) American Chemical Society

Fig. 15

Reprinted with permission from Ref. [119], copyright (2012) Elsevier. c TiO2, H-TiO2, N-TiO2 and H, N-TiO2 nanowire arrays. Reprinted with permission from Ref. [120], copyright (2012) American Chemical Society

Fig. 16

Reprinted with permission from Ref. [121], copyright (2014) Royal Society of Chemistry

Fig. 17

Reprinted with permission from Ref. [79], copyright (2018) Springer Nature. b Schematic of the synthesis of rutile TiO2 (R-TiO2) with a sulfurized surface along with photographs of R-TiO2-S, R’-TiO2-S-4 h and R’-TiO2-S annealed at 800 °C in an Ar atmosphere through Al reduction. Reprinted with permission from Ref. [123], copyright (2013) American Chemical Society. c Evolution from pristine TiO2 to TiO2−x and to x-doped TiO2−x (x = H, N, S, I). Reprinted with permission from Ref. [124], copyright (2014) Royal Society of Chemistry. d TiO2 obtained by adding 60 mg (sample 1), 120 mg (sample 2), 240 mg (sample 3) and 400 mg (sample 4) Mg powder. Reprinted with permission from Ref. [125], copyright (2017) John Wiley and Sons. e TiCl4 solutions in ethanol after adding Zn powder at different ratios and Mg, Al powder (Mg/Al:TiCl4 = 2:1). Reprinted with permission from Ref. [126], copyright (2013) Royal Society of Chemistry

Fig. 18

Reprinted with permission from Ref. [129], copyright (2017) IOP Publishing. b Formation mechanism of defective-LTO and c XRD of LTO calcined at 800 °C for various time periods. Reprinted with permission from Ref. [131], copyright (2017) John Wiley and Sons. d Photographs of (A) Ti glycolate gel and (B) black anatase TiO2−x with the Ti glycolate gel structure highlighted. Reprinted with permission from Ref. [134], copyright (2016) Royal Society of Chemistry. e Ti3+ self-doped TiO2 NT synthesis and f photographs of TiO2 NTs and detached ECR-TiO2 NT powders. Reprinted with permission from Ref. [136], copyright (2013) Royal Society of Chemistry

Fig. 19

Reprinted with permission from Ref. [76], copyright 2015, Elsevier

Fig. 20

Reprinted with permission from Ref. [144], copyright (2003) American Association for the Advancement of Science

Fig. 21

Reprinted with permission from Ref. [145], copyright 2012, Elsevier. b Pristine and defective LTO synthesized in a reducing atmosphere at 800 °C under high pressure. Reprinted with permission from Ref. [131], copyright (2017) John Wiley and Sons

Fig. 22

Reprinted with permission from Ref. [74], copyright (2012) American Chemical Society. c Ti K-edge XANES spectra and d EXAFS spectra of undoped Li4Ti5O12 in an oxidizing atmosphere (LTO-O), undoped Li4Ti5O12 in a reducing atmosphere (LTO-R) and Mo-doped Li4Ti5O12 in a reducing atmosphere (Mo-LTO-R). Reprinted with permission from Ref. [155] under Creative Commons

Fig. 23

Reprinted with permission from Ref. [157], copyright 2013, Royal Society of Chemistry. e Deconvolved XPS spectra of reference Li4Ti5O12 (R-LTO) and f Li4Ti5O12 with OVs (O-LTO) synthesized under 5 vol% H2/Ar atmosphere. Reprinted with permission from Ref. [158], copyright 2017, Elsevier

Fig. 24

Reprinted with permission from Ref. [161], copyright 2015, IOP Publishing. b Raman spectra of Li4Ti5O12 synthesized under different atmospheres. Reprinted with permission from Ref. [162], copyright 2011, Springer Nature. c FTIR spectra of undoped and Co2+ doped TiO2 nanoparticles. Reprinted with permission from Ref. [145], copyright 2012, Elsevier. d Gaussian peak fitted PL spectra of TiO2 nanotubes. Reprinted with permission from Ref. [166], copyright (2017) American Chemical Society. e EPR spectra of defective TiO2 nanoparticles reduced by L-ascorbic acid (0, 0.3 and 0.7 g corresponding to white, brown and black TiO2−x). Reprinted with permissions from Ref. [167] under Creative Commons. f Derivative EPR spectra of undoped LTO in oxidizing (LTO-O) and reducing atmospheres (LTO-R) as well as Mo-doped LTO in reducing atmosphere (Mo-LTO-R). Reprinted with permissions from Ref. [155] under Creative Commons

Fig. 25

Reprinted with permission from Ref. [111], copyright (2012) American Chemical Society

Fig. 26

Reprinted with permission from Ref. [179], copyright (2012) John Wiley and Sons

Fig. 27

Reprinted with permission from Ref. [161], copyright 2015, IOP Publishing. c 3D EELS spectra with the STEM image marked with positions in which EELS spectra were recorded in the left panel, and corresponding EELS spectra for Ti-L2,3 and O-K edges were recorded at various positions in the right panel. Reprinted with permission from Ref. [183], copyright (2016) American Chemical Society. d Cathodoluminescence spectra and Gaussian fitting results for sputter-deposited TiO2 nanowires. Reprinted with permission from Ref. [159], copyright (2010) American Chemical Society. e Thermal gravimetric analysis (TGA) and derivative thermogravimetry (DTG) of LTO nanoparticles under Ar or H2 atmosphere and f mass spectra signals of CO2 and H2O during annealing under H2 atmosphere. Reprinted with permissions from Ref. [186], copyright John Wiley and Sons

Fig. 28

Reprinted with permission from Ref. [196], copyright (2016) American Chemical Society. c Lattice structures of \({\text{Li}}_{4} {\text{Ti}}_{5} {\text{O}}_{12}\) and \({\text{Li}}_{7}\, {\text{Ti}}_{5}\, {\text{O}}_{12}\) with unit cells. d PDOS of \({\text{Li}}_{4}\, {\text{Ti}}_{5}\, {\text{O}}_{12}\) and \({\text{Li}}_{7}\, {\text{Ti}}_{5}\, {\text{O}}_{12}\) with two different structures from PBE results in which the Fermi level is aligned to 0 eV. Reprinted with permissions from Ref. [197] under Creative Commons

Fig. 29

Reprinted with permission from Ref. [231], copyright (2012) American Chemical Society. And b & c br, 3f(1), 3f(2) and 4f. Reprinted with permission from Ref. [229], copyright (2016) Elsevier

Fig. 30

Reprinted with permission from Ref. [228], copyright (2008) AIP Publishing

Fig. 31

Reprinted with permission from Ref. [203], copyright (2018) American Chemical Society

Fig. 32

Reprinted with permission from Ref. [131], copyright (2017) John Wiley and Sons

Fig. 33

Reprinted with permission from Ref. [196], copyright (2016) American Chemical Society. b Spin density differences ρplotted = ρup – ρdown in three Li-doped TiO2 polymorphs (Ti atoms: blue spheres, O atoms: red spheres, Li atoms: green spheres). The projection plane is (001) and (010) for anatase, (001) for rutile and (010) for TiO2(B). Reprinted with permission from Ref. [244], copyright (2015) Elsevier. c Supercell model of boron-doped rutile TiO2. d Calculated DOS of pristine and boron-doped rutile TiO2 with dopant concentrations of 0.5% and 1.0%. Reprinted with permission from Ref. [226], copyright (2014) Royal Society of Chemistry. e DOS of LTO and M-doped LTO (M = Cr, Fe, Ni and Mg) calculated with a \(2 \times 1 \times 1\) supercell and GGA functional. Reprinted with permission from Ref. [245], copyright (2006) John Wiley and Sons. f\(3 \times 1 \times 1\) supercell model for H-doped LTO and the calculated DOS for pristine and H-doped models from HSE06. Reprinted with permission from Ref. [110], copyright (2014) Royal Society of Chemistry

Fig. 34

Reprinted with permission from Ref. [229], copyright (2016) Elsevier. c Diffusion pathway between two octahedral sites in rutile. d Diffusion pathway between two octahedral sites in anatase. In c and d, light blue and red spheres represent Ti and O atoms, respectively. Reprinted with permission from Ref. [298], copyright (2015) Elsevier. Li diffusion pathways for e anatase and f rutile involving Li-ions hopping between two neighboring octahedral sites in each structure. Li diffusion pathways for TiO2(B) with Li atoms hopping between g two adjacent C sites, h two neighboring A1 sites and i two neighboring A2 sites. l–p Calculated energy profiles for Li-ion diffusion pathways in pristine and OV-defective models of l anatase, m rutile and for TiO2(B), n C–C, o A1–A1 and p A2–A2. Reprinted with permission from Ref. [203], copyright (2018) American Chemical Society

Fig. 35

Reprinted with permission from Ref. [77], copyright (2018) American Chemical Society. b Charge/discharge profiles (at the 20th cycle) for pristine TiO2 (the dotted line), Ar-1 h-TiO2−δ (the dashed line) and H2-1 h-TiO2−δ (the solid line) cycled at 0.2 C. Reprinted with permission from Ref. [219], copyright (2012) American Chemical Society. c Specific discharge capacities at various C rates for LTO and H-LTO NWAs. Reprinted with permission from Ref. [318], copyright (2012) John Wiley and Sons

Fig. 36

Reprinted with permission from Ref. [131], copyright (2017) John Wiley and Sons. c Rate capabilities of pure TiO2 anatase and Ti0.78□0.22O1.12F0.4(OH)0.48 electrodes. Reprinted with permission from Ref. [320], copyright (2015) American Chemical Society. d Initial charge/discharge profiles of undoped and V5+-doped TiO2 electrodes. Reprinted with permission from Ref. [322], copyright (2013) Elsevier

Fig. 37

Reprinted with permission from Ref. [325], copyright (2016) American Chemical Society. b Rate capabilities of S-TiO2/rGO, TiO2/rGO and S-TiO2 electrodes at different current densities. Reprinted with permission from Ref. [328], copyright (2018) Elsevier. c Structural models of Fe-doped-TiO2. d Rate capabilities of pristine and Fe-doped TiO2 at different currents. Reprinted (adapted) with permission from Ref. [329]. Copyright (2017) American Chemical Society

Fig. 38

Reprinted with permission from Ref. [339], copyright (2018) American Chemical Society. b Galvanostatic discharge–charge curves for TiO2 and Ti0.78□0.22O1.12F0.40(OH)0.48 versus Mg. Cells were cycled at 20 mA g−1 in the potential range 0.05–2.3 V versus Mg2+/Mg. c Galvanostatic discharge–charge curves for TiO2 and Ti0.78□0.22O1.12F0.40(OH)0.48 versus Al. Cells were cycled at 20 mA g−1 in the potential range 0.01–1.8 V versus Al3+/Al. Reprinted with permission from Ref. [340], copyright (2017) Springer Nature. d Rate performances of commercial white anatase TiO2 and black anatase TiO2 nanoleave electrodes at different current rates. Reprinted with permission from Ref. [341], copyright (2014) Royal Society of Chemistry

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Acknowledgements

We are grateful for the financial support from the Australia Research Council Discovery Projects DP170103721 and DP180102003, the National Key R&D Program of China (2016YFB0700600), the Soft Science Research Project of Guangdong Province (No. 2017B030301013) and the Shenzhen Science and Technology Research Grant (ZDSYS201707281026184). We would also like to thank Dr. Sean E. Lowe (Griffith University) for his contributions in polishing our manuscript.

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  1. Zhong Su and Jiahua Liu have contributed equally to this work.

Authors and Affiliations

  1. Centre for Clean Environment and Energy, School of Environment and Science, Griffith University, Gold Coast Campus, Gold Coast, QLD, 4222, Australia

    Zhong Su, Meng Li, Yuxuan Zhu, Shangshu Qian, Yulin Zhong & Shanqing Zhang

  2. School of Advanced Materials, Peking University Shenzhen Graduate School, Shenzhen, 518055, Guangdong, China

    Jiahua Liu, Mouyi Weng, Jiaxin Zheng & Feng Pan

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  1. Zhong Su
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Correspondence to Feng Pan or Shanqing Zhang.

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Su, Z., Liu, J., Li, M. et al. Defect Engineering in Titanium-Based Oxides for Electrochemical Energy Storage Devices. Electrochem. Energ. Rev. 3, 286–343 (2020). https://doi.org/10.1007/s41918-020-00064-5

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