Grain and grain boundary behaviors and electrical transport properties of TiO<sub>2</sub> nanowires under high pressure

Wang Yue; Shao Bo-Huai; Chen Shuang-Long; Wang Chun-Jie; Gao Chun-Xiao

doi:10.7498/aps.71.20212276

Abstract

In this work, anatase Titanium dioxide (TiO₂) nanowires are synthesized by the hydrothermal method, and its grain and grain boundary behaviors and electrical properties are investigated by alternating current (AC) impedance method under high pressure (up to 34.0 GPa). The relationship between the frequency dependence of impedance Z'' and pressure indicate that the conduction mechanism of anatase phase TiO₂ nanowires in the test pressure range is electronic conductivity. It should be noted that the characteristic peaks of Z'' move toward high frequency region with pressure increasing, demonstrating that the effect of grain interior on impedance becomes apparent. Additionally, the overall variation trends of grain and grain boundary resistance go downward with pressure increasing, and the descent rate of grain boundary is larger than those of grain before and after phase transition. However, in a range of phase transition (8.2–11.2 GPa, from anatase to baddeleyite phase), grain boundary resistance shows a discontinuously change (increases to 11.2 GPa and then decreases). Based on the different variation trends of grain and grain boundary resistance, it becomes obvious that the phase transition from anatase to baddeleyite phase first occurs at the surface of grain, and then extends to the interior of grain gradually. Also, as an intrinsic characteristic, the relaxation frequency is independent of the geometrical parameters. The pressure dependence of activation energy is obtained by fitting the pressure dependence of relaxation frequency. The activation energy of grain and grain boundary decrease with pressure increasing, implying that the contribution of pressure on the conductivity of sample is positive. Furthermore, the space charge potential for the whole test pressure range is positive, which is determined by the relationship between pressure and relaxation frequency. This fact illustrates that the anion defects are easily formed in the space charge region, and the oxygen defects are the main inducement for TiO₂ phase transformation.

Keywords:

Authors and contacts

1.
College of Physical Science and Technology, Bohai University, Jinzhou 121013, China
2.
State Key Laboratory of Superhard Materials, Jilin University, Changchun 130012, China

Corresponding author: Wang Chun-Jie, cjwang@foxmail.com

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 12004050) and the Research Foundation of the Education Department of Liaoning Province, China (Grant Nos. LJ2019013, LQ2020005).

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References

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[2]	Dong Z H, Song Y 2015 Can. J. Chem. 93 165 Google Scholar
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Cited By

图 1 经过650℃退火后的TiO₂纳米线　(a) XRD谱图; (b) SEM图片

Figure 1. TiO₂ nanowires after being annealing at 650 ℃: (a) XRD pattern; (b) SEM image.

DownLoad: Full-Size Img PowerPoint

图 2 TiO₂纳米线在不同压力下的阻抗谱　(a) 5.4 GPa; (b) 8.5 GPa; (c) 18.1 GPa; (d) 34.0 GPa

Figure 2. Impedance spectra of TiO₂ nanowires at different pressures: (a) 5.4 GPa; (b) 8.5 GPa; (c) 18.1 GPa; (d) 34.0 GPa.

DownLoad: Full-Size Img PowerPoint

图 3 TiO₂纳米线阻抗虚部Z" 随频率的演化关系　(a)在6.0—9.3 GPa范围内; (b) 在13.3—32.6 GPa范围内

Figure 3. Frequency dependence of impedance Z" plots of TiO₂ nanowires at different pressures: (a) In the range of 6.0–9.3 GPa; (b) in the range of 13.3–32.6 GPa.

DownLoad: Full-Size Img PowerPoint

图 4 不同压力下 TiO₂纳米线的Nyquist图　(a) 5.4 GPa; (b) 23.0 GPa

Figure 4. Nyquist impedance spectra of TiO₂ nanowires at different pressures: (a) 5.4 GPa; (b) 23.0 GPa.

DownLoad: Full-Size Img PowerPoint

图 5 TiO₂纳米线晶粒和晶界电阻随压力的变化关系

Figure 5. Pressure dependence of R_g and R_gb of TiO₂ nanowires

DownLoad: Full-Size Img PowerPoint

图 6 TiO₂纳米线晶粒和晶界驰豫频率随压力的变化关系

Figure 6. Variations of f_g and f_gbof TiO₂ nanowires as a function of pressure.

DownLoad: Full-Size Img PowerPoint

图 7 TiO₂纳米线晶界空间电荷势随压力的变化

Figure 7. Pressure dependence of space charge potential of TiO₂ nanowires.

DownLoad: Full-Size Img PowerPoint

表 1 TiO₂纳米线在不同压力区间的dH_g/dP和dH_gb/dP

Table 1. Fitting parameters from pressure dependence of active energy of grain and grain boundary of TiO₂ nanowires.

Pressure region/GPa dH/dP/(meV·GPa^–1)
Grain Grain boundary

1.6—8.2 –0.578 –0.433
9.5—34.0 –0.084 –0.069

DownLoad: CSV

[1]	Li Q J, Liu B B 2016 Chin. Phys. B 25 076107 Google Scholar
[2]	Dong Z H, Song Y 2015 Can. J. Chem. 93 165 Google Scholar
[3]	Swamy V, Kuznetsov A Y, Dubrovinsky L S, Kurnosov A, Prakapenka V B 2009 Phys. Rev. Lett. 103 075505 Google Scholar
[4]	Machon D, Daniel M, Pischedda V, Daniele S, Bouvier P, LeFloch S 2010 Phys. Rev. B 82 140102 Google Scholar
[5]	Machon D, Daniel M, Bouvier P, Daniele S, Floch S L, Melinon P, Pischedda V 2011 J. Phys. Chem. C 115 22286 Google Scholar
[6]	Li Q, Cheng B, Yang X, Liu R, Zou B 2013 J. Phys. Chem. C 117 8516 Google Scholar
[7]	Wang Z, Saxena S K 2001 Solid State Commun. 118 75 Google Scholar
[8]	Swamy V, Kuznetsov A, Dubrovinsky L S, Mcmillan P F, Prakapenka V B, Shen G, Muddle B C 2006 Phys. Rev. Lett. 96 135702 Google Scholar
[9]	Hearne G R, Zhao J, Dawe A M, Pischedda V, Comins J D 2004 Phys. Rev. B 70 134102 Google Scholar
[10]	Swamya V, Dubrovinsky L S, Dubrovinskaia N A, Simionovici A S, Drakopoulos M, Dmitriev V, Weber H P 2003 Solid State Commun. 125 111 Google Scholar
[11]	Swamy V, Dubrovinsky L S, Dubrovinskaia N A, Langenhorst F, Simionovici A, Drakopoulos M, Dmitriev V, Weber H P 2005 Solid State Commun. 134 541 Google Scholar
[12]	Arlt T, Bermejo M, Blanco M A, Gerward L, Jiang J Z, Olsen J S, Recio J M 2000 Phys. Rev. B 61 14414 Google Scholar
[13]	Haines J, Léger J M 1993 Physica B 192 233 Google Scholar
[14]	Lagarec K, Desgreniers S 1995 Solid State Commun. 94 519 Google Scholar
[15]	Li Q J, Liu B B, Wang L, Li D M, Liu R, Zou B, Cui T, Zou G T, Meng Y, Mao H K, Liu Z X, Liu J, Li J X 2010 J. Phys. Chem. Lett. 1 309 Google Scholar
[16]	Li Q J, Liu R, Cheng B Y, Wang L, Yao M G, Li D M 2012 Mater. Res. Bull. 47 1396 Google Scholar
[17]	Park S, Jang J, Cheon J, Lee H H, Lee D R, Lee Y 2008 J. Phys. Chem. C 112 9627 Google Scholar
[18]	Li Q, Cheng B, Tian B, Liu R, Liu B, Wang F, Chen Z, Zou B, Cui T, Liu B 2014 RSC Adv. 4 12873 Google Scholar
[19]	Dong Z, Xiao F, Zhao A, Liu L, Sham T K, Song Y 2016 RSC Adv. 6 76142 Google Scholar
[20]	Li Q, Ran L, Wang T, Ke X, Jing L 2015 AIP Adv. 5 097128 Google Scholar
[21]	Zhang Y, Wang Q, Zhang J, Wu X, Ma Y 2017 Nanotechnology 28 145705 Google Scholar
[22]	Liu B, Nakata K, Liu S, Sakai M, Ochia T, Murakami T, Takagi K, Fujishima A 2012 J. Phys. Chem. C 116 7471 Google Scholar
[23]	Tokudome H, Miyauchi M 2004 Chem. Commun. 8 958 Google Scholar
[24]	Wu J M, Shi H C, Wu W T 2006 Nanotechnology 17 105 Google Scholar
[25]	Rendón-Rivera A, Toledo-Antonio J A, Cortés-Jácome M A, Angeles-Chávez C 2011 Catal. Today 166 18 Google Scholar
[26]	Crossland E J W, Noel N, Sivaram V, Leijtens T, Alexander-Webber J A, Snaith H J 2013 Nature 495 215 Google Scholar
[27]	韩迪仪, 顾阳, 胡涛政, 董雯, 倪亚贤 2021 物理学报 70 038103 Google Scholar Han D Y, Gu Y, Hu T Z, Dong W, Ni Y X 2021 Acta Phys. Sin. 70 038103 Google Scholar
[28]	王春杰, 王月, 高春晓 2020 物理学报 69 147202 Google Scholar Wang C J, Wang Y, Gao C X 2020 Acta Phys. Sin. 69 147202 Google Scholar
[29]	曹楚南, 张鉴清 2002 电化学阻抗谱导论 (典藏版 1) (北京: 科学出版社) 第21页 Cao C N, Zhang J Q 2002 Introduction to Electrochemical Impedance Spectroscopy (Vol. 1) (Beijing: Science Press) p21 (in Chinese)
[30]	Watanabe T, Murakami T, Karashima S 1978 Scr. Metall. 12 361 Google Scholar
[31]	Dickey L E C 2004 Acta Mater. 52 809 Google Scholar
[32]	Zhang H, Zhang G, Wang J, Wang Q, Liu C 2021 J. Alloys Compd. 857 157482 Google Scholar
[33]	Wang Q, Wang X, Li J, Qin T, Sang D, Liu J, Ke F, Wang X, Li Y, Liu C 2021 J. Mater. Chem. C 9 4764 Google Scholar
[34]	Wang J, Zhang G, Liu H, Wang Q, Shen W, Yan Y, Liu C, Han Y, Gao C 2017 Appl. Phys. Lett. 111 031907 Google Scholar
[35]	Gerbig O, Merkle R, Maier J 2013 Adv. Mater. 25 3129 Google Scholar
[36]	Ali H, Karim S, Rafiq M A, Maaz K, Ahmad M 2014 J. Alloys Compd. 612 64 Google Scholar
[37]	Abouzari M, Berkemeier F, Schmitz G, Wilmer D 2009 Solid State Ionics 180 922 Google Scholar
[38]	Lü X, Yang W, Quan Z, Lin T, Bai L, Wang L, Huang F, Zhao Y 2014 J. Am. Chem. Soc. 136 419 Google Scholar
[39]	Wang Q, Li S, Peng F, Lei L, He D 2017 J. Appl. Phys. 121 215109 Google Scholar
[40]	Bai F, Bian K, Huang X, Wang Z, Fan H 2019 Chem. Rev. 119 7673 Google Scholar
[41]	Wang Q, He D, Peng F, Lei L, Xiong L, Wang P, Liu J 2014 High Pressure Res. 34 259 Google Scholar
[42]	Goncharov A F 1992 High Pressure Res. 8 607 Google Scholar
[43]	Popescu C, Sans J A, Errandonea D, Segura A, Sapia F 2014 Inorg. Chem. 53 11598 Google Scholar
[44]	Dutta A, Sinha T P, Shannigrahi S 2007 Phys. Rev. B 76 155113 Google Scholar
[45]	Buelbuel M M, Zeyrek S 2006 Microelectron. Eng. 83 2522 Google Scholar
[46]	Tolbert S H, Alivisatos A P 1995 J. Chem. Phys. 102 4642 Google Scholar
[47]	Brus L E, Harkless J A W, Stillinger F H 1996 J. Am. Chem. Soc. 118 4834 Google Scholar
[48]	Macdonald J R 1987 Impedance Spectrum (New York: Wiley) pp13–14, 205
[49]	Fleig J 2002 Solid State Ionics 150 181 Google Scholar
[50]	Henisch H K 1984 Semiconductor Contacts (Oxford: Clarendon Press) p85
[51]	Guo X 1995 Solid State Ionics 81 235 Google Scholar

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Grain and grain boundary behaviors and electrical transport properties of TiO₂ nanowires under high pressure

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Corresponding author: Wang Chun-Jie, cjwang@foxmail.com

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Pressure region/GPa	dH/dP/(meV·GPa^–1)
Pressure region/GPa	Grain	Grain boundary
1.6—8.2	–0.578	–0.433
9.5—34.0	–0.084	–0.069

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Grain and grain boundary behaviors and electrical transport properties of TiO2 nanowires under high pressure

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Corresponding author: Wang Chun-Jie, cjwang@foxmail.com

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Grain and grain boundary behaviors and electrical transport properties of TiO₂ nanowires under high pressure