Effects of different compositional ratios on physical structure and optical properties of thin films during alloying of Zn<sup>2+</sup> and TiO<sub>2</sub>

Xiao Wen-Yue; Dong Xiao-Shuo; Mamatrishat Mamat; Niu Na-Na; Li Guo-Dong; Zhu Ze-Tao; Bi Jie-Hao

doi:10.7498/aps.73.20240814

Abstract

A batch of TiO₂ films with different Zn²⁺ compositions are prepared on a single crystal silicon substrate by using sol-gel method to observe the changes in optical and photocatalytic properties in the alloying process of Zn²⁺ and TiO₂. X-ray diffractometer (XRD) is used to observe the changes in the crystal structures of the films in the alloying process and to track the formation of ZnTiO₃ compounds. Scanning electron microscope (SEM) and atomic force microscope (AFM) are used to observe the phenomena of a large number of holes on the surfaces of the films due to the limited solubility of the crystal lattice for Zn²⁺ in the alloying process. X-ray photoelectron spectroscopy (XPS) and optical bandgap are used to observe the changes at a level of the electronic structure of the films in the alloying process of Zn²⁺ with TiO₂. Finally, by degrading the methylene blue solution, it is shown that a small amount of Zn²⁺ doping is completely dissolved in TiO₂, destroying the TiO₂ crystalline quality. As the compositional share of Zn²⁺ continues to increase to 15%, the limited solubility of TiO₂ for Zn²⁺ is verified in the XPS peak fitting, resulting in a large number of hole structures in the film, and the active specific surface area of the film is enhanced, while Zn²⁺ effectively traps the photogenerated e^–/h⁺. In order to continue to observe the effect of Zn²⁺ concentration on TiO₂, we increase the concentration of Zn²⁺ to 40% and observe the phenomenon in the alloying process of Zn²⁺ with TiO₂. It is shown that the appearance of the compound ZnTiO₃ can act as a complex center for e^–/h⁺ and a significant decrease in the percentage of TiO₂ leads to a gradual decrease in the photocatalytic efficiency of the films after alloying.

Keywords:

Authors and contacts

1.
School of Physics and Technology, Xinjiang University, Urumqi 830017, China
2.
School of Materials Science and Engineering, Xinjiang University, Urumqi 830017, China

Corresponding author: Mamatrishat Mamat, rxtmmt@xju.edu.cn

Funds: Project supported by the Students Innovative-Research Training Program of Xinjiang University, China (Grant No. XJU-SRT-23114).

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References

[1]	Lukong V T, Ukoba K, Jen T C 2022 Int. J. Adv. Manuf. Technol. 122 3525 Google Scholar
[2]	李冬冬, 王丽莉 2012 物理学报 61 034212 Google Scholar Li D D, Wang L L 2012 Acta Phys. Sin. 61 034212 Google Scholar
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Cited By

图 1 不同Zn²⁺成分占比的薄膜的 XRD 图样

Figure 1. XRD patterns of thin films with different Zn²⁺ compositions.

DownLoad: Full-Size Img PowerPoint

图 2 不同Zn²⁺成分占比的薄膜的SEM图样

Figure 2. SEM patterns of thin films with different Zn²⁺ compositions.

DownLoad: Full-Size Img PowerPoint

图 3 (a)纯TiO₂以及(b)—(d) 3%, 15%和40% Zn²⁺成分占比的薄膜的二维和三维AFM图像

Figure 3. 2D and 3D AFM images of thin films with (a) pure TiO₂ and (b)–(d) 3%, 15% and 40% Zn²⁺ composition.

DownLoad: Full-Size Img PowerPoint

图 4 纯TiO₂以及3%, 15% 和 40%Zn²⁺成分占比的薄膜的XPS光谱

Figure 4. XPS spectra of pure TiO₂ and thin films with 3%, 15% and 40% Zn²⁺ compositions.

DownLoad: Full-Size Img PowerPoint

图 5 不同Zn²⁺成分占比的薄膜的(a)吸收光谱和(b) 光带隙能

Figure 5. (a) Absorption spectra and (b) optical band gap energy of films with different Zn²⁺ composition.

DownLoad: Full-Size Img PowerPoint

图 6 (a) 不同Zn²⁺成分占比的薄膜的吸收阈值波长和光带隙能; (b) 纯TiO₂和Zn²⁺成分占比为3%, 15% 和 40%的薄膜的价带

Figure 6. (a) Absorption threshold wavelengths and optical band gap energies of films with different Zn²⁺ compositions; (b) valence bands of pure TiO₂ and films with 3%, 15% and 40% Zn²⁺ compositions.

DownLoad: Full-Size Img PowerPoint

图 7 不同Zn²⁺成分占比的薄膜的能带位置示意图

Figure 7. Schematic representation of the energy band positions of films with different Zn²⁺ compositions.

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图 8 降解亚甲基蓝的光催化活性　(a) 随时间变化的降解量; (b) 相应的降解反应速率常数图

Figure 8. Photocatalytic activity for degradation of methylene blue: (a) Degradation amount with time; (b) corresponding degradation rate constant plots.

DownLoad: Full-Size Img PowerPoint

图 9 光催化反应速率(η)与光催化反应常数(K_app)的关系图

Figure 9. Plot of photocatalytic reaction rate (η) versus photocatalytic reaction constant (K_app).

DownLoad: Full-Size Img PowerPoint

表 1 从 XRD 图谱获得的结构参数

Table 1. Structural parameters obtained from XRD spectra.

Samples	(h k l )	FWHM β/(°)	D/nm
TiO₂	(1 0 1)	0.177	8.384
3% Zn-TiO₂	(1 0 1)	0.161	9.217
5% Zn-TiO₂	(1 0 1)	0.197	7.533
10% Zn-TiO₂	(1 0 1)	0.180	8.244
15% Zn-TiO₂	(1 0 1)	0.259	5.730
20% Zn-TiO₂	(1 0 1)	0.152	9.762
40% Zn-TiO₂	(1 0 1)	0.227	6.537

DownLoad: CSV

表 2 从AFM获得的粗糙度参数(R_a为算数平均粗糙度, R_MS为均方根粗糙度, R_Sk为粗糙度斜率, R_Ku为粗糙度峰度)

Table 2. Roughness parameters obtained from AFM (R_a, R_MS, R_Sk, R_Ku are the average, root- mean-square, Skewness, and Kurtosis values of surface roughness, respectively).

Samples	Roughness R_a/nm	Roughness R_MS/nm	Skewness R_Sk	Kurtosis R_Ku
TiO₂	3.515	4.359	–0.492	0.276
3%Zn-TiO₂	2.230	2.851	–0.077	0.089
15%Zn-TiO₂	5.590	6.990	–0.313	0.819
40%Zn-TiO₂	6.115	8.703	–1.079	3.318

DownLoad: CSV

[1]	Lukong V T, Ukoba K, Jen T C 2022 Int. J. Adv. Manuf. Technol. 122 3525 Google Scholar
[2]	李冬冬, 王丽莉 2012 物理学报 61 034212 Google Scholar Li D D, Wang L L 2012 Acta Phys. Sin. 61 034212 Google Scholar
[3]	Chinnarani M, Suresh S, Prabu K M, Kandasamy M, Pugazhenthiran N 2024 Inorg. Chim. Acta 560 121842 Google Scholar
[4]	Sanattalab E, Gürdağ G, Sığırcı B D 2023 Biomater. Adv. 148 213365 Google Scholar
[5]	Ziental D, Goslinska B C, Mlynarczyk D T, Sobotta A G, Stanisz B, Goslinski T L 2020 Nanomaterials 10 387 Google Scholar
[6]	Zhu Z W, Chen S F, Zhang Y, Wang W 2022 Prog. Org. Coat. 173 107226 Google Scholar
[7]	Alrowaili Z A, Alsohaimi I H, Betiha M A, Essawy A A, Mousa A A, Alruwaili S F, Hassan H M A 2020 Mater. Chem. Phys. 241 122403 Google Scholar
[8]	Ike P O, Ezugwu S, Chikwenze R, Nwanya A C, Ezugwu A E, Madiba I G, Ezekoye B A, Ahmed M S, Maaza M, Ezema F I 2019 Optik 191 1 Google Scholar
[9]	Aruna S T, Vismaya A, Balaji N 2021 Mater. Manuf. Processes 36 868 Google Scholar
[10]	Mittireddi R T, Makani N H, Prajapati D, Raj A, Banerjee R, Panda E 2023 Mater. Charact. 199 112818 Google Scholar
[11]	Sun N R, Wang J W, Yao J Z, Chen H M, Deng C H 2019 Microchim. Acta 186 159 Google Scholar
[12]	Zhang Q, Li C Y 2020 Nanomaterials 10 911 Google Scholar
[13]	Kusior A, Banas J, Zajac A T, Zubrzycka P, Ilnicka A M, Radecka M 2018 J. Mol. Struct. 1157 327 Google Scholar
[14]	Al-Tayeb M A-A, Khan M Y, Drmosh Q A, Hossain M K, Asim M, Dafalla H, Khan A 2023 Inorg. Chim. Acta 556 121611 Google Scholar
[15]	Ma Q, Qiu T, Liu S J, Weng L Q, Dong W Y 2010 Appl. Phys. A 104 365 Google Scholar
[16]	Liu Y, Peng Q, Zhou Z P, Yang G 2018 Chin. Phys. Lett. 35 048101 Google Scholar
[17]	Resende P D, Maria R, Silva J D, Azevedo I, Santos L A, Tadeu V 2020 J. Mater. Res. Technol. 9 10121 Google Scholar
[18]	Chen C C, Hu S H, Fu Y P 2015 J. Alloys Compd. 632 326 Google Scholar
[19]	Ahadi S, Moalej N S, Sheibani S 2019 Solid State Sci. 96 105975 Google Scholar
[20]	Yoon Y H, Lee S Y, Gwon J, Cho H J, Wu Q, Kim Y H, Lee W H 2018 Ceram. Int. 44 16647 Google Scholar
[21]	Qu X, Lin J B, Wei Q, Chen C T, Sun D P 2022 Chemosphere 308 136239 Google Scholar
[22]	Jaimy K B, Safeena V P, Ghosh S, Hebalkar N, Warrier K 2012 Dalton Trans. 41 4824 Google Scholar
[23]	Chen K T, Hsu C H, Jiang S C, Liang L S, Gao P, Qiu Y, Wu W Y, Zhang S, Zhu W Z, Lien S Y 2022 IEEE Trans. Electron Devices 69 1149 Google Scholar
[24]	Nair P K, Mizukami F, Nair J, Salou M, Oosawa Y, Izutsu H, Maeda K, Okubo T 1998 Mater. Res. Bull. 33 1495 Google Scholar
[25]	Chen P C, Chen C C, Chen S H 2017 Curr. Nanosci. 13 373 Google Scholar
[26]	Ren T Z, Yuan Z Y, Su B L 2004 Colloids Surf., A 241 67 Google Scholar
[27]	Lang J, Takahashi K, Kubo M, Shimada M 2022 Catalysts 12 365 Google Scholar
[28]	Mercado C C, Seeley Z M, Bandyopadhyay A, Bose S, McHale J L 2011 ACS Appl. Mater. Interfaces 3 2281 Google Scholar
[29]	Henderson M 2002 Surf. Sci. Rep. 46 1 Google Scholar
[30]	Dikici T, Yılmaz O, Akalin A S, Demirci S, Gültekin S, Yıldırım S, Yurddaşkal M 2022 J. Aust. Ceram. Soc. 58 1415 Google Scholar
[31]	Xu W, Li X J, Zhang S J, Wang J G, Xu Z K 2005 Trans. Nonferrous Met. Soc. China 15 119 Google Scholar
[32]	Wang C T, Lin H S, Wang W P 2019 Mater. Sci. Semicond. Process. 99 85 Google Scholar
[33]	Liao C Z, Li Y C, Tjong S C 2020 Nanomaterials 10 124 Google Scholar
[34]	Ismael M 2020 Sol. Energy 211 522 Google Scholar
[35]	Matsumoto Y, Katayama M, Abe T, Ohsawa T, Ohkubo I, Kumigashira H, Oshima M, Koinuma H 2010 J. Ceram. Soc. Jpn. 118 993 Google Scholar
[36]	Ribao P, Rivero M J, Ortiz I 2017 Environ. Sci. Pollut. Res. 24 12628 Google Scholar
[37]	Tang T, Wang T, Gao Y, Xiao H, Xu J H 2019 J. Mater. Sci. -Mater. Electron. 30 8471 Google Scholar
[38]	Xavier A M, Jacob I D, Surender S, Saravana kumaar M S S, Elangovan P 2022 Inorg. Chem. Commun. 146 110168 Google Scholar
[39]	Pecherskaya M D, Butanov K T, Ruzimuradov O N, Mamatkulov S I, Parpiev O 2022 Glass Phys. Chem. 48 327 Google Scholar
[40]	Heiba Z K, Mohamed M B, Badawi A, Abdellatief M 2022 J. Mater. Sci. -Mater. Electron. 33 10399 Google Scholar
[41]	Castellón E, Zayat M, Lévy D 2017 Adv. Funct. Mater. 28 04717 Google Scholar
[42]	Chu J Y, Sun Y C, Han X J, Zhang B, Du Y C, Song B, Xu P 2019 ACS Appl. Mater. Interfaces 11 18475 Google Scholar
[43]	Maleki K, Abdizadeh H, Golobostanfard M R, Adelfar R 2017 Appl. Surf. Sci. 394 37 Google Scholar

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Effects of different compositional ratios on physical structure and optical properties of thin films during alloying of Zn²⁺ and TiO₂

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Corresponding author: Mamatrishat Mamat, rxtmmt@xju.edu.cn

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Effects of different compositional ratios on physical structure and optical properties of thin films during alloying of Zn2+ and TiO2

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Authors and contacts

Corresponding author: Mamatrishat Mamat, rxtmmt@xju.edu.cn

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Effects of different compositional ratios on physical structure and optical properties of thin films during alloying of Zn²⁺ and TiO₂