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研究生： 高蒂雅
Deepa Kathiravan
論文名稱： ZnO-based Hybrid Nanomaterials for Multifunctional Sensing Applications
ZnO-based Hybrid Nanomaterials for Multifunctional Sensing Applications
指導教授： 黃柏仁
Bohr-Ran Huang
口試委員: 黃柏仁
周賢鎧
Yonhua Tzeng
Kung-Hwa Wei
學位類別： 博士
Doctor
系所名稱： 電資學院 - 電子工程系
Department of Electronic and Computer Engineering
論文出版年： 2019
畢業學年度： 107
語文別： 英文
論文頁數： 153
中文關鍵詞： ZnO NTs/N-UNCD 、ZnO NTs/graphene 、self-assembled heterostructure 、La-coated ZnO NRs 、ZnO-sericin 、detection of acetone in water 、UV photodetector 、H2 sensor
外文關鍵詞： ZnO NTs/N-UNCD, ZnO NTs/graphene, self-assembled heterostructure, La-coated ZnO NRs, ZnO-sericin, detection of acetone in water, UV photodetector, H2 sensor
相關次數： 點閱：306  下載：0 
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    • In this dissertation, ZnO nanorods (NRs) and nanotubes (NTs) have utilized as a common material to form hybrids for high-performance sensors. Each study has separated into different chapters, which focuses on the preparation of ZnO-based hybrid for specific sensor applications including the detection of acetone, H2 and UV light. First, the synthesis of nitrogen-incorporated ultra-nanocrystalline diamond (N-UNCD)/ZnO NTs nanohybrid and utilized for the detection of acetone in water using a novel strategy. No other reports are focused on the detection of acetone in water. The fascinating combination of these wide band gap semiconductor materials exhibit high sensor response (89 mV/mL), high stability and long-term reliability (tested after 60 days). Second, the self-assembled hierarchical interfaces of ZnO NTs and graphene with three novel heterostructures (SH1, SH2 andSH3) and utilizes as hydrogen sensors. This is the first study which focuses on ZnO NTs and graphene heterostructure with self-assembled morphologies for hydrogen sensor. The systematic investigation revealed that SH1 sensor exhibits an ultrahigh sensor response even at a low detection level of 10 ppm (14.3%) to 100 ppm (28.1%) compared to those of the SH2 and SH3 sensors. Third, the preparation of low-cost biofilms with the use of ZnO and silk-sericin protein (SSP) for the detection of H2 and UV sensors. This is the first study which presents the formation mechanism of ZnO and SSP based biofilms. The biofilm exhibits an ultra-fast response of 31.24% at 100 ppm while the UV sensor shows an effective switch-ratio (Iphoto/Idark) of 100 when compared to the as-prepared ZnO. Later, the preparation of La-coated ZnO NRs with the discontinuous lattice coating of La3+ on the surface of ZnO NRs and utilizes as multifunctional sensors to detect UV light and H2 gas. Moreover, this is the first study to focuses on the detection of H2 gas using La-coated ZnO NRs. An ultra-high H2 response of 63.8% was achieved even at a low detection level (ppm) with an ultra-fast response (15 s) and recovery time (9 s). Also, excellent UV sensing properties were observed with a high switch ratio (Iphoto/Idark) of 256.3. The salient features of this study are its reliability, simple synthesis method, and long-term stability, which makes each hybrid a promising candidate for new generation hydrogen sensors, acetone sensors, and UV photodetectors.

    In this dissertation, ZnO nanorods (NRs) and nanotubes (NTs) have utilized as a common material to form hybrids for high-performance sensors. Each study has separated into different chapters, which focuses on the preparation of ZnO-based hybrid for specific sensor applications including the detection of acetone, H2 and UV light. First, the synthesis of nitrogen-incorporated ultra-nanocrystalline diamond (N-UNCD)/ZnO NTs nanohybrid and utilized for the detection of acetone in water using a novel strategy. No other reports are focused on the detection of acetone in water. The fascinating combination of these wide band gap semiconductor materials exhibit high sensor response (89 mV/mL), high stability and long-term reliability (tested after 60 days). Second, the self-assembled hierarchical interfaces of ZnO NTs and graphene with three novel heterostructures (SH1, SH2 andSH3) and utilizes as hydrogen sensors. This is the first study which focuses on ZnO NTs and graphene heterostructure with self-assembled morphologies for hydrogen sensor. The systematic investigation revealed that SH1 sensor exhibits an ultrahigh sensor response even at a low detection level of 10 ppm (14.3%) to 100 ppm (28.1%) compared to those of the SH2 and SH3 sensors. Third, the preparation of low-cost biofilms with the use of ZnO and silk-sericin protein (SSP) for the detection of H2 and UV sensors. This is the first study which presents the formation mechanism of ZnO and SSP based biofilms. The biofilm exhibits an ultra-fast response of 31.24% at 100 ppm while the UV sensor shows an effective switch-ratio (Iphoto/Idark) of 100 when compared to the as-prepared ZnO. Later, the preparation of La-coated ZnO NRs with the discontinuous lattice coating of La3+ on the surface of ZnO NRs and utilizes as multifunctional sensors to detect UV light and H2 gas. Moreover, this is the first study to focuses on the detection of H2 gas using La-coated ZnO NRs. An ultra-high H2 response of 63.8% was achieved even at a low detection level (ppm) with an ultra-fast response (15 s) and recovery time (9 s). Also, excellent UV sensing properties were observed with a high switch ratio (Iphoto/Idark) of 256.3. The salient features of this study are its reliability, simple synthesis method, and long-term stability, which makes each hybrid a promising candidate for new generation hydrogen sensors, acetone sensors, and UV photodetectors.

    Abstract………………………………………………………………………...i Acknowledgments…………………………………………………………….ii Outline………………………………………………………………………….iii List of Figures………………………………………………………………….vii List of Tables…………………………………………………………………..xiv Chapter 1 Introduction 1.1 Overview of ZnO to nanohybrid-ZnO in sensor applications……1 1.2 Motivation……………………………………………………………3 1.3 Organization of this dissertation…………………………………4 Chapter 2 Literature review 2.1 Materials and applications……………………………………………5 2.1.1 Introduction of ZnO NRs/NTs …………………………………5 2.1.2 Introduction of nanodiamond materials…………………11 2.1.3 Introduction of graphene materials…………………………15 2.1.4 Introduction of SSP- A natural biopolymer…………………18 2.1.5 Introduction of La2O3 nanomaterials……………………………20 2.2 Acetone sensor applications…………………………………………21 2.3 Hydrogen sensor applications…………………………………………22 2.4 Ultra-violet photodetector applications………………………………24 Chapter 3 Experimental techniques and characterizations 3.1 Synthesis of materials……………………………………………………25 3.1.1 Synthesis of ZnO NRs/NTs…………………………………………26 3.1.2 Synthesis of Nanodiamonds and ZnO NTs/Nanodiamond hybrid…28 3.1.3 Synthesis of graphene and ZnO NTs/graphene heterostructures……30 3.1.4 Synthesis of SSP and ZnO-SSP biofilms…………………………31 3.1.5 Synthesis of La-doped ZnO NRs…………………………………32 3.2 Characterization of materials 3.2.1 Field emission scanning electron microscopy (FESEM) analysis…32 3.2.2 Transmission Electron microscopy (TEM) analysis………………32 3.2.3 Atomic force microscopy (AFM) analysis……………………………32 3.2.4 Raman studies…………………………………………………………33 3.2.5 X-ray photoelectron spectroscopy (XPS) analysis……………………33 3.2.6 UV-Visible spectroscopy investigations………………………………33 3.2.7 X-ray diffraction (XRD) spectrum analysis…………………………33 3.3 Electrochemical sensor fabrication and measurement system…………34 3.4 Gas sensor fabrication and measurement system………………………35 3.5 UV-photodetector fabrication and measurement system……………35 Chapter 4 Hybrid assembly of ZnO NTs and Nanodiamond for the detection of acetone in water 4.1 Research Background……………………………………………………37 4.2 Results and Discussion 4.2.1 Morphology and structural characterization…….…….…….……….39 4.2.2 Acetone sensing properties…….…….…….…….…….…….………42 4.2.3 Possible sensing mechanism…….…….…….…….…….…….………46 4.3 Summary…….…….…….…….…….…….…….…….…….…….……….53 Chapter 5 Hierarchical ZnO NTs and graphene interfaces of hydrogen sensing properties at room temperature 5.1 Research Background…….…….…….…….…….…….…….…………54 5.2 Results and Discussion…….…….…….…….…….…….…….…….……56 5.2.1 Morphology and structural characterization…….…….…….……….56 5.2.2 Hydrogen sensing properties…….…….…….…….…….…….…….63 5.2.3 Sensing mechanism…….…….…….…….…….…….…….…….….67 5.2.4 Stability measurements…….…….…….…….…….…….…….…….70 5.3 Summary…….…….…….…….…….…….…….…….…….…….………75 Chapter 6 Preparation of biofilms using SSP and ZnO for multisensing properties at room temperature 6.1 Research Background…….…….…….…….…….…….…….…….…….76 6.2 Results and Discussion…….…….…….…….…….…….…….…….……78 6.2.1 Morphology and structural characterization…….…….…….………..79 6.2.2 Gas sensing properties…….…….…….…….…….…….…….………86 6.2.3 UV sensing properties…….…….…….…….…….…….…….…….…90 6.2.4 Hydrogen and UV Sensing Mechanism…….…….…….…….……….94 6.3 Summary…….…….…….…….…….…….…….…….…….…….……….100 Chapter 7 Concurrent Enhancement in H2 and UV Sensing Properties of La3+-doped ZnO NRs 7.1 Research Background…….…….…….…….…….…….…….…….……101 7.2 Results and Discussion…….…….…….…….…….…….…….…….……101 7.2.1 Morphology and structural characterization…….…….…….……….103 7.2.2 H2 sensing properties…….…….…….…….…….…….…….……….109 7.2.3 UV sensing properties…….…….…….…….…….…….…….………116 7.2.4 UV and H2 sensing mechanism…….…….…….…….…….…….…...118 7.3 Summary…….…….…….…….…….…….…….…….…….…….……….122 Chapter 8 Conclusion and Future work…….…….…….…….…….……….123 8.1 Concluding remarks…….…….…….…….…….…….…….…….………123 8.2 Future work…….…….…….…….…….…….…….…….…….…….……125 References…….…….…….…….…….…….…….…….…….…….…….……126 Authors Biography............................152 List of Publications…….…….…….…….…….…….…….…….…….……...153

    Chapter 1

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    Chapter 4

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    Chapter 5

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    [16] Khan, M.; Tahir, M. N.; Adil, S. F.; Khan, H. U.; Rafiq, M.; Siddiqui, H.; Al-warthan, A. A.; Tremel, W. Graphene based Metal and Metal Oxide Nanocomposites: Synthesis, Properties and their Applications. J. Mater. Chem. A, Vol. 3, pp. 18753-18808 (2015).
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    [18] Zhang, Z.; Xue, Q.; Du, Y.; Ling, C.; Wei, X. Highly Enhanced Sensitivity of Hydrogen Sensors using Novel Palladium-Decorated Graphene Nanoribbon Film/SiO2/Si Structures, J. Mater. Chem. A, Vol. 2, pp. 15931–15937 (2014).
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    [29] Jiang, Q.; Yuru, G.; Baiyi, Z.; Yuxiang, L.; Xincun, D. Transition-Metal-Doped p-Type ZnO Nanoparticle-Based Sensory Array for Instant Discrimination of Explosive Vapors. Small, Vol. 12, pp. 1369–1377 (2016).

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    [39] Hsueh, T. J.; Chang, S. J.; Hsu, C. L.; Lin, Y. R.; Chend, I. C. ZnO Nanotube Ethanol Gas Sensors. J. Electrochem. Soc., Vol. 155, pp. 152-155 (2008).

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    Chapter 6

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    [2] Wang, Y. T.; Whang, W. T.; Chen, C. H. Hollow V2O5 Nano Assemblies for High-Performance Room-Temperature Hydrogen Sensors. ACS Appl. Mater. Interfaces, Vol. 7, pp. 8480−8487 (2015).

    [3] Vijayalakshmi, K.; Karthick, K. Growth of Highly c-Axis Oriented Mg: ZnO Nanorods on Al2O3 Substrate towards High-Performance H2 Sensing. Int. J. Hydrogen Energy, Vol. 39, pp. 7165-7172 (2014).
    [4] Shivani, S.; Kapil, S.; Neena, J. A Hydrogen Gas Sensor using a Pt-Sputtered MWCNTs/ZnO Nanostructure. Meas. Sci. Technol., Vol. 25, pp. 085103 (2014).
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    [6] Yang, Z.; Wang, M.; Song, X.; Yan, G.; Ding, Y.; Bai, J. High-Performance ZnO/Ag Nanowire/ZnO Composite Film UV Photodetectors with Large Area and Low Operating Voltage. J. Mater. Chem. C., Vol. 2, pp. 4312–4319 (2014).

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    [8] Tianyou, Z.; Xiaosheng, F.; Meiyong, L.; Xijin, X.; Haibo, Z.; Bando, Y.; Dmitri, G. A Comprehensive Review of One-Dimensional Metal-Oxide Nanostructure Photodetectors. Sensors, Vol. 9, pp. 6504-6529 (2009).
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    [17] Huang, H.; Gong, H.; Chow, C. L.; Guo, J.; White, T. J.; Tse, M. S.; Tan, O. K. Low-Temperature Growth of SnO2 Nanorod Arrays and Tunable n-p-n Sensing Response of a ZnO/SnO2 Heterojunctions for Exclusive Hydrogen Sensors. Adv. Funct. Mater., Vol. 21, pp. 2680−2686 (2011).
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    [19] Shewale, P. S.; Lee, N. K.; Lee, S. H.; Kang, K. Y.; Yu, Y. S.; Ti Doped ZnO Thin Film based UV Photodetector: Fabrication and Characterization. J. Alloys Compd., Vol. 624, pp. 251–257 (2015).
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    Chapter 7

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    [8] Chinh, N. D.; Quang, N. D.; Lee, H.; Hien, T. T.; Hieu, N. M.; Kim, D.; Kim, C.; Kim, D. NO gas sensing kinetics at room Temperature under UV Light Irradiation of In2O3 Nanostructures. Sci. Rep. Vol. 6, pp. 35066 (2016).

    [9] Miccoli, B.; Cauda, V.; Bonanno, A.; Sanginario, A.; Bejtka, K.; Bella, F.; Fontana, M.; Demarchi, D. One-Dimensional ZnO/Gold Junction for Simultaneous and Versatile Multisensing Measurements. Sci. Rep., Vol. 6, pp. 29763 (2016).

    [10] Kwiatkowski, M.; Bezverkhyya, I.; Skompska, M. ZnO Nanorods Covered with a TiO2 Layer: Simple Sol–gel Preparation, and Optical, Photocatalytic and Photoelectrochemical properties. J. Mater. Chem. A, Vol. 3, pp. 12748 (2015).

    [11] Lim, Y. R.; Song, W.; Lee, Y.B.; Kim, S. K.; Hana, J. K.; Myunga, S.; Leea, S. S.; Ana, K. S.; Choi, C. J.; Lim, J. Horizontally-Connected ZnO-Graphene Hybrid Films for
    Multifunctional Devices. App. Sur. Sci., Vol. 379, pp. 238–241 (2016).

    [12] Jaisutti, R.; Kim, J.; Park, S. K.; Kim, Y. H. Low-Temperature Photochemically Activated Amorphous Indium Gallium-Zinc Oxide for Highly Stable Room-Temperature Gas Sensors. ACS Appl. Mater. Interfaces, Vol. 8, pp. 20192−20199 (2016).

    [13] Postica, V.; Holken, I.; Schneider, V.; Kaidas, V.; Polonskyi, O.; Cretu, v.; Tiginyanu, I.; Faupel, F.; Adelung, R.; Lupan, O. Multifunctional Device based on ZnO: Fe Nanostructured films with enhanced UV and Ultra-Fast Ethanol Vapor Sensing. Mater. Sci. Semicond. Process. Vol. 49, pp. 20–33 (2016).

    [14] Mishra, Y. K.; Gaurav, M.; Cretu, V.; Postica, V.; Lupan, O.; Reimer, T.; Paulowicz, I.; Hrkac, V.; Benecke, W.; Kienle, L.; Adelung, R.; Direct Growth of Freestanding ZnO Tetrapod Networks for Multifunctional Applications in Photocatalysis, UV Photodetection, and Gas Sensing. ACS Appl. Mater. Interfaces, Vol. 7, pp. 14303−14316 (2015).

    [15] Zou, Y.; Chen, S.; Sun, J.; Liu, J.; Che, Y.; Liu, X.; Zhang, J.; Yang, D. Highly Efficient Gas Sensor Using a Hollow SnO2 Microfiber for Triethylamine Detection. ACS Sens., Vol. 2, pp. 897−902 (2017).

    [16] Li, D.; Qin, L.; Zhao, P.; Zhang, Y.; Liu, D.; Liu, F.; Kang, B.; Wang, Y.; Song, H.; Zhang, T.; Lu. G. Preparation and Gas-sensing Performances of ZnO/CuO Rough Nanotubular Arrays for Low-Working Temperature H2S detection. Sens. Actuators, B, Vol. 254, pp. 834–841 (2018).
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    [18] Zhu, L.; Li, Y.; Zeng, W. Enhanced Ethanol Sensing and Mechanism of Cr-doped ZnO nanorods: Experimental and Computational Study. Ceram. Int., Vol. 43, pp. 14873–14879 (2017).

    [19] Hsu, C. L.; Chang, S. J. ZnO Doped ZnO 1D Nanostructures: Synthesis, Properties, and Photodetector Application. Small, Vol. 10 (22), pp. 4562–4585 (2014).

    [20] Bhati, V.J.; Ranwa, S.; Fanetti, M.; Valant, M.; Kumar, M. Efficient Hydrogen Sensor based on Ni-Doped ZnO Nanostructures by RF Sputtering. Sens. Actuators, B, Vol. 255, pp. 588–597 (2018).

    [21] Hsu, C. L.; Li, H. H.; Hsueh, T. J. Water- and Humidity-Enhanced UV Detector by Using p‑Type La-Doped ZnO Nanowires on Flexible Polyimide Substrate. ACS Appl. Mater. Interfaces, Vol. 5, pp. 11142−11151 (2013).

    [22] Xua, X.L.; Chenb, Y.; Maa, S.Y.; Lia, W.Q.; Maoaa, Y. Z. Excellent Acetone Sensor of La-Doped ZnO Nanofibers with Unique Bead-like Structures. Sens. Actuators, B, Vol. 213, pp. 222–233 (2015).

    [23] Tian, S.; Zhang, Y.; Zeng, D.; Wang, H.; Li, N.; Xie, C.; Panc, C.; Zhao, X. Surface Doping of La ions into ZnO Nanocrystals to Lower the Optimal Working Temperature for HCHO Sensing Properties. Phys. Chem. Chem. Phys., Vol. 17, pp. 27437 (2015).

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