Nghiên cứu vật liệu nano siêu mỏng mos2 pha tạp nitơ và vật liệu tổng hợp graphene mos2 chế tạo bằng phương pháp điện hóa plasma ứng dụng cho phản ứng sản sinh hydrô

國立交通大學 材料科學與工程學系 博士論文 電漿電化學法製備氮摻雜二硫化鉬奈米片及石墨烯-二硫 化鉬複合材料及其產氫應用 Nitrogen Doped MoS2 Nanosheets and Graphene/MoS2 Composite Prepared by Electrolysis Plasma-Induced Process for Hydrogen Evolution Reaction 研究生: 阮文長 指導教授：韋光華 博士 中華民國一零九年四月 電漿電化學法製備氮摻雜二硫化鉬奈米片及石墨烯-二硫化鉬複合 材料及其產氫應用 Nitrogen Doped MoS2 Nanosheets and Graphene/MoS2 Composite Prepared by Electrolysis Plasma-Induced Process for Hydrogen Evolution Reaction 研究生：阮文長 Student: Nguyen Van Truong 指導教授：韋光華 博士 Advisor: Dr Kung-Hwa Wei 國立交通大學 材料科學與工程學系 博士論文 A Dissertation Submitted to Department of Materials Science and Engineering College of Engineering National Chiao Tung University in partial Fulfillment of the Requirements for the Degree of Doctor of Philosophy in Materials Science and Engineering March 2020 Hsinchu, Taiwan, Republic of China 中華民國一零九年四月 摘要 為了獲得可持續的富含地球的電催化劑材料，在氫析出反應（HER）中顯示出高性能， 在這裡我們提出了一種簡便的一鍋電漿電化學工藝，用於製造氮摻雜的二硫化鉬奈米 片和石墨烯/ 二硫化鉬複合材料。已經開發出一種有效的一步法，該方法涉及在短時間 內且在低溫（約 80°C）下同時進行二硫化鉬奈米片的電漿摻雜和剝落。特別地，可以 在浸沒的陰極尖端處產生有效的電漿區，以實現將氮原子摻雜到半導體性 2H-二硫化鉬 結構中。在二硫化鉬結構中氮摻雜和剝落的協同作用下調節電子和輸運性質，以增強 其催化活化作用。研究發現，在摻氮的二硫化鉬奈米片上，氮原子濃度為 5.2 at％時， 具有出色的催化氫析出反應，在 10 mA cm–2 的電流密度下，低過電位為 164 mV，Tafel 斜率較小，為 71 mV dec-1 –遠低於剝落的二硫化鉬奈米片（207 mV，82 mV dec-1）和塊 狀二硫化鉬（602 mV，198 mV dec-1），達到在 0.5 M 硫酸水溶液 25 小時內的長期穩定 性。有趣的是，在批量反應中通過簡單選擇陰極材料則可獲得兩種不同形態的石墨烯 片，其中可得到洋蔥狀的二硫化鉬奈米片（OGNs @ 二硫化鉬）和片狀的石墨烯包裹的 二硫化鉬複合物（GNs @ 二硫化鉬）。我們發現石墨烯片的存在似乎是增強 HER 能力 的關鍵。因此，我們得出的結論是，石墨烯-二硫化鉬奈米片界面上的電子耦合在增強 二硫化鉬奈米片界面上的電子耦合在增強 HER 活性方面也起著重要作用。我們的 OGNs @ 二硫化鉬複合材料表現出較高的 HER 性能，在 10 mA cm-2 的電流密度下具有 118 mV 的低過電位，Tafel 斜率在 dec-1 的 Tafel 斜率，以及長期的穩定性而不會降解。該性能 比片狀石墨烯包裹的二硫化鉬複合材料 GNs @ 二硫化鉬（182 mV，82 mV dec-1）要好得 多。這種方法似乎是一種有效且簡單的策略，不僅可以調節摻氮過渡金屬硫化物 （TMDCs）材料，還可以調節石墨烯和 TMDCs 複合材料的形貌，從而適用於廣泛的能 源應用。 i Nitrogen Doped MoS2 Nanosheets and Graphene/MoS2 Composite Prepared by Electrolysis Plasma-Induced Process for Hydrogen Evolution Reaction Student: Nguyen Van Truong Advisor: Prof Kung-Hwa Wei Department of Materials Science and Engineering National Chiao Tung University Abstract With the goal of obtaining sustainable earth-abundant electrocatalyst materials displaying high performance in the hydrogen evolution reaction (HER), here we propose a facile one-pot plasma-induced electrochemical process for the fabrication of both nitrogen-doped MoS2 nanosheets and graphene/MoS2 composite An efficient one-step approach that involves simultaneous plasma-induced doping and exfoliating of MoS2 nanosheets within a short time and at a low temperature (ca 80 °C) has been developed Particularly, an active plasma zone can be generated at the submerged cathode tip to achieve doping of nitrogen atoms into the semiconducting 2H-MoS2 structure The electronic and transport properties were modulated under the synergy of the nitrogen doping and exfoliation in the MoS2 structure to enhance their catalytic activation It is found that the N concentration of 5.2 at % at N-doped MoS2 nanosheets have excellent catalytic hydrogen evolution reaction where a low over-potential of 164 mV at a current density of 10 mA cm–2 and a small Tafel slope of 71 mV dec–1—much lower than those of exfoliated MoS2 nanosheets (207 mV, 82 mV dec–1) and bulk MoS2 (602 mV, 198 mV dec–1)—as well as an extraordinary long-term stability of >25 h in 0.5 M H2SO4 can be achieved Interestingly, through a simple selection of cathode materials in one-batch process, two different morphologies of graphene sheets were obtained, resulting in both onion-like covered MoS2 nanosheets (OGNs@MoS2) and sheets-like graphene wrapped MoS2 composites (GNs@MoS2) We found that the presence of the graphene sheets appeared to be a key aspect of the enhanced HER ability Therefore, we conclude that electronic coupling at the graphene– ii MoS2 nanosheet interfaces also played an important role in enhancing the HER activity Our OGNs@MoS2 composites exhibited high HER performance, characterized by a low overpotential of 118 mV at a current density of 10 mA cm–2, a Tafel slope of 73 mV dec–1, and long-time stability without degradation; this performance is much better than that of the sheetlike graphene-wrapped MoS2 composite GNs@MoS2 (182 mV, 82 mV dec–1) This approach appears to be an effective and simple strategy for tuning not only nitrogen-doped transition metal dichalcogenide (TMDCs) materials but also the morphologies of composites of graphene and TMDCs materials for a broad range of energy applications KEYWORDS: MoS2, Nitrogen doped MoS2, Onion-like graphene, Graphene/MoS2 composite, One-pot Plasma-Induced exfoliation, Hydrogen evolution reaction, electrocatalyst iii ACKNOWLEDGMENTS This dissertation presents a summary of my research work which has done in the Department of Materials Science and Engineering (MSE), National Chiao Tung University (NCTU) It is a pleasure to express my sincere gratitude to all the people who helped and supported me during my Ph.D study From bottom of my heart I express my deep sense of gratitude and profound respect to my supervisor Prof Kung-Hwa Wei He continually and convincingly conveyed a spirit of adventure in regard to research and scholarship, and an excitement in regard to teaching Without his generous encouragement and brief advice for those years, this dissertation would not have been completed My sincere thanks Prof Yu-Lun Chueh for his kind guidance and persistent help I would like to thank Dr Yen Po-Jen, Dr Cheng Hao-Wen, Dr Chen Hsiu-Cheng, Dr VanQui Le, Mr Phuoc Anh Le, Mr Chung-Hao Chen, Mr Tzu-Yi Yang, Mr Yung-Chi Hsu, Mr Bo-Hsien Lin for their kind supporting in my research Many thanks to all participants in Prof Kung-Hwa Wei’s lab who took part in the study and enabled this dissertation to be possible In addition, I would like to thank all members of Vietnamese Student Association-NCTU who made my life in Taiwan really pleasurable and joyful Finally, special thanks for my parent, my wife and my two angels who always standing by my side Thank you for always encouraging me to pursue my dreams I love you all so much, thanks for loving me too! Nguyen Van Truong Hsinchu, Taiwan April 2020 iv Table of Content 摘要 i Abstract ii Acknowledgment iv Table of Content v Figures list vii Tables list xi Chapter Introduction 1.1 Introduction of Transition metal dichalcogenides 1.2 Production of Transition Metal Dichalcogenides materials 1.3 Introduction of cathodic plasma exfoliation method 1.4 Introduction of Electrocatalytic Hydrogen Evolution Reaction 1.5 Introduction of nitrogen doped MoS2 12 1.6 Introduction of graphene/MoS2 composite 14 1.7 Strategies to enhancing MoS2 catalytic activity 16 1.8 Thesis outline 20 Chapter Production Nitrogen-Doped Molybdenum Disulfide nanosheets through Plasma-Induced process and their electrocatalyst performance 21 2.1 Introduction 21 2.2 Experimental section 24 2.3 Results and discussion 27 2.4 Conclusions 50 v Chapter Production Graphene/MoS2 composite through One-Pot Plasma-Induced process and their Electrocatalyst performance 51 3.1 Introduction 51 3.2 Experimental section 54 3.3 Results and discussion 58 3.4 Conclusions 83 Chapter Conclusions 84 References 87 Vita 99 Publications list 101 vi Figures list Figure 1.1 The periodic table with highlighted transition metal and chalcogenide elements that form layered TMDCs materials Figure 1.2 The crystal struture of TMDCs with Octahedral (1T), Trigonal prismatic (2H) and (3R) coordination Figure 1.3 Six main production methods of TMDCs and their content Figure 1.4 Several TMDCs nanosheets production methods Figure 1.5 Typical of plasma electrolysis and its applications Figure 1.6 Experimental setup and mechanism of cathodic plasma exfoliation Figure 1.7 Schematic representation of the proposed mechanism of plasma exfoliation and nitrogen-doping Figure 1.8 I-V curve of overall water splitting 10 Figure 1.9 Schematic of the covalent nitrogen doping in MoS2 upon N2 plasma surface treatment 13 Figure 1.10 (a) Schematic illustration of the electrochemical deposition set-up; (b) Comparison of MoS2-3D graphene hybrid in solution and solid state supercapacitor 15 Figure 1.11 Synthesis procedure and structural model for mesoporous MoS2 with a doublegyroid morphology 17 Figure 1.12 the schematic preparation process of MoS2/N-RGO nanocomposite 19 Figure 2.1 (a) Experimental setup for plasma-induced exfoliation and (b) proposed mechanism of exfoliation and nitrogen-doping process 27 Figure 2.2 FE-SEM images of bulk commercial samples of (a) MoS2, (b) MoSe2, (c) WS2 and (d) WSe2, respectively 29 vii Figure 2.3 SEM images of exfoliated (a) MoS2, (b) MoSe2, (c) WS2 and (d) WSe2 nanosheets AFM images of exfoliated (e) MoS2, (f) MoSe2 and (h) WSe2 nanosheets Raman spectra of exfoliated (i) MoS2, (j) MoSe2, (k) WS2 and (l) WSe2 nanosheets 31 Figure 2.4 UV–Vis spectra of (a) MoS2, (b) MoSe2, (c) WS2 and (d) WSe2 nanosheets 32 Figure 2.5 Low-magnification TEM images of (a) MoS2, (b) MoSe2, (c) WSe2 and (d) WS2 nanosheets Insets show the corresponding SAED patterns HRTEM images recorded along the [001] zone axis Insets: their filtered of (e) MoS2 (f) MoSe2, (g) WSe2, and (h) WS2 STEM bright-field images of (i) MoS2, (j) MoSe2, (k)WS2 and (l) WSe2 nanosheets, and their element mapping images, respectively 33 Figure 2.6 (a) Difference in frequency between E12g and A1g in Raman spectra and (b) the lateral size of exfoliated MoS2 using different applied biases 35 Figure 2.7 (a) Mechanism of the N-doped MoS2 nanosheets (b-f) Dark-field STEM images of undoped MoS2 and N-doped MoS2 nanosheets and the corresponding EELS elemental mapping images of Mo, S and N with different electrolytes and/or plasma-induced time, respectively 36 Figure 2.8 The statistical distribution of the lateral size of (a) undoped MoS2, (b) N-doped MoS2 and (c) the thickness of MoS2 nanosheets 38 Figure 2.0.21 XPS spectra (a) survey, (b) S 2p and (c) Mo 3d of Undoped MoS2 and N-doped MoS2 nanosheets, respectively 39 Figure 2.9 SEM images of N-doped MoS2 after the plasma-induced exfoliation at (a) 200 oC, (b) 300 oC (c) 500 oC and their BF-STEM images(d-f), respectively, correspond with EDS mapping of Mo, S and N elements 41 Figure 2.10 Raman spectra of N-doped MoS2 nanosheets after the thermal annealing at (a) 200, (b)300, and (c)500 oC, respectively 42 Figure 2.11 (a) LSV curves (recorded on a glassy-carbon electrode) of bulk MoS2, undoped MoS2 and N-doped MoS2 (b) Corresponding Tafel plots derived from (a) (c) Nyquist plots acquired at –200 mV vs RHE of the bulk MoS2, undoped MoS2 and N-doped MoS2 (d) Durability test of the N-doped MoS2 catalyst, performed at an overpotential of 165mV vs RHE 45 viii REFERENCES (1) Dickinson, R G.; 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(b) Schematic representation of the proposed mechanism of OGNs @MoS2 and GNs @MoS2 58