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| DC 欄位 | 值 | 語言 |
|---|---|---|
| dc.contributor.advisor | 郭錦龍 | zh_TW |
| dc.contributor.advisor | Chin-Lung Kuo | en |
| dc.contributor.author | 王宗翌 | zh_TW |
| dc.contributor.author | TSUNG-YI WANG | en |
| dc.date.accessioned | 2026-02-11T16:47:22Z | - |
| dc.date.available | 2026-02-12 | - |
| dc.date.copyright | 2026-02-11 | - |
| dc.date.issued | 2025 | - |
| dc.date.submitted | 2026-01-26 | - |
| dc.identifier.citation | [1] K.-F. Aguey-Zinsou and J.-R. Ares-Fernández. Hydrogen in magnesium: new perspectives toward functional stores. Energy & Environmental Science, 3(5):526–543,2010.
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| dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/101614 | - |
| dc.description.abstract | 氫能儲存的實際應用長期受限於材料的脫氫動力學遲滯與高能障問題。鎂氫化物(MgH2)因具備高氫含量與良好可逆性而被視為具潛力的儲氫材料，然而其強烈的鎂氫鍵結導致氫釋放困難，嚴重限制其脫氫效率。
本研究透過第一原理密度泛函理論，系統性探討石墨烯–氫化鎂異質接面對脫氫行為的影響，並比較完整石墨烯、含結構缺陷石墨烯以及硼摻雜石墨烯所形成之異質界面。藉由分析結構穩定性、氫空缺形成能、電子結構特性與反應路徑，釐清界面交互作用在氫釋放過程中的關鍵角色。 計算結果顯示，相較於純氫化鎂表面，石墨烯–氫化鎂異質接面可顯著降低氫空缺形成所需的能量；其中，缺陷與硼摻雜石墨烯界面能進一步穩定二配位氫空缺構型，顯示空缺能量行為高度依賴於界面原子結構。電子結構分析指出，異質界面產生明顯的電荷重新分佈，促進電子由氫化鎂向石墨烯轉移，進而降低氫移除相關能障。 反應路徑分析進一步顯示，完整石墨烯主要促進單階段脫氫機制，而缺陷與硼摻雜石墨烯則引入具較低能障的雙階段脫氫途徑。上述結果證實，石墨烯修飾不僅能提升氫化鎂的脫氫動力學，也會改變其脫氫反應機制。 本研究從原子尺度提供缺陷與摻雜石墨烯界面調控氫化鎂脫氫行為的關鍵見解，並為高效石墨烯基儲氫觸媒的設計提供理論依據。 | zh_TW |
| dc.description.abstract | Hydrogen storage remains constrained by slow kinetics and high activation barriers in magnesium-based hydrides, limiting their practical deployment. Magnesium hydride (MgH2) is attractive due to its high hydrogen capacity and reversibility; however, its dehydrogenation performance is hindered by strong Mg–H bonding and sluggish hydrogen release.
Density functional theory–based first-principles calculations were used to explore how pristine graphene, defect-engineered graphene, and boron-doped graphene modify the dehydrogenation behavior of MgH2. Structural stability, hydrogen vacancy formation energetics, electronic structure characteristics, and reaction pathways are analyzed to clarify the role of graphene–MgH2 interfacial interactions. The calculated results demonstrate that graphene–MgH2 heterojunctions substantially reduce the energetic cost associated with hydrogen vacancy formation compared with bare MgH2 surfaces. Defective and boron-doped graphene further enhance this effect by stabilizing twofold-coordinated hydrogen vacancy configurations. Electronic structure analyses indicate pronounced charge redistribution at the heterointerface, facilitating electron transfer from MgH2 to graphene and lowering the energy cost of vacancy formation. Reaction pathway calculations demonstrate that pristine graphene primarily promotes a one-stage hydrogen desorption mechanism, whereas defective and boron-doped graphene introduce an alternative two-stage pathway with reduced activation barriers. These findings confirm that graphene modification not only accelerates hydrogen release kinetics but also alters the underlying dehydrogenation mechanism of MgH2. This study provides atomistic-level insight into defect- and dopant-assisted graphene interfaces and offers practical design guidelines for graphene-based catalysts aimed at improving hydrogen storage performance. | en |
| dc.description.provenance | Submitted by admin ntu (admin@lib.ntu.edu.tw) on 2026-02-11T16:47:22Z No. of bitstreams: 0 | en |
| dc.description.provenance | Made available in DSpace on 2026-02-11T16:47:22Z (GMT). No. of bitstreams: 0 | en |
| dc.description.tableofcontents | Verification Letter from the Oral Examination Committee i
Acknowledgements iii 摘要 v Abstract vii Contents ix List of Figures xiii List of Tables xxi Denotation xxiii Chapter 1 Introduction 1 1.1 Background. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1 1.2 Hydrogen Storage System. . . . . . . . . . . . . . . . . . . . . .. . . 2 1.2.1 Hydrogen Storage Strategies. . . . . . . . . . . . . . . . . . . . . 2 1.2.2 Types of Metal Hydrides. . . . . . . . . . . . . . . . . . . . . . . 3 1.2.2.1 Interstitial Metal Hydrides. . . . . . . . . . . . . . . . 3 1.2.2.2 Non-Interstitial Metal Hydrides. . . . . . . . . . . . . 4 1.2.3 Hydrogenation and Dehydrogenation in Mg/MgH2 Systems. . . . . 6 1.3 Improvement Strategies for Mg/MgH2and Enhancement of Kinetic Performance. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6 1.3.1 Alloying Treatment. . . . . . . . . . . . . . . . . . . . . . . . . . 7 1.3.2 Nanosizing. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8 1.3.3 Catalyst Doping. . . . . . . . . . . . . . . . . . . . . . . . . . . . 10 1.3.4 Carbon-Based Catalysts in Hydrogen Storage. . . . . . . . . . . . 12 1.3.5 Defect Types in Reduced Graphene Oxide. . . . . . . . . . . . . . 14 1.4 Motivation and Objectives. . . . . . . . . . . . . . . . . . . . . . . 17 Chapter 2 Theoretical Background 19 2.1 Density Functional Theory (DFT). . . . . . . . . . . . . . . . . . . 19 2.1.1 Hohenberg–Kohn Theorem. . . . . . . . . . . . . . . . . . . . . . 20 2.2 Kohn-Sham Method. . . . . . . . . . . . . . . . . . . . . . . . . . 21 2.2.1 Exchange–Correlation Functional. . . . . . . . . . . . . . . . . . 26 2.2.2 Pseudopotential. . . . . . . . . . . . . . . . . . . . . . . . . . . . 27 2.3 Grimme DFT-D3 van der Waals correction. . . . . . . . . . . . . . 28 2.4 Transition State Search Methods. . . . . . . . . . . . . . . . . . . . 30 2.4.1 Nudged Elastic Band Method (NEB). . . . . . . . . . . . . . . . . 30 2.4.1.1 Climbing Image NEB Method (CI-NEB). . . . . . . . 31 2.4.2 Dimer Method. . . . . . . . . . . . . . . . . . . . . . . . . . . . . 32 Chapter 3 Methodology 35 3.1 Computational Details.........................35 3.2 Structure Construction. . . . . . . . . . . . . . . . . . . . . . . . . . 37 3.3 Atomic Labeling System. . . . . . . . . . . . . . . . . . . . . . . . 40 3.4 Hydrogen Vacancy Formation Energy. . . . . . . . . . . . . . . . . 45 3.5 Energy Calculations in Reaction Pathways. . . . . . . . . . . . . . 46 Chapter 4 Results and Discussion 49 4.1 Hydrogen Vacancy Formation. . . . . . . . . . . . . . . . . . . . . 49 4.1.1 Hydrogen Vacancy Formation Energy in MgH2 and Modified Graphene–MgH2 Systems. . . . . . . . . . . . . . . . . . . . . . . . . . . . 50 4.1.2 Electronic Properties of Hydrogen Vacancy Structures. . . . . . . . 54 4.1.3 Extended Influence of Defective and Boron-Doped Graphene on Hydrogen Vacancy Formation Energy. . . . . . . . . . . . . . . . . . 74 4.1.4 Electronic Properties of Hydrogen Vacancies at Sites Distant from Defects or Dopants. . . . . . . . . . . . . . . . . . . . . . . . . . 75 4.1.5 Summary. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 77 4.2 Hydrogen Desorption Mechanisms in Graphene–MgH2Systems. . . 78 4.2.1 One-Stage Desorption. . . . . . . . . . . . . . . . . . . . . . . . . 78 4.2.1.1 Electronic Properties of One-Stage Desorption. . . . . 90 4.2.2 Two-Stage Desorption. . . . . . . . . . . . . . . . . . . . . . . . 92 4.2.2.1 Electronic Properties of Two-Stage Desorption. . . . . 105 4.3 Migration of H2at the Graphene/MgH2 Interface. . . . . . . . . . . 108 4.4 Comparative Effects of Graphene Defects and Doping. . . . . . . . 111 4.4.1 Impact of DV(5–8–5) and 2SW Defects on Desorption Behavior. . 112 4.4.2 Influence of Boron Doping Concentration on Dehydrogenation. . . 114 Chapter 5 Conclusion 117 References 119 Appendix A — Supporting Information 127 A.1 Relaxed Structure of Hydrogen Adsorption on Graphene. . . . . . . 127 A.2 Hybridization of the Transition State in One-Stage Desorption. . . . 128 A.3 Hybridization of the Transition State in Two-Stage Desorption. . . . 129 A.4 Electronic Properties of DV(5–8–5)G/MgH2, 2SWG/MgH2, and 2BG/MgH2. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 131 A.5 Lattice Mismatch in Heterojunction Structures. . . . . . . . . . . . 133 A.5.1 Lattice Mismatch Influence on Vacancy Formation. . . . . . . . . 134 A.6 Hydrogen Storage Properties of Mg-Based Alloys. . . . . . . . . . 134 | - |
| dc.language.iso | en | - |
| dc.subject | 固態儲氫 | - |
| dc.subject | 密度泛函理論 | - |
| dc.subject | 氫化鎂 | - |
| dc.subject | 石墨烯 | - |
| dc.subject | 硼摻雜 | - |
| dc.subject | 缺陷石墨烯 | - |
| dc.subject | 氫脫附機制 | - |
| dc.subject | Solid-State Hydrogen Storage | - |
| dc.subject | Density Functional Theory | - |
| dc.subject | Magnesium Hydride | - |
| dc.subject | Graphene | - |
| dc.subject | Boron-doped | - |
| dc.subject | Defective Graphene | - |
| dc.subject | Hydrogen Desorption Mechanism | - |
| dc.title | 以第一原理計算探討缺陷石墨烯與硼摻雜石墨烯對氫化鎂之脫氫行為和機制的影響 | zh_TW |
| dc.title | First-Principles Study of the Effects of Defective Graphene and Boron-Doped Graphene on the Dehydrogenation Behavior and Mechanism of MgH2 | en |
| dc.type | Thesis | - |
| dc.date.schoolyear | 114-1 | - |
| dc.description.degree | 碩士 | - |
| dc.contributor.oralexamcommittee | 許文東;李明憲;吳鉉忠;陳馨怡 | zh_TW |
| dc.contributor.oralexamcommittee | Wen-Dung Hsu;Ming-Hsien Lee;Hsuan-Chung Wu;Hsin-Yi Chen | en |
| dc.subject.keyword | 固態儲氫,密度泛函理論氫化鎂石墨烯硼摻雜缺陷石墨烯氫脫附機制 | zh_TW |
| dc.subject.keyword | Solid-State Hydrogen Storage,Density Functional TheoryMagnesium HydrideGrapheneBoron-dopedDefective GrapheneHydrogen Desorption Mechanism | en |
| dc.relation.page | 134 | - |
| dc.identifier.doi | 10.6342/NTU202600185 | - |
| dc.rights.note | 同意授權(全球公開) | - |
| dc.date.accepted | 2026-01-27 | - |
| dc.contributor.author-college | 工學院 | - |
| dc.contributor.author-dept | 材料科學與工程學系 | - |
| dc.date.embargo-lift | 2031-01-19 | - |
| 顯示於系所單位： | 材料科學與工程學系 | |
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