| 摘要: | 本計畫研究具形態可控性之石墨烯，包含可控之結構、官能基團、邊界態、異質改質。這些特性會影響石墨烯許多基礎的界面特性並對後續的各領域實際應用有重要影響，特別是能解決長久以來各種奈米能源材料或石墨烯無法實際應用於儲能元件的缺失，如低能量密度與穩定性。本計劃提出新穎的合成方法、分析技術、組裝電極結構、功能化奈米觸媒等，期望於三年的研究歷程於多功能化石墨烯於能源應用的開展或突破侷限。研究內容第一年為石墨烯邊界態的功能化可控性之研究，包含: 建立合成規則性邊界態/官能基團可控性之新穎製程、邊界態臨場異質原子改質之製程建立、石墨烯超強附著力與防腐蝕效能增強。第二年主題為邊界型態可控石墨烯於儲能的機制的研究與效能評估，包含: 邊界選擇性改質與官能基對電解質與電子/離子傳導的模型建立、人工SEI膜於鋰金屬電極的效能與穩定性研究探討、低溫快速製備石墨烯核殼結構建立、發展可達高能量密度的石墨烯新穎電極結構。第三年主題為多形態石墨烯異質材料複合之前瞻觸媒研究評估，包含: 電泳沉積於臨場高方向性排列之氟化石墨烯功能複合材料、超快熱製程於合成均質之單原子觸媒的新方法、發展3D架構之石墨烯複合觸媒於電產氫之研究、共摻雜異質改質石墨烯的觸媒特性與應變增強觸媒活性、參雜異質原子於硫化鉬觸媒的穩定性增強。 ;The recent works with graphene for the clean energy-related applications have been found to block the practical usage due to the uncontrollable and complex nanostructure and chemical moieties. For example, the extremely high surface area of graphene are expected to ideal materials in an energy storage device like supercapacitor and LIB; however, it suddenly found that the lots of exposed edge state and versatile, functional groups intensively participate the electrochemical reaction that in turn facilitate the unstable and even degradation on device performance. Another issue is graphene shows lower energy density when restacking thus hinder practical use. All for these yet to be addressed due to the lack of controllable route for manipulation of graphene moieties (like macro/atomic structure, edge-state, selective functional groups, etc.) so as unable to realize their board applications.In this proposal, we develop a series of strategy and research protocol aim to manipulate graphene by inheriting the merits of both outperformed properties of graphene and homogenous while controllable graphene moieties with high working stability, where the fundamental physical/chemical properties and the further extended energy applications will be conducted. Here, the defined graphene moieties, including the fine tailoring of multi-structured graphene architecture, functional groups, edge state, and their heteroatomic doping. A newly developed method is proposed to create the regular graphene edges, hetero-atomic doping(N-, P-,B-,S- and co-doping) and selective functionalization through the proposed in-situ treatment through specious-selective remote plasma or rapid heating with precursors. The interface reactions against various electrolyte and their reliability, such as the artificial solid electrolyte interphase (SEIs), on energy storage devices (battery and supercapacitor) will be conducted. Moreover, we develop a method to prepare the single atomic catalysts (SACs) by comprising the graphene architecture as a catalyst supporting frameworks, and their heteroatomic doping, the catalyst activity and performance are investigated on HER and further extend to module and system applications. |
