本研究探討石墨烯之合成與多孔石墨烯電極在超級電容器上之應用。此外，研究中也分別利用化學還原法與化學氣相沉積法製備多孔石墨烯電極。
首先，本研究利用洛神花茶作為環保且無毒性的還原劑，開發低成本且具高效率的石墨烯化學還原製程。研究中也首次探討還原反應中花青素的參與，並提出可能的反應機制。而利用洛神花茶所還原製作出的可撓曲石墨烯薄膜電極，如果搭配家用微波爐進行數秒鐘的微波處理，即可使電極電阻大幅下降4個數量級，電極微結構由原本的層狀結構轉變為多孔結構，並使電極電容值上升至204.4 F g-1。
接著，研究中我們使用同樣富含花青素的黑豆水作為還原劑，藉由單一步驟製程的概念，同時達成還原氧化石墨烯與建構多孔複合材料的目的。本階段使用的多孔石墨烯複合電極，是利用黑豆水還原氧化石墨烯，並利用黑豆水中所含有的水溶性大豆蛋白質的熱誘導凝膠化特性，將還原後的混合溶液經冷卻與冷凍處理以製得水膠，該石墨烯與大豆蛋白質複合的水膠經微波處理後即成為多孔石墨烯複合電極。複合電極經微波處理後會在石墨烯表面產生均勻散布的奈米顆粒，並大幅提升電極導電性與電化學活性面積，該電極之電容值在充放電電流為0.1 A g-1時可達268.4 F g-1。
最後我們利用化學氣相沉積法，於活性碳纖維表面設計並製作出具3維多孔結構的聚苯胺/少層石墨烯包覆層。其中，藉由退火處理使活性碳纖維表面電鍍上的鎳顆粒形成網狀連通的結構，並作為石墨烯成長的基板。接著利用聚苯胺的包覆層保護成長在網狀鎳上的石墨烯層，將鎳金屬以蝕刻的方式移除，即可在活性碳纖維表面留下由聚苯胺/少層石墨烯包覆層所建構的空腔結構；包覆層在蝕刻中產生的破孔可使原本近似封閉的空腔結構轉為開放式的多孔空腔結構，除了可提升電極整體電化學活性表面積，也可使電解液更容易進入到電極的多孔結構中。因此，使此結構之電極可以在充放電電流為0.1 A g-1時達到400.2 F g-1的電容值與61.3 Wh kg-1的儲能量，
根據我們的研究顯示，含花青素的植物水性萃取物可作為具有相當潛力的氧化石墨烯還原劑。雖然利用這種製程製備出的石墨烯會因萃取物的吸附使表面產生改質，但同時也可以利用這種特性，輔以簡單快速的微波處理進而大幅改良電極微結構並提升電化學相關表現。此外，我們也利用化學氣相沉積法，在活性碳纖維表面包覆多孔的聚苯胺/少層石墨烯層，藉以製作出具有獨特多孔結構與優良電化學特性的可撓纖維電極。

In this dissertation, the studies on the graphene synthesis for graphene-based porous electrodes and their applications in supercapacitors have been investigated. Both the chemical reduced route and the chemical vapor deposition (CVD) method to synthesize graphene were used to design and fabricate the porous electrodes.
The aqueous extract of Hibiscus sabdariffa L., which is inherently non-toxic, environmentally friendly and cost effective, was used as a green reducing agent to chemically reduce graphene oxide (GO). And the investigation of anthocyanins during the reduction was first studied in our work. The flexible graphene film electrodes were fabricated using the synthesized graphene as a primary material. Furthermore, over four orders of magnitude in electric conductivity were achieved with an excellent specific capacitance of 204.4 F g-1 when the graphene film electrodes were treated in a household microwave oven.
Adopting an in situ construction strategy, green reduction of GO and the formation of an open porous structure are simultaneously completed in a one-pot process using an aqueous extract of another anthocyanin-containing plant, black soybean, as a green reducing agent. Graphene-based porous electrodes for supercapacitors were fabricated using the as-prepared graphene hydrogel as a primary material followed by microwave treating. Owing to the formation of uniformly dispersed nanoparticles on the graphene surface during microwave treating, both the electrical conductivity and the electroactive surface area were increased, as a consequence, the capacitance is significantly enhanced, reaching a capacitance of 268.4F g-1 at 0.1 A g-1.
Three-dimensional porous polyaniline/few-layer graphene-coated active carbon fiber (PANI/FLG-coated ACF) electrodes with the unique structure, where ACFs were covered with the open porous PANI/FLG layers, were investigated. Ni networks served as the template for graphene grown by annealing the electrodeposited Ni clusters on the surface of ACFs. After CVD, FLG was synthesized on the Ni surface which was subsequently coated with PANI serving as capacitive materials and supporting layers for FLG in the construction of shell structures during Ni etching. The surface combined pultruded structure and cavity network formed with the PANI/FLG coatings, where holes on the cavity increased the electroactive surface area and facilitated penetration of the electrolyte into the cavity networks. As a result, an average specific capacitance of 400.2 F g-1 and an energy density of 61.3 Wh kg−1 at a charging current of 0.1 A g−1 over the PANI/FLG-coated ACFs electrodes were achieved.
Based on the results, it is concluded that the extract of anthocyanin-containing plant can be a promising, potential, and green reducing agent for graphene synthesis. The porous graphene-based electrodes could be further improved by microwave treating owing to the naturally modification of graphene by the extract compounds. In addition, the porous PANI/FLG-coated ACFs with unique structure and good electrochemical performance could be easily designed and fabricated through the CVD method.

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