| 研究生: |
林怡君 LIN, YI-JYUN |
|---|---|
| 論文名稱: |
氧化鈷與硼摻雜還原氧化石墨烯之複合物在氧氣還原與氧氣析出反應之應用 Composite of Cobalt Oxide and B-doped Reduced Graphite Oxide for Oxygen Reduction and Evolution |
| 指導教授: |
楊明長
Yang, Ming-Chang |
| 學位類別: |
碩士 Master |
| 系所名稱: |
工學院 - 化學工程學系 Department of Chemical Engineering |
| 論文出版年: | 2016 |
| 畢業學年度: | 104 |
| 語文別: | 中文 |
| 論文頁數: | 138 |
| 中文關鍵詞: | 硼摻雜還原氧化石墨烯 、氧化鈷 、氧氣還原反應 、氧氣析出反應 、雙功能性觸媒 |
| 外文關鍵詞: | Boron-doped reduced graphite oxide, cobalt oxide, oxygen reduction reaction, oxygen evolution reaciotn, bifunctional catalyst |
| 相關次數: | 點閱:137 下載:3 |
| 分享至: |
| 查詢本校圖書館目錄 查詢臺灣博碩士論文知識加值系統 勘誤回報 |
為因應全球環保及低碳生活議題,開發新型可再生或替代能源已是未來產業趨勢,本研究致力於發展低成本、高效能之雙功能性催化觸媒材料,應用於氧氣還原反應 (oxygen reduction reaction, ORR) 和氧氣析出反應 (oxygen evolution reaction, OER)。燃料電池中陰極的氧氣反應為反應速率步驟,目前仍以貴金屬(如Pt, Ru)或其氧化物為主要觸媒,但其價格昂貴且資源有限。本研究使用水熱法,以硼酸 (H3BO3) 將硼摻雜在還原氧化石墨烯的同時,將氧化鈷擔載在此碳材上,成為CoOx/B-rGO複合材料。利用石墨烯的高表面積的特性有效分散氧化鈷,結合硼摻雜還原氧化石墨稀 (B-rGO) 所造成的正電荷缺陷,提升氧氣還原及氧氣析出反應活性。
由XRD分析結果顯示,本研究以水熱法製備之氧化鈷擔載於硼摻雜還原氧化石墨烯,同時具有四氧化三鈷(Co3O4)和氫氧化鈷(Co(OH)2)的氧化鈷結晶型態。比較不同觸媒,在0.1 M KOH中以1 mV/s掃描速率進行LSV電化學測試,CoOx/0.5M B-rGO在氧氣還原反應的起始電位為-0.112 V (vs. Ag/AgCl),正於Co3O4和0.5M B-rGO;在氧氣析出反應的起始電位為-0.516 V(vs. Ag/AgCl),負於Co3O4和0.5M B-rGO。硼摻雜能同時提升氧氣還原與氧氣析出活性。複合型觸媒會產生協同作用(synergistic effect),氧化鈷與硼摻雜還原氧化石墨烯會共同提升電化學活性。比較氧化鈷擔載於各種硼量摻雜還原氧化石墨烯,由LSV測試結果顯示,在氧氣還原反應,CoOx/0.5M B-rGO具有最正的起始電位-0.112 V (vs. Ag/AgCl);在氧氣析出反應,CoOx/1.5M B-rGO具有最負的起始電位0.505 V (vs. Ag/AgCl)。
氧化鈷擔載於各種硼量摻雜還原氧化石墨烯在熱處理後,所有複合型觸媒的氧氣還原反應活性皆下降,而CoOx/0.5M B-rGO的氧氣析出活性反而提高,有最負的起始電位0.479 V (vs. Ag/AgCl),由XRD分析圖發現Co(OH)2繞射峰消失,推測熱處理會破壞氫氧化鈷結構,造成電化學活性提升或下降。
The cobalt oxide on boron doped reduced graphite oxide (CoOx/B-rGO) was simultaneously synthesized by hydrothermal method in the presence of boric acid. The X-ray diffraction (XRD) and transmission electron microscopy (TEM) results revealed that the composite includes both Co3O4 and Co(OH)2 crystalline structure. The X-ray photoelectron spectroscopy (XPS) analysis demonstrated the boron atoms were successfully doped into reduced graphite oxide structure. In 0.1 M KOH electrolyte, the composite showed a more positive onset potential at -0.112 V for oxygen reduction reaction (ORR) and a more negative onset potential at -0.516 V for oxygen evolution reaction (OER) than either Co3O4 or boron doped reduced graphite oxide (B-rGO). Due to synergetic effect and unique boron doping active sites, CoOx/B-rGO was a high-performance non-precious bifunctional catalyst for both ORR and OER.
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