研究生: |
鐘幻苹 Huan-Ping Jhong |
---|---|
論文名稱: |
硒氰酸根鍵結過渡二硫族金屬修飾於多孔性碳材應用於提升氧氣還原反應效能 Enhanced Activity of Selenocyanate-containing Transition Metal Dichalcogenides Supported by Mesoporous Carbon for Oxygen Reduction |
指導教授: |
王丞浩
Chen-Hao Wang |
口試委員: |
施劭儒
Shao-Ju Shih 吳嘉文 Chia-Wen Wu 洪逸明 Yi-Ming Hong 廖英志 Ying-Chih Liao |
學位類別: |
碩士 Master |
系所名稱: |
工程學院 - 材料科學與工程系 Department of Materials Science and Engineering |
論文出版年: | 2019 |
畢業學年度: | 107 |
語文別: | 中文 |
論文頁數: | 116 |
中文關鍵詞: | 氧氣還原反應 、燃料電池 、二硒化鈷 、硒氰酸根 |
外文關鍵詞: | Anion Alkaline Exchange Fuel Cells (AAEMFC), Oxygen Reduction Reaction (ORR), Cobalt Diselenide (CoSe2), Selenocyanate (SeCN-) |
相關次數: | 點閱:436 下載:0 |
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本研究透過控制含有鈷以及硒之前驅物比例,再搭配界面活性劑與溶劑的使用,經水熱法處理後可得一特殊形貌之二硒化鈷。而利用此實驗流程,加入適當比例之碳材及尿素後,再使用化學氣相沉積儀燒結至特定溫度,即可製備出最佳條件之觸媒(CoSe2/NC)。經電化學量測後得知,該觸媒具有最佳之氧氣還原活性且其電子轉移數可達3.994,非常接近理想之電子轉移數4.0。另外,觸媒在經過線性掃描法(Linear Sweep Voltammetry)方式30000圈穩定性測試後,其半波電位衰退率僅5.9%,可知此觸媒在反應的過程中具備極佳之穩定性。同時也在鹼性陰離子交換膜燃料電池(Anion Alkaline Exchange Membrane Fuel Cell)測試中,達到146.3 mW cm-2 的高輸出功率。
此具有高催化活性及穩定性的觸媒可歸因於兩個因素,首先從氮的近邊X射線吸收細微結構(Near Edge X-Ray Absorption Fine Structure)圖譜中得知,有一特徵峰顯現為Co-N鍵結在鍵結能396.3eV的位置。因為氮原子本身具有的高電負度與二價鈷提供的空軌域,有效地促進電子轉移,進而增加活性。再者,硒氰酸根(SeCN-)的結構也因為其具有較高的氧化電位,因此可提升氧氣還原反應進行的效率。
利用此簡易的方法製備出具有獨特形貌之新穎高效率電催化觸媒,相信應用在其他電化學反應或系統中,也是極具發展潛力的選擇。
Cobalt diselenide is used to synthesize a transition metal with an active center that is supported by nitrogen-doped carbon materials—CoSe2/NC. CoSe2/NC demonstrates an excellent oxygen reduction reaction (ORR) ability with an electron-transfer number of 3.994, which is approximately equal to the ideal electron-transfer number 4.0. In an electrochemical measurement, CoSe2/NC presents excellent durability after 30,000 cycles linear sweep voltammetry (LSV) scan. When an anion (alkaline) exchange membrane fuel cell uses CoSe2/NC, superior performance is achieved in terms of the current generation. Moreover, a maximum power density of 146.3 mW cm−2 is obtained when a Fumapem® FAA-3 membrane is used.
The high catalytic performance of CoSe2/NC is due to two reasons—1) presence of selenocyanate (SeCN−) bonding in CoSe2/NC that promotes electron transfer and 2) presence of Co-N structures that act as active sites in an ORR. These characteristics of CoSe2/NC enhance the performance of the active sites and increase the kinetic reaction rate during the ORR, thus causing CoSe2/NC to be a promising catalyst.
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