高效電化學二氧化碳還原觸媒及其應用於H型反應槽及流通槽之最佳化研究

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研究生：	許家偉 Chia-Wei Hsu
論文名稱：	高效電化學二氧化碳還原觸媒及其應用於H型反應槽及流通槽之最佳化研究 The Optimization of Highly Effective Carbon Dioxide Reduction Reaction Catalysts Applied in H-cells and Flow Cells
指導教授：	王冠文 Kuan-Wen Wang
口試委員:
學位類別：	碩士 Master
系所名稱：	工學院 - 材料科學與工程研究所 Graduate Institute of Materials Science & Engineering
論文出版年：	2022
畢業學年度：	110
語文別：	英文
論文頁數：	62
中文關鍵詞：	銅、氧化銦、二氧化碳還原反應、法拉第效率、玻碳電極、氣體擴散電極、質量傳輸、H型反應槽、流通槽
外文關鍵詞：	Cu, In2O3, CO2 reduction reaction, faradaic efficiency, glassy carbon electrode, gas diffusion electrode, mass transfer, H-cells, flow cells
相關次數：	點閱：12 下載：0
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在過去的一個世紀裡，大氣中的二氧化碳 (carbon dioxide, CO2) 排放量急劇增加。 CO2 還原反應 (CO2 reduction reaction, CO2RR) 是減少全球碳足跡最有希望的解決方案之一。具有高選擇性 (selectivity) 和活性的催化劑已在H型反應槽(H-cells)中得到廣泛研究。然而CO2RR在H-cells 的應用因其產量低，電流密度通常小於10 mA/cm2，限制其商業化應用。
因此，本研究將銅、氧化銦 (Cu-In2O3) 觸媒塗佈於H-cells和流通槽(flow cells)中的玻碳電極 (glassy carbon electrode, GCE)以及氣體擴散電極 (gas diffusion electrode, GDE)上，並研究其CO2 還原成一氧化碳 (carbon monoxide, CO) 的選擇性以及電流密度。在H-cells 的測試中， GCE 和 GDE 上的觸媒在 -0.7 V (vs. RHE) 下有著96和 92 % 的高CO法拉第效率 (faradaic efficiency, FE)，其電流密度分別為 3 和 6 mA/cm2。此外，在液體和氣體進料的flow cells中，CO FE 分別為 89和 86 %，具有 30 和 90 mA/cm2 的高電流密度，遠高於 H-cells 5 倍和 15 倍的電流密度。因H-cell的設計改善了質量傳輸 (mass transfer) 問題並降低了電極之間的電阻，使其觸媒效能有著極大的提升，本研究提供了一種有效的方式，可將實驗室規模的 CO2RR 朝向工業應用發展。

The carbon dioxide (CO2) emission in the atmosphere has increased dramatically in the past century. The CO2 reduction reaction (CO2RR) is one of the most promising solutions to reduce the global carbon footprint. The catalysts which have high selectivity and activity have been widely studied in H-cells. However, the application of H-cells is still far from the commercialization of CO2RR because of its low productivity (< 10 mA/cm2).
In this study, a comparative study of Cu-In2O3 catalysts immobilized onto glassy carbon electrode (GCE), gas diffusion electrode (GDE) in H-cells and flow cells is conducted to selectively reduce CO2 to carbon monoxide (CO). In the setup of H cells, catalysts on GCE and GDE exhibit a high CO faradaic efficiency (FE) of 96 and 92 % with a current density of 3 and 6 mA/cm2, respectively, at -0.7 V vs. RHE. Furthermore, in liquid and gas feed flow cells configurations, the CO FE is 89 and 86 % with an extraordinarily high current density of 30 and 90 mA/cm2, which increase by the factor of 5 and 15 compared with that in H-cells, respectively. These outstanding catalyst activities have been achieved through the flow cell design that overcomes the mass transfer issues and reduces the resistance between the electrodes. This study provides an effective strategy to move CO2RR in lab scale towards industrial application.

摘要    i
Abstract    ii
致謝    iii
Table of Contents    v
List of Figures    vii
List of Tables    ix
Chapter 1 Introduction    1
1.1 Mechanism of CO2RR    3
1.2 The electrodes for H-cells    6
1.3 Flow cell reactors    9
1.4 Motivation and Approach    12
Chapter 2 Experimental Section    13
2.1 Materials    13
2.2 Preparation of Catalysts    14
2.3 Physical Characterizations of Catalyst    15
2.4 Flow cell design    16
2.5 CO2RR measurement    18
2.5.1 H-cell measurement    18
2.5.2 Flow-cell  measurement    20
2.5.3 Gas chromatographic system    20
2.5.4 Standard preparation    21
Chapter 3 Results and Discussion    22
3.1 Catalysts characterization    22
3.2 The optimization of CO2RR in H-cell    26
3.2.1 The effect of carbon papers    26
3.2.2 CO2RR performance in H-cell    29
3.2.3 Summary    32
3.3 Flow cell CO2RR performance    33
3.3.1 The cathode flow-field plate    33
3.3.2 CO2RR performance in the flow cell    33
3.3.3 Summary    40
Chapter 4 Conclusions    41
References    42
                                

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