單原子之二維雙摻雜觸媒應用於陰離子交換膜燃料電池

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研究生：	Francisca Tania Deviani Wijaya Francisca Tania Deviani Wijaya
論文名稱：	單原子之二維雙摻雜觸媒應用於陰離子交換膜燃料電池 2-Dimensional Dual-Doped Single Atomic Electrocatalyst for Anion-Exchange Membrane Fuel Cell
指導教授：	王丞浩 Chen-Hao Wang
口試委員:	郭俞麟 Yu-Lin Kuo 黃信智 Hsin-Chih Huang 林律吟 Lu-Yin Lin 林昇佃 Shawn D. Lin 王丞浩 Chen-Hao Wang
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：	2023
畢業學年度：	111
語文別：	英文
論文頁數：	61
中文關鍵詞：	陰離子交換膜燃料電池、氮磷共摻雜碳、單原子活性位點、氧還原反應、電催化劑
外文關鍵詞：	AEMFC, N-P co-doped carbon, Single-atomic active site, Oxygen reduction reaction, Electrocatalyst
相關次數：	點閱：254 下載：2
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上一筆

長期以來，能源一直被認為是日常生活中最重要的必需品之一。由於我們嚴重依賴化石燃料來生產能源，隨著能源需求逐年增加，二氧化碳排放量也隨之增加。因此，我們必須轉而發展可更永續的能源，以減少二氧化碳排放。燃料電池為綠色可再生能源，受到科學家們的歡迎，但燃料電池的主要問題是氧氣還原反應之速率緩慢，目前大多採用鉑基觸媒，使成本大幅增加。在這項研究中，我們合成了一種二維多孔奈米片觸媒來幫助陰離子交換膜燃料電池中的氧氣還原反應，當中鐵單原子活性位點由氮磷共摻雜碳材料支撐。
利用三聚氰胺和雙氰胺作為氮摻雜的碳前驅體，並與二苯基膦酸以濕式合成法混合，經 1000°C 碳化下，形成具有足夠缺陷數量的多孔碳奈米片結構。XPS 證明了吡啶氮和石墨氮以及磷物種等存在，透過添加 4 wt% 的鐵前驅體，並在 800°C 的氮氣和氨氣下進行熱處理，即可得到最佳鐵單原子觸媒。單原子特性可藉由 XRD 中無任何峰出現、 XAS 中沒有 Fe-Fe 鍵以及 TEM 成像等得到證明。在鹼性條件下，MDP-4-Fe-800 樣品的 Eonset 為 0.97 V、E1/2 為 0.86 V、Jlimiting 為 5.5 mA/cm2、其電化學活性超過了商用 Pt/C。此外，在30,000次循環後、其穩定性良好、Jlimiting 僅下降 0.39 mA/cm2、Eonset 和 E1/2 均僅下降 30 mV。儘管 MDP-4-Fe-800 的 AEMFC 燃料電池結果尚未超過商業化的 Pt/C 、但它可以達到 244 mW/cm2 的最大功率密度。

Energy has long been considered one of the most important necessities in our daily lives. Because we rely heavily on fossil fuels to generate energy, CO2 emissions rise proportionally as energy demand rises year after year. As a result, we must shift to more sustainable energy production to reduce CO2 emissions. Hydrogen fuel cells are a type of green and renewable energy that has gained popularity among scientists. The main issue for the hydrogen fuel cell is the slow ORR rate, which currently employs Pt-based catalysts, increasing the cost significantly. Researchers are primarily attempting to create low-cost electrocatalysts to replace Pt. In this research, we have synthesized a 2D porous nanosheet electrocatalyst to aid ORR in AEMFC with Fe single atomic active sites being supported by an N-P co-doped carbon material.
Melamine and dicyandiamide were used as the N-doped carbon precursor, which was then mixed with diphenyl phosphinic acid in a wet synthesis method. The mixtures were then carbonized at the temperature of 1000°C to create the porous carbon nanosheet structure with an adequate number of defects, as proven by SEM, XRD, and Raman. The existence of pyridinic-N and graphitic-N, as well as P species, was proven by XPS. The best results were then used as carbon supports for the Fe single-atomic catalyst by adding 4 wt% of Fe precursor and heat treating them at 800°C in N2 and NH3 environments. The single-atomic property of the electrocatalyst could be proven by the non-existent peak in XRD, the lack of Fe-Fe bonding in XAS, as well as TEM imaging. The electrochemical activity of the material was shown by the MDP-4-Fe-800 sample with an Eonset of 0.97 V, an E1/2 of 0.86 V, and a Jlimiting of 5.5 mA/cm2 in an alkaline condition, which surpasses the commercial Pt/C in the same condition. It also has good stability after 30,000 cycles with only a 0.39 mA/cm2 decrease in Jlimiting and a 30 mV decrease of both Eonset and E1/2. Even though the AEMFC fuel cell result of MDP-4-Fe-800 has not surpassed that of commercialized Pt/C, it could reach 244 mW/cm2.

ABSTRACT    I
中文摘要    III
ACKNOWLEDGEMENTS    IV
TABLE OF CONTENTS    V
LIST OF FIGURES    VII
LIST OF TABLES    X
CHAPTER 1 INTRODUCTION    1
1    Research Background    1
2    Hydrogen Fuel Cell    3
2.1    Types of Hydrogen Fuel Cells    5
2.2    Anion-Exchange Membrane Fuel Cell    6
2.3    Electrochemistry of Oxygen Reduction Reaction    7
3    Electrocatalyst for ORR    11
CHAPTER 2 LITERATURE REVIEW    13
1    Non-Precious Metal-based Electrocatalysts for ORR    13
1.1    Iron-based Single Atomic Catalysts for ORR    18
2    Metal-free Electrocatalytic Materials for ORR    21
2.1    Dual-doped N, P Catalysts for ORR    23
CHAPTER 3 EXPERIMENTAL DETAILS    25
1    Materials and Chemicals    25
2    Experimental Procedure    26
2.1    Synthesis of N, P-doped Carbon    26
2.2    Synthesis of Fe Single Atomic Catalyst    27
3    Characterization of Materials and Basic Principle of Instruments    28
3.1    X-Ray Diffraction    28
3.2    Scanning Electron Microscopy    29
3.3    Transmission Electron Microscopy    29
3.4    X-Ray Photoelectron Spectroscopy    30
3.5    X-Ray Absorption Spectroscopy    31
3.6    Brunauer-Emmett-Teller Analysis    32
4    Electrochemical Test Measurements    32
CHAPTER 4 RESULTS AND DISCUSSION    35
1    N, P-Doped Carbon    35
1.1    Different Heat Treatment Temperature    35
1.2    Different N-C Precursors    39
2    Fe Single Atomic Catalyst    44
2.1    Different Carbon Supports (MDP and DDP)    44
2.2    Different Weight Percentages of Fe Precursor    51
2.3    Stability and Single-Cell Test    54
CHAPTER 5 CONCLUSION    56
BIBLIOGRAPHY    58


                                

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