博碩士論文 107389602 詳細資訊



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姓名 利亞 普(Pouria Dadvari)  查詢紙本館藏   畢業系所 材料科學與工程研究所
論文名稱 應用於電催化析氧反應之高性能多金屬尖晶石 合成及其機理動力學模擬研究
(Synthesis of High-Performance Multimetallic Spinel for Oxygen Evolution Reaction Electrocatalysis and Mechanistic Kinetic Modeling)
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摘要(中) 開發用於析氧反應（OER）的高效穩定且價格低廉的電催化劑對於發展用於生產可持
續氫燃料的水電解槽技術至關重要。
高熵陶瓷具有獨特的性質，例如晶格畸變和高構型熵， 有益於催化反應。本工作透過
溶膠-凝膠自燃法，製備了五種含有 3d 過渡金屬和鋁（ (AlCrCoNiFe2)O）的金屬尖晶
石，並與其他合成的多金屬和單金屬氧化物在鹼性條件下的 OER 電催化性能進行了
比較。電化學分析表明，合成的五種金屬尖晶石在泡沫鎳基板上產生最低的電荷轉移
電阻（1.666 V vs RHE 時為 0.49 (Ω)）、塔菲爾斜率(43 mV.dec-1
) 和過電位(η10=320
mV)主要歸因於缺陷晶體結構產生的空間電荷界面極化，可以增加反應界面金屬-氧
（M-O）鍵斷裂的局部電場強度， M-O 鍵溫和的共價特性，快速的電荷傳輸和較小
的距離活躍站點。總體而言， 這些因素都可以增加活性位點的形成、中間體之間的碰
撞和 O2 形成的速率。
將 五 種不同金屬摻入晶體結構中所產生的高構形熵也可以提高 OER 的相穩定性。
動力學建模也可驗證多金屬尖晶石表面可能的反應機制。
摘要(英) The development of efficient and stable electrocatalysts with low prices for the oxygen evolution reaction (OER) is pivotal in the advancement of water electrolyzer technologies for production of sustainable hydrogen fuel. High entropy ceramics have distinctive properties such as lattice distortion and high configurational entropy which can be very useful for catalytic purposes. In this work, through the application of the sol-gel auto-combustion method, five metal spinel containing 3d transition metals and Aluminum ((AlCrCoNiFe2)O) were prepared, and their electrocatalytic performance in comparison with other synthesized multi-metal and monometallic oxides for OER within an alkaline medium was analyzed. The electrochemical analysis revealed that the synthesized five metal spinel yielded the lowest charge transfer resistance (0.49 (Ω) at 1.666 V vs RHE ), Tafel slope (43 mV.dec-1), and overpotential (η10=320 mV) with nickel foam substrate outcomes mainly can be attributed to the space charge interfacial polarization stemming from defective crystal structure which can increase local electric field strength for metal-oxygen (M-O) bond breakage at reaction interface, mild covalency character of M-O bonds, fast charge transport and a small distance between active site. Totally all these factors can increase the rate of active sites formation, collision between intermediates, and O2 formation. High configurational entropy coming from the incorporation of five dissimilar metals into the crystal structure can also increase phase stability for OER. Kinetic modeling also can be a useful method for testifying possible reaction mechanism on the surface of multi-metal spinel.
Key words: Oxygen Evolution Reaction (OER), High Entropy Ceramics (HEC), Cocktail effect, Sol-gel auto-combustion method, Multimetallic spinel, Tafel slope, Overpotential, Space charge-interfacial polarization, Defective crystal structure, Local electric field strength, Metal-oxygen covalency, Charge transport, Active sites, Kinetic model, Reaction mechanism.
關鍵字(中) ★ 析氧反應
★ 高熵陶瓷
★ 動力學模型		 關鍵字(英) ★ Oxygen Evolution Reaction
★ High Entropy Ceramic
★ Kinetic Model
論文目次 摘要…………………………………………………………………………………………...….......I
Abstract……………………………………..…………………………………………………...…....II
Table of content………………………………………………………………………….………..…III
Table of figures……………………………………………………………………………...……..…V
List of Tables………………………………………………………………………………….…...VIII
Chapter 1 Introduction………………………………………………………………………...……….1
1.1 Disordered crystalline materials and their advantage for electrocatalytic purposes……...….…2
1.2 High entropy materials……………………………………………………………………....…3
1.2.1 Characteristics of high entropy material……………………………………………...…..…4
1.2.1.1 Thermodynamics: high entropy effect………………………………………………..…4
1.2.1.2 Kinetic: sluggish diffusion effect……………………………………………………..…4
1.2.1.3 Structure: severe lattice distortion………………………………………………..….…..4
1.2.1.4 Cocktail effect…………………………………………………………………………...5
1.3 Spinel…………………………………………………………………………………….……...5
1.4 Adsorption isotherm………………………………………………………………………....….5
1.4.1 Langmuir isotherm……………………………………………………………….……....….5
1.4.2 Frumkin isotherm………………………………………………………………………........6
1.4.3 Frumkin-Temkin isotherm……………………………………………….………….……....6
Chapter 2 Literature review…………………………………………………………………….…..…8
2.1 OER electrocatalysts………………………………………………………………………..…..8
2.2 Recent works related to high entropy materials for OER ……………………………………...9
2.3 Suggested descriptors proposed for OER efficiency of catalysts…………………………..…..9
2.4 Different OER mechanisms in alkaline environment…………………………………….……11
Chapter 3 Experimental methodology…………………………………………………….….............12
3.1 Materials and preparation methods……………………………………………….....….......…12
3.2 Characterization…………………………………………………………………………..…...12
3.2.1 X-ray powder diffraction (XRD) ……………….……………………………………….....12
3.2.1.1 X-ray diffraction refinement and crystallite size estimation…………….…….……....12
3.2.2 X-ray photoelectron spectroscopy (XPS)…………………………………….……..….......12
3.2.3 Transmission electron microscopy (TEM), scanning electron microscopy (SEM) and
energy dispersive X-ray spectroscopy (EDS)……………………....………………..…….13
3.3 Electrochemical measurement…………………………………………….…….……….….…13
3.4 Impedance spectroscopy analysis for space charge measurement……………….…...….........14
3.5 Faraday efficiency…………………………………………………………………………......14
Chapter 4 Results and discussion…………………………………………………………….………15
4.1 Mixing or configurational entropy………………………………………………………....…..15
4.2 Morphology, composition and crystallographic structure analysis……………….……......…..15
4.3 Electroanalytical results……………………………………………………...………….…..…16
4.4 Factors affecting activity of catalysts…………………………………………………….….....17
4.4.1 Space charge-interfacial and charge transport polarization………………...……....….......17
4.4.2 Covalency character of metal-oxygen bond in oxides……….……………………....….....18
4.4.3 Distance between active sites………………………………………………….....….…......19
4.5 Stability and efficiency…………………………………………………………...….…….......19
4.6 Derivation of kinetic model for possible OER mechanisms……………….……………..........20
4.6.1 Derivation of impedance function with Langmuir adsorption isotherm…………………...20
4.6.2 Surface coverage versus applied electric potential…………………………………….......20
4.6.3 Charge balance equation for Krasil′shchikov path………………………………………....21
4.6.4 Mass balance equations for intermediates of Krasil′shchikov path………….……..….......22
4.6.5 Kinetic model for layered double hydroxide (LDH) mechanism………………...………..26
4.6.6 Kinetic model for Nørskov mechanism…………………………...………………….....…31
4.7 Active sites and turn over frequency………………………………………………………..….34
4.8 Gibbs free energy changes…………………………………………………………………..….35
4.9 Correspondence of kinetic model with experimental results……………………………….......36
Chapter 5 Conclusion…….………………………………………………………………...……...…37
References……………………..……………………………………………………………..…..…116
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指導教授 做實驗 洪緯璿(Kuan-Wen Wang Wei-Hsuan Hung) 審核日期 2024-7-6
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