研究生: |
徐啟寧 Chi-Ning Hsu |
---|---|
論文名稱: |
以電沉積技術開發用於整體水分解的層狀雙氫氧化物電極 Layered Double Hydroxide Electrode Developed by Electrodeposition Technique for Overall water splitting |
指導教授: |
郭東昊
Dong-Hau Kuo |
口試委員: |
薛人愷
Ren-Kae Shiue 柯文政 Wen-Cheng Ke |
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: | 2020 |
畢業學年度: | 108 |
語文別: | 中文 |
論文頁數: | 118 |
中文關鍵詞: | 電沉積 、層狀雙氫氧化物 、薄膜 、電催化性能 、整體水分解 |
外文關鍵詞: | electrodeposition, Layered Double Hydroxide, thin film, electrical property, overall water splitting |
相關次數: | 點閱:370 下載:14 |
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本研究使用電沉積技術成功製備出具高電催化特性的雙功能NiFe-LDH/Ni(OH)2雙層薄膜,並在實驗中,探討不同的層狀雙氫氧化物的電催化性能,以及不同的電沉積參數對薄膜的電化學特性與表面特徵之影響。透過SEM、XRD、Raman及XPS來分析薄膜的表面特徵,並使用雙頻道恆電位/電流/交流阻抗儀來量測其電催化性能。
本實驗改變電沉積電壓與時間製備單層之NF3b薄膜與雙層之NF3b/N2與NF3b/N3薄膜。由SEM結果得知NF3b薄膜呈現出直立片狀結構; NF3b/N2呈現出表面具有微小顆粒的直立片狀結構;NF3b/N3呈現出表面平整光滑的直立片狀結構。拉曼量測結果得知NF3b薄膜為NiFe-LDH結構;NF3b/N2與NF3b/N3薄膜為Ni(OH)2結構。
電化學量測結果顯示,NF3b/N2具有最佳的OER電催化性能,
LSV量測可以得到,在200 mA/cm2的電流下,過電勢為257 mV,Tafel斜率值為126 mV/dec。NF3b/N3則具有最佳的HER性能,在-10 mA/cm2的電流下,過電勢為-151 mV,Tafel斜率值為86 mV/dec。本實驗將NF3b/N2薄膜與NF3b/N3薄膜作為電極,使用1 M KOH作為電解質,組裝成簡易的鹼性電解槽,並測試用於整體水分解的電催化性能,在LSV量測中得到,在10 mA/cm2的電流下,所需電壓為1.63 V,在CstC的測試中也顯現出良好的穩定性。
In this research, 1st-layer Ni-Fe-LDH/2nd-layer Ni(OH)2 composite thin films were fabricated and utilized for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) to simultaneously conduct electrocatalytic water splitting process. The composite thin films were deposited on Ni foam by electrodeposition technique. To find out the optimum performances of the catalysts, the first layer was fabricated with different voltages of -0.7 – -1.15 V and fixed deposition time of 2.5 min. The second layer was done with a fixed potential at -1 V and different deposition times of 1 – 3 min. The electrochemical properties and characteristics of the as-deposited composite thin films were analyzed with XRD, SEM, Raman, XPS measurements, and electrocatalytically tested with HER and OER as well as overall water splitting.
It was found that the morphology of 1st-layer Ni-Fe LDH with deposition potential at -1 V and time at 2.5 min showed as the lamellar sheets standing perpendicularly to Ni foam substrate. The first layer LDH was then electrodeposited with Ni to form a thin second layer of Ni(OH)2 which was confirmed with Raman spectroscopy analysis. The performance of the composite thin films were tested with Ni(OH)2 deposited with different deposition times. The electrochemical measurements indicated the NF3b/N2 thin film electrode exhibited the best properties for OER. With the current density of 200 mA/cm2, the overpotential and Tafel slope for oxygen evolution reaction were 257 mV and 126 mV/dec, respectively. On the other hand, the NF3b/N3 thin film electrode exhibited the best properties for HER. The best HER performance exhibited with the overpotential of -151 mV and Tafel slope of 86 mV/dec at current density of -10 mA/cm2. To show the overall water splitting process, NF3b/N2 and NF3b/N3 thin film electrodes were repectively utilized as anode and cathode with 1 M KOH as electrolyte. For the overall water splitting reaction, the electrolytic cell had the overpotantial of 1.63 V at 10 mA/cm2, while it has 348 mA/cm2 at 2.0 V. At the constant currednt test for cell stability, the cell gradually reached stable overpotential of 1.84 V at 20 mA/cm2. This work contributed to a simple electrodeposition method to fabricate double-layer composite thin film for a promising and stable electrocatalytic water splitting reaction in alkaline solution.
[1] N.T. Suen, S.F. Hung, Q. Quan, N. Zhang, Y.J. Xu, H.M. Chen, Electrocatalysis for the Oxygen Evolution Reaction: Recent Development and Future Perspectives, Chem Soc Rev, 46 (2017) 337-365.
[2] 黃秉鈞,李健成《科學發展》2005年2月,386期,56 ~ 61頁.
[3] 林國興,賴建銘,張嵩駿,林俊男, 氫能趨勢分析與儲能應用新思維. 工業材料雜誌376期, 2018.
[4] M.A. Khan, H. Zhao, W. Zou, Z. Chen, W. Cao, J. Fang, J. Xu, L. Zhang, J. Zhang, Recent Progresses in Electrocatalysts for Water Electrolysis, Electrochemical Energy Reviews, 1 (2018) 483-530.
[5] Y. Lee, J. Suntivich, K.J. May, E.E. Perry, Y. Shao-Horn, Synthesis and Activities of Rutile IrO2 and RuO2 Nanoparticles for Oxygen Evolution in Acid and Alkaline Solutions, The Journal of Physical Chemistry Letters, 3 (2012) 399-404.
[6] T. Reier, M. Oezaslan, P. Strasser, Electrocatalytic Oxygen Evolution Reaction (OER) on Ru, Ir, and Pt Catalysts: A Comparative Study of Nanoparticles and Bulk Materials, ACS Catalysis, 2 (2012) 1765-1772.
[7] E. Antolini, Iridium As Catalyst and Cocatalyst for Oxygen Evolution/Reduction in Acidic Polymer Electrolyte Membrane Electrolyzers and Fuel Cells, ACS Catalysis, 4 (2014) 1426-1440.
[8] R. Kötz, Anodic Iridium Oxide Films, Journal of The Electrochemical Society, 131 (1984) 72.
[9] S. Cherevko, S. Geiger, O. Kasian, N. Kulyk, J.-P. Grote, A. Savan, B.R. Shrestha, S. Merzlikin, B. Breitbach, A. Ludwig, K.J.J. Mayrhofer, Oxygen and Hydrogen Evolution Reactions on Ru, RuO2, Ir, and IrO2 Thin Film Electrodes in Acidic and Alkaline Electrolytes: A Comparative Study on Activity and Stability, Catalysis Today, 262 (2016) 170-180.
[10] M.M. Najafpour, S. Madadkhani, M. Tavahodi, Manganese Oxides Supported on Nano-sized Metal Oxides as Water-Oxidizing Catalysts for Water-Splitting Systems: 3-Electrochemical Studies, International Journal of Hydrogen Energy, 42 (2017) 60-67.
[11] C. Pan, T. Takata, K. Domen, Overall Water Splitting on the Transition‐Metal Oxynitride Photocatalyst LaMg1/3Ta2/3O2N over a Large Portion of the Visible‐Light Spectrum, Chemistry – A European Journal, 22 (2016) 1854-1862.
[12] E. Ha, L.Y.S. Lee, J. Wang, F. Li, K.Y. Wong, S.C.E. Tsang, Significant Enhancement in Photocatalytic Reduction of Water to Hydrogen by Au/Cu2ZnSnS4 Nanostructure, Advanced Materials, 26 (2014) 3496-3500.
[13] I. Tsuji, Y. Shimodaira, H. Kato, H. Kobayashi, A. Kudo, Novel Stannite-type Complex Sulfide Photocatalysts AI2-Zn-AIV-S4 (AI = Cu and Ag; AIV = Sn and Ge) for Hydrogen Evolution under Visible-Light Irradiation, Chemistry of Materials, 22 (2010) 1402-1409.
[14] H. Abdullah, D.-H. Kuo, X. Chen, High Efficient Noble Metal Free Zn(O,S) Nanoparticles for Hydrogen Evolution, International Journal of Hydrogen Energy, 42 (2017) 5638-5648.
[15] H. Zhou, F. Yu, Q. Zhu, J. Sun, F. Qin, L. Yu, J. Bao, Y. Yu, S. Chen, Z. Ren, Water Splitting by Electrolysis at High Current Densities Under 1.6 volts, Energy & Environmental Science, 11 (2018) 2858-2864.
[16] H. Zhou, F. Yu, J. Sun, R. He, S. Chen, C.-W. Chu, Z. Ren, Highly Active Catalyst Derived from a 3D Foam of Fe(PO3)2/Ni2P for Extremely Efficient Water Oxidation, Proceedings of the National Academy of Sciences, 114 (2017) 5607.
[17] X. Zou, Y. Zhang, Noble Metal-Free Hydrogen Evolution Catalysts for Water Splitting, Chemical Society Reviews, 44 (2015) 5148-5180.
[18] Y. Yan, B.Y. Xia, B. Zhao, X. Wang, A Review on Noble-Metal-Free Bifunctional Heterogeneous Catalysts for Overall Electrochemical Water Splitting, Journal of Materials Chemistry A, 4 (2016) 17587-17603.
[19] Y. Jiao, Y. Zheng, M. Jaroniec, S.Z. Qiao, Design of Electrocatalysts for Oxygen- and Hydrogen-Involving Energy Conversion Reactions, Chemical Society Reviews, 44 (2015) 2060-2086.
[20] D.U. Lee, P. Xu, Z.P. Cano, A.G. Kashkooli, M.G. Park, Z. Chen, Recent Progress and Perspectives on Bifunctional Oxygen Electrocatalysts for Advanced Rechargeable Metal–Air Batteries, Journal of Materials Chemistry A, 4 (2016) 7107-7134.
[21] L. Jörissen, Bifunctional Oxygen/Air Electrodes, Journal of Power Sources, 155 (2006) 23-32.
[22] C. Hu, L. Zhang, J. Gong, Recent Progress Made in the Mechanism Comprehension and Design of Electrocatalysts for Alkaline Water Splitting, Energy & Environmental Science, 12 (2019) 2620-2645.
[23] Q. Wang, D. O’Hare, Recent Advances in the Synthesis and Application of Layered Double Hydroxide (LDH) Nanosheets, Chemical Reviews, 112 (2012) 4124-4155.
[24] G. Fan, F. Li, D.G. Evans, X. Duan, Catalytic Applications of Layered Double Hydroxides: Recent Advances and Perspectives, Chem Soc Rev, 43 (2014) 7040-7066.
[25] D.G. Evans, R.C.T. Slade, Structural Aspects of Layered Double Hydroxides, in: X. Duan, D.G. Evans (Eds.) Layered Double Hydroxides, Springer Berlin Heidelberg, Berlin, Heidelberg, 2006, pp. 1-87.
[26] M. Gong, H. Dai, A Mini Review of NiFe-Based Materials as Highly Active Oxygen Evolution Reaction Electrocatalysts, Nano Research, 8 (2015) 23-39.
[27] R.M.M. Santos, J. Tronto, V. Briois, C.V. Santilli, Thermal Decomposition and Recovery Properties of ZnAl–CO3 Layered Double Hydroxide for Anionic Dye Adsorption: Insight into the Aggregative Nucleation and Growth Mechanism of the LDH Memory Effect, Journal of Materials Chemistry A, 5 (2017) 9998-10009.
[28] P. Refait, M. Abdelmoula, L. Simon, J.-M.R. Génin, Mechanisms of Formation and Transformation of Ni–Fe Layered Double Hydroxides in SO32− and SO42− Containing Aqueous Solutions, Journal of Physics and Chemistry of Solids, 66 (2005) 911-917.
[29] P. Luo, K. Xu, R. Zhang, L. Huang, J. Wang, W. Xing, J. Huang, Highly Efficient and Selective Reduction of Nitroarenes with Hydrazine over Supported Rhodium Nanoparticles, Catalysis Science & Technology, 2 (2012) 301-304.
[30] M. Gong, Y. Li, H. Wang, Y. Liang, J.Z. Wu, J. Zhou, J. Wang, T. Regier, F. Wei, H. Dai, An Advanced Ni–Fe Layered Double Hydroxide Electrocatalyst for Water Oxidation, Journal of the American Chemical Society, 135 (2013) 8452-8455.
[31] Z. Lu, W. Xu, W. Zhu, Q. Yang, X. Lei, J. Liu, Y. Li, X. Sun, X. Duan, Three-Dimensional NiFe Layered Double Hydroxide Film for High-Efficiency Oxygen Evolution Reaction, Chemical Communications, 50 (2014) 6479-6482.
[32] N. Jiang, B. You, M. Sheng, Y. Sun, Electrodeposited Cobalt-Phosphorous-Derived Films as Competent Bifunctional Catalysts for Overall Water Splitting, Angew Chem Int Ed Engl, 54 (2015) 6251-6254.
[33] J. Luo, J.-H. Im, M.T. Mayer, M. Schreier, M.K. Nazeeruddin, N.-G. Park, S.D. Tilley, H.J. Fan, M. Grätzel, Water Photolysis at 12.3% Efficiency via Perovskite Photovoltaics and Earth-Abundant Catalysts, Science, 345 (2014) 1593.
[34] L.-A. Stern, L. Feng, F. Song, X. Hu, Ni2P as a Janus Catalyst for Water Splitting: the Oxygen Evolution Activity of Ni2P Nanoparticles, Energy & Environmental Science, 8 (2015) 2347-2351.
[35] Y. Yan, L. Thia, B.Y. Xia, X. Ge, Z. Liu, A. Fisher, X. Wang, Construction of Efficient 3D Gas Evolution Electrocatalyst for Hydrogen Evolution: Porous FeP Nanowire Arrays on Graphene Sheets, Advanced Science, 2 (2015) 1500120.
[36] P. Jiang, Q. Liu, Y. Liang, J. Tian, A.M. Asiri, X. Sun, A Cost-Effective 3D Hydrogen Evolution Cathode with High Catalytic Activity: FeP Nanowire Array as the Active Phase, Angewandte Chemie International Edition, 53 (2014) 12855-12859.
[37] F. Gloaguen, J.D. Lawrence, T.B. Rauchfuss, Biomimetic Hydrogen Evolution Catalyzed by an Iron Carbonyl Thiolate, Journal of the American Chemical Society, 123 (2001) 9476-9477.
[38] J. Bao, X. Zhang, B. Fan, J. Zhang, M. Zhou, W. Yang, X. Hu, H. Wang, B. Pan, Y. Xie, Ultrathin Spinel-Structured Nanosheets Rich in Oxygen Deficiencies for Enhanced Electrocatalytic Water Oxidation, Angewandte Chemie International Edition, 54 (2015) 7399-7404.
[39] B.C.M. Martindale, E. Reisner, Bi-Functional Iron-Only Electrodes for Efficient Water Splitting with Enhanced Stability through In Situ Electrochemical Regeneration, Advanced Energy Materials, 6 (2016) 1502095.
[40] X. Zhang, Y. Liang, Nickel Hydr(oxy)oxide Nanoparticles on Metallic MoS2 Nanosheets: A Synergistic Electrocatalyst for Hydrogen Evolution Reaction, Advanced Science, 5 (2018) 1700644.
[41] S. Jiao, Z. Yao, M. Li, C. Mu, H. Liang, Y.-J. Zeng, H. Huang, Accelerating Oxygen Evolution Electrocatalysis of Two-Dimensional NiFe Layered Double Hydroxide Nanosheets via Space-Confined Amorphization, Nanoscale, 11 (2019) 18894-18899.
[42] C. Tang, H.-S. Wang, H.-F. Wang, Q. Zhang, G.-L. Tian, J.-Q. Nie, F. Wei, Spatially Confined Hybridization of Nanometer-Sized NiFe Hydroxides into Nitrogen-Doped Graphene Frameworks Leading to Superior Oxygen Evolution Reactivity, Advanced Materials, 27 (2015) 4516-4522.
[43] Y. Wang, C. Jiang, Y. Le, B. Cheng, J. Yu, Hierarchical Honeycomb-Like Pt/NiFe-LDH/rGO Nanocomposite with Excellent Formaldehyde Decomposition Activity, Chemical Engineering Journal, 365 (2019) 378-388.
[44] Y.-Z. Su, K. Xiao, N. Li, Z.-Q. Liu, S.-Z. Qiao, Amorphous Ni(OH)2 @ Three-Dimensional Ni Core–Shell Nanostructures for High Capacitance Pseudocapacitors and Asymmetric Supercapacitors, Journal of Materials Chemistry A, 2 (2014) 13845-13853.