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標題: | 金屬修飾鎳金屬有機骨架/鎳網電極用於鹼性電催化水解之研究 Metal-decorated Ni-MOF-74/Ni foam electrocatalysts for alkaline water electrolysis |
作者: | 王心慧 Xin-Huei Wang |
指導教授: | 蔡豐羽 Feng-Yu Tsai |
關鍵字: | 全水分解,產氫反應,產氧反應,金屬有機骨架,電催化劑,一步驟水熱法, water-splitting reaction,hydrogen/oxygen evolution reaction,metal-organic frameworks,electrocatalyst,one-pot hydrothermal process, |
出版年 : | 2023 |
學位: | 碩士 |
摘要: | 金屬奈米顆粒表面修飾的金屬有機骨架(Metal-organic framework, MOF)是一具有發展前景的電催化劑,其中的奈米金屬顆粒具備許多有助於水電解催化反應的性質,如高比表面積、多活性點以及低成本等。本研究利用一步驟水熱法(One-pot hydrothermal process)合成新穎的雙金屬(Pd及Ru)修飾MOF/鎳網(NF)電極,做為鹼性水電解反應之催化劑。在合成的雙金屬Pd及Ru修飾之MOF/鎳網電極(Pd/Ru@Ni-MOF-74/NF)中,Pd及Ru奈米金屬顆粒均勻分佈並透過與MOF中的有機連接配體產生化學鍵結而修飾於電極表面。相較於以同方式合成之單金屬(Pd或Ru)修飾電極,Pd/Ru@Ni-MOF-74/NF在鹼性水電解產氫反應中展現顯著提升的電催化反應效果—低的過電位及Tafel斜率。此催化劑優異的催化效果歸因於文獻報導之理論預測Pd與Ru雙金屬間的協同效應,於本研究中展現實際的實驗結果。MOF/NF以最佳的金屬含量與比例修飾後得到極低的過電位值14.1 mV及Tafel斜率12.0 mV/dec,此結果已低於文獻報導的商用Pt/C電極的46mV及~42mV/dec與其他金屬修飾的MOF/NF電極。本研究中亦展示了電極的微波碳化處理以及部分非貴金屬置換的初步研究結果,將會做為本研究未來的改進及發展方向。 Metal-decorated metal-organic frameworks (MOFs), where metal nanoparticles are distributed on the surface of MOFs, are a promising approach for developing high-performance electrocatalysts for water electrolysis, as they combine the advantages of MOFs—high specific surface area, abundant active sites, and low cost—with the excellent catalytic property of metal nanoparticles. This study demonstrated synthesis of a novel dual-metal Pd/Ru-decorated Ni-MOF-74 supported on a nickel foam (NF) substrate using a one-pot hydrothermal reaction for use as electrocatalysts for alkaline water electrolysis. The synthesized Pd/Ru@Ni-MOF-74/NF contained uniformly decorated Pd and Ru nanoparticles which were chemically bonded to Ni-MOF-74 through the linker molecules. The Pd/Ru@Ni-MOF-74/NF exhibited significantly improved electrocatalytic performance—lowered over-potential and Tafel slope—for the hydrogen evolution reaction (HER) over those of single metal Pd- or Ru-decorated Ni-MOF/NF’s, which were also synthesized as bases of comparison. The superior HER performance of the Pd/Ru@Ni-MOF-74/NF was attributed to a theoretically predicted synergistic mechanism between Pd and Ru, for which there result herein provided experimental evidence. Upon optimization of the ratio and loading content of the decorating Pd/Ru, an exceptionally low over-potential of 14.1 mV and Tafel slope of 12.0 mV/dec was obtained from the Pd/Ru@Ni-MOF-74/NF, which were substantial improvements over not only those reported for commercial Pt/C catalysts (~46 mV and ~42 mV/dec, respectively) but also those of other types of metal-decorated MOF’s. Microwave treatments and substitution of Pd with Co of the dual-metal-decorated Ni-MOF-74/NF were also preliminarily studied to provide a basis for future refinements of the dual-metal-decoration approach. |
URI: | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/90568 |
DOI: | 10.6342/NTU202302917 |
全文授權: | 同意授權(全球公開) |
顯示於系所單位: | 材料科學與工程學系 |
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ntu-111-2.pdf 此日期後於網路公開 2028-08-04 | 22.4 MB | Adobe PDF |
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