非晶質金屬有機框架衍生物支撐之釕基觸媒 應用於酸性與鹼性海水介質中之析氫反應研究;Amorphous Metal-Organic Framework-Derived Ru-Based Catalysts for Hydrogen Evolution Reaction in Both Acidic and Alkaline Seawater Media

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Title:	非晶質金屬有機框架衍生物支撐之釕基觸媒應用於酸性與鹼性海水介質中之析氫反應研究;Amorphous Metal-Organic Framework-Derived Ru-Based Catalysts for Hydrogen Evolution Reaction in Both Acidic and Alkaline Seawater Media
Authors:	張家語;Chang, Chia-Yu
Contributors:	材料科學與工程研究所
Keywords:	金屬有機框架;析氫反應;海水電解;釕;鎳;鉑;metal-organic frameworks (MOFs);hydrogen evolution reaction (HER);seawater electrolysis;ruthenium;nickel;platinum
Date:	2025-06-25
Issue Date:	2025-10-17 11:45:32 (UTC+8)
Publisher:	國立中央大學
Abstract:	氫能作為一種潔淨且永續的替代能源，受到廣泛的關注。傳統的水分解反應通常在額外添加電解質的淡水中進行，然而淡水資源短缺，已成為氫能大規模應用的重大挑戰。近年來，海水電解逐漸被視為一具潛力的永續產氫策略，然而，其實際應用仍面臨諸多挑戰，包括鹽類沉積與高腐蝕性等關鍵問題，急需有效解決以實現海水電解的應用。本研究設計並製備了用於0.5 M H2SO4與鹼性模擬海水中的高效析氫反應(hydrogen evolution reaction, HER)電催化觸媒，以金屬有機框架(metal-organic frameworks, MOFs)衍生物作為載體，構築了釕(Ru)為主的催化系統。其中，選用Ni-BTC(1,3,5-苯三甲酸，H3BTC)作為基材，因其多孔結構可提供大量活性位點，具備優異的結構穩定性與快速的離子傳導能力，可有效提升HER活性。透過策略性地引入鉑(Pt)與均勻分散的鎳(Ni)，調節氫吸附能並促進反應動力學。其中RuPt0.3@Ni/C與Ru@Ni/C在酸性與鹼性模擬海中皆展現出優異的性能，在電流密度10 mA cm-2下的過電位(η10)分別僅為25和14 mV，Tafel斜率分別為14和33 mV dec-1，質量活性分別高達527和596 A g⁻¹ Ru+Pt。為深入探討觸媒的催化機制，進行了臨場X光吸收光譜(in-situ X-ray absorption spectroscopy, XAS)分析，以解析HER過程中的活性位點，同時利用電感耦合電漿發射光譜(inductively coupled plasma optical emission spectrometry, ICP-OES)評估穩定性測試後觸媒的金屬殘留率。此外，透過CO剝離(CO-stripping)實驗，進一步揭示了鹼性模擬海水中的水解離行為。臨場XAS與ICP-OES實驗結果證實，Ni-BTC衍生物載體提供穩定的結構，能有效抑制Cl-誘發的腐蝕反應並防止反應過程中金屬的溶解。CO剝離實驗結果進一步表明，適量引入Pt可調節氫吸附能，從而促進水解反應並提升HER活性。本研究成果為開發高效能HER觸媒與海水產氫技術提供了可行的設計策略與理論依據。;Hydrogen energy has attracted significant attention as a clean and sustainable alternative energy source. Tractional water splitting is typically conducted in freshwater with added electrolytes. However, the limited availability of freshwater poses a major challenge for the large-scale implementation of hydrogen energy. Recently, seawater electrolysis has emerged as a promising strategy for continuous hydrogen production. Nonetheless, critical challenges such as salt precipitation and high corrosiveness must be addressed to realize its full potential. In this study, efficient Ru-based electrocatalysts supported on metal-organic frameworks (MOFs)-derived structures were prepared for the hydrogen evolution reaction (HER) in both 0.5 M H2SO4 and alkaline simulated seawater. The Ni-BTC (1,3,5-benzenetricarboxylic acid, H3BTC)-derived support provides a porous structure with abundant active sites, excellent structural stability, and rapid ion transport, all of which enhance HER activity. Strategic incorporation of Pt and well-dispersed Ni modulates hydrogen adsorption energy and accelerates reaction kinetics. Notably, RuPt0.3@Ni/C and Ru@Ni/C catalysts exhibit remarkable performance in acidic and alkaline simulated seawater media, achieving overpotentials of 25 and 14 mV at 10 mA cm-2, Tafel slopes of 14 and 33 mV dec-1, and mass activities of 527 and 596 A g-1 Ru+Pt, respectively. To elucidate the catalytic mechanisms, in situ X-ray absorption spectroscopy (XAS) was performed to clarify the active sites during the HER process, while inductively coupled plasma optical emission spectrometry (ICP-OES) was used to evaluate metal retention during stability tests. The CO-stripping analysis further provides insights into water dissociation behavior in alkaline simulated seawater media. In-situ XAS and ICP-OES results confirm that the Ni-BTC-derived support offers a structurally stable framework, effectively mitigates Cl- induced corrosion, and prevents the dissolution of metals during the HER process. Additionally, CO-stripping experiments demonstrate that the moderate incorporation of Pt modulates hydrogen adsorption energy, thereby facilitating water dissociation and enhancing HER performance. These findings offer a practical design strategy for high-performance HER catalysts and advancing seawater-based hydrogen energy technologies.
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