水氧化催化劑之合成與應用

Synthesis and application of water oxidation catalysts

10.6342/NTU201704193

童敬維

水分解 ； 人工光合作用 ； 產氧反應 ； water splitting ； oxygen evolution reaction ； artificial photosynthesis

國立臺灣大學化學系學位論文

2017年

博士

陳浩銘

英文

本研究著重於人工光合作用材料之合成及與實驗設計，並利用同步輻射X光光源技術對催化劑在進行水分解同時臨場檢測分析，深入了解其反應機制，並加以改良合成之策略，提升催化效能及穩定性，量測條件及材料皆以符合綠色能源的原則下設計。 研究材料的方向分為三個部分，金屬氧化物、有機金屬分子及微米結構吸光材料。相較於有機金屬分子，金屬氧化物在嚴苛的催化環境下有較高的穩定性並較為廣泛應用在電催化系統。我們發展出具有表面活性緩衝層之單晶奈米粒子催化劑，此結構在反覆的氧化還原過程中並不會對其主體造成影響，因此大大提升催化過程中的穩定性，且經過一千小時的連續產氧反應後，其活性僅衰退5個百分比。另一方面，我們發展出具有微米級方格孔洞的導電玻璃，有助於有機金屬分子在高電壓及強鹼的電催環境下進行產氧反應，並藉由臨場X光吸收分析技術觀測其金屬中心的結構變化，而目前結果顯示對於不同配位基組成的有機金屬分子，其反應過程的活性物種有明顯的不同。吸光材料的部分，本實驗室成功合成出微米柱體結構的矽晶圓面板，利用電沉積技術在矽基板表面製備出鎳奈米粒子，且在光催水氧化系統下具有高活性及穩定性。

Our research has focused on the newly developed strategy to improve the activity and stability of artificial photosynthesis materials. The in situ synchrotron X-ray techniques provides a powerful method to the investigation of the truly active species of catalysts during water splitting and can be applied in studying both homogeneous and heterogeneous system. To achieve practical use of large scale renewable energy, abundant and low cost first-low transition metal for water splitting are required. At First, we reported a single-crystal Co3O4 nanocube underlay with an adapting thin CoO layer result in a high-stability electrocatalyst in oxygen evolution reaction. An in-situ X-ray diffraction method is developed to observe the formation of active metal oxyhydroxide phase, and further revealed that CoO thin layer could protect underlay electrocatalyst through reversible transformation to active phase. In the other hand, we also investigated an in-situ X-ray absorption method provide an information of the real active species in the formation from various ligand-based iron complexes during electrocatalysis water oxidation. Third, Ni-dispersed on silicon microwire photoanode by electrodeposition was successfully fabricated, and performed high activity and stability for PEC test.

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