氫（H2）作為一種無碳乾淨的能源，是緩解現今與未來社會能源需求中最有吸引力和最環保的選擇。其中電解水產氫是最突出和前衛的技術，但它需要較高的過電位來驅動緩慢的陽極析氧反應。本論文展示了三種將水電解與只需要較低的過電位使更易氧化的陽極化學原料混合的方法。
在第一種方法中，我們通過使用碘化物氧化反應開發了一種新型混合電解材料，我們製造了釕錫表面合金氧化物作為碘化物輔助混合水電解的陽極電催化劑。 以乙二醇為還原劑，通過金紅石型氧化錫與釕離子的水熱反應，在金紅石型氧化錫表面製備釕-錫合金氧化物。將IOR電解與OER電解以釕-錫表面合金氧化物作為陽極電催化劑進行比較，在雙電極系統中，釕-錫表面合金氧化物陽極上在IOR 的電解表現出1.01 V的超低電壓，以達到10 mA cm-2的基準電流密度，而在水電解OER的電解則是需要電壓為1.58 V，才能實現相同的電流密度。該系統在陰極產生了具有達到將近100 %法拉第效率的氫能。
在第二種方法中，我們成功加入負載在三維網狀材料上之混合合金氧化物來提高IOR電催化的穩定性。在本實驗中，我們展示了一種在3D網狀二氧化鈦上開發自支撐釕鈦混合合金氧化物(RuTiO)的簡便方法用於IOR電解。即使與熱力學析氧反應電位相比，在IOR系統中達到10 mA cm-2電流密度的電位也顯著降低了 220 mV，由於碘化物氧化的熱力學特性，開發的RuTiO需要1.09 V的超低電壓，才能為酸性介質進行IOR電解以提供10 mA cm-2的基準電流密度。在IOR的電解中，陰極電極處產生H2的法拉第效率幾乎為100%，也獲得了36小時持久穩定性測試，表明釕-鈦混合氧化物可作為陽極電催化劑用於IOR的節能電解生產高附加價值H2。這一發現將為設計其他低成本的過渡金屬混合合金氧化物電催化劑鋪路，該催化劑基於3D網狀二氧化鈦，具有更高的催化活性和更長的IOR電解穩定性。
在第三種方法中，我們研究了單原子合金催化劑的合成，以提高IOR催化活性並降低貴金屬含量。在這裡，我們展示了一種簡單的合成釕鈦單原子合金催化劑的步驟，該催化劑嵌入二氧化鈦（Ru SAAC）以改善碘化物氧化反應。因此，Ru SAAC 表現出優異的IOR活性，提供100 mV的低過電位以實現10 mA cm-2的電流密度和36 mV dec-1 的小Tafel斜率，表明在酸性電解質條件下具有熱力學有利和動力學快速的催化性能。與第一項和第二項工作相比，Ru SAAC表現出84.4%的最高法拉第效率，這表明由於最大原子效率，在IOR的電解中具有快速動力學。

Hydrogen (H2), as a non-carbon clean energy source, is the most attractive and environmentally friendly option to alleviate the future energy demand of society. Its production by water electrolysis is the most prominent and a front-running technology, but it requires the high overpotential to drive the sluggish anodic oxygen evolution reaction. This thesis has demonstrated three approaches to hybridize water electrolysis with more readily oxidizable anodic chemical feedstocks requiring low overpotentials.
In the first approach, we have developed a new type of hybrid electrolysis by employing iodide oxidation reaction. We fabricated the ruthenium-tin surface alloy oxide as anode electrocatalyst for iodide-assisted hybrid water electrolysis. The ruthenium-tin surface alloy oxide was prepared on the surface of rutile tin oxide through hydrothermal reaction of rutile tin oxide with the ruthenium ions in the presence of ethylene glycol as reducing agent. IOR-based electrolysis was compared with OER-based electrolysis over ruthenium-tin surface alloyed oxide as anode electrocatalyst. In a two-electrode system, the IOR-based electrolysis on ruthenium-tin surface alloyed oxide anode exhibits an ultra-low cell voltage of 1.01 V to reach a benchmark current density of 10 mA cm-2 compared OER-based electrolysis which needs a cell voltage of 1.58 V to achieve the same current density by the same anode electrocatalyst. This system produced a value-added hydrogen at the cathode with  100% Faradic efficiency.
In the second approach, we improved the IOR stability of the active electrocatalyst by incorporating mixed alloy oxide supported on three-dimensional web-like material. Here, we show a facile process to develop a self-supported ruthenium-titanium mixed alloy oxide (RuTiO) on a 3D web-like titania for IOR-based electrolysis. The potential for IOR to reach the current density of 10 mA cm-2 is remarkably reduced by 220 mV even compared to the thermodynamic oxygen evolution reaction potential. Because of the thermodynamic feature of iodide oxidation, the developed RuTiO require, an ultralow cell voltage of 1.09 V to afford a benchmark current density of 10 mA cm-2 for IOR-based electrolysis in acidic media. The Faradaic efficiency for H2 production is almost 100% at the cathode electrode in the IOR-based electrolysis. The long-lasting stability without degradation for 36 hours was obtained indicating that the ruthenium-titanium mixed oxide could be used as anode electrocatalyst in energy-saving IOR-based electrolysis for a value-added H2 production. This finding will pave a route to design other low-cost transition metal mixed alloy oxide electrocatalysts engineered on 3D web-like titania with improved catalytic activity and prolonged stability for IOR-based electrolysis.
In the third approach, we studied the synthesis of single-atom alloy catalyst to increase the IOR catalytic activity and to reduce the precious metal content. Here, we show a simple route for synthesis of ruthenium-titanium single-atom alloy catalyst embedded on titania (Ru SAAC) for improved iodide oxidation reaction. Thus, the Ru SAAC exhibited an excellent IOR activity which provided a low overpotential of 100 mV to achieve a current density of 10 mA cm-2 and a small Tafel slopes of 36 mV dec-1 indicating thermodynamically favorable and kinetically fast catalytic property in acidic electrolyte. The Ru SAAC exhibited the highest voltage efficiency of 84.4 % compared to the first and the second work which indicates its fast kinetics for IOR-based electrolysis due to the maximum atom efficiency.

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