水中微量污染物、能源危機和溫室氣體(greenhouse gas)排放為目前全球所面臨的三個最為息息相關的環境威脅。為有效降這些環境污染問題，光電催化反應(photoelectrocatalysis)為最為彈性且具兼備高效率的處理方式之一，其提供更卓越的氧化還原催化效能，進一步擴展與應用至水處理技術、氫能源開發以及碳還原技術等。
目前多數的光電催化研究著重於半導體材料之創新，較缺少反應系統設計的探討，進而衍生催化劑對於光捕獲與光電轉換效率不足的缺陷。因此本研究的主要目的在建構三種新型光電催化系統，包括串聯式光電化學系統、光纖維電極和雙纖維光催化系統，並將之應用於污染物處理、水裂解產氫以及二氧化碳還原。在串聯光電催化系統中，本研究利用TAB3Bi2Br7I2 perovskite/g-C3N4為陽極，phosphorene/g-C3N4為陰極，在陽極進行廢水中污染物的光電催化降解，陰極進行水裂解產氫研究，研究發現於模擬廢水的條件(COD於50 mg L-1)下，環丙沙星於陽極系統高達73%之降解效率，產氫效能於陰極系統仍擁有~2 mmol h-1 g-1。其次，光纖維電極之開發由聚合物光纖(polymeric optical fiber)、氧化銦錫半導體材料與可見光材料於Nafion-PVDF聚合物表面上方分層組成，突破光纖固有之絕緣特性。與相同製備過程之玻璃光電極反應面積(2 cm2)與量子效率(1.5%)相比，此項光纖電極分別大幅增進了7倍(14.1 cm2)與9倍(13.1%)之表現性。最後，雙纖維光催化系統集成了鐵金屬有機架構物-聚合物光纖以及高效率氣體傳輸之中空膜纖維(hollow membrane fiber)，提升CO2(aq)分子與光響應奈米材料層吸附機會，加速碳還原應用之生成效率。相較於光催化漿料反應之甲酸(formic acid)產率(5 mM h-1 g-1)，此系統之產率增加至16倍(82 mM h-1 g-1)，並實現對甲酸生成之高選擇性(> 99%)。根據上述三項創新的光(電)催化系統之突破性與潛力，本研究成功提出針對光電催化系統的開發與創新，並且實現將低環境負荷目標以及可持續發展的處理平台，以高效處理潛在的污染問題，同時修復目前所面臨的環境挑戰。

Micropollutants in water, the energy crisis, and greenhouse gas (GHG) emissions are three pressing environmental challenges confronting the world today. As technological advancements continue, the detection limitations of these pollutants have become increasingly critical. Nevertheless, the fundamental treatment processes currently in use are proving insufficient. Therefore, it is imperative to rapidly discover solutions to these intricate water pollution problems, reduce the dependence on fossil energy, and effectively address GHG issues. Photoelectrocatalytic processes (PECs) combine photocatalysis and electrochemical principles to enhance charge carrier migration. Nano-enabled PECs can be used for water purification, hydrogen (H2) production, and CO2 reduction.
While most PEC studies focus on nanomaterial (NM) developments, the reactor design of PEC is also important to maximize the conversion efficiency of photons and electrons. To develop a low-cost, sustainable, and flexible catalytic platform under photo(electro)catalysis, we create three novel PEC systems: tandem PEC devices, optoelectrode fiber, and dual-fiber system. First, the tandem PEC system combines the TAB3Bi2Br7I2 perovskite/g-C3N4 anode and phosphorene/g-C3N4 photocathode. This enhances the interaction of electrons, holes, and protons for redox reactions. Our study discovered that when simulating wastewater conditions with a COD of 50 mg L-1, ciprofloxacin photoelectrocatalytic degradation showed an impressive efficiency of up to 73% within the anode system. Furthermore, the cathode system exhibited a H2 production performance of ~2 mmol h-1 g-1. Second, optoelectrode fiber, polymeric optical fiber (POF) integrated with indium tin oxide (ITO) NM plus visible-photocatalysts in the Nafion-PVDF polymers surface layer, break through the original insulation property to add an electrically-conductivity for PEC utilization. Compared to glass photoelectrodes within the same NMs deposition, this PEC-POF architecture achieves 7- and 9-fold in the catalytic reaction area (i.e., 2 cm2 → 14.1 cm2) and quantum efficiency (i.e., 1.5% → 13.1%), respectively. Last, the photocatalytic dual-fiber system, incorporated with NH2-MIL-101(Fe)-optical- and CO2-delivering hollow membrane-fiber, forms a sustainable CO2(aq) delivered into the catalysts, accelerating the reactive capability in carbon reduction. The CO2-to-HCOOH conversion rates (82 mM h-1 g-1) were >16-fold higher than the photocatalytic slurry reaction (~5 mM h-1 g-1), and the HCOOH selectivity was up to 99%. Drawing on the groundbreaking advancements and potential of the three innovative photo(electro)catalytic systems, this study has successfully introduced novel approaches to the development of PEC architectures. This achievement establishes an environmentally friendly and sustainable processing platform that efficiently addresses pollution concerns and current environmental challenges.

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