水污染日趨嚴重，高級氧化法應用於有機廢水處理受到廣泛注意。雙氧水為綠色化學氧化劑，可誘導高反應性物質(例如：∙OH)生成。但目前商業化製造雙氧水之蒽醌法受制於複雜操作、安全顧慮及有機溶劑二次污染等問題。因此本研究重點包括: (1)利用原位紫外/可見光譜即時監測代表性有機物之反應動力學；(2)發展新穎平面碳點修飾之碳氮複合物(GCN/PDI/CDs)應用於光驅動同時產生雙氧水及有機物氧化；及(3)利用改良之熱縮合法，將富氮單體併入酚醛樹酯，以提升太陽光驅動生成雙氧水之產率。建立原位紫外/可見光譜的量測方法，可達到同時氧化及監測有機物之目的，但廢水代表性有機污染物：苯、氯苯、萘、布洛酚及亞甲藍與雙氧水吸光度部分重疊干擾，採一階動力修正方法使之達到最小化，以獲得之反應動力參數：擬一階反應動力常數(kt)介於0.0026~0.0338 min-1，二階反應動力常數(k·OH)介於1.756×1011~1.78×1012 M-1min-1。經由簡單的熱沉浸法製備新穎平面GCN/PDI/CDs，改質之碳氮複合物於5小時可見光照射可以生成252 μM之雙氧水，此外，亞甲藍經3小時可見光照射，可有效光催化氧化，碳點具有優良的電子傳遞能力，可以有效降低電子與電洞再結合率，並活化雙氧水產生高反應性物質。另外，透過簡單酸化程序，將蜜勒單體與間苯二酚進行共聚合製備新穎球型富氮樹酯(RFM)促進光驅動雙氧水生成反應發生，吸收光譜分析顯示富氮樹酯可吸收可見光達700 nm、能隙約為1.8-2 eV。富氮樹酯經5小時可見光照射下可以生成195 μM之雙氧水，此外，相較於三嗪單體，庚嗪單體具有更好的導電性及光反應活性位置，結果清楚顯示此新型有機聚合物可應用於光驅動雙氧水生成及有機物氧化。所開發之原位紫外/可見光譜法可以提高有機物動力學研究之便捷性，並提供反應程序設計之重要參考依據，新穎碳催化劑具低成本及環境友善之優勢，可應用於有機物廢水處理。

Advanced oxidation processes (AOPs) for organic wastewater treatments have received widely attention. Hydrogen peroxide (H2O2), being a green oxidant, is an important precursor to induce formation of highly reactive species (such as ∙OH) for AOPs. However, H2O2 has been produced by anthraquinone (AO) process which has many disadvantages such as complicated operation, high safety risk, and organic solvents pollution. Regardless of the high H2O2 yield rate in the AO process, high energy consumption is still the main challenge for the tolerable cost for AOPs. Thus, the major objectives of this study were: (1) Real-time determination for photocatalytic oxidation kinetic of presentative organic pollutants by in situ UV/Vis spectroscopy; (2) Simultaneously photocatalytic generation of H2O2 and on-site utilization for AOP by the new 2D planar carbon dot dispersed carbon nitride composite (GCN/PDI/CDs); (3) Photocatalytic H2O-to-H2O2 by the novel melem incorporated 3D spherical nitrogen-enriched resin photocatalysts by incorporation of melem into phenolic resin. An in situ UV/Vis spectroscopic cell was used to simultaneous monitor the oxidation of representative organic pollutants such as benzene, chlorobenzene, naphthalene, methylene blue and ibuprofen in wastewater. The interference of the UV/Vis absorption overlap between H2O2 and representative organic pollutants was minimized by justified raw kinetic data. The pseudo first-order rate constants (kt) were in the range of 0.0026-0.0338 min-1. The second-order rate constants (k·OH) for the reaction between representative organic pollutants and hydroxyl free radicals were 1.756×1011-1.78×1012 M-1min-1. The new 2D planar carbon dot (CD) dispersed carbon nitride (GCN/PDI/CD) composites were prepared by the facile impregnation-thermal method. Accumulated 252 μM of H2O2 were yielded in a 5-h visible light irradiation in the presence of the GCN/PDI/CD composites. Additionally, methylene blue could be photocatalytically oxidized within a 3-h visible light irradiation. Carbon dot, being an excellent electrons conductor, can effectively reduce the recombination of photo-excited electron and hole, and activate H2O2 to yield high reactive species such as ·OH.
The novel 3D spherical nitrogen-enriched resin photocatalyst was prepared by copolymerization of resorcinol and melem via a simple acidification process for facilitating the photocatalytic H2O-to-H2O2 reaction. Their UV/Vis spectra show that the nitrogen-enriched resin have a strong absorbance between 200-700 nm, corresponding to a band gap energy of 1.8-2 eV under the visible light irradiation. Accumulated 195 μM of H2O2 can be yielded in a 5-h irradiation by the resin photocatalysts. In addition, the phenolic resin copolymerized with heptazine possessing a better conductivity and more photo-active sites has a high photocatalytic effectiveness. The developed in situ UV/Vis spectroscopic method can provide a fast reaction kinetic study for processes design. The novel carbon photocatalysts, having the advantages of a relatively low-cost and eco-friendly, can be used for the treatments of organic wastewater.

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