本文選題：過一硫酸鹽 + 硫酸根自由基�。� 參考：《合肥工業(yè)大學(xué)》2015年碩士論文

【摘要】：本文針對持久性有機污染物難以治理的技術(shù)難題,開展以催化材料為核心的新型類Fenton技術(shù)研究,圍繞類Fenton催化劑的理性設(shè)計和基礎(chǔ)科學(xué)問題,構(gòu)建基于硫酸根自由基(SO.-)的石墨烯基復(fù)合催化劑(Mn3O4-rGO, Co-rGO和Co(OH)2)/PMS耦合催化氧化去除水中有機物,以活性自由基基團生成速率與生成效率為優(yōu)化指標(biāo),設(shè)計并制備出新型石墨烯基復(fù)合催化劑,揭示了催化劑生長機理和結(jié)構(gòu)控制途徑,探明了礦化有機物的反應(yīng)機理,詮釋了催化材料的組成—結(jié)構(gòu)—表/界面性質(zhì)—催化性能間的構(gòu)效關(guān)系,在新型類Fenton的基礎(chǔ)理論和應(yīng)用兩個方面均取得了較好的成績。本論文的主要研究內(nèi)容如下所示：(1)以鱗片石墨為原料,采用改進的Hummers法制備氧化石墨,以所制備的氧化石墨作為前驅(qū)體,在水溶液中用原位合成技術(shù)成功制備了納米Mn3O4-rGO復(fù)合物催化劑,并研究了其活化PMS降解有機污染物金橙Ⅱ的性能。采用FESEM、EDS、TEM、XRD、Raman、XPS和TGA對所制備的催化劑進行相關(guān)的表征測試,表征的結(jié)果表明Mn304納米顆粒成功負(fù)載到石墨烯表面,Mn3O4-rGO雜化材料中的Mn304納米顆粒的平均粒徑為29.2 nm。催化性能測試表明,常溫條件下,濃度為0.5g/L的Mn304-rGO催化劑能在120 min內(nèi)將30 mg/L的金橙II完全降解。此外,金橙II的降解效率隨溫度(25-55℃)、pH值(4.0.11.0)PMS濃度(0.25-1.5g/L)的升高而升高,但隨金橙II溶液初始濃度(30-90 mg/L)的升高而降低。同時,催化劑在循環(huán)4次后仍可在120 min內(nèi)反應(yīng)完全,顯示出良好的穩(wěn)定性。(2)以氧化石墨為原料,采用原位合成技術(shù)制備出Co-rGO催化劑的前驅(qū)體,再通過氫氣還原成功制備Co-rGO催化劑,并以此構(gòu)建了納米Co-rGO/PMS的新型高級氧化體系。研究發(fā)現(xiàn),在納米Co-rGO復(fù)合物中,Co納米顆粒與石墨烯的結(jié)合在催化活性方面起到了協(xié)同作用。與純Co納米顆粒相比,納米Co-rGO復(fù)合物對PMS分解反應(yīng)的催化活性更強,更有利于有機污染物的氧化降解。在相同催化劑(Co-rGO)和PMS(0.2g/L)用量下,Co-rGO/PMS體系中金橙Ⅱ(60mg/L)的降解遵循準(zhǔn)一級反應(yīng)動力學(xué),速率常數(shù)k為0.0747 min-1,是Co/PMS體系中表觀速率常數(shù)k (0.0357 min-1)的2.1倍。(3)采用簡單的水熱合成法,以葡萄糖為氧化石墨烯的還原劑,成功制備出α-Co(OH)2-rGO的雜化材料,并對利用該催化劑活化PMS降解苯酚的性能進行了研究。催化劑的表征結(jié)果表明α-Co(OH)2納米顆粒隨機的、無規(guī)律的負(fù)載在石墨烯片層上。催化劑的催化性能研究發(fā)現(xiàn),在催化劑濃度為0.02 g/L, PMS濃度為0.5g/L的條件下,α-Co(OH)2-rGO/PMS體系在40 min內(nèi)對30 mg/L苯酚溶液的降解率達到了99%。當(dāng)α-Co(OH)2-rGO濃度提高到0.1 g/L,10min即可將等量的苯酚溶液完全降解。最后,利用HPLC技術(shù),檢測了α-Co(OH)2-rGO/PMS體系降解苯酚的中間產(chǎn)物,并給出了苯酚降解的機理。
[Abstract]:In this paper, aiming at the technical problems of persistent organic pollutants (pops) being difficult to control, a new type of Fenton technology with catalytic material as its core is developed, which focuses on the rational design and basic science of Fenton-like catalysts. A graphene based composite catalyst based on sulphate radical (SO.-) was constructed for the removal of organic compounds in water by coupled catalytic oxidation of mn _ 3O _ 4-rGO. Co-rGO and Co(OH)2)/PMS. The formation rate and efficiency of active radical groups were taken as the optimization index. A novel graphene based composite catalyst was designed and prepared. The mechanism of catalyst growth and structure control was revealed, and the reaction mechanism of mineralized organic matter was explored. The structure-activity relationship between the composition, structure, surface / interface properties and catalytic properties of the catalytic materials was explained, and good results were obtained in the basic theory and application of the new Fenton. The main contents of this thesis are as follows: (1) using flake graphite as raw material, graphite oxide was prepared by improved Hummers method, and graphite oxide was used as precursor. Nano-sized Mn3O4-rGO complex catalysts were successfully prepared by in-situ synthesis in aqueous solution, and their catalytic properties for the degradation of gold orange 鈪，

本文編號：1966481