三维网络结构石墨烯/Fe@δ-MnO2水凝胶低温高活性催化矿化苯酚的研究

Thorough removal of organic pollutants in water with energy-saving method at room temperature is one of the important water pollutant control research. The catalyst δ-MnO2 is widely used in the catalytic degradation of low concentration organic compounds owing to strong oxidation. However, there are still many problems such as high catalytic reaction temperature, weak mineralization ability and need separation. In order to achieve complete mineralization and removal of organic pollutants, we prepared three-dimension network structure graphene /Fe@ δ-MnO2 with high activity and strong oxidation which could adsorb and enrich low concentration organic pollutants in water and the problems of separation and continuous flow degradation were solved. The imbedding of the catalyst MnO2 has realized the self regeneration of the adsorbents, the three-dimensional graphene structure solves the enrichment of phenol and accelerates the catalytic reaction rate. The local high temperature (200-300℃) produced by the contact interface between Fe and δ-MnO2 promotes the fracture of the chemical bond of phenol, accelerates the catalytic oxidation process and realizes complete mineralization. Based on the three-dimensional network structure of graphene /Fe@ δ-MnO2 with high surface area, the mechanism of in situ adsorption enrichment and degradation of low concentration organic pollutants in water was revealed. The law of formation of three-dimensional network structure and its influence on adsorption performance were revealed. The influence of anchoring location of catalyst and pollutant adsorption and enrichment at low temperature was revealed, providing a theoretical basis for wastewater treatment.

常温条件下以节能方式彻底净化工业排放含酚废水，是水污染物控制研究中的重要内容之一。能净化苯酚的强氧化δ-MnO2存在催化反应温度高、矿化能力弱、需要分离等问题亟待解决。本课题拟通过结构调控研制出石墨烯/Fe@δ-MnO2三维网络结构，对水中低浓度苯酚进行吸附富集-室温定点催化氧化降解，实现苯酚彻底矿化去除的研究，解决了二次污染、分离和连续流动降解问题。催化剂MnO2的嵌入实现了吸附材料自再生问题、三维石墨烯结构解决了苯酚的富集，加速了催化反应速率。 利用金属Fe吸光与δ-MnO2接触界面产生的局域高温（200-300℃），促进苯酚化学键的断裂，加速催化氧化过程，实现完全矿化。揭示催化材料的结构调控对含酚废水的吸附富集性能以及催化降解规律。揭示三维网络结构的形成规律以及对吸附性能的影响规律，揭示催化剂的锚定位置与污染物吸附富集低温催化降解的影响规律，为废水治理提供理论依据。

常温条件下以节能方式彻底净化工业排放含酚废水，是水污染物控制研究中的重要内容之一。能净化苯酚的强氧化δ-MnO2存在催化反应温度高、矿化能力弱、需要分离等问题亟待解决。酚类污染物的室温深度矿化是目前解决煤化工污染的重要难题。本文通过MnO2的优势暴露晶面(001)调节生长，产生的Jahn-Teller 效应诱导了晶面势调控，实现了室温条件下酚类污染物的深度矿化。研究结果发现纳米花结构MnO2具有密排堆积的层状结构，(100)晶面MnO2具有纳米球形貌且具有开口通道的晶体学结构。苯酚降解实验表明(100) MnO2较 (001) MnO2具有3倍的速率，超过30%的降解度，降低了约11KJ/mol 的反应活化能，60 ℃矿化度为37%。通过ESR以及DFT共同证实：(001) 晶面MnO2通过氧气与其表面空位耦合发生1个电子的转移产生超氧活性物种，(100)晶面MnO2通过氧气与其表面空位耦合发生2个电子的转移产生过氧活性物种，此活性物种为(100) MnO2 较(001) MnO2在反应速度提高，矿化度增加，及反应活化能降低的本质。此工作已经发表在了Applied catalytic B environment. 利用三维石墨烯结构可以实现对污染物的吸附富集-光催化协同原位净化。本文通过制备高氧化度的氧化石墨烯进一步增强了石墨烯复合磷酸铋气凝胶的光催化活性。根据对复合材料进行的SEM、FTIR、Raman、XRD、DRS等表征探究了氧化石墨烯对复合材料的形貌、结构以及光吸收特性的影响。高氧化度BiPO4/GA复合材料降解苯酚的表观速率常数约为商业复合材料的1.88倍。结果证实，高氧化度的氧化石墨烯大大提高了复合材料的光催化性能。此工作已经发表到Chemical Engineering Journal.

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