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水钠锰矿催化邻苯二酚、对苯二酚和间苯二酚的氧化降解及相关矿化作用。

Oxidative degradation and associated mineralization of catechol, hydroquinone and resorcinol catalyzed by birnessite.

作者信息

Chang Chien S W, Chen H L, Wang M C, Seshaiah K

机构信息

Department of Environmental Engineering and Management, Chaoyang University of Technology, Wufong Township, Taichung County 41349, Taiwan, ROC.

出版信息

Chemosphere. 2009 Feb;74(8):1125-33. doi: 10.1016/j.chemosphere.2008.10.007. Epub 2008 Nov 22.

Abstract

Abiotic degradation and mineralization of catechol, hydroquinone, and resorcinol catalyzed by birnessite (delta-MnO2) was investigated. Studies were carried out by monitoring changes of pE versus time and pH versus time of the reaction systems during the initial 10 h reaction period and release of CO2 and associated reactions at the end of a 90 h reaction period. The reactions under anoxic condition were compared with aeration condition. The reactions were carried out in suspensions at initial pH of 6.0 under air and N2 atmosphere at room temperature and free of microbial activity. These results indicated that kinetic-related changes of pE versus time and pH versus time were dependent on structural characteristics of phenolic compound and aeration or anoxic condition in the reaction system. The sequence of the mineralization of phenolic compounds catalyzed by delta-MnO2 in presence of air expressed by CO2 release was catechol > hydroquinone > or = resorcinol and the differences were significant. However, under an N2 atmosphere the amounts of CO2 released were drastically reduced with insignificant differences among the three reaction systems. Further, phenolic compound degradations, dissolved and adsorbed Mn, and oxidation state of Mn in delta-MnO2 were also determined to elucidate the catalytic efficacy mediated by both O2 and delta-MnO2 in the reaction systems.

摘要

研究了水钠锰矿(δ-MnO₂)催化邻苯二酚、对苯二酚和间苯二酚的非生物降解及矿化作用。通过监测反应体系在初始10小时反应期内pE随时间和pH随时间的变化,以及在90小时反应期结束时二氧化碳的释放及相关反应来开展研究。将缺氧条件下的反应与曝气条件下的反应进行了比较。反应在室温下于空气和氮气气氛中、初始pH为6.0的悬浮液中进行,且无微生物活性。这些结果表明,pE随时间和pH随时间的动力学相关变化取决于酚类化合物的结构特征以及反应体系中的曝气或缺氧条件。在有空气存在的情况下,由δ-MnO₂催化的酚类化合物矿化作用以二氧化碳释放量表示的顺序为邻苯二酚>对苯二酚≥间苯二酚,且差异显著。然而,在氮气气氛下,二氧化碳的释放量大幅减少,三个反应体系之间的差异不显著。此外,还测定了酚类化合物的降解、溶解和吸附的锰以及δ-MnO₂中锰的氧化态,以阐明反应体系中氧气和δ-MnO₂介导的催化效果。

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