基于氨基多羧酸螯合铁催化氧化硫化氢技术的研究进展  

Study on Catalyst Oxidetion H_2S with Aminopolycarboxylic Chelating Iron

作　　者：张世光[1,2] 罗莹[1,2] 郭芳[1,2] 

机构地区：[1]中北大学超重力化工山西省重点实验室,山西太原030051 [2]中北大学山西省超重力化工工程技术研究中心,山西太原030051

出　　处：《中北大学学报（自然科学版）》2016年第6期625-632,共8页Journal of North University of China(Natural Science Edition)

基　　金：国家自然科学基金资助项目(21376229)

摘　　要：基于络合铁法脱硫的催化氧化技术用于脱除恶臭污染物H2S气体已成为能源加工业的研究热点.本文综述了30年来国外脱硫过程中的络合化学、反应机理及动力学等研究内容.首先提出适宜螯合剂的平衡常数范围,指出有氧供体的配体生成的Fe(Ⅲ)/Fe(Ⅱ)螯合剂的稳定性高;其次认为吸收反应过程中各中间产物存在形态是pH值的函数,Fe(Ⅲ)通过羟基化的途径来增强反应活性,中间物反应活性的差异与pH值、螯合剂中配位基团的结构、数量有关.同时通过对螯合剂降解机理的比较分析指出配体被OH·氧化攻击的地方是在-亚甲基与羧酸盐基团之间,亚甲基在乙烯桥中连接两个氮原子,从而为如何抑制络合剂的降解提供了参考;最后对我国络合铁法脱硫当前存在的问题及未来的研究方向进行了探讨.Gas desulfurization processes based on iron chelate chemistry as a catalytic oxidization technology for the removal of H2 S in energy processing industries has received increasing attention.Complex chemistry,mechanism and dynamics of desulfurization processes based on iron chelate are reviewed in recent 30 years.Firstly,an unexpected result of this study is that favorable redox reactions are associated with conditional constants that vary over a wide range of numerical values,ligands that form suitable iron complexes as catalysts have oxygen donors.Then,it is the hydroxyl radical that has ability to oxidation Fe（Ⅲ）chelates whereas ferryl has not.It is seen that pH has significant impact on the ferric chelate complexs on the reactive absorption rate of H2 S,and the phenomenon of increasing reactivity of ferric chelates with hydroxylation is shown too.The observation indicates that pH,the number and structure of coordinating groups on chelates are related to the difference of intermediate reactivity.Furthermore,the intermediates and products of the oxidative degradation of each chelating agent are described and compared.During the reoxidation of the ferrous formed and which in turn generates the hydroxyl radical by reaction with ferrous ion.The site of oxidative attack by the hydroxyl radical on these ligands seems to be the-CH2- groups a to the carboxylate groups,as well as the-CH2- groups in the ethylene bridges between the nitrogen.Lastly,the current problems as well as the corresponding research directions are discussed.

关 键 词：螯合铁 氧化还原 硫化氢 催化氧化 降解 

分 类 号：TQ028.8[化学工程]