| 罗莹,祁极冰,郭芳.化学通报,2016,79(7):597-603. |
| 络合铁法脱硫再生机理研究进展 |
| Research Progress on the Mechanism of Regeneration of Chelated Iron Desulfurization Solution |
| 投稿时间：2015-10-08 修订日期：2016-02-04 |
| DOI： |
| 中文关键词: 螯合亚铁 硫化氢 再生 羟基自由基 化学计量数 |
| 英文关键词:Chelating Ferrous hydrogen sulfide regeneration hydroxyl radical stoichiometry |
| 基金项目:国家自然科学(21376229)；山西省科学技术发展计划(工业部分)(20130321035-02)。 |
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| 中文摘要: |
| 络合铁法脱硫实现了催化剂的循环利用,其中亚铁离子再生是整个技术的核心。再生过程中,由于反应速率常数比值的不同,Fe2+的反应级数出现1级、2级乃至其间变化的各种结果；分子氧(O2)及其衍生物(如：超氧化物(Hn+O2.-),过氧化氢(H2O2),羟基(OH.))或高价的含氧铁中间体(如(L)Fe4+=O、(L﹒+) Fe4+=O和(L)nFe4+ (OH)(OOH))均可以氧化亚铁离子；典型配体EDTA、HEDTA和NTA亚铁的氧化机制是一致的。再生过程中配体有一个适宜的pH值范围,配体NTA过量时,其活性依赖pH值和NTA的浓度,NTA量的差别导致不同的反应途径。同时,由于氧化过程中配体消耗了过量的氧发生降解,从而造成化学反应计量数的偏差。 |
| 英文摘要: |
| The chelated iron desulfurization has realized the catalyst recycling, in which ferrous ion regeneration is the core of the whole technology. In the regeneration process, authors found the reaction to be first order, second order in Fe2 , and even found a transition in reaction order from 1 to 2, due to the different reaction rate constant ratio; The ferrous ion can be oxidized by molecular oxygen (O2) and its derivatives (such as: superoxide (Hn O2.-), hydrogen peroxide (H2O2), hydroxyl (OH.)) or high valence state of iron containing oxygen intermediates (such as (L)Fe4 =O、(L﹒ ) Fe4 =O and (L)nFe4 (OH)(OOH)). The oxidation mechanism of ferrous NTA appeared to be similar to that of ferrous chelates of EDTA and HEDTA. In the regeneration process, there was a suitable pH range for the ligand. When ligand NTA was excessive, its activity dependent on the pH and the concentration of the NTA, and the differences of the NTA concentration lead to different reaction pathways. In the oxidation reactions, the excess oxygen consumption was caused by the ligand, ligand degradation was occured, which leads to the deviation of the stoichiometry. |
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