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采用改进的低pH值液体氧化还原硫回收(LRSR)工艺并通过铁催化剂对的电化学再生来去除硫化氢(H2S)气体。

H2S(g) removal using a modified, low-ph liquid redox sulfur recovery (LRSR) process with electrochemical regeneration of the Fe catalyst couple.

作者信息

Gendel Youri, Levi No'omi, Lahav Ori

机构信息

Faculty of Civil and Environmental Engineering, Technion, Haifa, 32000, Israel.

出版信息

Environ Sci Technol. 2009 Nov 1;43(21):8315-9. doi: 10.1021/es901594j.

DOI:10.1021/es901594j
PMID:19924962
Abstract

A modified pH 1.0 liquid redox sulfur recovery (LRSR) process, based on reactive absorption of H(2)S((g)) in an acidic (pH 1.0) iron solution ([Fe(III)] = 9-8 g L(-1), [Fe(II)] = 1-2 g L(-1)) and electrochemical regeneration of the Fe(III)/Fe(II) catalyst couple, is introduced. Fe(II) was oxidized in a flow-through electrolytic cell by Cl(2(aq)) formed on a Ti/RuO(2) anode. pH 1.0 was applied to retard the potential precipitation of predominantly jarosite group Fe(III) species. At pH 1.0, the presence of chloride ions at [Cl(-)] = 30 g L(-1) allows for both efficient (indirect) electrochemical oxidation of Fe(II) and efficient H(2)S((g)) reactive absorption. The latter observation was hypothesized to be associated with higher concentrations of Fe(III)-Cl complexes that are more highly reactive toward H(2)S((aq)) than are free Fe(III) ions and Fe-SO(4) complexes that otherwise dominate pH 1.0 Fe(III) solutions in the absence of a significant Cl(-) concentration. At the described operational conditions the rate of Fe(II) oxidation in the experimental system was 0.793 kg Fe h(-1) per m(2) anode surface area, at a current efficiency of 58%. Electricity cost within the electrochemical step was approximated at $0.9 per kg H(2)S((g)) removed.

摘要

介绍了一种改进的pH 1.0液体氧化还原硫回收(LRSR)工艺,该工艺基于在酸性(pH 1.0)铁溶液([Fe(III)] = 9 - 8 g L⁻¹,[Fe(II)] = 1 - 2 g L⁻¹)中对H₂S(g)进行反应吸收以及Fe(III)/Fe(II)催化剂对的电化学再生。Fe(II)在流通式电解池中被Ti/RuO₂阳极上形成的Cl₂(aq)氧化。采用pH 1.0来抑制主要为黄钾铁矾族Fe(III)物种的潜在沉淀。在pH 1.0时,[Cl⁻] = 30 g L⁻¹的氯离子的存在既允许Fe(II)进行高效的(间接)电化学氧化,也允许H₂S(g)进行高效的反应吸收。据推测,后一种观察结果与较高浓度的Fe(III)-Cl络合物有关,这些络合物对H₂S(aq)的反应性比游离Fe(III)离子和Fe-SO₄络合物更高,否则在没有显著Cl⁻浓度的情况下,Fe-SO₄络合物在pH 1.0的Fe(III)溶液中占主导地位。在所描述的操作条件下,实验系统中Fe(II)的氧化速率为每平方米阳极表面积0.793 kg Fe h⁻¹,电流效率为58%。电化学步骤中的电费估计为每去除一千克H₂S(g) 0.9美元。

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