高等学校化学学报
高等學校化學學報
고등학교화학학보
CHEMICAL JOURNAL OF CHINESE UNIVERSITIES
2014年
4期
760-765
,共6页
硫化氢%有机胺型铁基离子液体%湿法氧化
硫化氫%有機胺型鐵基離子液體%濕法氧化
류화경%유궤알형철기리자액체%습법양화
H2 S%Amine Fe-based ionic liquid%Wet oxidation
合成了有机胺型铁基离子液体1.6Et3 NHCl·FeCl3,研究了其热稳定性和对H2 S的吸收与再生性能.考察了H2 S浓度为832 mg/m3,温度为40~180℃,气体流速分别为100,300,400和500 mL/min条件下H2 S的去除率,结果表明当气体流速小于400 mL/min时,吸收率可达100%;随着温度升高,吸收效率提高并趋于恒定.在最优条件下测得1.6Et3 NHCl·FeCl3离子液体的硫容量为6.36 g/L,远高于[ Bmim] FeCl4离子液体.通过比较吸收H2 S前后的红外光谱图,进一步确定了氧化反应的发生.采用密度泛函理论从分子水平上研究了H2S与1.6Et3NHCl·FeCl3和[Bmim]FeCl4两种铁基离子液体以及Fe3+水溶液的相互作用,从理论上比较了脱硫剂中的基质对H2 S吸收的影响,确定了胺基对H2 S吸收的促进作用.通过对脱硫产物的XRD分析,确定了斜方晶体(α-硫)的生成,与传统水相湿法氧化脱硫得到的产物相同.通入空气可快速有效地对1.6Et3 NHCl·FeCl3离子液体进行再生.
閤成瞭有機胺型鐵基離子液體1.6Et3 NHCl·FeCl3,研究瞭其熱穩定性和對H2 S的吸收與再生性能.攷察瞭H2 S濃度為832 mg/m3,溫度為40~180℃,氣體流速分彆為100,300,400和500 mL/min條件下H2 S的去除率,結果錶明噹氣體流速小于400 mL/min時,吸收率可達100%;隨著溫度升高,吸收效率提高併趨于恆定.在最優條件下測得1.6Et3 NHCl·FeCl3離子液體的硫容量為6.36 g/L,遠高于[ Bmim] FeCl4離子液體.通過比較吸收H2 S前後的紅外光譜圖,進一步確定瞭氧化反應的髮生.採用密度汎函理論從分子水平上研究瞭H2S與1.6Et3NHCl·FeCl3和[Bmim]FeCl4兩種鐵基離子液體以及Fe3+水溶液的相互作用,從理論上比較瞭脫硫劑中的基質對H2 S吸收的影響,確定瞭胺基對H2 S吸收的促進作用.通過對脫硫產物的XRD分析,確定瞭斜方晶體(α-硫)的生成,與傳統水相濕法氧化脫硫得到的產物相同.通入空氣可快速有效地對1.6Et3 NHCl·FeCl3離子液體進行再生.
합성료유궤알형철기리자액체1.6Et3 NHCl·FeCl3,연구료기열은정성화대H2 S적흡수여재생성능.고찰료H2 S농도위832 mg/m3,온도위40~180℃,기체류속분별위100,300,400화500 mL/min조건하H2 S적거제솔,결과표명당기체류속소우400 mL/min시,흡수솔가체100%;수착온도승고,흡수효솔제고병추우항정.재최우조건하측득1.6Et3 NHCl·FeCl3리자액체적류용량위6.36 g/L,원고우[ Bmim] FeCl4리자액체.통과비교흡수H2 S전후적홍외광보도,진일보학정료양화반응적발생.채용밀도범함이론종분자수평상연구료H2S여1.6Et3NHCl·FeCl3화[Bmim]FeCl4량충철기리자액체이급Fe3+수용액적상호작용,종이론상비교료탈류제중적기질대H2 S흡수적영향,학정료알기대H2 S흡수적촉진작용.통과대탈류산물적XRD분석,학정료사방정체(α-류)적생성,여전통수상습법양화탈류득도적산물상동.통입공기가쾌속유효지대1.6Et3 NHCl·FeCl3리자액체진행재생.
Amine Fe-based ionic liquid 1.6Et3NHCl·FeCl3 was synthesized with ideal H2S absorption ca-pacity and good thermostability. H2 S removal efficiency was tested under the condition with H2 S concentration of 832 mg/m3 , temperature ranging from 40 ℃ to 180 ℃, and gas flow of 100, 300, 400 or 500 mL/min. The results showed that when the gas flow was less than 400 mL/min, H2 S removal efficiency could reach 100%; H2 S removal efficiency increased with the increasing in temperature and tended to approach an asymp-totic value. Under the optimal conditions, the sulfur capacity of 1.6Et3NHCl·FeCl3 was 6.36 g/L, higher than that of [ Bmim] FeCl4 . Comparing the FTIR spectra before and after H2 S absorption, redox reaction be-tween 1.6Et3NHCl·FeCl3 and H2S was confirmed. The interaction between H2S and 1.6Et3NHCl·FeCl3/[ Bmim] FeCl4/H2 O has been studied at the molecular level using density functional theory, and the influence of the substrate on H2 S absorption was illustrated to be responsible for the enhancement of H2 S absorption by aminal group. The product after H2 S absorption was orthorhombic crystal sulfur(α) , which is the same as the product from traditional aqueous phase oxidation desulfurization. 1.6Et3NHCl·FeCl3ionic liquid can be re-used efficiently after quick regeneration by air flow.