首页|期刊导航|煤炭转化|热活化耦合铁负载改性埃洛石吸附剂联合脱除气态铅和铬的实验与机理研究

热活化耦合铁负载改性埃洛石吸附剂联合脱除气态铅和铬的实验与机理研究OA

Experimental and mechanistic study on the synergistic removal of gaseous lead and chromium using thermally activated coupled iron-loaded modified halloysite sorbents

中文摘要英文摘要

燃烧烟气中高浓度铅和铬的排放会对人体及环境造成严重危害,亟需加强对铅和铬的排放控制.采用900℃热活化耦合2 0%(质量分数)铁负载复合改性方法制备得到改性埃洛石(Fe-HNT)吸附剂.基于实验和密度泛函理论计算,系统探究了 Fe-HNT对铅和铬的联合脱除性能和吸附机理.实验结果表明,在800 ℃~1 100 ℃范围内,随温度升高,Fe-HNT对铅和铬的吸附效率先升高后降低,1 000℃为最佳吸附温度,铅和铬的吸附效率分别为77.59%和75.10%.联合脱除时,Fe-HNT对铅和铬的吸附效率略有降低,吸附效率分别为71.49%和73.39%.进一步采用XRD探究吸附产物的晶相组成及吸附机理,发现在吸附铅和铬的过程中,Fe-HNT与铅和铬发生了化学反应,吸附产物主要为铅和铬的硅铝酸盐、铁酸盐以及铬酸铁.采用密度泛函理论计算从微观层面揭示铅和铬在Fe-HNT表面的吸附机理,结果表明,吸附剂表面的Al、O和Fe原子均为铅和铬的活性吸附位点,由于铅和铬在吸附剂表面的活性位点相同,二者之间存在竞争吸附.其中铅易与埃洛石结合,铬则与Fe-HNT上的Fe2O3的结合能力更强,更易吸附在Fe2O3上.

High concentrations of lead and chromium in combustion flue gas pose serious risks to human health and the environment.Therefore,their emissions require effective control.A modified halloysite(Fe-HNT)adsorbent was prepared using a composite modification method combining thermal activation at 900 ℃ with 20%iron loading.The combined removal performance and adsorption mechanisms of Fe-HNT for lead and chromium were systematically investigated through a combination of experiments and density functional theory(DFT)calculations.The experimental results show that the adsorption efficiencies of Fe-HNT for lead and chromium first increase and then decrease as the temperature increases from 800 ℃ to 1 100 ℃.The optimal adsorption temperature is 1 000 ℃,with adsorption efficiencies of 77.59%for lead and 75.10%for chromium.During the combined removal of lead and chromium,the adsorption efficiencies of Fe-HNT decrease slightly,reaching 71.49%for lead and 73.39%for chromium.The crystalline phase composition of the adsorption products was further analyzed by XRD.During the adsorption process,Fe-HNT reacts chemically with lead and chromium.The adsorption products mainly consist of lead and chromium silicoaluminates,ferrites,and iron chromate.The adsorption mechanism of lead and chromium on the surface of Fe-HNT was revealed at the microscopic level using DFT calculations.The results indicate that the Al,O and Fe atoms on the Fe-HNT surface are active adsorption sites for lead and chromium.There is competitive adsorption between lead and chromium because they share the same active sites on the adsorbent.Lead preferentially binds to halloysite,whereas chromium exhibits a stronger binding affinity for Fe2O3 on Fe-HNT,making it more readily adsorbed onto Fe2O3.

张艾嘉;刘晶;杨应举;邸刘阳;胡艳军

浙江工业大学能源与碳中和科教融合学院,310014杭州||华中科技大学煤燃烧与低碳利用全国重点实验室,430074武汉华中科技大学煤燃烧与低碳利用全国重点实验室,430074武汉华中科技大学煤燃烧与低碳利用全国重点实验室,430074武汉华中科技大学煤燃烧与低碳利用全国重点实验室,430074武汉浙江工业大学能源与碳中和科教融合学院,310014杭州||浙江省清洁能源转化与利用重点实验室,310014杭州

资源环境

改性埃洛石联合脱除吸附机理密度泛函理论

leadchromiummodified hayllositecombined removaladsorption mechanismdensity functional theory

《煤炭转化》 2026 (4)

101-110,10

国家自然科学基金项目(U21A20142、523B2064、52236008)和湖北省自然科学基金重点项目(2023AFA039)

10.19726/j.cnki.ebcc.202604010

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