摘要
选用桑蚕废弃物蚕沙为碳源,利用ZnCl2和FeCl2作为活化剂,通过一步合成法获得一种Fe掺杂高石墨化多孔生物炭材料Fe/Z-ASE,并测定香精化合物分子苯乙醇和茴香醚在Fe/Z-ASE上的吸附和缓释动力学行为,然后再通过量子化学计算分析苯乙醇、茴香醚与Fe/Z-ASE的作用关系以及苯乙醇、茴香醚分子间作用力。结果发现:蚕沙多孔炭Fe/Z-ASE孔隙结构发达,表面石墨化碳含量高,Fe元素分布均匀,其BET比表面积为950.9 m^2/g且中孔占60%以上,是一种表面疏水并呈现弱极性的多级孔生物炭材料;在苯乙醇和茴香醚的扩散和控释过程中,茴香醚具有比苯乙醇更高的吸附量(510 mg/g)和扩散动力学常数(1.7×10^-2 min^-1),而且在不同初始茴香醚吸附量下(150~500 mg/g)其都能获得较好的控释效果。随后通过密度泛函DFT模拟计算可知,茴香醚和苯乙醇都是弱碱,能与Fe/Z-ASE材料上的弱酸性吸附位(Fe-C)产生相互作用,而且由于茴香醚的碱性更弱,所以与Fe/Z-ASE的作用力更强。然后再通过分子动力学分析可知,苯乙醇分子间能产生强氢键作用而茴香醚分子间不存在强相互作用,所以苯乙醇分子在高初始吸附量下不易被脱附,而茴香醚分子在高/低初始吸附量下都能获得较高脱附保留率。
The silkworm waste from the silkworm was selected as the carbon source,and ZnCl2 and FeCl2 were used as activators to obtain a Fe-doped highly graphitized porous biochar material Fe/Z-ASE through a one-step synthesis method.The fabricated Fe/Z-ASE was tested for the adsorption and sustained-release kinetics of pheneylethanol and anisole while their mutual interaction and intermolecular interactions were evaluated by quantum chemical calculation.The silkworm feces exhibited a well-developed pore structure,high surface graphitized carbon content,high BET surface area(950.9 m^2/g),more than 60%mesopores and uniform distribution of Fe.Fe/Z-ASE exhibited hydrophobic surface and weak polarity,while anisole realized higher adsorption capacity(510 mg/g)and diffusion rate of 1.7×10^-2 min^-1 than that of phenylethanol under variable anisole adsorption amounts(150—510 mg/g).Density functional simulations suggested anisole and phenylethanol as weak bases and hence interacted with the weakly acidic adsorption sites(Fe-C)on the Fe/Z-ASE,while the relatively higher basicity of anisole endorsed it stronger interaction with Fe/Z-ASE.Molecular dynamics analysis showed strong hydrogen bonding between pheneylethanol molecules while no such interaction existed among anisole molecules,which hindered the desorption of pheneylethanol molecules under high initial adsorption capacity as compared to those of anisole.
作者
陈功
武煜翔
卢真保
王炳锋
杨东晓
赵钟兴
黄艳
CHEN Gong;WU Yuxiang;LU Zhenbao;WANG Bingfeng;YANG Dongxiao;ZHAO Zhongxing;HUANG Yan(Huabao Flavor Company Limited by Shares,Lhasa 850000,Tibet,China;Guangzhou Huafang Tobacco Flavor Company Limited by Shares,Guangzhou 510530,Guangdong,China;School of Chemistry&Chemical Engineering,Guangxi University,Nanning 530004,Guangxi,China;College of Materials and Energy,South China Agricultural University,Guangzhou 510642,Guangdong,China)
出处
《化工学报》
EI
CAS
CSCD
北大核心
2020年第12期5628-5635,共8页
CIESC Journal
基金
国家自然科学基金项目(21666004)
广西高校大学生创新创业训练计划项目(201910593044)。
关键词
Fe基蚕沙生物炭
吸附
脱附
苯乙醇
茴香醚
分子模拟
Fe-based silkworm excrement biocarbon
adsorption
desorption
pheneylethanol
anisole
molecular simulation
作者简介
通信作者:黄艳(1976-),女,博士,高级工程师,13352827425@189.cn;通信作者:赵钟兴(1979-),男,副教授,zhaozhongxing@gxu.edu.cn;第一作者:陈功(1996-),男,硕士研究生,844649803@qq.com。
