苯二胺改性氧化石墨烯膜制备及其渗透汽化性能
作者:陆莹莹,桑蕾,崔鹏
单位: 合肥工业大学 化学与化工学院,安徽省可控化学与材料化工重点实验室,合肥 230009
关键词: 苯二胺;氧化石墨烯;膜;渗透汽化
DOI号:
分类号: TQ028.8
出版年,卷(期):页码: 2020,40(2):39-44

摘要:
分别采用邻苯二胺(OPD)、间苯二胺(MPD)、对苯二胺(PPD)共价改性氧化石墨烯(GO)片层,采用真空抽滤法制备苯二胺改性GO膜,研究三种不同结构的苯二胺对GO膜结构和性能的影响。研究结果表明,不同结构苯二胺对GO的改性作用不同:OPD的反应活性低,对GO含氧官能团的消耗较少,可有效拓展GO膜的层间距;MPD消耗GO的含氧官能团多于OPD,也对GO膜层间距有较好的增大;PPD消耗更多的GO含氧官能团,其对位氨基的高反应活性导致GO片层产生堆积作用,对膜层间距无明显影响。OPD、MPD和PPD改性GO膜对90 wt%乙醇/水体系的渗透通量分别为0.55 kg/(m2?h)、0.56 kg/(m2?h)和0.42 kg/(m2?h),分离因子分别为90.58、30.78和34.49,证明苯二胺对GO有一定的改性作用。
O-phenylenediamine (OPD), m-phenylenediamine (MPD) and p-phenylenediamine (PPD) were selected for covalently modifying graphene oxide (GO) sheets to prepare phenylenediamines modified GO membranes by vacuum filtration, and the effects of three phenylenediamines on the structure and properties of GO membrane were studied. The results show that phenylenediamines of different structures have different modification effects on GO: OPD has low reactivity and consumes less oxygen-containing functional groups of GO, which can effectively extend the interlayer distance (d-spacing) of GO membrane; MPD consumes more oxygen-containing functional groups of GO than OPD, and also increases the d-spacing of GO membrane; PPD consumes most of GO oxygen-containing functional groups due to high reactivity of the para-amino group, resulting in the accumulation of the GO sheets, and there is no significant change in the d-spacing of GO membrane. Pervaporation separation performance of three modified membranes for 90 wt% ethanol/water system shows that the permeation flux of OPD, MPD and PPD modified GO membranes are 0.55 kg/(m2?h), 0.56 kg/(m2?h) and 0.42 kg/(m2?h), the separation factor are 90.58, 30.78 and 34.49, respectively. It is proved that phenylenediamines have certain modification effects on GO.

基金项目:
国家自然科学基金项目(21476055)

作者简介:
第一作者简介:陆莹莹(1995-),女,安徽省铜陵市人,在读硕士研究生,主要研究方向为膜分离过程与装备,E-mail:2018110454@mail.hfut.edu.cn 通讯作者,E-mail:cuipeng@hfut.edu.cn

参考文献:
[1] Liu G, Jin W. Graphene oxide membrane for molecular separation: challenges and opportunities[J]. Science China Materials, 2018, 61(8):1021-1026.
[2] Nair R R, Wu H A, Jayaram P N, et al. Unimpeded permeation of water through helium-leak-tight graphene-based membranes[J]. Science, 2012, 335(6067):442-444.
[3] Thebo K H, Qian X, Zhang Q, et al. Highly stable graphene-oxide-based membranes with superior permeability[J]. Nat Commun, 2018, 9(1):1486.
[4] Hung W S, Tsou C H, De Guzman M, et al. Cross-linking with diamine monomers to prepare composite graphene oxide-framework membranes with varying d-spacing[J]. Chem Mater, 2014, 26(9):2983-2990.
[5] Hua D, Rai R K, Zhang Y, et al. Aldehyde functionalized graphene oxide frameworks as robust membrane materials for pervaporative alcohol dehydration[J]. Chem Eng Sci, 2017, 161:341-349.
[6] Huang K, Liu G, Lou Y, et al. A graphene oxide membrane with highly selective molecular separation of aqueous organic solution[J]. Angew Chem Int Ed Engl, 2014, 53(27):6929-6932.
[7] Chen X, Liu G, Zhang H, et al. Fabrication of graphene oxide composite membranes and their application for pervaporation dehydration of butanol[J]. Chin J Chem Eng, 2015, 23(7):1102-1109.
[8] Lou Y, Liu G, Liu S, et al. A facile way to prepare ceramic-supported graphene oxide composite membrane via silane-graft modification[J]. Appl Surf Sci, 2014, 307:631-637.
[9] Hu M, Mi B. Enabling graphene oxide nanosheets as water separation membranes[J]. Environ Sci Technol, 2013, 47(8):3715-3723.
[10] Qian X, Li N, Wang Q, et al. Chitosan/graphene oxide mixed matrix membrane with enhanced water permeability for high-salinity water desalination by pervaporation[J]. Desalination, 2018, 438:83-96.
[11] Shen H, Wang N, Ma K, et al. Tuning inter-layer spacing of graphene oxide laminates with solvent green to enhance its nanofiltration performance[J]. J Membr Sci, 2017, 527:43-50.
[12] Lecaros R L G, Mendoza G E J, Hung W S, et al. Tunable interlayer spacing of composite graphene oxide-framework membrane for acetic acid dehydration[J]. Carbon, 2017, 123:660-667.
[13] Roy C D, Singh C, Paul A. Role of graphite precursor and sodium nitrate in graphite oxide synthesis[J]. RSC Advances, 2014, 4(29):15138.
[14] Shanmugharaj A M, Yoon J H, Yang W J, et al. Synthesis, characterization, and surface wettability properties of amine functionalized graphene oxide films with varying amine chain lengths[J]. J Colloid Interface Sci, 2013, 401:148-154.
[15] Jia Z, Wang Y. Covalently crosslinked graphene oxide membranes by esterification reactions for ions separation[J]. J Mater Chem A, 2015, 3(8):4405-4412.
[16] Zhang Y, Zhang S, Chung T S. Nanometric graphene oxide framework membranes with enhanced heavy metal removal via nanofiltration[J]. Environ Sci Technol, 2015, 49(16):10235-10242.
[17] Kumar A, Khandelwal M. Amino acid mediated functionalization and reduction of graphene oxide-synthesis and the formation mechanism of nitrogen-doped graphene[J]. New J Chem., 2014, 38(8):3457-3467.
[18] 赵小龙, 孙红娟, 彭同江. 对苯二胺功能化还原氧化石墨烯的结构和官能团变化[J]. 高等学校化学学报, 2016, 37(4): 728-735.

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