摘要
采用甲基修饰的含氮辅助配体,与间苯二甲酸和六水硝酸锌在水热条件下合成一个水相稳定的金属有机框架物:{[Zn(BDC)(dmbpy)]·4H2O}n(1)(BDC=间苯二甲酸,dmbpy=3,3′-二甲基-4,4′-联吡啶),并对该化合物进行结构表征。X射线粉末衍射和差热分析结果显示该化合物表现出良好的热稳定性和水相稳定性。化合物1为二维结构,沿b轴方向存在0.92 nm×0.83nm和0.82 nm×0.39 nm的孔道。该化合物对5-氟尿嘧啶的包封率(质量分数)高达14.2%,并且在模拟体液中可缓慢释放70 h(37℃下,释放率在pH值为7.4和6.0时分别为94.5%和99%)。体内斑马鱼和体外MTT法结果显示该化合物浓度达到500μg·mL-1时生理依然安全。
By using a methyl-functionalized N-donor ligand, a water-stable zinc-based MOF {[Zn(BDC)(dmbpy)]·4H_2O}n(1)(BDC=isophthalate, dmbpy=3,3′-dimethyl-4,4′-bipyridine) was synthesized and structurally characterized. TGA and PXRD results show high thermal and water stability for 1. 1 exhibits a 2D(4,4) net with channels of 0.92 nm×0.83 nm and 0.82 nm×0.39 nm along the b axis, respectively. De-solvated 1 adsorbs around 14.2%(w/w) 5-fluorouracil(5-FU) and the cumulative release value of 5-FU after 70 h was about 94.5% and 99% in PBS(pH=7.4 and pH=6.0) at 37 ℃, respectively. The in vivo zebrafish toxicity tests and in vitro MTT assays of 1 at different concentrations results reveal that 1 is nontoxic(cell viability>80%) up to concentrations of 500 μg·mL-1.
引文
[1]Banerjee D,Elsaidi S K,Thallapally P K.J.Mater.Chem.A,2017,5:16611-16615
[2]Lee S J,Kim S,Kim E J,et al.Chem.Eng.J.,2018,335345-351
[3]Medishetty R,Zareba J K,Mayer D,et al.Chem.Soc.Rev.2017,46:4976-5004
[4](a)Chen L F,Xu Q.Science,2017,358:304-305(b)LIU Yuan-Yuan(刘媛媛)),LI Xin-Shu(李欣书),ZHANGHui-Min(张慧敏),et al.Chinese J.Inorg.Chem.(无机化学学报),2018,35(12):2280-2290
[5]Espallargas G M,Coronado E.Chem.Soc.Rev.,2018,47533-557
[6](a)Zheng K,Liu Z Q,Chen F,et al.Sens.Actuators B:Chem.2018,257:705-713(b)LU Yan-Lei(卢延磊),ZHU Ning(朱宁),ZHAO Yu-Meng(赵宇萌),et al.Chinese J.Inorg.Chem.(无机化学学报)2019,35(4):720-728
[7]Ma D Y,Xie J,Zhu Z,et al.Inorg.Chem.Commun.,201786:128-132
[8]Zhang X J,Wang W J,Hu Z J,et al.Coord.Chem.Rev.2015,284:206-235
[9]Yu Y J,Yu C,Niu Y Z,et al.Biosens.Bioelectron.,2018101:297-303
[10]Assen A H,Yassine O,Shekhah O.ACS Sens.,2017,21294-1301
[11]Ma D Y,Li Y W,Li Z.Chem.Commun.,2011,47:7377-7379
[12]Mitra S,Sasmal H S,Kundu T,et al.J.Am.Chem.Soc.2017,139:4513-4520
[13]Keskin S,Kizilel S.Ind.Eng.Chem.Res.,2011,4:1799-1812
[14]Horcajada P,Serre C,Vallet-Regi M,et al.Angew.Chem.Int.Ed.,2006,118:6120-6124
[15]APEXⅡSoftware,Vers.6.3.1,Bruker AXS Inc,Madison,Wisconsin,USA,2004.
[16]Sheldrick G M.Acta Crystallogr.Sect.A:Found.Crystallogr.2008,A64:112-122
[17]Spek A L.PLATON,A Multipurpose Crystallographic Tool Utrecht University,The Netherlands,2005.
[18]Wang J,Ma D Y,Liao W L,et al.CrystEngComm,2017,195244-5250
[19]Chalati T,Horcajada P,Couvreur P,et al.Nanomedicine2011,6:1683-1695
[20]Zhao X S,Wang S T,Wu Y,et al.Aquat.Toxicol.,2013136-137:49-59
[21]Chen T H,Lin C C,Meng P J.J.Hazard.Mater.,2014,277134-140
[22]Ma D Y,Lu K,Qin L,et al.Inorg.Chim.Acta,2013,39684-91
[23]Sun C Y,Qin C,Wang C G,et al.Adv.Mater.,2011,235629-5632
[24]Li Q L,Wang J P,Liu W C,et al.Inorg.Chem.Commun.2015,55:8-10
[25]Bag P P,Wang D,Chen Z,et al.Chem.Commun.,2016,523669-3672
[26]Liu J Q,Li X F,Gu C Y,et al.Dalton Trans.,2015,4419370-19382
[27]Liu J Q,Wu J,Jia Z B,et al.Dalton Trans.,2014,43:17265-17273