摘要
将催化反应引入光谱传感体系中可大大提高其灵敏度,因此,开展催化生荧/催化生色传感研究具有重要意义.将组成固定并具有孔隙结构的金属有机框架材料(MOFs)用于催化光谱传感研究,有助于理解催化剂与传感性能之间的关系.然而,目前涉及此方面研究的报道相当有限.本文采用水热合成法制备了一种比表面积和空隙率大、催化活性高的Fe-MOFs材料(Fe-MIL-101).以3,3′,5,5′-四甲基联苯胺(TMB)为底物分子,在H2O2的存在下,系统地研究了该Fe-MOFs材料催化TMB生色反应的实验条件以及其催化反应机理.在此基础上,借助谷胱甘肽(GSH)与其他巯基化合物在清除·OH自由基能力方面的显著性差异,建立了一种高效、高选择性、高灵敏度的GSH催化光谱传感体系.这种高选择性明显优于以往的GSH光谱传感与识别体系.
Since introducing catalytic reactions can greatly improve the sensitivity of spectral sensing systems,developing catalytic chromogenic/fluorescence sensing systems has important influence. By introducing metal-organic frameworks(MOFs) with fixed composition and good porous structure into traditional spectral sensing, it is helpful for understanding the relationship between catalyst and its sensing performance. However, very limited examples involved in this field at present. In this article, Fe-MOFs(Fe-MIL-101) with large surface area and high porosity were successfully synthesized by using a hydrothermal synthesis method. The Fe-MOF could exhibit outstanding catalytic activity towards the traditional enzyme substrate 3,3′,5,5′-tetramethylbenzidine(TMB). The experimental conditions and catalytic reactions mechanism of Fe-MOF catalyzing the oxidation reaction of the TMB-H_2O_2 system were systematically studied. On the basis of these findings, and taking together the fact that glutathione(GSH) serving as a better free radical scavenger than other traditional thiols, a highly efficient GSH sensing system with high selectivity and sensitivity could be successfully established.
引文
1 Okuhara T,Mizuno N,Misono M.Adv Catal,1996,41:113-252
2 Lloyd Spetz A,Tobias P,Unéus L,Svenningstorp H,Ekedahl LG,Lundstr?m I.Sens Actuat B-Chem,2000,70:67-76
3 Weckhuysen BM.Chem Commun,2002,0:97-110
4 Liang Y,Li Y,Wang H,Zhou J,Wang J,Regier T,Dai H.Nat Mater,2011,10:780-786
5 Wu Q,Anslyn EV.J Am Chem Soc,2004,126:14682-14683
6 Zaupa G,Mora C,Bonomi R,Prins LJ,Scrimin P.Chem Eur J,2011,17:4879-4889
7 Lin Y,Ren J,Qu X.Acc Chem Res,2014,47:1097-1105
8 Wei H,Wang E.Chem Soc Rev,2013,42:6060-6093
9 Wu J,Wang X,Wang Q,Lou Z,Li S,Zhu Y,Qin L,Wei H.Chem Soc Rev,2019,48:1004-1076
10 Wang W,Wu Y,Lin X,Chen W,Liu A,Peng H.Chin J Anal Chem,2018,46:1545-1551(in Chinese).[王文俊,吴燕虹,林秀玲,陈伟,刘爱林,彭花萍.分析化学,2018,46:1545-1551]
11 Xu Y,Wu XQ,Shen JS,Zhang HW.RSC Adv,2015,5:92114-92120
12 Xu Z,Baek KH,Kim HN,Cui J,Qian X,Spring DR,Shin I,Yoon J.J Am Chem Soc,2010,132:601-610
13 Zhang Y,Zhou X,Hu J,Chen S M,Ma Z,Chen X.Chin J Struct Chem,2013,32:1291-1296
14 Neves A,Lanznaster M,Bortoluzzi AJ,Peralta RA,Casellato A,Castellano EE,Herrald P,Riley MJ,Schenk G.J Am Chem Soc,2007,129:7486-7487
15 Fernández-Moreira V,Thorp-Greenwood FL,Coogan MP.Chem Commun,2010,46:186-202
16 Soroka K,Vithanage RS,Phillips DA,Walker B,Dasgupta PK.Anal Chem,1987,59:629-636
17 Jv Y,Li B,Cao R.Chem Commun,2010,46:8017-8019
18 Bonomi R,Cazzolaro A,Sansone A,Scrimin P,Prins LJ.Angew Chem Int Ed,2011,50:2307-2312
19 Jiang H,Chen Z,Cao H,Huang Y.Analyst,2012,137:5560-5564
20 Ma X,Sun M,Lin Y,Liu Y,Luo F,Guo L,Qiu B,Zhenyu L,Chen G.Chin J Anal Chem,2018,46:1-10
21 Gao L,Zhuang J,Nie L,Zhang J,Zhang Y,Gu N,Wang T,Feng J,Yang D,Perrett S,Yan X.Nat Nanotech,2007,2:577-583
22 Wei H,Wang E.Anal Chem,2008,80:2250-2254
23 Dai Z,Liu S,Bao J,Ju H.Chem Eur J,2009,15:4321-4326
24 Wu Z,Wu J,Sun X,Liu B,Shen J.Sci Sin-Chim,2017,47:1226-1232(in Chinese)[吴振龙,邬佳佳,孙向英,刘斌,沈江珊.中国科学:化学,2017,47:1226-1232]
25 Hu Y,Geng X,Zhang L,Huang Z,Ge J,Li Z.Sci Rep,2017,7:5849
26 Wang DM,Gao MX,Gao PF,Yang H,Huang CZ.J Phys Chem C,2013,117:19219-19225
27 Zhu S,Zhao XE,You J,Xu G,Wang H.Analyst,2015,140:6398-6403
28 Hu XB,Liu YL,Wang WJ,Zhang HW,Qin Y,Guo S,Zhang XW,Fu L,Huang WH.Anal Chem,2018,90:1136-1141
29 Lee JY,Farha OK,Roberts J,Scheidt KA,Nguyen SBT,Hupp JT.Chem Soc Rev,2009,38:1450-1459
30 Gole B,Bar AK,Mallick A,Banerjee R,Mukherjee PS.Chem Commun,2013,49:7439-7441
31 Huang K,Xu Y,Wang L,Wu D.RSC Adv,2015,5:32795-32803
32 Cheng H,Liu Y,Hu Y,Ding Y,Lin S,Cao W,Wang Q,Wu J,Muhammad F,Zhao X,Zhao D,Li Z,Xing H,Wei H.Anal Chem,2017,89:11552-11559
33 Imaz I,Rubio-Martínez M,García-Fernández L,García F,Ruiz-Molina D,Hernando J,Puntes V,Maspoch D.Chem Commun,2010,46:4737-4739
34 Du M,Li CP,Chen M,Ge ZW,Wang X,Wang L,Liu CS.J Am Chem Soc,2014,136:10906-10909
35 Sanz R,Martínez F,Orcajo G,Wojtas L,Briones D.Dalton Trans,2013,42:2392-2398
36 Shekhah O,Belmabkhout Y,Chen Z,Guillerm V,Cairns A,Adil K,Eddaoudi M.Nat Commun,2014,5:4228
37 Panella B,Hirscher M,Pütter H,Müller U.Adv Funct Mater,2006,16:520-524
38 Kreno LE,Leong K,Farha OK,Allendorf M,Van Duyne RP,Hupp JT.Chem Rev,2012,112:1105-1125
39 He L,Liu Y,Liu J,Xiong Y,Zheng J,Liu Y,Tang Z.Angew Chem Int Ed,2013,52:3741-3745
40 Wang Y,Zhu Y,Binyam A,Liu M,Wu Y,Li F.Biosens Bioelectron,2016,86:432-438
41 Cheng H,Zhang L,He J,Guo W,Zhou Z,Zhang X,Nie S,Wei H.Anal Chem,2016,88:5489-5497
42 Qin L,Wang X,Liu Y,Wei H.Anal Chem,2018,90:9983-9989
43 Liu F,Xu Y,Zhao L,Zhang L,Guo W,Wang R,Sun D.J Mater Chem A,2015,3:21545-21552
44 Lin XM,Niu JL,Wen PX,Pang Y,Hu L,Cai YP.Cryst Growth Des,2016,16:4705-4710
45 Lu J,Xiong Y,Liao C,Ye F.Anal Methods,2015,7:9894-9899
46 Wu XQ,Xu Y,Chen YL,Zhao H,Cui HJ,Shen JS,Zhang HW.RSC Adv,2014,4:64438-64442
47 Chen D,Li B,Jiang L,Duan D,Li Y,Wang J,He J,Zeng Y.RSC Adv,2015,5:97910-97917
48 Skobelev IY,Sorokin AB,Kovalenko KA,Fedin VP,Kholdeeva OA.J Catal,2013,298:61-69
49 Gao P,Sun XY,Liu B,Lian HT,Liu XQ,Shen JS.J Mater Chem C,2018,6:8105-8114
50 Murata A,Suenaga H,Hideshima S,Tanaka Y,Kato F.Agric Biol Chem,1986,50:1481-1487
51 Wang W,Schuchmann MN,Schuchmann HP,Knolle W,von Sonntag J,von Sonntag C.J Am Chem Soc,1999,121:238-245
52 Harbour JR,Issler SL.J Am Chem Soc,1982,104:903-905
53 Schaap AP,Thayer AL,Faler GR,Goda K,Kimura T.J Am Chem Soc,1974,96:4025-4026
54 Dennany L,Gerlach M,O’Carroll S,Keyes TE,Forster RJ,Bertoncello P.J Mater Chem,2011,21:13984-13990
55 Mohammadi S,Khayatian G.Spectrochim Acta Part A-Mol Biomol Spectr,2017,185:27-34
56 Liu X,Wang Q,Zhang Y,Zhang L,Su Y,Lv Y.New J Chem,2013,37:2174-2178
57 Huang H,Shi F,Li Y,Niu L,Gao Y,Shah SM,Su X.Sens Actuat B-Chem,2013,178:532-540
58 Hu Z,Jiang X,Xu F,Jia J,Long Z,Hou X.Talanta,2016,158:276-282
59 Wangpradit O,Rahaman A,Mariappan SVS,Buettner GR,Robertson LW,Luthe G.Environ Sci Pollut Res,2016,23:2138-2147
60 Feng J,Huang P,Shi S,Deng KY,Wu FY.Anal Chim Acta,2017,967:64-69
61 Di W,Zhang X,Qin W.Appl Surf Sci,2017,400:200-205
62 Ma Y,Zhang Z,Ren C,Liu G,Chen X.Analyst,2011,137:485-489
63 Zou H,Yang T,Lan J,Huang C.Anal Methods,2017,9:841-846
64 Cai QY,Li J,Ge J,Zhang L,Hu YL,Li ZH,Qu LB.Biosens Bioelectron,2015,72:31-36
65 Li W,Wang J,Zhu J,Zheng YQ.J Mater Chem B,2018,6:6858-6864
66 Zhang X,Mao X,Li S,Dong W,Huang Y.Sens Actuat B-Chem,2018,258:80-87
67 Wang Y,Liu Y,Ding F,Zhu X,Yang L,Zou P,Rao H,Zhao Q,Wang X.Anal Bioanal Chem,2018,410:4805-4813
68 Li S,Wang L,Zhang X,Chai H,Huang Y.Sens Actuat B-Chem,2018,264:312-319