EDTA-壳聚糖对小鼠模型中Cd(Ⅱ)脱除作用
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摘要
镉污染通过食物链传递严重威胁人类健康,因而探索安全、有效脱除生物体内镉的方法具有重要意义。本文制备得到乙二胺四乙酸(EDTA)酰化改性的壳聚糖衍生物(ETC),并采用热分析技术表征了其稳定性。通过连续和不连续两种染毒方法,腹腔注射1 mg/kg CdCl_2,建立Cd~(2+)污染的小鼠模型。然后以ETC与EDTA和壳聚糖(CTS)等进行染毒小鼠脱镉,取小鼠眼球血、心、肝及肾脏器等,计算脏器系数及检测眼球中血、肝脏、肾脏、及心的镉含量。结果表明,不同染毒方式对小鼠体重及急性毒性作用存在显著差异。EDTA、ETC、CTS对血镉脱除率分别达58.94%、51.68%、37.43%;但ETC对小鼠各脏器镉的脱除率远高于其他脱镉剂,其中对心、肾镉脱除率分别高达63.90%、45.00%。相关研究结果为壳聚糖衍生物脱除重金属提供了一种参考方法。
Cadmium pollution through the food chain is a serious threat to human health, and it is thus of great significance to explore safe and effective ways to remove cadmium from organisms. In this paper, chitosan derivatives(ETC) were prepared via acylation with EDTA. The stability of ETC was characterized using TG-DSC technique. A mouse model of Cd contamination was established by intraperitoneal injection of 1 mg/kg Cd Cl2, according to two continuous and discontinuous exposure processes. The removal of cadmium in mice was determined when exposed to ETC, EDTA, and chitosan(CTS). The eyeballs were excised from living body. Heart, liver and kidney were excised by sacrificed mice. To track the cadmium in mice, the cadmium contents in blood, eyeball, liver, kidney, and heart were determined. The results showed that there were significant differences in the body weight and acute toxicity effects of different exposure methods on mice. The cadmium removal rates on the blood of EDTA, ETC, and CTS were 58.94%, 51.68%, and 37.43%, respectively. The removal rate of cadmium in mouse organs by ETC was much higher than that by other cadmium removal agents. The removal rates of cadmium in hearts and kidneys by ETC were 63.90% and 45.00%, respectively. The results provide a reference for the removal of heavy metals using chitosan derivatives.
Cadmium pollution through the food chain is a serious threat to human health, and it is thus of great significance to explore safe and effective ways to remove cadmium from organisms. In this paper, chitosan derivatives(ETC) were prepared via acylation with EDTA. The stability of ETC was characterized using TG-DSC technique. A mouse model of Cd contamination was established by intraperitoneal injection of 1 mg/kg Cd Cl2, according to two continuous and discontinuous exposure processes. The removal of cadmium in mice was determined when exposed to ETC, EDTA, and chitosan(CTS). The eyeballs were excised from living body. Heart, liver and kidney were excised by sacrificed mice. To track the cadmium in mice, the cadmium contents in blood, eyeball, liver, kidney, and heart were determined. The results showed that there were significant differences in the body weight and acute toxicity effects of different exposure methods on mice. The cadmium removal rates on the blood of EDTA, ETC, and CTS were 58.94%, 51.68%, and 37.43%, respectively. The removal rate of cadmium in mouse organs by ETC was much higher than that by other cadmium removal agents. The removal rates of cadmium in hearts and kidneys by ETC were 63.90% and 45.00%, respectively. The results provide a reference for the removal of heavy metals using chitosan derivatives.
引文
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[12]Repo E,Warchol J K,Kurniawan T A,et al.Adsorption of Co(II)and Ni(II)by EDTA-and/or DTPA-modified chitosan:Kinetic and equilibrium modeling[J].Chemical Engineering Journal,2010,161(1-2):73-82
[13]Repo E,Warchol J K,Bhatnagar A,et al.Heavy metals adsorption by novel EDTA-modified chitosan-silica hybrid materials[J].Journal of Colloid and Interface Science,2011,358(1):261-267
[14]Tian X,Yun S,Zhou S,et al.The weight of main organs and organ coefficient in db/db and+/db mice[J].Chinese Journal of Comparative Medicine,2006,4:220-222
[15]袁本利.药物安全评价中脏器系数的意义及不足[J].中国新药杂志,2003,12(11):960-963YUAN Ben-li.Significance and deficiency of organ coefficient in drug safety evaluation[J].Chinese Journal of New Drugs,2003,12(11):960-963
[16]El-Sharif A A,Hussain M H M.Chitosan-EDTA new combination is a promising candidate for treatment of bacterial and fungal infections[J].Current Microbiology,2011,62(3):739-745
[17]Loretz B,Bernkopschnürch A.In vitro evaluation of chitosan-EDTA conjugate polyplexes as a nanoparticulate gene delivery system[J].Aaps Journal,2006,8(4):756-764
[18]贾之慎,李奇彪.双突跃电位滴定法测定壳聚糖脱乙酰度[J].化学世界,2001,5:240-241JIA Zhi-Shen,LI Qi-biao.Determination of the degree of deacetylation of chitosan by double jump potential titration[J].Chemical World,2001,5:240-241
[19]郑丝柳,徐阳,周颖梅.羧甲基壳聚糖制备的反应条件对最优取代度的影响研究[J].化工技术与开发,2016,44(6):31-35ZHENG Si-liu,XU Yang,ZHOU Ying-mei.Effect of reaction conditions on the optimal degree of substitution for preparation of carboxymethyl chitosan[J].Chemical Technology&Development,2016,44(6):31-35
[20]Pawlak A,Mucha M.Thermogravimetric and FTIR studies of chitosan blends[J].Thermochimica Acta,2003,396(1-2):153-166
[21]吴永琴,关存杰,刘洪茂,等.镉诱导小鼠急性肝损伤模型的研究[J].安徽医科大学学报,2015,50(10):1443-1447WU Yong-qin,GUAN Cun-jie,LIU Hong-mao,et al.Study on the model of acute liver injury induced by cadmium in mice[J].Journal of Anhui Medical University,2015,50(10):1443-1447
[22]房传栋,张宾,徐君辉,等.紫贻贝金属硫蛋白对小鼠体内镉富集的拮抗及排出功效研究[J].食品安全质量检测学报,2017,8(7):2723-2728FANG Chuan-dong,ZHANG Bin,XU Jun-hui,et al.Antagonism and efficacy of metallothionein in mice in vivo[J].Journal of Food Safety&Quality,2017,8(7):2723-2728
[23]王志华,江阳阳,余晓华,等.壳聚糖及其水溶性衍生物对小鼠免疫功能的影响[J].食品科学,2016,37(1):198-202WANG Zhi-hua,JIANG Yang-yang,YU Xiao-hua,et al.Effects of chitosan and its water-soluble derivatives on immune function in mice[J].Food Science,2016,37(1):198-202
[24]Liu J,Liu Y,Habeebu S M,et al.Chronic combined exposure to cadmium and arsenic exacerbates nephrotoxicity,particularly in metallothionein-I/II null mice[J].Toxicology,2000,147(3):157-166
[25]王海健,万久琴,韩毓,等.锌对镉致小鼠肝肾睾丸病理损伤的保护作用[J].毒理学杂志,2009,23(4):296-299WANG Hai-jian,WAN Jiu-qin,HAN Yu,et al.Protective effects of zinc on pathological damage of liver and kidney testis in mice induced by cadmium[J].Toxicology,2009,23(4):296-299
[26]林霖,杨国栋,汪纪仓.虎杖苷对镉致小鼠睾丸氧化应激损伤的保护作用[J].食品科学,2015,36(23):275-278LIN Lin,YANG Guo-dong,WANG Ji-cang.Protective effect of polydatin on oxidative stress induced by cadmium in mice testis[J].Food Science,2015,36(23):275-278
[27]Caldas N M,Oliveira S R D,Neto J A G,et al.Direct and simultaneous determination of Cd,Cu,and Se in blood samples by graphite furnace atomic absorption spectrometry[J].Atomic Spectroscopy-Norwalk Connecticut,2009,30(4):115-119
[28]Anitha A,Rani V V D,Krishna R,et al.Synthesis,characterization,cytotoxicity and antibacterial studies of chitosan,-carboxymethyl and,-carboxymethyl chitosan nanoparticles[J].Carbohydrate Polymers,2009,78(4):672-677
[29]Bernkop-Schnürch A,Paikl C,Valenta C.Novel bioadhesive chitosan-EDTA conjugate protects leucine enkephalin from degradation by aminopeptidase N[J].Pharmaceutical Research,1997,14(7):917-922
[30]Tachi M,Katagiri Y.Determination of cadmium in organs by atomic absorption spectrophotometry[J].Igaku to Seibutsugaku Medicine and Biology,1970,81(3):131-137
[31]Iavicoli I,Carelli G,Castellino N,et al.The determination of low lead levels in the bone of lead-depleted mice by graphite furnace atomic absorption spectrometry[J].Fresenius Journal of Analytical Chemistry,2001,370(8):1100
[32]Sabaa M W,Mohamed N A,Mohamed R R,et al.Synthesis,characterization and antimicrobial activity of poly(-vinyl imidazole)grafted carboxymethyl chitosan[J].Carbohydrate Polymers,2010,79(4):998-1005
[33]Bernkop-Schnürch A,Paikl C,Valenta C.Novel bioadhesive chitosan-EDTA conjugate protects leucine enkephalin from degradation by aminopeptidase N[J].Pharmaceutical Research,1997,14(7):917-922
[34]田金花,杨华,迟光伟,等.壳聚糖和壳寡糖的磷酸化研究[J].化学研究与应用,2010,22(5):554-558TIAN Jin-hua,YANG Hua,CHI Guang-wei,et al.Phosphorylation of chitosan and chitooligosaccharides[J].Chemical Research and Application,2010,22(5):554-558
[35]朱圣陶,傅春玲,江伟威,等.某些营养素对短期染毒铅镉汞在小鼠体内分布的影响[J].工业卫生与职业病,2005,31(5):305-309ZHU Sheng-tao,FU Chun-ling,JIANG Wei-wei,et al.Effects of certain nutrients on short-term exposure to lead,cadmium,mercury in mice[J].Industrial Health and Occupational Diseases,2005,31(5):305-309
[36]李子琪,孟倩,孙凤清,等.壳聚糖及其衍生物脱除贝类中重金属的机理及应用研究进展[J].食品与机械,2016,2:188-192LI Zi-qi,MENG Qian,SUN Feng-qing,et al.Research progress on the mechanism and application of removal of heavy metals from shellfish by chitosan and its derivatives[J].Food and Machinery,2016,2:188-192
[2]张建辉,王芳斌,汪霞丽,等.湖南稻米镉和土壤镉锌的关系分析[J].食品科学,2015,36(22):156-160ZHANG Jian-hui,WANG Fang-bin,WANG Xia-li,et al.Analysis of Cadmium and cadmium in soil of Hunan[J].Food Science,2015,36(22):156-160
[3]毛伟杰,任惠峰,樊佳欢,等.日本扇贝加工废弃物中镉的脱除技术研究现状[J].安徽农业科学,2017,45(7):73-75MAO Wei-jie,REN Hui-feng,FAN Jia-huan,et al.Research status of cadmium removal technology in processing waste of scallops in Japan[J].Journal of Anhui Agricultural Sciences,2017,45(7):73-75
[4]吴佳林,鲍纬,程云雷,等.EDTA螯合树脂对镉离子的吸附性能探究[J].安徽化工,2017,43(4):28-30WU Jia-lin,BAO Wei,CHENG Yun-lei,et al.Study on adsorption performance of cadmium ion on EDTA chelating resin[J].Anhui Chemical Industry,2017,43(4):28-30
[5]李光先,钟志勇,陈嘉兴,等.乙二胺四乙酸驱镉对慢性镉、中毒大鼠、小鼠的肾毒性[J].实验动物与比较医学,2015,31(1):56-60LI Guang-xian,ZHONG Zhi-yong,CHEN Jia-xing,et al.Nephrotoxicity of ethylenediaminetetraacetic acid as a repellent to chronic cadmium poisoning in rats and mice[J].Laboratory Animal and Comparative Medicine,2015,31(1):56-60
[6]Shukla S K,Mishra A K,Arotiba O A,et al.Chitosan-based nanomaterials:a state-of-the-art review[J].International Journal of Biological Macromolecules,2013,59(4):46
[7]Juang R S,Wu F C,Tseng R L.Solute adsorption and enzyme immobilization on chitosan beads prepared from shrimp shell wastes[J].Bioresource Technology,2001,80(3):187-193
[8]Liu X L,Xie W C,Yang X H,et al.Optimization of adsorption technology of chitosan with Paralytic shellfish poisoning(PSP)by response surface methodology(RSM)[J].Advanced Materials Research,2011,236-238:2673-2678
[9]吕丹娜,许丽,刘正伟.壳聚糖的生物学作用及在体内代谢的研究进展[J].中国畜牧兽医,2006,33(8):15-18LV Dan-na,XU Li,LIU Zheng-wei.Biological effects of chitosan and its research progress in vivo metabolism[J].China Animal Husbandry and Veterinary Medicine,2006,33(8):15-18
[10]王林.EDTA-壳聚糖的制备及对Cd2+、Pb2+的吸附研究[D].湛江:广东海洋大学,2013WANG Lin.Preparation of EDTA-chitosan and its adsorption for Cd2+and Pb2+[D].Zhanjiang:Ocean University of Guangdong,2013
[11]Ren Y,Abbood H A,He F,et al.Magnetic EDTA-modified chitosan/Si O2/Fe3O4,adsorbent:Preparation,characterization,and application in heavy metal adsorption[J].Chemical Engineering Journal,2013,226(12):300-311
[12]Repo E,Warchol J K,Kurniawan T A,et al.Adsorption of Co(II)and Ni(II)by EDTA-and/or DTPA-modified chitosan:Kinetic and equilibrium modeling[J].Chemical Engineering Journal,2010,161(1-2):73-82
[13]Repo E,Warchol J K,Bhatnagar A,et al.Heavy metals adsorption by novel EDTA-modified chitosan-silica hybrid materials[J].Journal of Colloid and Interface Science,2011,358(1):261-267
[14]Tian X,Yun S,Zhou S,et al.The weight of main organs and organ coefficient in db/db and+/db mice[J].Chinese Journal of Comparative Medicine,2006,4:220-222
[15]袁本利.药物安全评价中脏器系数的意义及不足[J].中国新药杂志,2003,12(11):960-963YUAN Ben-li.Significance and deficiency of organ coefficient in drug safety evaluation[J].Chinese Journal of New Drugs,2003,12(11):960-963
[16]El-Sharif A A,Hussain M H M.Chitosan-EDTA new combination is a promising candidate for treatment of bacterial and fungal infections[J].Current Microbiology,2011,62(3):739-745
[17]Loretz B,Bernkopschnürch A.In vitro evaluation of chitosan-EDTA conjugate polyplexes as a nanoparticulate gene delivery system[J].Aaps Journal,2006,8(4):756-764
[18]贾之慎,李奇彪.双突跃电位滴定法测定壳聚糖脱乙酰度[J].化学世界,2001,5:240-241JIA Zhi-Shen,LI Qi-biao.Determination of the degree of deacetylation of chitosan by double jump potential titration[J].Chemical World,2001,5:240-241
[19]郑丝柳,徐阳,周颖梅.羧甲基壳聚糖制备的反应条件对最优取代度的影响研究[J].化工技术与开发,2016,44(6):31-35ZHENG Si-liu,XU Yang,ZHOU Ying-mei.Effect of reaction conditions on the optimal degree of substitution for preparation of carboxymethyl chitosan[J].Chemical Technology&Development,2016,44(6):31-35
[20]Pawlak A,Mucha M.Thermogravimetric and FTIR studies of chitosan blends[J].Thermochimica Acta,2003,396(1-2):153-166
[21]吴永琴,关存杰,刘洪茂,等.镉诱导小鼠急性肝损伤模型的研究[J].安徽医科大学学报,2015,50(10):1443-1447WU Yong-qin,GUAN Cun-jie,LIU Hong-mao,et al.Study on the model of acute liver injury induced by cadmium in mice[J].Journal of Anhui Medical University,2015,50(10):1443-1447
[22]房传栋,张宾,徐君辉,等.紫贻贝金属硫蛋白对小鼠体内镉富集的拮抗及排出功效研究[J].食品安全质量检测学报,2017,8(7):2723-2728FANG Chuan-dong,ZHANG Bin,XU Jun-hui,et al.Antagonism and efficacy of metallothionein in mice in vivo[J].Journal of Food Safety&Quality,2017,8(7):2723-2728
[23]王志华,江阳阳,余晓华,等.壳聚糖及其水溶性衍生物对小鼠免疫功能的影响[J].食品科学,2016,37(1):198-202WANG Zhi-hua,JIANG Yang-yang,YU Xiao-hua,et al.Effects of chitosan and its water-soluble derivatives on immune function in mice[J].Food Science,2016,37(1):198-202
[24]Liu J,Liu Y,Habeebu S M,et al.Chronic combined exposure to cadmium and arsenic exacerbates nephrotoxicity,particularly in metallothionein-I/II null mice[J].Toxicology,2000,147(3):157-166
[25]王海健,万久琴,韩毓,等.锌对镉致小鼠肝肾睾丸病理损伤的保护作用[J].毒理学杂志,2009,23(4):296-299WANG Hai-jian,WAN Jiu-qin,HAN Yu,et al.Protective effects of zinc on pathological damage of liver and kidney testis in mice induced by cadmium[J].Toxicology,2009,23(4):296-299
[26]林霖,杨国栋,汪纪仓.虎杖苷对镉致小鼠睾丸氧化应激损伤的保护作用[J].食品科学,2015,36(23):275-278LIN Lin,YANG Guo-dong,WANG Ji-cang.Protective effect of polydatin on oxidative stress induced by cadmium in mice testis[J].Food Science,2015,36(23):275-278
[27]Caldas N M,Oliveira S R D,Neto J A G,et al.Direct and simultaneous determination of Cd,Cu,and Se in blood samples by graphite furnace atomic absorption spectrometry[J].Atomic Spectroscopy-Norwalk Connecticut,2009,30(4):115-119
[28]Anitha A,Rani V V D,Krishna R,et al.Synthesis,characterization,cytotoxicity and antibacterial studies of chitosan,-carboxymethyl and,-carboxymethyl chitosan nanoparticles[J].Carbohydrate Polymers,2009,78(4):672-677
[29]Bernkop-Schnürch A,Paikl C,Valenta C.Novel bioadhesive chitosan-EDTA conjugate protects leucine enkephalin from degradation by aminopeptidase N[J].Pharmaceutical Research,1997,14(7):917-922
[30]Tachi M,Katagiri Y.Determination of cadmium in organs by atomic absorption spectrophotometry[J].Igaku to Seibutsugaku Medicine and Biology,1970,81(3):131-137
[31]Iavicoli I,Carelli G,Castellino N,et al.The determination of low lead levels in the bone of lead-depleted mice by graphite furnace atomic absorption spectrometry[J].Fresenius Journal of Analytical Chemistry,2001,370(8):1100
[32]Sabaa M W,Mohamed N A,Mohamed R R,et al.Synthesis,characterization and antimicrobial activity of poly(-vinyl imidazole)grafted carboxymethyl chitosan[J].Carbohydrate Polymers,2010,79(4):998-1005
[33]Bernkop-Schnürch A,Paikl C,Valenta C.Novel bioadhesive chitosan-EDTA conjugate protects leucine enkephalin from degradation by aminopeptidase N[J].Pharmaceutical Research,1997,14(7):917-922
[34]田金花,杨华,迟光伟,等.壳聚糖和壳寡糖的磷酸化研究[J].化学研究与应用,2010,22(5):554-558TIAN Jin-hua,YANG Hua,CHI Guang-wei,et al.Phosphorylation of chitosan and chitooligosaccharides[J].Chemical Research and Application,2010,22(5):554-558
[35]朱圣陶,傅春玲,江伟威,等.某些营养素对短期染毒铅镉汞在小鼠体内分布的影响[J].工业卫生与职业病,2005,31(5):305-309ZHU Sheng-tao,FU Chun-ling,JIANG Wei-wei,et al.Effects of certain nutrients on short-term exposure to lead,cadmium,mercury in mice[J].Industrial Health and Occupational Diseases,2005,31(5):305-309
[36]李子琪,孟倩,孙凤清,等.壳聚糖及其衍生物脱除贝类中重金属的机理及应用研究进展[J].食品与机械,2016,2:188-192LI Zi-qi,MENG Qian,SUN Feng-qing,et al.Research progress on the mechanism and application of removal of heavy metals from shellfish by chitosan and its derivatives[J].Food and Machinery,2016,2:188-192
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