基于纳米银负载氧化石墨烯的新型聚乙烯复合材料

doi:10.15541/jim20180372

无机材料学报 ›› 2019, Vol. 34 ›› Issue (6): 633-640.DOI: 10.15541/jim20180372

基于纳米银负载氧化石墨烯的新型聚乙烯复合材料

张峰^1,²,张凯立¹,周明明²,陈超³,蔡志威³,魏国辉⁴,姜兴茂^4,⁵,张诚¹,劳伦·鲁尔曼⁶,吕耀康¹()

^1. 浙江工业大学化学工程学院, 杭州 310014
^2. 浙江大学医学院附属儿童医院, 杭州 310052
^3. 浙江省食品药品检验研究院, 杭州 310052
^4. 常州英中纳米科技有限公司, 常州 213000
^5. 武汉工程大学化工与制药学院, 武汉 430205
^6. 斯特拉斯堡大学化学研究所, 斯特拉斯堡 67081

收稿日期:2018-08-09 修回日期:2018-09-04 出版日期:2019-06-20 网络出版日期:2019-05-23
作者简介:张峰(1980-), 男, 副主任医师. E-mail: zfwl@zju.edu.cn
基金资助:
国家自然科学基金(21501148);浙江省药品接触材料质量控制研究重点实验室开放基金;浙江省自然科学基金(LY19B01000)

A New Polyethylene Composite Material Based on Nano Silver Particels Loaded Graphene Oxide

Feng ZHANG^1,²,Kai-Li ZHANG¹,Ming-Ming ZHOU²,Chao CHEN³,Zhi-Wei CAI³,Guo-Hui WEI⁴,Xing-Mao JIANG^4,⁵,Cheng ZHANG¹,RUHLMANN Laurent⁶,Yao-Kang LÜ¹()

^1. School of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310014, China
^2. The Children's Hospital, Zhejiang University School of Medicine, Hangzhou 310052, China
^3. Zhejiang Institute for Food and Drug Control, Hangzhou, 310052, China
^4. Changzhou Yingzhong Nano Technology Co., Ltd, Changzhou 213000, China
^5. School of Chemical Engineering & Pharmacy, Wuhan Institute of Technology, Wuhan 430205, China;
^6. Institut de Chimie, Université de Strasbourg, Strasbourg 67081, France;

Received:2018-08-09 Revised:2018-09-04 Published:2019-06-20 Online:2019-05-23
Supported by:
National Natural Science Foundation of China(21501148);Open Funding from Zhejiang Provincial Key Laboratory for Quality Control of Drug Contact Materials;Zhejiang Provincial Natural Science Foundation(LY19B01000)

摘要/Abstract

摘要：

通过超声波辅助液相法将纳米银(AgNPs)与氧化石墨烯(GO)结合制得了一种新的负载纳米银的氧化石墨烯材料AgNPs@GO。分析表明在该材料中AgNPs主要被锚接在GO片层的含氧基团和缺陷上, 部分Ag单质被氧化为Ag ⁺离子并有部分GO被还原。AgNPs@GO能有效抑制铜绿假单胞菌生长, 其抑菌能力显著强于AgNPs和GO。将AgNPs@GO作为添加剂引入聚乙烯(PE)基体, 进一步制备了新型的AgNPs@GO掺杂PE复合材料0.48wt%-AgNPs@GO/PE, 相比PE和AgNPs掺杂PE复合材料, 0.48wt%-AgNPs@GO/PE具有更好的抑菌能力和更强的阻隔水蒸气性能, 并且在水和乙醇溶液中都具有较好的耐溶出性能。

关键词: 纳米银, 氧化石墨烯, 铜绿假单胞菌, 聚乙烯, 抑菌, 阻隔水蒸气性能

Abstract:

A new nano silver particels loaded graphene oxide (AgNPs@GO) was obtained through ultrasonic assisted liquid phase method. In AgNPs@GO, nano silver particels (AgNPs) are mainly anchored at oxygen containing groups and defects of graphene oxide (GO) sheets, part of GO sheets are reduced and some Ag(0) atoms have been oxidized to Ag ⁺ ions. AgNPs@GO exhibits significantly stronger ability for inhibiting Pseudomonas aeruginosa than that of AgNPs and GO. Therefore, AgNPs@GO was further introduced to polyethylene (PE) matrix as an additive to prepare a new composite material 0.48wt%-AgNPs@GO/PE. Compare with bare PE and AgNPs doped PE composites, 0.48wt%-AgNPs@GO/PE not only has a better antibacterial ability and stronger water vapor barrier property, but also dissolves out less nonvolatile substance than PE in water and ethanol solution.

Key words: nano silver particels, graphene oxide, pseudomonas aeruginosa, polyethylene, antibacterial ability, water vapor barrier property

中图分类号:

O614

张峰, 张凯立, 周明明, 陈超, 蔡志威, 魏国辉, 姜兴茂, 张诚, 劳伦·鲁尔曼, 吕耀康. 基于纳米银负载氧化石墨烯的新型聚乙烯复合材料[J]. 无机材料学报, 2019, 34(6): 633-640.

Feng ZHANG, Kai-Li ZHANG, Ming-Ming ZHOU, Chao CHEN, Zhi-Wei CAI, Guo-Hui WEI, Xing-Mao JIANG, Cheng ZHANG, RUHLMANN Laurent, Yao-Kang LÜ. A New Polyethylene Composite Material Based on Nano Silver Particels Loaded Graphene Oxide[J]. Journal of Inorganic Materials, 2019, 34(6): 633-640.

图/表 16

图1 AgNPs@GO的制备流程图

Fig. 1 Schematic illustration for the preparation of AgNPs@GO

图2 AgNPs@GO粉末(a)和其溶胶(b)的照片

Fig. 2 Photographs of AgNPs@GO powder (a) and its sol (b)

图S1 AgNPs、GO和AgNPs@GO水分散液的紫外-可见吸收光谱

Fig. S1 UV-Vis spectra of AgNPs、GO and AgNPs@GO aqueous dispersions

图S2 PE、0.48wt%-AgNPs/PE、2.88wt%-AgNPs/PE和0.48wt%-AgNPs@GO/PE的紫外-可见吸收光谱

Fig. S2 UV-Vis spectra of PE, 0.48wt%-AgNPs/PE, 2.88wt% -AgNPs/PE, and 0.48wt%-AgNPs@GO/PE

图3 AgNPs@GO的TEM(a,b)和HRTEM(c)照片以及AgNPs@GO上负载的AgNPs粒径分布的统计结果(d)

Fig. 3 TEM (a, b) and HRTEM (c) images of AgNPs@GO, and statistical result of the particle size distribution of AgNPs loaded on AgNPs@GO (d)

图4 GO和AgNPs@GO的XRD图谱(a); GO的XPS C1s图谱(b); AgNPS@GO的C1s(c)、O1s(d)、Ag3d(e)的XPS图谱和Ag(f)的AES 能谱

Fig. 4 XRD patterns of GO and AgNPs@GO(a); XPS C1s spectra of GO (b); XPS spectra C1s (c), O1s (d), Ag3d(e) of AgNPS@GO, and AES energy spectrum (f) of Ag

图S3 PE、0.48wt%-AgNPs/PE、2.88wt%-AgNPs/PE和0.48wt%-AgNPs@GO/PE的红外光谱

Fig. S3 IR spectra of PE, 0.48wt%-AgNPs/PE, 2.88wt%- AgNPs/PE, and 0.48wt%-AgNPs@GO/PE

图5 AgNPs@GO、GO和AgNPs的铜绿假单胞菌的抑菌圈实验照片(a)((1)涂有AgNPs@GO的纸片, (2)涂有GO的纸片, (3)涂有AgNPs的纸片)和抑菌圈实验数据结果图(b)

Fig. 5 Photograph of inhibition zone of Pseudomonas aeruginosa ((1) paper coated with AgNPs@GO, (2) paper coated with GO, (3) paper coated with AgNPs) (a) and results of experimental data of inhibition zone of AgNPs@GO, GO and AgNPs (b)

图6 不同时间取菌液接种于营养琼脂平板上进行的细菌培养照片(a)及其在不同时间的各试管中菌液的浊度(测量上限为4 MCF)(b) 和计数曲线(c)

Fig. 6 Photos (a) and turbidity (b) of the bacteria liquid in each test tube at different time (The upper limit of turbidity measurement is 4 MCF) and its counting curves of the bacterial culture on the nutrient agar plate at different time (c)

图7 抑制铜绿假单胞菌生长实验结果

Fig. 7 Inhibition of Pseudomonas aeruginosa growth test results Line 1: Blank control group; Line 2: 0.48wt%-AgNPs/PE; Line 3: 2.88wt%-AgNPs/PE; Line 4: 0.48wt%-AgNPs@GO/PE

图8 水蒸气透过率实验结果 A: PE; B: 0.48wt%-AgNPs/PE; C: 2.88wt%-AgNPs/PE; D: 0.48wt%- AgNPs@GO/PE

Fig. 8 The results of water vapor transmission rate experiments

图S4 PE薄片的水蒸气透过率数据图, 其水蒸气透过率为0.03885 g/(m2?d)

Fig. S4 Water vapor transmittance data of PE sheet is 0.03885 g/(m2?d)

图S5 0.48wt%-AgNPs/PE薄片的水蒸气透过率数据图, 其水蒸气透过率为0.07477 g/(m2?d)

Fig. S5 Water vapor transmittance data of 0.48wt%-AgNPs/PE sheet is 0.07477 g/(m2?d)

图S6 2.88wt%-AgNPs/PE薄片的水蒸气透过率数据图, 其水蒸气透过率为0.09484 g/(m2?d)

Fig. S6 Water vapor transmittance data of 2.88wt%-AgNPs/ PE sheet, 0.09484 g/(m2?d)

图S7 0.48wt%-AgNPs@GO/PE薄片的水蒸气透过率数据图, 其水蒸气透过率为0.02410 g/(m2?d)

Fig. S7 Water vapor transmittance data of 0.48wt%-AgNPs@GO/PE sheet, 0.02410 g/(m2?d)

图9 溶出物实验结果 A: PE; B: 0.48wt%-AgNPs/PE; C: 2.88wt%-AgNPs/PE; D: 0.48wt%- AgNPs@GO/PE

Fig. 9 The results of the dissolution tests

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基于纳米银负载氧化石墨烯的新型聚乙烯复合材料

A New Polyethylene Composite Material Based on Nano Silver Particels Loaded Graphene Oxide

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