光/磁热Fe2SiO4/Fe3O4双相生物陶瓷及其复合电纺丝膜制备及抗菌性能研究

doi:10.15541/jim20210659

无机材料学报 ›› 2022, Vol. 37 ›› Issue (9): 983-990.DOI: 10.15541/jim20210659

光/磁热Fe₂SiO₄/Fe₃O₄双相生物陶瓷及其复合电纺丝膜制备及抗菌性能研究

盛丽丽¹^,²(), 常江¹^,²()

1.中国科学院上海硅酸盐研究所高性能陶瓷与超微结构国家重点实验室, 上海 200050
2.中国科学院大学材料与光电研究中心, 北京 100049

收稿日期:2021-10-25 修回日期:2022-12-24 出版日期:2022-09-20 网络出版日期:2022-01-24
通讯作者: 常江, 研究员. E-mail: jchang@mail.sic.ac.cn
作者简介:盛丽丽(1992-), 女, 博士研究生. E-mail: lilissic@163.com
基金资助:
国家重点研发计划(2016YFC1100201);上海市科学技术委员会项目(19441902300)

Photo/Magnetic Thermal Fe₂SiO₄/Fe₃O₄ Biphasic Bioceramic and Its Composite Electrospun Membrane: Preparation and Antibacterial

SHENG Lili¹^,²(), CHANG Jiang¹^,²()

1. State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China
2. Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China

Received:2021-10-25 Revised:2022-12-24 Published:2022-09-20 Online:2022-01-24
Contact: CHANG Jiang, professor. E-mail: jchang@mail.sic.ac.cn
About author:SHENG Lili (1992-), female, PhD candidate. E-mail: lilissic@163.com
Supported by:
National Key Research and Development Program of China(2016YFC1100201);Funding of Science and Technology Commission of Shanghai Municipality(19441902300)

摘要/Abstract

摘要：

兼具抗菌和组织修复活性的生物材料在再生医学领域具有广阔的应用前景。以光热和磁热为基础的热疗技术都具有抗菌作用, 但光的穿透能力有限, 磁热试剂的热转换效率较低, 限制了其在生物医学领域的应用。本研究合成了Fe₂SiO₄/Fe₃O₄双相复合生物陶瓷粉体, 不仅同时具有良好的光热和磁热效应, 还能有效释放活性的铁和硅酸根离子。用陶瓷粉体与明胶/聚己内酯复合制备的电纺丝膜不仅具有良好的细胞相容性, 而且具有光热和磁热效应。复合膜在相对温和的条件下近红外光(808 nm, 0.36 W·cm^-2)与交变磁场(506 kHz, 837 A·m^-1)同时处理15 min后, 与单独近红外光或磁场热处理相比, 具有更强的细菌抑制活性。因此, 这种集光热、磁热功能于一体且具有细胞相容性的Fe-Si基生物陶瓷及其复合材料在再生医学领域具有潜在的应用前景。

关键词: Fe, 硅酸盐, 双相生物陶瓷, 静电纺丝, 抗菌性能

Abstract:

Biomaterials with both antibacterial and tissue repair activity have promising applications in the field of regenerative medicine. Both photothermal and magnetothermal-based techniques have antimicrobial effects, but the limited penetration capacity of light and the low thermal conversion efficiency of magnetothermal reagents limit their applications in biomedical fields. Here, we synthesized Fe₂SiO₄/Fe₃O₄ biphasic composite bioceramic powders, which not only display good photothermal and magnetothermal effects, but also effectively release active Fe and silicate ions, and prepared electrospun membranes by combining ceramic powders with gelatin/polycaprolactone, which not only exhibit good cytocompatibility, but also, importantly, possess both photothermal and magnetothermal properties. The composite membranes, under conditions of being irradiated with near-infrared light (808 nm, 0.36 W·cm^-2) and placed in alternating magnetic field (506 kHz, 837 A·m^-1) for 15 min simultaneously, are able to inhibit bacterial activity more effectively than the thermal treatment with near-infrared light or magnetic field alone. Therefore, this Fe-Si-based bioceramic and its composite material with photothermal, magnetothermal, antimicrobial, and biocompatible properties, have potential application in the field of regenerative medicine.

Key words: Fe, silicate, biphasic bioceramic, electrospun, antibacterial

中图分类号:

TQ174

盛丽丽, 常江. 光/磁热Fe₂SiO₄/Fe₃O₄双相生物陶瓷及其复合电纺丝膜制备及抗菌性能研究[J]. 无机材料学报, 2022, 37(9): 983-990.

SHENG Lili, CHANG Jiang. Photo/Magnetic Thermal Fe₂SiO₄/Fe₃O₄ Biphasic Bioceramic and Its Composite Electrospun Membrane: Preparation and Antibacterial[J]. Journal of Inorganic Materials, 2022, 37(9): 983-990.

图/表 11

图1 (a)空气气氛和(b)氩气气氛中凝胶粉体的TG-DTA曲线

Fig. 1 TG-DTA curves of gel powders tested in (a) air and (b) argon atmosphere

图2 800 ℃不同气氛条件下FF煅烧产物的XRD图谱

Fig. 2 XRD patterns of FF products calcined at 800 ℃ in different atmospheres FF-1: the product obtained by calcining without argon gas; FF-2-FF-4: the product obtained by calcining with argon gas at 10, 25 and >25 kPa in the furnace, respectively.

表1 不同条件下粉体产物在ECM中24 h的离子释放量

Table 1 Ion release of powders prepared under different conditions after 24 h being submersed in cell culture medium ECM

Powder	Fe ion/(μg·mL^-1)	Silicate ion/(μg·mL^-1)
FF-1	43.96	70.12
FF-2	28.37	40.23
FF-3	13.62	27.16
FF-4	5.76	12.68

图3 不同煅烧条件制备的粉体产物的磁热和光热性能

Fig. 3 Magnetothermal and photothermal properties of powder products after being calcined under different conditions (a) Magnetic analysis results; (b) Results of thermal performance of different powders under alternating magnetic field intensity of 506 kHz at 837 A·m-1; (c) Photothermal performance of different powders under 808 nm near-infrared light irradiation at a density of 0.36 W·cm-2. FF-1: the product obtained by calcining without argon gas; FF-2-FF-4: the product obtained by calcining with argon gas at 10, 25 and >25 kPa in the furnace, respectively. 1 emu=103 A·m-1, 1 Oe=1000/4π A/m Colorful figures are available on website

图4 FF-2粉体的粒度表征

Fig. 4 Particle size characterization of FF-2 powders

图5 FF-2粉体的SEM和TEM照片。

Fig. 5 SEM and TEM images of FF-2 powders (a, b) SEM images at low (a) and high (b) magnification; (c) TEM high-resolution image of the powder with inset showing electron diffraction pattern of the powder

图6 不同FF-2粉体含量的复合电纺丝膜的形貌

Fig. 6 Morphologies of composite electrospun membranes with different FF-2 powder compositing amounts (a) Optical photos; (b) SEM images. 0, 10, 20, 30, and 40 in the figures represent composite membranes with powder contents of 0, 10%, 20%, 30%, and 40%, respectively

表2 不同粉体含量的复合电纺丝膜的离子释放性能

Table 2 Ion release properties of composite electrospun films with different powder contents in cell culture medium ECM

Powder content/%	Fe ion/(μg·mL^-1)	Silicate ion/(μg·mL^-1)
0	0	0
10	0.05	0.27
20	0.13	1.45
30	0.32	2.76
40	0.61	5.98

图7 不同粉体含量的复合膜的光热和磁热性能

Fig. 7 Photothermal and magnetothermal properties of composite membranes with different powder contents (a) Under NIR light (0.36 W·cm-2) irradiation at a wavelength of 808 nm; (b) In an alternating magnetic field (506 kHz, 837A·m-1); (c) Composite film with 30% powder content under laser, alternating magnetic field and laser in combination with alternating magnetic field, respectively. 0, 10, 20, 30, and 40 in the figures represent composite membranes with powder contents of 0, 10%, 20%, 30%, and 40%, respectively. MTT: magnetothermal; PTT: photothermal; MTT+PTT: combined photothermal and magnetothermal

图8 FG-30复合电纺丝膜的细胞相容性

Fig. 8 Cytocompatibility of FG-30 composite electrospun membranes (a-f) SEM images of cell adhesion on FG-0 membrane (a-c) and FG-30 composite membrane (d-f) after 24 h of HUVEC culture, respectively; (g) Effect of composite membrane on HUVECs proliferation. Blank, FG-0, and FG-30 in the figures indicate blank control group, FG-0 electrospun membrane group, and FG-30 composite electrospun membrane group, respectively. * indicates p<0.05 which means significant difference between groups

图9 FG-30复合膜对金黄色葡萄球菌的光/磁热联合抑制作用

Fig. 9 Combined photo/magneto-thermal inhibition of S.aureus by FG-30 composite membrane (a) Optical photographs of colony coated plates; (b) Statistical results of inhibition rate. Blank, FG-0, FG-30, FG-30 (MTT), FG-30 (PTT), and FG-30 (MTT+PTT) denote blank control, FG-0 membrane, FG-30 membrane, FG-30 membrane with magnetothermal, FG-30 membrane with photothermal, FG-30 membrane with combined photothermal and magnetothermal, respectively. * indicates p<0.05 which means significant difference between groups

参考文献 26

[1]	BELKAID Y, TAMOUTOUNOUR S. The influence of skin microorganisms on cutaneous immunity. Nature Reviews Immunology, 2016, 16(6): 353-366. DOI URL
[2]	FALANGA V. Wound healing and its impairment in the diabetic foot. Lancet, 2005, 366(9498): 1736-1743. DOI URL
[3]	ROBSON M. Wound infection - a failure of wound healing caused by an imbalance of bacteria. Surgical Clinics of North America, 1997, 77(3): 637-650. DOI URL
[4]	LI P L, HAN F X, CAO W W, et al. Carbon quantum dots derived from lysine and arginine simultaneously scavenge bacteria and promote tissue repair. Applied Materials Today, 2020, 19(1): 100601. DOI URL
[5]	XIE X, WU J R, CAI X J, et al. Photothermal/pH response B-CuS-DOX nanodrugs for chemo-photothermal synergistic therapy of tumor. Journal of Inorganic Materials, 2020, 36(1): 81-87. DOI URL
[6]	ZENG Y L, CHEN J J, TIAN Z F, et al. Preparation of mesoporous organosilica-based nanosystem for in vitro synergistic chemo-and photothermal therapy. Journal of Inorganic Materials, 2020, 35(12): 1365-1372. DOI URL
[7]	ZHAO L Y, LIU Y M, XING R R, et al. Supramolecular photothermal effects: a promising mechanism for efficient thermal conversion. Angewandte Chemie International Edition, 2020, 59(10): 3793-3801. DOI URL
[8]	WU G Z, WU Z Y, LIU L, et al. NIR light responsive MoS₂ nanomaterials for rapid sterilization: optimum photothermal effect via sulfur vacancy modulation. Chemical Engineering Journal, 2022, 427(1): 132007. DOI URL
[9]	CHEN R, ROMERO G, CHRISTIANSEN M G, et al. Wireless magnetothermal deep brain stimulation. Science, 2015, 347(6229): 1477-1480. DOI URL
[10]	LI W, WEI W Y, WU X P, et al. The antibacterial and antibiofilm activities of mesoporous hollow Fe₃O₄ nanoparticles in an alternating magnetic field. Biomaterials Science, 2020, 8(16): 4492-4507. DOI URL
[11]	ZHUANG H, LIN R C, LIU Y Q, et al. 3D-printed bioceramic scaffolds with osteogenic activity for simultaneous photo-magnetothermal therapy of bone tumor. ACS Biomaterials Science and Engineering, 2019, 5(12): 6725-6734. DOI URL
[12]	FU D P, LIU J L, REN Q L, et al. Magnetic iron sulfide nanoparticles as thrombolytic agents for magnetocaloric therapy and photothermal therapy of thrombosis. Frontiers in Materials, 2019, 6(1): 316. DOI URL
[13]	LIU J C, GUO X, ZHAO Z, et al. Fe₃S₄ nanoparticles for arterial inflammation therapy: integration of magnetic hyperthermia and photothermal treatment. Applied Materials Today, 2020, 18(1): 100457. DOI URL
[14]	LI H Y, CHANG J. Stimulation of proangiogenesis by calcium silicate bioactive ceramic. Acta Biomaterialia, 2013, 9(2): 5379-5389. DOI URL
[15]	ZHAI W Y, LU H X, CHEN L, et al. Silicate bioceramics induce angiogenesis during bone regeneration. Acta Biomaterialia, 2012, 8(1): 341-349. DOI URL
[16]	YU Q Q, CHANG J, WU C. Silicate bioceramics: from soft tissue regeneration to tumor therapy. Journal of Material Chemistry B, 2019, 7(36): 5449-5460. DOI URL
[17]	MAO L X, XIA L G, CHANG J, et al. The synergistic effects of Sr and Si bioactive ions on osteogenesis, osteoclastogenesis and angiogenesis for osteoporotic bone regeneration. Acta Biomaterialia, 2017, 61(1): 217-232. DOI URL
[18]	GAO L, ZhOU Y L, PENG J L, et al. A novel dual-adhesive and bioactive hydrogel activated by bioglass for wound healing. NPG Asia Materials, 2019, 11: 66.
[19]	WEINTRAUB L R, GORAL A, GRASSO J, et al. Collagen biosynthesis in iron overload. Annals of the New York Academy of Sciences, 1988, 526(1): 179-184.
[20]	SHENG L, ZHANG Z, ZHANG Y, et al. A novel “hot spring”-mimetic hydrogel with excellent angiogenic properties for chronic wound healing. Biomaterials, 2020, 264(1): 120414. DOI URL
[21]	XING M, HUAN Z G, LI Q, et al. Containerless processing of Ca-Sr-Si system bioactive materials: thermophysical properties and ion release behaviors. Ceramics International, 2017, 43(6): 5156-5163. DOI URL
[22]	LI H Y, CHANG J. Bioactive silicate materials stimulate angiogenesis in fibroblast and endothelial cell co-culture system through paracrine effect. Acta Biomaterialia, 2013, 9(6): 6981-6991. DOI URL
[23]	XING M, WANG X Y, WANG E D, et al. Bone tissue engineering strategy based on the synergistic effects of silicon and strontium ions. Acta Biomaterialia, 2018, 72(1): 381-395. DOI URL
[24]	ZHANG J, SHI H S, LIU J Q, et al. Good hydration and cell-biological performances of superparamagnetic calcium phosphate cement with concentration-dependent osteogenesis and angiogenesis induced by ferric iron. Journal of Materials Chemistry B, 2015, 3(45): 8782-8795. DOI URL
[25]	WU M, DEOKAR A R, LIAO J, et al. Graphene-based photothermal agent for rapid and effective killing of bacteria. ACS Nano, 2013, 7(2): 1281-1290. DOI URL
[26]	IBELLI T, TEMPLETON S, LEVI-POLYACHENKO N. Progress on utilizing hyperthermia for mitigating bacterial infections. International Journal of Hyperthermia, 2018, 34(2): 144-156. DOI URL

光/磁热Fe₂SiO₄/Fe₃O₄双相生物陶瓷及其复合电纺丝膜制备及抗菌性能研究

Photo/Magnetic Thermal Fe₂SiO₄/Fe₃O₄ Biphasic Bioceramic and Its Composite Electrospun Membrane: Preparation and Antibacterial

RichHTML

PDF (PC)

可视化

摘要/Abstract

引用本文

使用本文

图/表 11

参考文献 26

相关文章 15

编辑推荐

Metrics

本文评价

[1]	吴锐, 张敏慧, 金成韵, 林健, 王德平. 光热核壳TiN@硼硅酸盐生物玻璃纳米颗粒的降解和矿化性能[J]. 无机材料学报, 2023, 38(6): 708-716.
[2]	王世怡, 冯爱虎, 李晓燕, 于云. Fe₃O₄负载Ti₃C₂T_x对Pb(II)的吸附性能研究[J]. 无机材料学报, 2023, 38(5): 521-528.
[3]	范栋, 钟鑫, 王亚文, 张振忠, 牛亚然, 李其连, 张乐, 郑学斌. 富铝CMAS对稀土硅酸盐环境障涂层的腐蚀行为与机制研究[J]. 无机材料学报, 2023, 38(5): 544-552.
[4]	罗淑文, 马名生, 刘峰, 刘志甫. Ca-B-Si体系LTCC材料腐蚀行为及腐蚀机理[J]. 无机材料学报, 2023, 38(5): 553-560.
[5]	王磊, 李建军, 宁军, 胡天玉, 王洪阳, 张占群, 武琳馨. CoFe₂O₄@Zeolite催化剂活化过一硫酸盐对甲基橙的强化降解: 性能与机理[J]. 无机材料学报, 2023, 38(4): 469-476.
[6]	钱新宇, 王无敌, 宋青松, 董永军, 薛艳艳, 张晨波, 王庆国, 徐晓东, 唐慧丽, 曹桂新, 徐军. 0.6%Pr, x%La:CaF₂的发光性能研究和Judd-Ofelt分析[J]. 无机材料学报, 2023, 38(3): 357-362.
[7]	王如意, 徐国良, 杨蕾, 邓崇海, 储德林, 张苗, 孙兆奇. p-n异质结BiVO₄/g-C₃N₄光阳极的制备及其光电化学水解性能[J]. 无机材料学报, 2023, 38(1): 87-96.
[8]	庞力斌, 王德平. 介孔硼硅酸盐玻璃微球药物载体的制备及其性能表征[J]. 无机材料学报, 2022, 37(7): 780-786.
[9]	陈士昆, 王楚楚, 陈晔, 李莉, 潘路, 文桂林. 磁性Ag₂S/Ag/CoFe_1.95Sm_0.05O₄ Z型异质结的制备及光催化降解性能[J]. 无机材料学报, 2022, 37(12): 1329-1336.
[10]	陈铖, 丁晶鑫, 王会, 王德平. 掺钕介孔硼硅酸盐生物活性玻璃陶瓷骨水泥的制备与性能表征[J]. 无机材料学报, 2022, 37(11): 1245-1258.
[11]	刘城, 赵倩, 牟志伟, 雷洁红, 段涛. 新型铋基SiOCNF复合膜对放射性气态碘的吸附性能[J]. 无机材料学报, 2022, 37(10): 1043-1050.
[12]	张晓山, 王兵, 吴楠, 韩成, 刘海燕, 王应德. 高红外遮蔽SiZrOC纳米纤维膜的制备及其性能研究[J]. 无机材料学报, 2022, 37(1): 93-100.
[13]	马玲玲, 常江. Nd掺杂硅酸钙及其复合电纺丝膜的制备及性能研究[J]. 无机材料学报, 2021, 36(9): 974-980.
[14]	王袁杰, 裴学良, 李好义, 徐鑫, 何流, 黄政仁, 黄庆. 自由基引发活性聚碳硅烷交联及其在制备SiC纤维中的应用[J]. 无机材料学报, 2021, 36(9): 967-973.
[15]	朱子旻, 张敏慧, 张轩宇, 姚爱华, 林健, 王德平. 硼硅酸盐生物活性玻璃在直流电场下的体外矿化性能[J]. 无机材料学报, 2021, 36(9): 1006-1012.