Please wait a minute...
Frontiers of Materials Science

ISSN 2095-025X

ISSN 2095-0268(Online)

CN 11-5985/TB

Postal Subscription Code 80-974

2018 Impact Factor: 1.701

Front. Mater. Sci.    2019, Vol. 13 Issue (4) : 399-409    https://doi.org/10.1007/s11706-019-0484-x
RESEARCH ARTICLE
Upconversion luminescence Ca--Mg--Si bioactive glasses synthesized using the containerless processing technique
Qin LI1, Min XING1, Lan CHANG1,2, Linlin MA1, Zhi CHEN3, Jianrong QIU3, Jianding YU1(), Jiang CHANG1()
1. State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China
2. School of Pharmacy, Fudan University, Shanghai 201203, China
3. State Key Laboratory of Luminescent Materials and Devices, South China University of Technology, Guangzhou 510640, China
 Download: PDF(2908 KB)   HTML
 Export: BibTeX | EndNote | Reference Manager | ProCite | RefWorks
Abstract

In this study, a series of Er3+/Yb3+ co-doped Ca--Mg--Si glasses were prepared via the containerless processing. Phase composition and luminescent properties of the prepared materials were investigated through XRD and spectrometry, and bioactivity, biocompatibility and cytotoxicity were evaluated. The XRD patterns indicated that akermanite (AKT) ceramic powders were completely transformed into the glassy phase (AKT-G, EYA) through the containerless processing, which exhibit upconversion luminescence, and the luminescence intensity increased with the increase of the doping amount of Er3+ and Yb3+. High amount of Yb3+ doping and existence of Ca2+ in glasses resulted in more intensive red-light emission. The SEM observation, combined with EDS analysis, and cell culture experiments showed that the as-prepared glasses were nontoxic, biocompatible and bioactive. All these results demonstrated that the contai-nerless processing is a facile method for preparing homogeneous luminescent bioactive glasses. Furthermore, this luminescent Ca--Mg--Si glasses may be used as bone implant materials to study the in vivo distribution of degradation products of bone implants, which may be of great significance for the development and clinical application of new bone grafting materials.

Keywords containerless processing      akermanite      Er3+/Yb3+ codoped Ca--Mg--Si glass      upconversion luminiscence      bioactivity     
Corresponding Author(s): Jianding YU,Jiang CHANG   
Online First Date: 27 November 2019    Issue Date: 04 December 2019
 Cite this article:   
Qin LI,Min XING,Lan CHANG, et al. Upconversion luminescence Ca--Mg--Si bioactive glasses synthesized using the containerless processing technique[J]. Front. Mater. Sci., 2019, 13(4): 399-409.
 URL:  
https://academic.hep.com.cn/foms/EN/10.1007/s11706-019-0484-x
https://academic.hep.com.cn/foms/EN/Y2019/V13/I4/399
Sample c(Er2O3)/mol.% c(Yb2O3)/mol.% c(AKT)/mol.%
AKT-G 0 0 100
EYA-1 0.79 6.36 92.85
EYA-2 1.62 13.14 85.24
EYA-3 2.54 20.38 77.09
EYA-4 3.52 28.12 68.36
Tab.1  Nominal compositions of Er3+/Yb3+ co-doped Ca–Mg–Si glasses (after conversion to molar ratio)
Fig.1  Ca–Mg–Si glasses prepared by the containerless processing: (a) AKT-G; (b) EYA-1; (c) EYA-2; (d) EYA-3; (e) EYA-4.
Fig.2  XRD patterns of as-prepared samples AKT-G, EYA-1, EYA-2, EYA-3 and EYA-4. The inset illustrates the XRD pattern of AKT-P raw material.
Fig.3  Luminescence photos of as-prepared glasses excited by 980 nm laser: (a) EYA-1; (b) EYA-2; (c) EYA-3; (d) EYA-4.
Fig.4  Upconversion luminescence spectra of Er3+/Yb3+ co-doped bioactive glasses: EYA-1, EYA-2, EYA-3 and EYA-4.
Fig.5  Relationship between the upconversion luminescence and the Er3+/Yb3+ doping concentration under the same power 0.95 A.
Fig.6  Morphologies of as-prepared (a) EYA-2 before soaking in SBF, and (b) EYA-1, (c) EYA-2, (d) EYA-3 and (e) EYA-4 after soaking in SBF for 14 d.
Fig.7  EDS results of as-prepared (a) EYA-2 before soaking in SBF, and (b) EYA-1, (c) EYA-2, (d) EYA-3 and (e) EYA-4 after soaking in SBF for 14 d.
Fig.8  (a) The proliferation of HUVECs in the ionic extracts of glasses after culturing for 5 d. The cells cultured in medium without ionic extracts of glasses were treated as the control group. (b) The proliferation of HDFs in the ionic extracts of glasses after culturing for 7 d. The cells cultured in medium without ionic extracts of glasses were treated as the control group. (*p<0.05)
Fig.9  Expression of angiogenesis related genes including (a) VEGF and (b) KDR in HUVECs cultured with ionic extracts of glasses after 3 d. Expression of angiogenesis related genes including (c) VEGF and (d) bFGF in HDFs cultured with ionic extracts of glasses after 3 d. The cells cultured in medium without ionic extracts of glasses were treated as the control group. (*p<0.05)
Fig.10  (a) The cell migration of HDFs in ionic extracts of glasses after scratching (0 h) and migration for 26 h. (b) The migration ratios of HDFs cultured with ionic extracts of glasses. The cells cultured in medium without ionic extracts of glasses were treated as the control group. (*p<0.05)
Fig.11  (a) The cell migration of HUVECs in ionic extracts of glasses after scratching (0 h) and migration for 26 h. (b) The migration ratios of HUVECs cultured with ionic extracts of glasses. The cells cultured in medium without ionic extracts of glasses were treated as the control group. (*p<0.05)
1 C Wu, J Chang. Degradation, bioactivity, and cytocompatibility of diopside, akermanite, and bredigite ceramics. Journal of Biomedical Materials Research Part B: Applied Biomaterials, 2007, 83B(1): 153–160
https://doi.org/10.1002/jbm.b.30779 pmid: 17318828
2 N Y Iwata, G H Lee, Y Tokuoka, et al.. Sintering behavior and apatite formation of diopside prepared by coprecipitation process. Colloids and Surfaces B: Biointerfaces, 2004, 34(4): 239–245
https://doi.org/10.1016/j.colsurfb.2004.01.007 pmid: 15261063
3 J Ou, Y Kang, Z Huang, et al.. Preparation and in vitro bioactivity of novel merwinite ceramic. Biomedical Materials, 2008, 3(1): 015015
https://doi.org/10.1088/1748-6041/3/1/015015 pmid: 18458502
4 L Radev, H Vladimir, I Michailova, et al.. Sol-gel bioactive glass-ceramics Part II: Glass-ceramics in the CaO–SiO2–P2O5–MgO system. Central European Journal of Chemistry, 2009, 7(3): 322–327
https://doi.org/10.2478/s11532-009-0014-2
5 P Siriphannon, Y Kameshima, A Yasumori, et al.. Formation of hydroxyapatite on CaSiO3 powders in simulated body fluid. Journal of the European Ceramic Society, 2002, 22(4): 511–520
https://doi.org/10.1016/S0955-2219(01)00301-6
6 C Wu, Y Ramaswamy, D Kwik, et al.. The effect of strontium incorporation into CaSiO3 ceramics on their physical and biological properties. Biomaterials, 2007, 28(21): 3171–3181
https://doi.org/10.1016/j.biomaterials.2007.04.002 pmid: 17445881
7 W Renooij, H A Hoogendoorn, W J Visser, et al.. Bioresorption of ceramic strontium-85-labeled calcium phosphate implants in dog femora. A pilot study to quantitate bioresorption of ceramic implants of hydroxyapatite and tricalcium orthophosphate in vivo. Clinical Orthopaedics and Related Research, 1985, (197): 272–285
https://doi.org/10.1097/00003086-198507000-00034 pmid: 4017341
8 T Matsuoka, J Hildreth, D H Wisner. Liver injury as a model of uncontrolled hemorrhagic shock: resuscitation with different hypertonic regimens. The Journal of Trauma, 1995, 39(4): 674–680
https://doi.org/10.1097/00005373-199510000-00010 pmid: 7473953
9 J Kónya, N M Nagy. Chapter 8: Radioactive tracer methods. In: Nuclear and Radiochemistry (Second Edition), 2018, 187–245
10 F Wang, R Deng, J Wang, et al.. Tuning upconversion through energy migration in core–shell nanoparticles. Nature Materials, 2011, 10(12): 968–973
https://doi.org/10.1038/nmat3149 pmid: 22019945
11 G Chen, T Y Ohulchanskyy, R Kumar, et al.. Ultrasmall monodisperse NaYF4:Yb3+/Tm3+ nanocrystals with enhanced near-infrared to near-infrared upconversion photoluminescence. ACS Nano, 2010, 4(6): 3163–3168
https://doi.org/10.1021/nn100457j pmid: 20509664
12 M Haase, H Schäfer. Upconverting nanoparticles. Angewandte Chemie International Edition, 2011, 50(26): 5808–5829
https://doi.org/10.1002/anie.201005159 pmid: 21626614
13 X J Kang, Z Y Cheng, C X Li, et al.. Core–shell structured up-conversion luminescent and mesoporous NaYF4:Yb3+/Er3+@nSiO2@mSiO2 nanospheres as carriers for drug delivery. The Journal of Physical Chemistry C, 2011, 115(32): 15801–15811
https://doi.org/10.1021/jp203039t
14 J Shen, L Zhao, G Han. Lanthanide-doped upconverting luminescent nanoparticle platforms for optical imaging-guided drug delivery and therapy. Advanced Drug Delivery Reviews, 2013, 65(5): 744–755
https://doi.org/10.1016/j.addr.2012.05.007 pmid: 22626980
15 C Wang, L Cheng, Z Liu. Drug delivery with upconversion nanoparticles for multi-functional targeted cancer cell imaging and therapy. Biomaterials, 2011, 32(4): 1110–1120
https://doi.org/10.1016/j.biomaterials.2010.09.069 pmid: 20965564
16 Q Li, M Xing, Z Chen, et al.. Er3+/Yb3+ co-doped bioactive glasses with up-conversion luminescence prepared by contai-nerless processing. Ceramics International, 2016, 42(11): 13168–13175
https://doi.org/10.1016/j.ceramint.2016.05.108
17 N Sezer, Z Evis, S M Kayhan, et al.. Review of magnesium-based biomaterials and their applications. Journal of Magnesium and Alloys, 2018, 6(1): 23–43
https://doi.org/10.1016/j.jma.2018.02.003
18 N-E L Saris, E Mervaala, H Karppanen, et al.. Magnesium. An update on physiological, clinical and analytical aspects. Clinica Chimica Acta, 2000, 294(1–2): 1–26
https://doi.org/10.1016/S0009-8981(99)00258-2 pmid: 10727669
19 L Xia, Z Zhang, L Chen, et al.. Proliferation and osteogenic differentiation of human periodontal ligament cells on akermanite and β-TCP bioceramics. European Cells & Materials, 2011, 22: 68–83
https://doi.org/10.22203/eCM.v022a06 pmid: 21761393
20 H Sun, C Wu, K Dai, et al.. Proliferation and osteoblastic differentiation of human bone marrow-derived stromal cells on akermanite-bioactive ceramics. Biomaterials, 2006, 27(33): 5651–5657
https://doi.org/10.1016/j.biomaterials.2006.07.027 pmid: 16904740
21 Q Liu, L Cen, S Yin, et al.. A comparative study of proliferation and osteogenic differentiation of adipose-derived stem cells on akermanite and β-TCP ceramics. Biomaterials, 2008, 29(36): 4792–4799
https://doi.org/10.1016/j.biomaterials.2008.08.039 pmid: 18823660
22 C Wu, J Chang. A novel akermanite bioceramic: preparation and characteristics. Journal of Biomaterials Applications, 2006, 21(2): 119–129
https://doi.org/10.1177/0885328206057953 pmid: 16443628
23 C Wu, J Chang, S Ni, et al.. In vitro bioactivity of akermanite ceramics. Journal of Biomedical Materials Research Part A, 2006, 76A(1): 73–80
https://doi.org/10.1002/jbm.a.30496 pmid: 16224776
24 Y Huang, X Jin, X Zhang, et al.. In vitro and in vivo evaluation of akermanite bioceramics for bone regeneration. Biomaterials, 2009, 30(28): 5041–5048
https://doi.org/10.1016/j.biomaterials.2009.05.077 pmid: 19545889
25 M Montazerian, B E Yekta, V K Marghussian, et al.. Bioactivity and cell proliferation in radiopaque gel-derived CaO–P2O5–SiO2–ZrO2 glass and glass-ceramic powders. Materials Science and Engineering C, 2015, 55: 436–447
https://doi.org/10.1016/j.msec.2015.05.065 pmid: 26117775
26 T Kokubo, H Takadama. How useful is SBF in predicting in vivo bone bioactivity? Biomaterials, 2006, 27(15): 2907–2915
https://doi.org/10.1016/j.biomaterials.2006.01.017 pmid: 16448693
27 Y Josset, F Nasrallah, E Jallot, et al.. Influence of physicochemical reactions of bioactive glass on the behavior and activity of human osteoblasts in vitro. Journal of Biomedical Materials Research Part A, 2003, 67A(4): 1205–1218
https://doi.org/10.1002/jbm.a.20035 pmid: 14624507
28 M Xing, X Wang, E Wang, et al.. Bone tissue engineering strategy based on the synergistic effects of silicon and strontium ions. Acta Biomaterialia, 2018, 72: 381–395
https://doi.org/10.1016/j.actbio.2018.03.051 pmid: 29627679
29 L Yang, Y Zhang, L Hu, et al.. Synthesis, characterization and cell imaging properties of rare earth compounds based on hydroxamate ligand. Journal of Rare Earths, 2018, 36(4): 418–423
https://doi.org/10.1016/j.jre.2017.11.004
30 M J Zhu, J D Yu, M H Zhang, et al.. Upconversion luminescence of Er3+/Yb3+ Co-doped La2O3–TiO2–ZrO2 glasses prepared by containerless processing. Journal of Inorganic Materials, 2015, 30(4): 391–396
31 J Yu, Y Arai, T Masaki, et al.. Fabrication of BaTi2O5 glass-ceramics with unusual dielectric properties during crystallization. Chemistry of Materials, 2006, 18(8): 2169–2173
https://doi.org/10.1021/cm0525555
32 J Yu, P F Paradis, T Ishikawa, et al.. Giant dielectric constant of hexagonal BaTiO3 crystal grown by containerless processing. Chemistry of Materials, 2004, 16(21): 3973–3975
https://doi.org/10.1021/cm0487526
33 M Zhang, J Yu, X Pan, et al.. Bifunction in Er3+/Yb3+ co-doped BaTi2O5–Gd2O3 glasses prepared by aerodynamic levitation method. Materials Research Bulletin, 2013, 48(11): 4729–4732
https://doi.org/10.1016/j.materresbull.2013.08.009
34 H W Song, B J Sun, T Wang, et al.. Three-photon upconversion luminescence phenomenon for the green levels in Er3+/Yb3+ co-doped cubic nanocrystalline yttria. Solid State Communications, 2004, 132(6): 409–413
https://doi.org/10.1016/j.ssc.2004.07.044
35 D Matsuura. Red, green, and blue upconversion luminescence of trivalent-rare-earth ion-doped Y2O3 nanocrystals. Applied Physics Letters, 2002, 81(24): 4526–4528
https://doi.org/10.1063/1.1527976
36 D Solis, E De la Rosa, O Meza, et al.. Role of Yb3+ and Er3+ concentration on the tunability of green–yellow–red upconversion emission of co-doped ZrO2:Yb3+–Er3+ nanocrystals. Journal of Applied Physics, 2010, 108(2): 023103
https://doi.org/10.1063/1.3465325
37 Y Q Li, G De With, H T Hintzen. The effect of replacement of Sr by Ca on the structural and luminescence properties of the red-emitting Sr2Si5N8:Eu2+ LED conversion phosphor. Journal of Solid State Chemistry, 2008, 181(3): 515–524
https://doi.org/10.1016/j.jssc.2007.11.037
38 A L Antaris, H Chen, K Cheng, et al.. A small-molecule dye for NIR-II imaging. Nature Materials, 2016, 15(2): 235–242
https://doi.org/10.1038/nmat4476 pmid: 26595119
39 J Green. Cytosolic pH regulation in osteoblasts. Mineral and Electrolyte Metabolism, 1994, 20(1–2): 16–30
pmid: 8202049
40 A El-Ghannam, P Ducheyne, I M Shapiro. Bioactive material template for in vitro synthesis of bone. Journal of Biomedical Materials Research, 1995, 29(3): 359–370
https://doi.org/10.1002/jbm.820290311 pmid: 7615587
41 S Maeno, Y Niki, H Matsumoto, et al.. The effect of calcium ion concentration on osteoblast viability, proliferation and differentiation in monolayer and 3D culture. Biomaterials, 2005, 26(23): 4847–4855
https://doi.org/10.1016/j.biomaterials.2005.01.006 pmid: 15763264
42 E Gentleman, Y C Fredholm, G Jell, et al.. The effects of strontium-substituted bioactive glasses on osteoblasts and osteoclasts in vitro. Biomaterials, 2010, 31(14): 3949–3956
https://doi.org/10.1016/j.biomaterials.2010.01.121 pmid: 20170952
43 W Götz, C Reichert, L Canullo, et al.. Coupling of osteogenesis and angiogenesis in bone substitute healing — A brief overview. Annals of Anatomy, 2012, 194(2): 171–173
https://doi.org/10.1016/j.aanat.2011.10.002 pmid: 22055938
[1] Ya-Wei DU,Li-Nan ZHANG,Zeng-Tao HOU,Xin YE,Hong-Sheng GU,Guo-Ping YAN,Peng SHANG. Physical modification of polyetheretherketone for orthopedic implants[J]. Front. Mater. Sci., 2014, 8(4): 313-324.
[2] Qiang WEI, Zhen-Duo CUI, Xian-Jin YANG, Lian-Yun ZHANG, Jia-Yin DENG, . Design and characterization of bioceramic coating materials for Ti6Al4V[J]. Front. Mater. Sci., 2010, 4(2): 171-174.
[3] WANG Lin, YU Bing, SUN Li-ping, REN Lei, ZHANG Qi-qing. Microsphere-integrated gelatin-siloxane hybrid scaffolds for bone tissue engineering: bioactivity & antibacterial activity[J]. Front. Mater. Sci., 2008, 2(2): 172-178.
[4] WU Qisheng, CHENG Futao, WEI Wuji. Study on the mechanical and biological property of PMMA bone cement modified with ultra-fine glass fibers and nano-hydroxyapatite[J]. Front. Mater. Sci., 2007, 1(3): 247-251.
[5] QI Yumin, CUI Chunxiang, LIU Shuangjin, WANG Huifen, HE Yun. Fabrication and biocompatibility in vitro of potassium titanate biological thin film/titanium alloy biological composite[J]. Front. Mater. Sci., 2007, 1(3): 252-257.
Viewed
Full text


Abstract

Cited

  Shared   
  Discussed