骨骼是一種高度再生的組織，損傷後可以自行再生。但是，當損傷太嚴重時，骨骼很難自行修復。因此，近來對人造骨的需求不斷增加，而生物活性玻璃是另一種表現出優異的生物活性、生物相容性和生物降解性的材料。然而，在實際應用中，存在對其機械強度較弱的擔憂。在人工骨移植物中添加壓電元件可以提供更好的生物反應並有助於骨癒合過程。

在本實驗中，生物活性玻璃 (BG) 和鈦酸鋇 (BT) 複合材料進行了造粒，並通過噴霧熱解 (SP) 和噴霧乾燥 (SD) 對其進行了表徵。採用X射線衍射和掃描電子顯微鏡分析了噴霧熱解製備的76SBG (SiO2 80 mo%, CaO 15 mol% P2O5 5 mol%) 顆粒的晶體結構和顆粒狀態。然後使用噴霧乾燥將 BT 和 BG 複合材料造粒。在製粒過程中使用這種濃度為 1.0 wt% 的聚乙烯醇 (PVA) 以試圖控製粒徑而不被巨噬細胞檢測到。通過 X 射線衍射、掃描電子顯微鏡、傅里葉變換光譜和 MTT 測定對顆粒狀樣品的相組成、形態、生物活性、細胞毒性和生物降解性進行了表徵。

在本研究中，通過結合 SP 和 SD 成功實現了造粒。使用傅里葉變換光譜儀通過體外試驗證實製備的BG產生羥基磷灰石。在所有樣品中均未觀察到細胞毒性，表明噴霧熱解和噴霧乾燥相結合是一種有效的製粒方法。

Bone is a highly regenerative tissue that can regenerate on its own after damage. However, when the damage is too severe, it is difficult for bone to repair on its own. Therefore, the need for artificial bone has been increasing recently, and Bioactive glass is another material that exhibits excellent bioactivity, biocompatibility, and biodegradability. However, in terms of practical application, there are concerns about its weak mechanical strength. Adding piezoelectric components to artificial bone grafts can provide better biological response and help in the bone healing process.

In this experiment, bioactive glass (BG) and barium titanate (BT) composites were granulated and characterized by spray pyrolysis (SP) and spray drying (SD). 76SBG (SiO2 80 mo%, CaO 15 mol% P2O5 5 mol%) particles prepared by spray pyrolysis were analyzed for crystal structure and particle state by X-ray diffraction and scanning electron microscopy. The BT and BG composites were then granulated using spray drying. This polyvinyl alcohol (PVA) concentration of 1.0 wt% was used during granulation in an attempt to control particle size without detection by macrophages. The granulated samples were characterized for phase composition, morphology, bioactivity, cytotoxicity, and biodegradability by X-ray diffraction, scanning electron microscopy, Fourier transform infrared spectroscopy, and MTT assay.

In this study, granulation was successfully achieved by combining SP and SD. The prepared BG was confirmed to produce hydroxyapatite by in vitro tests using a Fourier transform spectrometer. No cytotoxicity was observed in all samples, indicating that the combination of spray pyrolysis and spray drying is an effective granulation method.

[1] Joana Caetano-Lopes, Helena Canhão, João Eurico Fonseca “Osteoblasts and Bone Formation” Article in Acta Reumatologica Portuguesa, April 2007
[2] Atsushi Irie, Masamichi Takami, Hideo Kubo, Naoko Sekino-Suzuki, Kohji Kasahara, Yutaka Sanai “Heparin enhances osteoclastic bone resorption by inhibiting osteoprotegerin activity” Bone Volume 41, Issue 2, August 2007, Pages 165-174
[3] Akira Myoui “History of Artificial Bones and Latest Design Concepts” Artificial Organs Vol. 40, No. 1 2011
[4] Liu-Gu Chen, Yu-Hsuan Huang, Yu-Jen Chou. Preparation and characterization of spray-dried granulated bioactive glass micron spheres. Applied Ceramic TECHNOLOGY. DOI: 10.1111/ijac.13715
[5] Tetsuya Kameyame. Bioceramics: Minor Special Issue on Ceramics and Surface Treatment. Vo1.45, No 4,1994
[6] Zohaib Khurshid, Shehriar Husain, Hessah Alotaibi, Rabiya Rehman, Muhammad S. Zafar, Imran Farooq, Abdul S. Khan. Novel Techniques of Scaffold Fabrication for Bioactive Glasses. 2019 Elsevier Ltd. All rights reserved. Chapter 18
[7] Chikara Ohtsuki and Toshiki Miyazaki, Graded Structure on Artificial Bone Having Bone-Bonding Ability, J. Jpn. Soc. Powder Powder Metallurgy Vol. 51, No. 4, Received December 10, 2003
[8] R. Li, A.E. Clark, and L. L. Hench “An Investigation of Bioactive Glass Powders by Sol-Gel Processing” Journdl of Applied Biomdterinl5, Vol 2, 231 239 (1991)
[9] Gene H. Haertling “Ferroelectric Ceramics: History and Technology” J. Am. Ceram. Soc., 82 [4] 797–818 (1999)
[10] Eiichi Fukada, Iwao Yasuda “On the piezoelectric effect of bone” Journal of the physical society of Japan Vol. 12, No. 10, October 1957
[11] M. Acosta, N. Novak, V. Rojas, S. Patel, R. Vaish, J. Koruza, G. A. Rossetti, Jr.
and J. Rodel “BaTiO3-based piezoelectrics: Fundamentals, current status, and perspectives” APPLIED PHYSICS REVIEWS 4, 041305 (2017)
[12] Fu-Cheng Kao, Ping-Yeh Chiu, Tsung-Ting Tsai, Zong-Hong Lin “The application of nanogenerators and piezoelectricity in osteogenesis” Science and Technology of Advanced Materials. Volume 20, 2019 - Issue 1
[13] M. Acosta, N. Novak, V. Rojas, S. Patel, R. Vaish, J. Koruza, G. A. Rossetti, Jr.,
and J. Rodel “BaTiO3-based piezoelectrics: Fundamentals, current status, and perspectives” APPLIED PHYSICS REVIEWS 4, 041305 (2017)
[14] Cijun Shuai, Guofeng Liu, Youwen Yang, Wenjing Yang, Chongxian He, Guoyong Wang, Zheng Liu, Fangwei Qi, Shuping Peng “Functionalized BaTiO3 enhances piezoelectric effect towards cell response of bone scaffold” Colloids and Surfaces B: Biointerfaces Volume 185, 1 January 2020, 110587
[15] Deepak Khare, Bikramjit Basu, Ashutosh Kumar Dubey “Electrical stimulation and piezoelectric biomaterials for bone tissue engineering applications” Biomaterials Volume 258, November 2020, 120280
[16] NikeWalter, Theresia Stich, Denitsa Docheva, Volker Alt, Markus Rupp “Evolution of implants and advancements for osseointegration: A narrative review” Injury Available online 4 August 2022
[17] Shao-Ju Shih • Yu-Jen Chou • I-Chen Chien. One-step synthesis of bioactive glass by spray pyrolysis. J Nanopart Res (2012) 14:1299. DOI 10.1007/s11051-012-1299-1
[18] Gary L. Messing, Shi-Chang Zhang, and Gopal V. Jayanthi “Ceramic Powder Synthesis by Spray Pyrolysis” Journal J. AM. Ceram. Soc, 76 [11] 2707-26 1993
[19] Reinhard Vehringa, Willard R. Fossb, David Lechuga-Ballesteros. Particle formation in spray drying. Aerosol Science 38 (2007) 728 – 746
[20] Liu-Gu Chen, Yu-Hsuan Huang, Yu-Jen Chou. Preparation and characterization of spray-dried granulated bioactive glass micron spheres. Applied Ceramic TECHNOLOGY. DOI: 10.1111/ijac.13715
[21] M. Meskinfam “17 - Polymer scaffolds for bone regeneration” Characterization of Polymeric Biomaterials 2017, Pages 441-475
[22] https://kovodym.blogspot.com/2014/04/33-compact-bone-tissue-diagram.html
[23] Xiaoming Li, Shuang Yang, Shaochuan Wang, Shidan, Li, Hao Jiang, Wenhui Hu, Ping Liu, Qijie Dai, Bo Zhang, Yanfeng Luo, Shiwu Dong “A hierarchical biomimetic periosteum combined immunomodulatory and osteogenic functions for bone regeneration” Composites Part B: Engineering Volume 243, 15 August 2022, 110099
[24] Wentao Zhang, Naiguo Wang, Ming Yang, Tianze Sun, Jing Zhang, Yantao Zhao, Na Huo, Zhonghai Li “Periosteum and development of the tissue-engineered periosteum for guided bone regeneration” Journal of Orthopaedic Translation
Volume 33, March 2022, Pages 41-54
[25] Yuhe Yang, Jingdong Rao, Huaqian Liu, Zhifei Dong, Zhen Zhang, Ho-Pan Bei, Chunyi Wen, Xin Zhao “Biomimicking design of artificial periosteum for promoting bone healing ” Journal of Orthopaedic Translation
Volume 36, September 2022, Pages 18-32
[26] Kara Rogers “carpal bone anatomy” The Editors of Encyclopaedia Britannica • Edit History
[27] Ian H. Parkinson, Nicola L. Fazzalari “Characterisation of Trabecular Bone Structure”
Skeletal Aging and Osteoporosis January 2012
[28] Shigeo Niwa “Recent Trends and Development of Biomaterials for Artificial Bone” December 2003.
[29] H. ROESLER “THE HISTORY OF SOME FUNDAMENTAL CONCEPTS IN
BONE BIOMECHANICS” J. Biomechanics Vol. 20 No. 11 12. Pp. 1025-1034. 1987. Printed in Great Britain
[30] Hench LL. Bioceramics: From concept to clinic. J Am Ceram Soc. 1991;74:1487–510.
[31] Vera B. Morthenn, Gottfried Lemperle,, and Richard L. Gallo. Phagocytosis of different Particulate Dermal Filler Substances by Human Macrophages and Skin Cells. Dermatol Surg 28:6:June 2002
[32] Hashmat Gul, Maria Khan, Abdul Samad Khan “Bioceramics: types and clinical
Applications” Handbook of Ionic Substituted Hydroxyapatites 2020
[33] X. ZHAO. Introduction to bioactive materials in medicine. UK–China Research Academy of Bioactive Molecules and Materials (RABMM), UK
[34] D. F. Williams. The Williams Dictionary of Biomaterials, 1999, p. 42. Liverpool, UK: Liverpool University Press.
[35] Eugeni Cañas, María José Orts, Enrique Sánchez, Devis Bellucci, Valeria Cannillo “Deposition of bioactive glass coatings based on a novel composition containing strontium and magnesium” Journal of the European Ceramic Society Volume 42, Issue 13, October 2022, Pages 6213-6221
[36] Imran Farooq, Saqib Ali, Shehriar Husain, Erum Khan, Robert G.Hill5 “17 - Bioactive glasses—structure and applications” Advanced Dental Biomaterials 2019, Pages 453-476
[37] Mahdieh Hajian Monfared, Faezeh Esmaeili Ranjbar, Maryam Torbati, S. Ali Poursamar, Nasrin Lotfibakhshaiesh, Jafar Ai, Somayeh Ebrahimi-Barough, Mahmoud Azami “Preparation and characterization of 3D nanocomposite scaffold from bioactive glass/β-tricalcium phosphate via Robocasting method for bone tissue engineering” Journal of Non-Crystalline Solids Volume 593, 1 October 2022, 121769
[38] L. L. Hench, R. J. Splinter, W. C. Allen and T. K. Greenlee, Jr. Bonding mechanisms at the interface of ceramic prosthetic materials. J. Biomed. Mater. Res., 1971, 2, 117–141.
[39] Fengjie Li, Yue Jiang, Minghui Chen, Bin Yu, Jinlong Wang, Fuhui Wang “Effect of ZrO2 addition on in-vitro bioactivity and mechanical properties of SiO2–Na2O–CaO–P2O5 bioactive glass-ceramic” Ceramics International Volume 48, Issue 13, 1 July 2022, Pages 18541-18550
[40] Andrada Ioana, Damian-Buda, Georgeta Voicu, Bogdan Stefan Vasile, Adela Banciu, Florin Iordache, Lucian Toma Ciocan “Development of mesoporous borosilicate bioactive glass nanoparticles containing Mg2+ and Zn2+: biocompatibility, bioactivity and antibacterial activity” Journal of Non-Crystalline Solids Volume 594, 15 October 2022, 121819
[41] Marcelo da Silva Mantini Viana, Thalita MarcolanValverde, Breno Rocha Barrioni, Alfredo Miranda de Goes, Marcos Augusto de Sá, Marivalda de Magalhães Pereira “Binary SiO2–CoO spherical bioactive glass nanoparticles for tissue engineering applications” Ceramics International Available online 12 August 2022
[42] Marcelo da Silva Mantini Viana, Thalita Marcolan Valverde, Breno Rocha Barrioni, Alfredo Miranda de Goes, Marcos Augusto de Sá, Marivalda de Magalhães Pereira “Binary SiO2–CoO spherical bioactive glass nanoparticles for tissue engineering applications” Ceramics International Available online 12 August 2022
[43] Hideki Aoki, Masaru Akao, Atsuo Ito and Satoshi Nakamura “Crystal Chemistry of Hydroxyapatite” Division of Inorganic Materials, Institute for Medical and Dental Engineering , Tokyo Medical and Dental University 1988
[44] C.C. Silva, H.H.B. Rocha, F.N.A. Freire, M.R.P. Santos, K.D.A. Saboia,
J.C. Goes, A.S.B. Sombra “Hydroxyapatite screen-printed thick films: optical
and electrical properties” Materials Chemistry and Physics 92 (2005) 260–268
[45] V. P. Orlovskii, V. S. Komlev and S. M. Barinov “Hydroxyapatite and Hydroxyapatite-Based Ceramics” Inorganic Materials, Vol. 38, No. 10, 2002, pp. 973–984
[46] Yu-Jen Chou, Chih-Wei Hsiao, Nien-Ti Tsou , Meng-Huang Wu and Shao-Ju Shih “Preparation and in Vitro Bioactivity of Micron-sized Bioactive Glass Particles Using Spray Drying Method” Article in Applied Sciences · December 2018
[47] Roland Wetzel, Delia S. Brauer “Apatite formation of substituted Bioglass 45S5: SBF vs. Tris” Materials Letters Volume 257, 15 December 2019, 126760
[48] F.Wudy, C.Stock, H.J.Gores “MEASUREMENT METHODS | Electrochemical: Quartz Microbalance” Reference Module in Chemistry, Molecular Sciences and Chemical Engineering Encyclopedia of Electrochemical Power Sources 2009, Pages 660-672
[49] Nike Walter, Theresia Stich, Denitsa Docheva, Volker Alt, Markus Rupp “Evolution of implants and advancements for osseointegration: A narrative review” Injury　Available online 4 August 2022
[50] Yohko F. YANO. Nanodroplets Generated by Ultrasonic Atomization. Earozoru Kenkyu, 26 (1), 18-23 (2011)
[51] Nobuo Kieda “Preparation and Microstnlcture Control of Fine Particles
by Spray Pyrolysis” Inorganic Materials, Vol.5, Mar. 103-112(1998)
[52] Chao-Kuang Kuo, Liu-Gu Chen, Chun-Fu Tseng, Yu-Jen Chou “Influences of acid catalysts on the microstructure, bioactivity and cytotoxicity of bioactive glass nanoparticles prepared by spray pyrolysis” Journal of Non-Crystalline Solids 560 (2021) 120710 Available
[53] Hidefumi Yoshii “The Structure and Properties of Spray-dried Powder. Journal of the Japanese Society for Food Technology” Vol. 14, No. 3, pp. 119 - 124, Sep. 2013
[54] Giulia Molino, Alessandra Bari, Francesco Baino, Sonia Fiorilli, and Chiara Vitale-Brovarone “Electrophoretic deposition of spray-dried Sr-containing mesoporous bioactive glass spheres on glass–ceramic scaffolds for bone tissue regeneration” J Mater Sci (2017) 52:9103–9114
[55] Yoshio Kukita “Spray Drying” UDC 66.047.791.1 1973
[56] M. Weller, T. Overton, J. Rourke, and F. Armstrong, Schreiber Atkins Inorganic Chemistry (Upper), 6th edition, Tokyo Kagaku Doujin, Inc 2016
[57] Makoto Takagi, Basic Analytical Chemistry, Chemical Dojin 2006
[58] Lewi Peter Richardo “The bioactivity, antibacterial properties and cell-viability effects of Sr on Ag-containing mesoporous bioactive glass” 2020 July
[59] S. Petit, J. Madejova “Chapter 2.7 - Fourier Transform Infrared Spectroscopy” Developments in Clay Science Volume 5, 2013, Pages 213-231
[60] S.A., Husseina, Reham Roshdya, Mohammed Ezzeldienb, M.S., Abd-sadeka “Effect of mixed ions of (Zr+2 and Ti+2) on the physical properties of B2O3-SiO2-P2O5 single bond Na2O single bond CaO as bioactive glass system” Journal of Non-Crystalline Solids Available online 7 December 2021, 121324
[61] Jianhui Chenabc, Lei Zengb, Xiaofeng Chenabc, Tianshun Liaoabc, Jiafu Zheng” Preparation and characterization of bioactive glass tablets and evaluation of bioactivity and cytotoxicity in vitro” Bioactive Materials, Volume 3, Issue 3, September 2018, Pages 315-321
[62] A. Hodzic “Re-use, recycling and degradation of composites” Green Composites
Polymer Composites and the Environment Woodhead Publishing Series in Composites Science and Engineering 2004, Pages 252-271
[63] Sanzhong Xu, Xianyan Yang, Xiaoyi Chen, Huifeng Shao, Yong He, Lei Zhang, Guojing Yang, Zhongru Gou “Effect of borosilicate glass on the mechanical and biodegradation properties of 45S5-derived bioactive glass-ceramics” Journal of Non-Crystalline Solids Volume 405, 1 December 2014, Pages 91-99