Black tantalic oxide submicro-particles coating on PEEK fibers woven into fabrics as artificial ligaments with photothermal antibacterial effect and osteogenic activity for promoting ligament-bone healing

doi:10.1016/j.jmst.2022.05.054

Abstract

Abstract:

Design of artificial ligaments possessing both osteogenic activity and antibacterial effect that promotes ligament-bone healing and prevents bacterial infection in bone tunnels for anterior cruciate ligament (ACL) reconstruction remains a significant challenge. In this study, black tantalic oxide (BTO) submicro-particles with oxygen vacancies and structure defects were fabricated by using traditional white tantalic oxide (WTO) through magnesium thermal reduction (MTR) method, and BTO was coated on polyetheretherketone (PEEK) fibers (PKF), which were woven into fabrics (PBT) as artificial ligaments. PBT with BTO coating exhibited excellent photothermal performance, which possessed not only antibacterial effects in vitro but also anti-infective ability in vivo. PBT with optimized surface properties (e.g., submicro-topography and hydrophilicity) not only significantly facilitated rat bone mesenchymal stem cells (BMSC) responses (e.g., proliferation and osteogenic differentiation) in vitro but also stimulated new bone formation for ligament-bone healing in vivo. The presence of oxygen vacancies and structure defects in BTO did not change the surface properties and osteogenic activity of BPT while displaying an outstanding photothermal antibacterial effect. In summary, BPT with osteogenic activity and photothermal antibacterial effect promoted bone regeneration and prevented bacterial infection, thereby promoting ligament-bone healing. Therefore, PBT would have tremendous potential as a novel artificial ligament for ACL reconstruction.

Key words: Black tantalic oxide, PEEK fibers, Artificial ligament, Photothermal antibacterial effects, Ligament-bone healing

Fan Wang, Mengyao Wang, Qingsong He, Xuehong Wang, Ping Sun, Yinjun Ji, Yunfei Niu, Fengqian Li, Jie Wei. Black tantalic oxide submicro-particles coating on PEEK fibers woven into fabrics as artificial ligaments with photothermal antibacterial effect and osteogenic activity for promoting ligament-bone healing[J]. J. Mater. Sci. Technol., 2023, 133: 195-208.

Figures/Tables 9

Fig. 1. (A) Digital photos, (B) SEM images (scale bar: 500 nm), (C) TEM images (scale bar: 1 nm), (D) IFFT images (scale bar: 1 nm), (E) XRD patterns (* represents TO characteristic peaks), (F) XPS spectra (Ta narrow scan), (G) EPR and (H) UV-vis-NIR absorption spectrum, and (I) photothermal curves in the dry environment of WTO and BTO, (J) photothermal stability curve of BTO, and (K) thermal images of WTO and BTO, NIR irradiation (5 min, 808 nm, 1 W/cm2).

Fig. 2. (A) Digital photos, (B) SEM images (scale bar: 8 μm) and (C) SEM images of B under high magnification (scale bar: 1 μm) of the samples (PKF, PWT and PBT).

Fig. 3. (A) FTIR spectrum, (B) XRD patterns (* represents TO characteristic peaks, ○ represents PEEK characteristic peaks), (C) photothermal curves in the dry environment under NIR irradiation (5 min, 808 nm and 1 W/cm2), (D) protein adsorption, (E) water and diiodomethane contact angles and (F) surface energy of the samples (PKF, PWT and PBT).

Fig. 4. (A) SEM images (scale bar: 25 μm), (B) CLSM (scale bar: 20 μm) of the morphology of BMSC on the samples (PKF, PWT and PBT) at 1 and 3 d after culturing, (C) adhesion ratio of the cells on samples at 4, 6 and 12 h after culturing, and (D) proliferation of the cells on samples at 1, 3 and 7 d after culturing. * represents p < 0.05, compared with PKF.

Fig. 5. (A) Views of ALP staining (scale bar: 300 μm), (B) quantitative evaluation of ALP activity, (C-F) expression of osteogenic-associated genes (OPN, OCN, Runx2 and ALP) of BMSC on the samples (PKF, PWT and PBT) at 7 and 14 d after culturing. * represents p < 0.05, compared with PKF.

Fig. 6. (A, D) Bacterial live dead staining images (scale bar: 20 μm), (B, E) photos of colonies and (C, F) antibacterial ratio of S. aureus (A-C) and E.coli (D-F) cultivated on the samples (PKF, PWT and PBT) with NIR or without NIR irradiation. * represents p < 0.05, compared with PKF, # represents p < 0.05, compared with PWT.

Fig. 7. (A) Thermal images and (B) photothermal curves of sample implantation area under NIR irradiation (808 nm, 1 W/cm2, 5 min), (C) representative images of the bacteria detached from samples at 14 days, and (D) antibacterial ratio of S. aureus; (E) X-ray images of rat femurs with PKF, PWT and PBT at day 14 after implantation, red arrow represents cortical bone destruction and periosteal reaction. * represents p < 0.05, compared with PKF, # represents p < 0.05, compared with PWT.

Fig. 8. Micro-CT 2D images of bone tunnels area in both femur (A) and tibial (B) at 4 and 12 w after implantation of the samples (PKF, PWT and PBT), scale bar: 2 mm; micro-CT 3D reconstructed images of bone tunnels area in both femur (C) and tibial (D) at 4 and 12 w after implantation of the samples, scale bar: 3 mm; Quantitative analysis of BV/TV for femoral (E) and tibial (F), femoral bone tunnel area (G), tibial bone tunnel area (H), and failure load (I) at 4 and 12 w after implantation of the samples. * represents p < 0.05, compared with PKF.

Fig. 9. Photos of histological images of H&E (A) and Masson (B) staining of the samples (PKF, PWT and PBT) at 4 and 12 w after implantation. NB: new bone, G: implantable samples, IF: interface.

References 67

[1]	Y. Kawakami, K. Nonaka, N. Fukase, A. D’Amore, Y. Murata, P. Quinn, S. Luketich, K. Takayama, K.G. Patel, T. Matsumoto, J.H. Cummins, M. Kurosaka, K. Kuroda, W.R. Wagner, F.H. Fu, J. Huard, Acta Biomater. 121 (2021) 275-287. DOI PMID
[2]	Y. Li, S.C. Fu, Y.C. Cheuk, Y.T. Ong, H. Feng, S.H. Yung, J. Orthop. Transl. 24 (2020) 183-189.
[3]	Y.J. No, M. Castilho, Y. Ramaswamy, H. Zreiqat, Adv. Mater. 32 (2019) 1904511. DOI URL
[4]	T.W. Chen, P. Zhang, J.W. Chen, Y.H. Hua, S.Y. Chen, Am. J. Sport. Med. 45 (2017) 2739-2750. DOI URL
[5]	Y. Luo, C. Zhang, J. Wang, F.F. Liu, K.W. Chau, L. Qin, J.L. Wang, Bioact. Mater. 10 (2021) 3231-3243.
[6]	H.G. Li, J.B. Fan, L.G. Sun, X.C. Liu, P.Z. Cheng, H.B. Fan, Biomaterials 106 (2016) 180-192.
[7]	H. Li, J.Y. Li, J. Jiang, F. Lv, J. Chang, S.Y. Chen, C.T. Wu, Acta Biomater. 54 (2017) 399-410. DOI URL
[8]	Y.M. Li, X.M. Guo, S.K. Dong, T.H. Zhu, Y.S. Chen, S. Zhao, G.M. Xie, J. Jiang, H.Y. He, C.S. Liu, J.Z. Zhao, Acta Biomater. 115 (2020) 160-175. DOI URL
[9]	M. Reijman, V. Eggerding, E.E. Van, A.E. Van, D.B.I. Van, L.J. Van, J. Zijl, E. Waarsing, S. Bierma-Zeinstra, D. Meuffels,BMJ Brit. Med. J. 372 (2021) n375.
[10]	D. Porrelli, M. Mardirossian, N. Crapisi, M. Urban, N.A. Ulian, L. Bevilacqua, G. Turco, M. Maglione, J. Mater. Sci. Technol. 95 (2021) 213-224. DOI
[11]	M.M. He, Y. Huang, H. Xu, G.J. Feng, L.M. Liu, Y.B. Li, D. Sun, L. Zhang, Acta Biomater. 129 (2021) 18-32. DOI URL
[12]	J.Y. Hou, Z.H. Xiao, Z.Q. Liu, H.W. Zhao, Y.K. Zhu, L. Guo, Z.F. Zhang, R.O. Ritchie, Y. Wei, X.L. Deng, Adv. Mater. 33 (2021) 2103727. DOI URL
[13]	Z.G. Yuan, T. long, J. Zhang, Z. Lyu, W. Zhang, X.C. Meng, J. Qi, Y. Wang, J. Or- thop. Transl. 33 (2022) 90-106.
[14]	Z. Yuan, Y. He, C.C. Lin, P. Liu, K.Y. Cai, J. Mater. Sci. Technol. 78 (2021) 51-67. DOI URL
[15]	Y.Z. Wu, Q. Liao, L. Wu, Y.X. Luo, W. Zhang, M. Guan, H.B. Pan, L.P. Tong, P.K. Chu, H.Y. Wang, ACS Nano 12 (2021) 17854-17869.
[16]	Y. Wu, Y.H. Zhang, R. Zhang, S.Y. Chen, Front. Bioeng. Biotechnol. 9 (2021) 630745. DOI URL
[17]	P. Ma, T.W. Chen, X.P. Wu, Y.D. Hu, K. Huang, Y.F. Wang, H.L. Dai, J. Mater. Chem. B 9 (2021) 6600-6613.
[18]	Q. Wu, X.M. Liu, B. Li, L. Tan, Y. Han, Z.Y. Li, Y.Q. Liang, Z.D. Cui, S.L. Zhu, S. L. Wu, Y.F. Zheng, J. Mater. Sci. Technol. 67 (2021) 70-79. DOI URL
[19]	J. Liu, L. Li, R. Zhang, Z.P. Xu, J. Mater. Sci. Technol. 63 (2021) 73-80. DOI URL
[20]	J. Song, J. Li, X.R. Bai, L. Kang, L.Y. Ma, N.Q. Zhao, S.L. Wu, Y. Xue, J.J. Li, X.J. Ji, J.W. Sha, J. Mater. Sci. Technol. 87 (2021) 83-94. DOI
[21]	Y. Huang, P.J. Wang, W.M. Tan, W.K. Hao, L.W. Ma, J.K. Wang, T. Liu, F. Zhang, C. H. Ren, W. Liu, D.W. Zhang, J. Mater. Sci. Technol. 107 (2022) 34-42. DOI
[22]	Z. Yang, F.J. Zhao, W. Zhang, Z.Y. Yang, M. Luo, L. Liu, X.D. Cao, D.F. Chen, X. F. Chen, Chem. Eng. J. 419 (2021) 129520. DOI URL
[23]	L.P. Tong, Q. Liao, Y.T. Zhao, H. Huang, A. Gao, W. Zhang, X.Y. Gao, W. Wei, M. Guan, P.K. Chu, H.Y. Wang, Biomaterials 193 (2019) 1-11.
[24]	X.C. Wang, J.M. Xue, B. Ma, J.F. Wu, J. Chang, M. Gelinsky, C.T. Wu, Adv. Mater. 48 (2020) 2005140.
[25]	Z.M. Wang, J. Zhao, W.Z. Tang, L.Q. Hu, X. Chen, Y.P. Su, C. Zou, J.H. Wang, W.W. Lu, W.X. Zhen, R.H. Zhang, D.Z. Yang, S.L. Peng, Small 15 (2019) 1901560.
[26]	X.M. Zhang, Y. Li, Y.X. Gu, C.N. Zhang, H.C. Lai, J.Y. Shi, Int. J. Nanomed. 14 (2019) 8693-8706. DOI URL
[27]	M.M. Momeni, M. Mirhosseini, M. Chavoshi, Ceram. Int. 42 (2016) 9133-9138. DOI URL
[28]	L.L. Liu, J. Xu, S.Y. Jiang, Metals 6 (2016) 221 (Basel).
[29]	K. McNamara, S. Beloshapkin, K.M. Hossain, M.S. Dhoubhadel, S.A.M. Tofail, Appl. Surf. Sci. 535 (2021) 147621. DOI URL
[30]	S.Q. Mei, F. Wang, X.L. Hu, K. Yang, D. Xie, L.L. Yang, Z.Y. Wu, J. Wei, Biomater. Sci. 9 (2021) 167-185. DOI URL
[31]	H.L. Huang, Y.Y. Chang, H.J. Chen, Y.K. Chou, C.H. Lai, M.Y.C. Chen, J. Vac. Sci. Technol. A 32 (2014) 02B117. DOI URL
[32]	N. Koufaki, A. Ranella, K.E. Aifantis, M. Barberoglou, S. Psycharakis, C. Fotakis, E. Stratakis,Biofabrication 3 (2011) 045004.
[33]	K. Stapelfeldt, S. Stamboroski, P. Mednikova, D. Bruggemann,Biofabrication 11 (2019) 025010.
[34]	S.C. Huo, F. Wang, Z.C. Lyu, Q.M. Hong, B.E. Nie, J. Wei, Y. Wang, J. Zhang, B. Yue, Chem. Eng. J. 426 (2021) 130806. DOI URL
[35]	X. Wu, C. Luo, P. Hao, T. Sun, R.S. Wang, C.L. Wang, Z.G. Hu, Y.W. Li, J. Zhang, G. Bersuker, L.T. Sun, K. Pey, Adv. Mater. 30 (2018) 1703025. DOI URL
[36]	A .M. Diez-Pascual, A .L. Diez-Vicente, ACS Appl. Mater. Interfaces 7 (2015) 5561-5573.
[37]	M. Qasim, K. Asghar, D. Das, Ceram. Int. 45 (2019) 24971-24981. DOI
[38]	C.F. Almeida Alves, L. Fialho, S.M. Marques, S. Pires, P. Rico, C. Palacio, S. Car- valho, Sci. Eng. C 124 (2021) 112008.
[39]	M.M. Ye, J. Jia, G.A. Ozin, Adv. Energy Mater. 7 (2017) 1601811. DOI URL
[40]	J.C. Ruiz-Cornejo, J.F. Vivo-Vilches, D. Sebastián, M.V. Martínez-Huerta, M. J. Lázaro, Renew. Energy 178 (2021) 307-317.
[41]	K. Manthiram, A.P. Alivisatos, J. Am. Chem. Soc. 134 (2012) 3995-3998. DOI PMID
[42]	L.H.Z. Li, G.Z. Li, Y. Wu, Y.C. Lin, Y.C. Qu, Y. Wu, K.Y. Lu, Y. Zou, H. Chen, Q. Yu, Y. X. Zhang, J. Mater. Sci. Technol. 110 (2022) 14-23. DOI URL
[43]	K.H. Ye, K.S. Li, Y.R. Lu, Z.J. Guo, N. Ni, H. Liu, Y.C. Huang, H.B. Ji, P.S. Wang, TrAC Trends Anal. Chem. 116 (2019) 102-108.
[44]	V. Khanal, N.O. Balayeva, C. Günnemann, Z. Mamiyev, R. Dillert, D.W. Bahne- mann, V. Subramanian, Appl. Catal. B-Environ. 291 (2021) 119974. DOI URL
[45]	M. Wang, G.Q. Tan, Y. Wang, B.X. Zhang, H.J. Ren, L. Lv, S.J. Feng, M.Y. Dang, J. Alloy. Compd. 891 (2021) 161928. DOI URL
[46]	Y.Y. Ma, J. Tan, H.F. Zhang, G.G. Zhang, F. Liu, M.C. Liu, Y. Wang, Y.Q. Zheng, J. Alloy. Compd. 889 (2021) 161767. DOI URL
[47]	Z. Yuan, Y. He, C.C. Lin, P. Liu, K.Y. Cai, J. Mater. Sci. Technol. 78 (2021) 51-67. DOI URL
[48]	Y. Dai, H. Guo, L.Y. Chu, Z.H. He, M.Q. Wang, S.H. Zhang, X.F. Shang, J. Orthop. Transl. 24 (2020) 198-208.
[49]	E.M. Hetrick, M.H. Schoenﬁsch, Chem. Soc. Rev. 35 (2006) 780-789.
[50]	L. Han, Y.N. Zhang, X. Lu, K.F. Wang, Z.M. Wang, H.P. Zhang, ACS Appl. Mater. Interfaces 8 (2016) 29088-29100. DOI URL
[51]	Q. Ding, Y. Liu, T. Chen, X.Y. Wang, Z.C. Feng, X.L. Wan, M. Dupuis, C. Li, J. Mater. Chem. A 8 (2020) 6 812-6 821.
[52]	J.W. Fu, Z.H. Chen, M.H. Wang, S.J. Liu, J.H. Zhang, J.N. Zhang, R.P. Han, Q. Xu, Chem. Eng. J. 259 (2015) 53-61. DOI URL
[53]	M. Rinaldi, T. Ghidini, F. Cecchini, A. Brandao, F. Nanni, Compos. Part B-Eng. 145 (2018) 162-172. DOI URL
[54]	X.J. Dou, X.W. Wei, G. Liu, S. Wang, Y.X. Lv, J.L. Li, Z.J. Ma, G.S. Zheng, Y.K. Wang, M.H. Hu, W.T. Yu, D.W. Zhao, J. Orthop. Transl. 19 (2019) 81-93.
[55]	C.F.A. Alves, A. Cavaleiro, S. Carvalho, Mater. Sci. Eng. C 58 (2016) 110-118. DOI URL
[56]	H. Liu, R. Liu, I. Ullah, S.Y. Zhang, Z.Q. Sun, L. Ren, K. Yang, J. Mater. Sci. Technol. 48 (2020) 130-139. DOI URL
[57]	D.D. Zhang, J.L. Zhou, F. Peng, J. Tan, X.M. Zhang, S. Qian, Y.Q. Qiao, Y. Zhang, X. Y. Liu, J. Mater. Sci. Technol. 105 (2022) 57-67. DOI URL
[58]	Q. Wu, S.X. Xu, X. Wang, B. Jia, Y. Han, Y.F. Zhuang, Y. Sun, Z.Y. Sun, Y.P. Guo, H. M. Kou, C.Q. Ning, K.R. Dai, Biomaterials 268 (2021) 120553.
[59]	M. Zhang, J.T. Zhang, L.N. Ban, L.X. Qiu, J.S. Chen, Z.H. Zhu, Y. Wan,Biofabrica- tion 12 (2020) 035022.
[60]	T. Ni, Y.M. Zhu, L. Hao, Y. Chen, T. Cheng, Mater. Des. 217 (2022) 110643. DOI URL
[61]	Z.Z. Feng, X.M. Liu, L. Tan, Z.D. Cui, X.J. Yang, Z.Y. Li, Y.F. Zheng, K.W.K. Yeung, S. L. Wu, Small 14 (2018) 1704347.
[62]	F.J. Zhao, W.H. Xie, W. Zhang, X.L. Fu, W.D. Gao, B. Lei, X.F. Chen, Adv. Healthc. Mater. 7 (2018) 1800361. DOI URL
[63]	J.Y. Cai, Q.Q. Zhang, J.B. Chen, J. Jiang, X.M. Mo, C.L. He, J.Z. Zhao, Bioact. Mater. 6 (2021) 783-793.
[64]	G. Criscenti, A. Longoni, A. Di Luca, C. De Maria, C.A. Van Blitterswijk, G. Vozzi, L. Moroni,Biofabrication 8 (2016) 015009.
[65]	Y. Luo, C. Zhang, J. Wang, F.F. Liu, K.W. Chau, L. Qin, J.L. Wang, Bioact. Mater. 6 (2021) 3231-3243.
[66]	H.D. Jung, T.S. Jang, J.E. Lee, S.J. Park, Y. Son, S.H. Park,Biofabrication 11 (2019) 045014.
[67]	X. He, Y. Li, J.X. Guo, J.K. Xu, H.Y. Zu, L. Huang, M.T.Y. Ong, P.S.H. Yung, L. Qin, Biomaterials 269 (2021) 120625.