{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,5,12]],"date-time":"2026-05-12T02:04:06Z","timestamp":1778551446218,"version":"3.51.4"},"reference-count":42,"publisher":"MDPI AG","issue":"3","license":[{"start":{"date-parts":[[2022,2,4]],"date-time":"2022-02-04T00:00:00Z","timestamp":1643932800000},"content-version":"vor","delay-in-days":0,"URL":"https:\/\/creativecommons.org\/licenses\/by\/4.0\/"}],"funder":[{"DOI":"10.13039\/501100001691","name":"Japan Society for the Promotion of Science","doi-asserted-by":"publisher","award":["JP19H02549"],"award-info":[{"award-number":["JP19H02549"]}],"id":[{"id":"10.13039\/501100001691","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100001691","name":"Japan Society for the Promotion of Science","doi-asserted-by":"publisher","award":["JP21K05175"],"award-info":[{"award-number":["JP21K05175"]}],"id":[{"id":"10.13039\/501100001691","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100002241","name":"Japan Science and Technology Agency","doi-asserted-by":"publisher","award":["JPMJMI21EE"],"award-info":[{"award-number":["JPMJMI21EE"]}],"id":[{"id":"10.13039\/501100002241","id-type":"DOI","asserted-by":"publisher"}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":["Nanomaterials"],"abstract":"<jats:p>Nanofibrillated bacterial cellulose (NFBC), a type of cellulose nanofiber biosynthesized by Gluconacetobacter sp., has extremely long (i.e., high-aspect-ratio) fibers that are expected to be useful as nanofillers for fiber-reinforced composite resins. In this study, we investigated a composite of NFBC and poly(methyl methacrylate) (PMMA), a highly transparent resin, with the aim of improving the mechanical properties of the latter. The abundant hydroxyl groups on the NFBC surface were silylated using 3-(methacryloyloxy)propyltrimethoxysilane (MPTMS), a silane coupling agent bearing a methacryloyl group as the organic functional group. The surface-modified NFBC was homogeneously dispersed in chloroform, mixed with neat PMMA, and converted into PMMA composites using a simple solvent-casting method. The tensile strength and Young\u2019s modulus of the composite increased by factors of 1.6 and 1.8, respectively, when only 0.10 wt% of the surface-modified NFBC was added, without sacrificing the maximum elongation rate. In addition, the composite maintained the high transparency of PMMA, highlighting that the addition of MPTMS-modified NFBC easily reinforce PMMA. Furthermore, interactions involving the organic functional groups of MPTMS were found to be very important for reinforcing PMMA.<\/jats:p>","DOI":"10.3390\/nano12030537","type":"journal-article","created":{"date-parts":[[2022,2,6]],"date-time":"2022-02-06T20:38:40Z","timestamp":1644179920000},"page":"537","update-policy":"https:\/\/doi.org\/10.3390\/mdpi_crossmark_policy","source":"Crossref","is-referenced-by-count":15,"title":["Reinforcing Poly(methyl methacrylate) with Bacterial Cellulose Nanofibers Chemically Modified with Methacryolyl Groups"],"prefix":"10.3390","volume":"12","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-5675-3157","authenticated-orcid":false,"given":"Hiroyuki","family":"Kono","sequence":"first","affiliation":[{"name":"Division of Applied Chemistry and Biochemistry, National Institute of Technology, Tomakomai College, Tomakomai 059-1275, Japan"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Haruto","family":"Tsujisaki","sequence":"additional","affiliation":[{"name":"Division of Applied Chemistry and Biochemistry, National Institute of Technology, Tomakomai College, Tomakomai 059-1275, Japan"},{"name":"Graduate School of Chemical Sciences and Engineering, Hokkaido University, Sapporo 060-8628, Japan"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3238-813X","authenticated-orcid":false,"given":"Kenji","family":"Tajima","sequence":"additional","affiliation":[{"name":"Faculty of Engineering, Hokkaido University, Sapporo 060-8628, Japan"}],"role":[{"role":"author","vocabulary":"crossref"}]}],"member":"1968","published-online":{"date-parts":[[2022,2,4]]},"reference":[{"key":"ref_1","doi-asserted-by":"crossref","first-page":"678","DOI":"10.1080\/15583724.2015.1031377","article-title":"A review of the properties and applications of poly (methyl methacrylate) (PMMA)","volume":"55","author":"Ali","year":"2015","journal-title":"Polym. Rev."},{"key":"ref_2","doi-asserted-by":"crossref","unstructured":"Aldegheishem, A., AlDeeb, M., Al-Ahdal, K., Helmi, M., and Alsagob, E.I. (2021). Influence of reinforcing agents on the mechanical properties of denture base resin: A systematic review. Polymers, 13.","DOI":"10.3390\/polym13183083"},{"key":"ref_3","doi-asserted-by":"crossref","unstructured":"Zafar, M.S. (2021). Prosthodontic applications of polymethyl methacrylate (PMMA): An update. Polymers, 13.","DOI":"10.3390\/polym12102299"},{"key":"ref_4","doi-asserted-by":"crossref","first-page":"3801","DOI":"10.2147\/IJN.S130722","article-title":"PMMA denture base material enhancement: A review of fiber, filler, and nanofiller addition","volume":"12","author":"Gad","year":"2017","journal-title":"Int. J. Nanomed."},{"key":"ref_5","doi-asserted-by":"crossref","first-page":"1045","DOI":"10.1016\/S1359-835X(99)00021-4","article-title":"Mechanical properties of glass-fibre mat\/PMMA functionally gradient composite","volume":"30","author":"Jang","year":"1999","journal-title":"Compos. Part A Appl. Sci. Manuf."},{"key":"ref_6","doi-asserted-by":"crossref","first-page":"311","DOI":"10.30684\/etj.35.4A.2","article-title":"Preparation and characterization of PMMA-HDPE and HDPE-PMMA binary polymer blends","volume":"35","author":"Salih","year":"2017","journal-title":"J. Eng. Technol."},{"key":"ref_7","doi-asserted-by":"crossref","first-page":"808","DOI":"10.1039\/C6BM00939E","article-title":"A novel botryoidal aramid fiber reinforcement of a PMMA resin for a restorative biomaterial","volume":"5","author":"He","year":"2017","journal-title":"Biomater. Sci."},{"key":"ref_8","doi-asserted-by":"crossref","first-page":"759","DOI":"10.1002\/pen.24611","article-title":"Preparation of poly(methyl methacrylate)-Silica nanoparticles via differential microemulsion polymerization and physical properties of NR\/PMMA-SiO2 hybrid membranes","volume":"58","author":"Tumnantong","year":"2018","journal-title":"Polym. Eng. Sci."},{"key":"ref_9","first-page":"453","article-title":"The mechanical andoptical properties of injection-moulded PMMA, filled with glass particles of a matching refractive index","volume":"25","author":"Wildner","year":"2017","journal-title":"Polym. Polym. Compos."},{"key":"ref_10","doi-asserted-by":"crossref","first-page":"21308","DOI":"10.1021\/am5062823","article-title":"Improved adhesion between PMMA and stainless steel modified with PMMA brushes","volume":"6","author":"Shimizu","year":"2014","journal-title":"ACS Appl. Mater. Interfaces"},{"key":"ref_11","doi-asserted-by":"crossref","unstructured":"Kim, G.H., Hwang, S.W., Jung, B.N., Kang, D., Shim, J.K., and Seo, K.H. (2020). Effect of PMMA\/Silica hybrid particles on interfacial adhesion and crystallization properties of poly(lactic acid)\/block acrylic elastomer composites. Polymers, 12.","DOI":"10.3390\/polym12102231"},{"key":"ref_12","doi-asserted-by":"crossref","first-page":"41","DOI":"10.1080\/09276440.2018.1467167","article-title":"Enhanced interfacial adhesion between PMMA and carbon fiber by graphene oxide coating","volume":"26","author":"Yanli","year":"2019","journal-title":"Compos. Interfaces"},{"key":"ref_13","doi-asserted-by":"crossref","first-page":"29561","DOI":"10.1021\/acsomega.0c04533","article-title":"Nanofibrillated bacterial cellulose modified with (3-Aminopropyl)trimethoxysilane under aqueous conditions: Applications to poly(methyl methacrylate) fiber-reinforced nanocomposites","volume":"5","author":"Kono","year":"2020","journal-title":"ACS Omega"},{"key":"ref_14","doi-asserted-by":"crossref","first-page":"960","DOI":"10.1016\/j.dental.2006.08.003","article-title":"Effect of fiber architecture on flexural characteristics and fracture of fiber-reinforced dental composites","volume":"23","author":"Karbhari","year":"2007","journal-title":"Dent. Mater."},{"key":"ref_15","doi-asserted-by":"crossref","first-page":"762","DOI":"10.1016\/j.msec.2016.02.001","article-title":"Electrospun nanofiber reinforcement of dental composites with electromagnetic alignment approach","volume":"62","author":"Uyar","year":"2016","journal-title":"Mater. Sci. Eng. C"},{"key":"ref_16","doi-asserted-by":"crossref","unstructured":"Park, S.Y., Yook, S., Goo, S., Im, W., and Youn, H.J. (2020). Preparation of transparent and thick CNF\/epoxy composites by controlling the properties of cellulose nanofibrils. Nanomaterials, 10.","DOI":"10.3390\/nano10040625"},{"key":"ref_17","doi-asserted-by":"crossref","first-page":"277","DOI":"10.1016\/j.compositesb.2015.08.040","article-title":"Mechanical characterization of scalable cellulose nano-fiber based composites made using liquid composite molding process","volume":"84","author":"Barari","year":"2016","journal-title":"Compos. Part B Eng."},{"key":"ref_18","doi-asserted-by":"crossref","first-page":"310","DOI":"10.2115\/fiberst.2020-0039","article-title":"Cellulose Nanofibers: Recent progress and future prospects","volume":"76","author":"Isogai","year":"2020","journal-title":"J. Fiber Sci. Technol."},{"key":"ref_19","doi-asserted-by":"crossref","first-page":"63","DOI":"10.1016\/j.carbpol.2019.05.008","article-title":"Bacterial cellulose production, properties and applications with different culture methods\u2014A review","volume":"219","author":"Wang","year":"2019","journal-title":"Carbohydr. Polym."},{"key":"ref_20","doi-asserted-by":"crossref","unstructured":"Swingler, S., Gupta, A., Gibson, H., Kowalczuk, M., Heaselgrave, W., and Radecka, I. (2021). Recent advances and applications of bacterial cellulose in biomedicine. Polymers, 13.","DOI":"10.3390\/polym13030412"},{"key":"ref_21","doi-asserted-by":"crossref","first-page":"1605","DOI":"10.1002\/nano.202100044","article-title":"Recent development in bacterial cellulose production and synthesis of cellulose based conductive polymer nanocomposites","volume":"2","author":"Poddar","year":"2021","journal-title":"Nano Sel."},{"key":"ref_22","doi-asserted-by":"crossref","first-page":"581","DOI":"10.1021\/acs.biomac.9b01328","article-title":"Detailed structural analyses of nanofibrillated bacterial cellulose and its application as binder material for a display device","volume":"21","author":"Tajima","year":"2019","journal-title":"Biomacromolecules"},{"key":"ref_23","doi-asserted-by":"crossref","first-page":"3432","DOI":"10.1021\/acs.biomac.7b01100","article-title":"One-step production of amphiphilic nanofibrillated cellulose using a cellulose-producing bacterium","volume":"18","author":"Tajima","year":"2017","journal-title":"Biomacromolecules"},{"key":"ref_24","doi-asserted-by":"crossref","first-page":"2971","DOI":"10.1007\/s10570-013-0050-0","article-title":"One-step production of nanofibrillated bacterial cellulose (NFBC) from waste glycerol using Gluconacetobacter intermedius NEDO-01","volume":"20","author":"Kose","year":"2013","journal-title":"Cellulose"},{"key":"ref_25","doi-asserted-by":"crossref","first-page":"8232","DOI":"10.1021\/acsanm.0c01670","article-title":"Nanofibrillated bacterial cellulose surface modified with methyltrimethoxysilane for fiber-reinforced composites","volume":"3","author":"Kono","year":"2020","journal-title":"ACS Appl. Nano Mater."},{"key":"ref_26","doi-asserted-by":"crossref","first-page":"1745","DOI":"10.3390\/ma6051745","article-title":"Nanofibrillated cellulose surface modification: A review","volume":"6","author":"Missoum","year":"2013","journal-title":"Materials"},{"key":"ref_27","doi-asserted-by":"crossref","first-page":"9909","DOI":"10.2147\/IJN.S266103","article-title":"Surface-modified nanocellulose for application in biomedical engineering and nanomedicine: A review","volume":"ume 15","author":"Tortorella","year":"2020","journal-title":"Int. J. Nanomed."},{"key":"ref_28","doi-asserted-by":"crossref","first-page":"34107","DOI":"10.1021\/acsomega.1c05603","article-title":"Facile post-carboxymethylation of cellulose nanofiber surfaces for enhanced water dispersibility","volume":"6","author":"Kono","year":"2021","journal-title":"ACS Omega"},{"key":"ref_29","doi-asserted-by":"crossref","unstructured":"Delgado, A.H.S., and Young, A.M. (2021). Methacrylate peak determination and selection recommendations using ATR-FTIR to investigate polymerisation of dental methacrylate mixtures. PLoS ONE, 16.","DOI":"10.1371\/journal.pone.0252999"},{"key":"ref_30","doi-asserted-by":"crossref","first-page":"7506","DOI":"10.1021\/ja010704o","article-title":"CP\/MAS 13C NMR study of cellulose and cellulose derivatives. 1. Complete assignment of the CP\/MAS 13C NMR spectrum of the native cellulose","volume":"124","author":"Kono","year":"2002","journal-title":"J. Am. Chem. Soc."},{"key":"ref_31","doi-asserted-by":"crossref","first-page":"11454","DOI":"10.1021\/jp048927z","article-title":"A 29Si and 13C CP\/MAS NMR study on the surface species of gas-phase-deposited \u03b3-aminopropylalkoxysilanes on heat-treated silica","volume":"108","author":"Ek","year":"2004","journal-title":"J. Phys. Chem. B"},{"key":"ref_32","doi-asserted-by":"crossref","first-page":"1","DOI":"10.1038\/s41467-020-15669-z","article-title":"Origin of micro-scale heterogeneity in polymerisation of photo-activated resin composites","volume":"11","author":"Sirovica","year":"2020","journal-title":"Nat. Commun."},{"key":"ref_33","doi-asserted-by":"crossref","first-page":"106840","DOI":"10.1016\/j.compositesb.2019.05.051","article-title":"Analysis of mechanical behavior of 3D printed heterogeneous particle-polymer composites","volume":"173","author":"Joyee","year":"2019","journal-title":"Compos. Part B Eng."},{"key":"ref_34","doi-asserted-by":"crossref","first-page":"304","DOI":"10.1016\/j.compositesa.2014.10.014","article-title":"Heterogeneity of discontinuous carbon fibre composites: Damage initiation captured by Digital Image Correlation","volume":"68","author":"Johanson","year":"2015","journal-title":"Compos. Part A Appl. Sci. Manuf."},{"key":"ref_35","doi-asserted-by":"crossref","first-page":"83","DOI":"10.1016\/j.compositesb.2016.10.084","article-title":"Characterization of silylated modified clay nanoparticles and its functionality in PMMA","volume":"110","author":"Bee","year":"2017","journal-title":"Compos. Part B Eng."},{"key":"ref_36","doi-asserted-by":"crossref","first-page":"610","DOI":"10.4012\/dmj.2012-040","article-title":"Effects of silane coupling agents and solutions of different polarity on PMMA bonding to alumina","volume":"31","author":"Chaijareenont","year":"2012","journal-title":"Dent. Mater. J."},{"key":"ref_37","doi-asserted-by":"crossref","first-page":"623","DOI":"10.4012\/dmj.2012-056","article-title":"Effect of different amounts of 3-methacryloxypropyltrimethoxysilane on the flexural properties and wear resistance of alumina reinforced PMMA","volume":"31","author":"Chaijareenont","year":"2012","journal-title":"Dent. Mater. J."},{"key":"ref_38","doi-asserted-by":"crossref","first-page":"7617","DOI":"10.1021\/acsami.0c22584","article-title":"A mussel-inspired polydopamine-filled cellulose aerogel for solar-enabled water remediation","volume":"13","author":"Zou","year":"2021","journal-title":"ACS Appl. Mater. Interfaces"},{"key":"ref_39","doi-asserted-by":"crossref","first-page":"26","DOI":"10.1016\/j.jobab.2020.11.002","article-title":"Plant extract-loaded bacterial cellulose composite membrane for potential biomedical applications","volume":"6","author":"Fatima","year":"2021","journal-title":"J. Bioresour. Bioprod."},{"key":"ref_40","doi-asserted-by":"crossref","first-page":"75","DOI":"10.1016\/j.jobab.2021.01.003","article-title":"Preparation and properties of cellulose nanocomposite fabrics with in situ generated silver nanoparticles by bioreduction method","volume":"6","author":"Deeksha","year":"2021","journal-title":"J. Bioresour. Bioprod."},{"key":"ref_41","doi-asserted-by":"crossref","first-page":"14045","DOI":"10.1021\/la303091k","article-title":"Amine modification of thermally carbonized porous silicon with silane coupling chemistry","volume":"28","author":"Bimbo","year":"2012","journal-title":"Langmuir"},{"key":"ref_42","doi-asserted-by":"crossref","first-page":"806","DOI":"10.1016\/j.compositesa.2010.03.005","article-title":"Silane coupling agents used for natural fiber\/polymer composites: A review","volume":"41","author":"Xie","year":"2010","journal-title":"Compos. Part A Appl. Sci. Manuf."}],"container-title":["Nanomaterials"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/www.mdpi.com\/2079-4991\/12\/3\/537\/pdf","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2025,10,10]],"date-time":"2025-10-10T22:14:14Z","timestamp":1760134454000},"score":1,"resource":{"primary":{"URL":"https:\/\/www.mdpi.com\/2079-4991\/12\/3\/537"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2022,2,4]]},"references-count":42,"journal-issue":{"issue":"3","published-online":{"date-parts":[[2022,2]]}},"alternative-id":["nano12030537"],"URL":"https:\/\/doi.org\/10.3390\/nano12030537","relation":{},"ISSN":["2079-4991"],"issn-type":[{"value":"2079-4991","type":"electronic"}],"subject":[],"published":{"date-parts":[[2022,2,4]]}}}