{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,10,27]],"date-time":"2026-10-27T19:19:51Z","timestamp":1793128791459,"version":"4.5.0"},"reference-count":40,"publisher":"MDPI AG","issue":"6","license":[{"start":{"date-parts":[[2026,3,13]],"date-time":"2026-03-13T00:00:00Z","timestamp":1773360000000},"content-version":"vor","delay-in-days":0,"URL":"https:\/\/creativecommons.org\/licenses\/by\/4.0\/"}],"funder":[{"DOI":"10.13039\/501100001809","name":"National Natural Science Foundation of China","doi-asserted-by":"publisher","award":["52472096"],"award-info":[{"award-number":["52472096"]}],"id":[{"id":"10.13039\/501100001809","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100021171","name":"Guangdong Basic and Applied Basic Research Foundation","doi-asserted-by":"crossref","award":["2024A1515011656"],"award-info":[{"award-number":["2024A1515011656"]}],"id":[{"id":"10.13039\/501100021171","id-type":"DOI","asserted-by":"crossref"}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":["Polymers"],"abstract":"<jats:p>The precursor infiltration and pyrolysis (PIP) route is widely adopted to fabricate carbon fiber-reinforced silicon carbide (Cf\/SiC) composites; however, the atomic-scale restructuring of the pyrolytic carbon\/silicon carbide (PyC\/SiC) interface during ceramization\u2014and its impact on mechanical integrity\u2014remains elusive. Here, reactive molecular dynamics (ReaxFF MD) simulations elucidate the coupled thermochemical\u2013mechanical evolution of polycarbosilane (PCS) precursors on PyC substrates with orientation angles (OAs) of 0\u00b0, 25\u00b0, 55\u00b0, and 85\u00b0. Dynamic pyrolysis triggers a pivotal transition from sp2 to sp3 hybridization at the interface. High-OA substrates (55\u00b0 and 85\u00b0) present a dense population of reactive edge sites, fostering extensive cross-interfacial covalent bonding. Subsequent shear loading reveals that these pyrolysis-induced chemical bridges govern failure modes, shifting from interlayer sliding dominated by weak non-bonded interactions (0\u00b0) to ductile fracture featuring uniform plasticity and crack deflection. The OA = 55\u00b0 interface attains a theoretical peak shear strength of 15 GPa and exhibits the most favorable combination of high strength and ductile failure under tensile loading, owing to an optimal balance between reactive site availability and interlayer steric openness. In contrast, the OA = 85\u00b0 interface, despite comparable peak stress, fails via brittle crack penetration into the SiC matrix. By correlating atomistic structure with macroscopic performance, this study provides a bottom-up framework for engineering Cf\/SiC composites via interfacial texturing and optimized pyrolysis protocols.<\/jats:p>","DOI":"10.3390\/polym18060702","type":"journal-article","created":{"date-parts":[[2026,3,13]],"date-time":"2026-03-13T11:12:25Z","timestamp":1773400345000},"page":"702","update-policy":"https:\/\/doi.org\/10.3390\/mdpi_crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Structural Evolution and Mechanical Modulation of Cf\/SiC Interfaces During PIP Ceramization: A ReaxFF Molecular Dynamics Study"],"prefix":"10.3390","volume":"18","author":[{"given":"Yue","family":"Zhan","sequence":"first","affiliation":[{"name":"School of Materials Science and Engineering, South China University of Technology, Guangzhou 510640, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xudong","family":"Wang","sequence":"additional","affiliation":[{"name":"Xi\u2019an Aerospace Propulsion Institute, Xi\u2019an 710100, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5619-6290","authenticated-orcid":false,"given":"Kang","family":"Guan","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering, South China University of Technology, Guangzhou 510640, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7896-2750","authenticated-orcid":false,"given":"Ming","family":"Lv","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering, South China University of Technology, Guangzhou 510640, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Cheng","family":"Peng","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering, South China University of Technology, Guangzhou 510640, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaohui","family":"Yang","sequence":"additional","affiliation":[{"name":"Xi\u2019an Aerospace Propulsion Institute, Xi\u2019an 710100, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Longteng","family":"Bai","sequence":"additional","affiliation":[{"name":"Xi\u2019an Aerospace Propulsion Institute, Xi\u2019an 710100, China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"1968","published-online":{"date-parts":[[2026,3,13]]},"reference":[{"key":"ref_1","doi-asserted-by":"crossref","first-page":"117","DOI":"10.1016\/j.jmst.2016.08.004","article-title":"Design, Preparation and Properties of Carbon Fiber Reinforced Ultra-High Temperature Ceramic Composites for Aerospace Applications: A Review","volume":"33","author":"Tang","year":"2017","journal-title":"J. Mater. Sci. Technol."},{"key":"ref_2","doi-asserted-by":"crossref","first-page":"109816","DOI":"10.1016\/j.engfracmech.2023.109816","article-title":"Fatigue Life Prediction Considering Individual Modulus for Unidirectional Needled C\/SiC Composites under Variable Amplitude Loading","volume":"295","author":"Yin","year":"2024","journal-title":"Eng. Fract. Mech."},{"key":"ref_3","doi-asserted-by":"crossref","first-page":"635","DOI":"10.1016\/j.matdes.2015.11.024","article-title":"Impact Resistance of 2D Plain-Woven C\/SiC Composites at High Temperature","volume":"90","author":"Yang","year":"2016","journal-title":"Mater. Des."},{"key":"ref_4","doi-asserted-by":"crossref","first-page":"305","DOI":"10.1111\/ijac.12631","article-title":"Pressure-Less Joining of C\/SiC and SiC\/SiC by a MoSi2\/Si Composite","volume":"14","author":"Gianchandani","year":"2017","journal-title":"Int. J. Appl. Ceram. Technol."},{"key":"ref_5","doi-asserted-by":"crossref","first-page":"5557","DOI":"10.1016\/j.ceramint.2021.11.100","article-title":"Understanding the Machining Characteristic of Plain Weave Ceramic Matrix Composite in Ultrasonic-Assisted Grinding","volume":"48","author":"Zhang","year":"2022","journal-title":"Ceram. Int."},{"key":"ref_6","doi-asserted-by":"crossref","first-page":"1900269","DOI":"10.1002\/adem.201900269","article-title":"Polymer-Derived Ultra-High Temperature Ceramics (UHTCs) and Related Materials","volume":"21","author":"Ionescu","year":"2019","journal-title":"Adv. Eng. Mater."},{"key":"ref_7","doi-asserted-by":"crossref","first-page":"263","DOI":"10.1111\/j.1744-7402.2009.02424.x","article-title":"Single- and Multilayered Interphases in SiC\/SiC Composites Exposed to Severe Environmental Conditions: An Overview","volume":"7","author":"Naslain","year":"2010","journal-title":"Int. J. Appl. Ceram. Technol."},{"key":"ref_8","doi-asserted-by":"crossref","first-page":"905","DOI":"10.1016\/S0008-6223(01)00225-1","article-title":"Thermal Shock Behavior of 3-Dimensional C\/SiC Composite","volume":"40","author":"Yin","year":"2002","journal-title":"Carbon"},{"key":"ref_9","doi-asserted-by":"crossref","first-page":"1805","DOI":"10.1111\/j.1551-2916.2010.03876.x","article-title":"Polymer-Derived Ceramics: 40 Years of Research and Innovation in Advanced Ceramics","volume":"93","author":"Colombo","year":"2010","journal-title":"J. Am. Ceram. Soc."},{"key":"ref_10","first-page":"499","article-title":"Ceramic Composite Interfaces: Properties and Design","volume":"27","author":"Faber","year":"1997","journal-title":"Annu. Rev. Mater. Res."},{"key":"ref_11","doi-asserted-by":"crossref","first-page":"3857","DOI":"10.1007\/BF00355946","article-title":"The Physics and Mechanics of Fibre-Reinforced Brittle Matrix Composites","volume":"29","author":"Evans","year":"1994","journal-title":"J. Mater. Sci."},{"key":"ref_12","doi-asserted-by":"crossref","unstructured":"Pask, J.A., and Evans, A.G. (1987). Interfacial Chemistry and Bonding in Fiber Reinforced Glass and Glass-Ceramic Matrix Composites. Ceramic Microstructures \u201986: Role of Interfaces, Springer.","DOI":"10.1007\/978-1-4613-1933-7"},{"key":"ref_13","doi-asserted-by":"crossref","first-page":"179","DOI":"10.1016\/j.jeurceramsoc.2013.08.027","article-title":"Influence of Surface Fibre Properties and Textural Organization of a Pyrocarbon Interphase on the Interfacial Shear Stress of SiC\/SiC Minicomposites Reinforced with Hi-Nicalon S and Tyranno SA3 Fibres","volume":"34","author":"Buet","year":"2014","journal-title":"J. Eur. Ceram. Soc."},{"key":"ref_14","doi-asserted-by":"crossref","first-page":"012030","DOI":"10.1088\/1757-899X\/213\/1\/012030","article-title":"Prediction of Elastic Properties of Pyrolytic Carbon Based on Orientation Angle","volume":"213","author":"Song","year":"2017","journal-title":"IOP Conf. Ser. Mater. Sci. Eng."},{"key":"ref_15","doi-asserted-by":"crossref","first-page":"288","DOI":"10.1016\/j.carbon.2013.01.076","article-title":"The Effect of Heat Treatment on the Strength and Toughness of Carbon Fiber\/Silicon Carbide Composites with Different Pyrolytic Carbon Interphase Thicknesses","volume":"57","author":"Mei","year":"2013","journal-title":"Carbon"},{"key":"ref_16","doi-asserted-by":"crossref","first-page":"16282","DOI":"10.1016\/j.ceramint.2021.02.207","article-title":"Influence of Pyrolytic Carbon Interphase and Pyrolysis Temperature on the Mechanical and Tribological Properties of Cf\/SiC after Heat Treatment at 1800 \u00b0C","volume":"47","author":"Zhang","year":"2021","journal-title":"Ceram. Int."},{"key":"ref_17","doi-asserted-by":"crossref","first-page":"2171","DOI":"10.1111\/jace.18193","article-title":"Effect of Pyrocarbon Interphase Texture and Thickness on Tensile Damage and Fracture in T-700TM Carbon Fiber-Reinforced Silicon Carbide Minicomposites","volume":"105","author":"Duan","year":"2022","journal-title":"J. Am. Ceram. Soc."},{"key":"ref_18","doi-asserted-by":"crossref","first-page":"766","DOI":"10.1016\/j.combustflame.2012.12.007","article-title":"Comparison of Thermal and Catalytic Cracking of 1-Heptene from ReaxFF Reactive Molecular Dynamics Simulations","volume":"160","year":"2013","journal-title":"Combust. Flame"},{"key":"ref_19","doi-asserted-by":"crossref","first-page":"107","DOI":"10.1016\/j.fuproc.2017.03.016","article-title":"ReaxFF Molecular Dynamics Simulation of Pyrolysis and Combustion of Pyridine","volume":"161","author":"Liu","year":"2017","journal-title":"Fuel Process. Technol."},{"key":"ref_20","doi-asserted-by":"crossref","first-page":"3971","DOI":"10.1021\/acs.jpca.8b01256","article-title":"Thermal Decomposition Mechanism of CL-20 at Different Temperatures by ReaxFF Reactive Molecular Dynamics Simulations","volume":"122","author":"Wang","year":"2018","journal-title":"J. Phys. Chem. A"},{"key":"ref_21","doi-asserted-by":"crossref","first-page":"106147","DOI":"10.1016\/j.fuproc.2019.106147","article-title":"ReaxFF-Based Molecular Dynamics Simulation of the Initial Pyrolysis Mechanism of Lignite","volume":"195","author":"Xu","year":"2019","journal-title":"Fuel Process. Technol."},{"key":"ref_22","doi-asserted-by":"crossref","first-page":"109534","DOI":"10.1016\/j.polymdegradstab.2021.109534","article-title":"In-Depth Understanding on the Early Stage of Phenolic Resin Thermal Pyrolysis through ReaxFF-Molecular Dynamics Simulation","volume":"186","author":"Xing","year":"2021","journal-title":"Polym. Degrad. Stab."},{"key":"ref_23","doi-asserted-by":"crossref","first-page":"3308","DOI":"10.1021\/jp3078002","article-title":"Toward a Process-Based Molecular Model of SiC Membranes. 1. Development of a Reactive Force Field","volume":"117","author":"Naserifar","year":"2013","journal-title":"J. Phys. Chem. C"},{"key":"ref_24","doi-asserted-by":"crossref","first-page":"3320","DOI":"10.1021\/jp307799p","article-title":"Toward a Process-Based Molecular Model of SiC Membranes. 2. Reactive Dynamics Simulation of the Pyrolysis of Polymer Precursor to Form Amorphous SiC","volume":"117","author":"Naserifar","year":"2013","journal-title":"J. Phys. Chem. C"},{"key":"ref_25","doi-asserted-by":"crossref","first-page":"5767","DOI":"10.1021\/acs.jpcc.7b12287","article-title":"Reactive Dynamics Simulation Study on the Pyrolysis of Polymer Precursors to Generate Amorphous Silicon Oxycarbide Structures","volume":"122","author":"Gao","year":"2018","journal-title":"J. Phys. Chem. C"},{"key":"ref_26","doi-asserted-by":"crossref","unstructured":"Lu, K., and Chaney, H. (2025). Understanding Polysiloxane Polymer to Amorphous SiOC Conversion During Pyrolysis Through ReaxFF Simulation. Materials, 18.","DOI":"10.3390\/ma18071412"},{"key":"ref_27","doi-asserted-by":"crossref","first-page":"1645","DOI":"10.1021\/acs.jpcc.5c05359","article-title":"Atomistic-Scale Simulations of the High-Temperature Chemistry of Si\/C\/O\/H-Based Polymers and Their Conversion to Si\/C Solid Materials","volume":"130","author":"Hosna","year":"2026","journal-title":"J. Phys. Chem. C"},{"key":"ref_28","doi-asserted-by":"crossref","unstructured":"Li, Y., Hou, D., Chen, C., Jiang, J., Li, Y., Xu, C., and Zhang, Z. (2026). Fundamental Understanding of Carbon Evolution in Polycarbosilane Derived SiC Ceramics: A ReaxFF Molecular Dynamics Study. J. Mater. Chem. A.","DOI":"10.1039\/D5TA09086E"},{"key":"ref_29","doi-asserted-by":"crossref","first-page":"266","DOI":"10.1016\/j.commatsci.2017.02.006","article-title":"Tensile Mechanical Properties Study of SiC\/Graphene Composites Based on Molecular Dynamics","volume":"131","author":"Zhan","year":"2017","journal-title":"Comput. Mater. Sci."},{"key":"ref_30","doi-asserted-by":"crossref","unstructured":"Zhou, Y., Ye, T., Ma, L., Lu, Z., Yang, Z., and Liu, S. (2019). Investigation on Cf\/PyC Interfacial Properties of C\/C Composites by the Molecular Dynamics Simulation Method. Materials, 12.","DOI":"10.3390\/ma12040679"},{"key":"ref_31","doi-asserted-by":"crossref","first-page":"085008","DOI":"10.1088\/1361-651X\/ac2478","article-title":"Molecular Dynamics Simulation on PyC Interfacial Failure Mechanism and Shear Strength of SiC\/SiC Composites","volume":"29","author":"Niu","year":"2021","journal-title":"Model. Simul. Mater. Sci. Eng."},{"key":"ref_32","doi-asserted-by":"crossref","first-page":"107742","DOI":"10.1016\/j.compositesa.2023.107742","article-title":"Microstructure of PyC Dominates Interfacial Shear Failure in SiCf\/SiC Composites: From Localized Sliding to Uniform Plasticity","volume":"174","author":"Wang","year":"2023","journal-title":"Compos. Part Appl. Sci. Manuf."},{"key":"ref_33","doi-asserted-by":"crossref","unstructured":"Kil, T., Cho, Y., Bae, J.-H., Lee, J.E., Won, J.S., Lee, M.Y., and Lee, H.I. (2026). A Multiscale Modeling Approach for the Prediction of the Mechanical Properties of C\/SiC Composites Fabricated by the CVI Process. Materials, 19.","DOI":"10.3390\/ma19030623"},{"key":"ref_34","doi-asserted-by":"crossref","first-page":"110445","DOI":"10.1016\/j.engfracmech.2024.110445","article-title":"Exploring the Toughening Mechanisms of PyC Interphase in SiCf\/SiC Composites through Molecular Dynamics and Mesoscale Stochastic Simulations","volume":"310","author":"Wang","year":"2024","journal-title":"Eng. Fract. Mech."},{"key":"ref_35","doi-asserted-by":"crossref","first-page":"111530","DOI":"10.1016\/j.engfracmech.2025.111530","article-title":"Trans-Scale Temperature-Dependent Cohesive Zone Model for C\/PyC\/SiC Interface","volume":"329","author":"Shang","year":"2025","journal-title":"Eng. Fract. Mech."},{"key":"ref_36","doi-asserted-by":"crossref","first-page":"9396","DOI":"10.1021\/jp004368u","article-title":"ReaxFF:\u2009 A Reactive Force Field for Hydrocarbons","volume":"105","author":"Dasgupta","year":"2001","journal-title":"J. Phys. Chem. A"},{"key":"ref_37","doi-asserted-by":"crossref","first-page":"16111","DOI":"10.1021\/jp306391p","article-title":"Oxidation of Silicon Carbide by O2 and H2O: A ReaxFF Reactive Molecular Dynamics Study, Part I","volume":"116","author":"Newsome","year":"2012","journal-title":"J. Phys. Chem. C"},{"key":"ref_38","doi-asserted-by":"crossref","first-page":"549","DOI":"10.1016\/j.carbon.2019.12.096","article-title":"Micromechanical Properties of Pyrolytic Carbon with Interlayer Crosslink","volume":"159","author":"Chen","year":"2020","journal-title":"Carbon"},{"key":"ref_39","doi-asserted-by":"crossref","first-page":"055502","DOI":"10.1103\/PhysRevLett.89.055502","article-title":"Structural Relaxation of Amorphous Silicon Carbide","volume":"89","author":"Ishimaru","year":"2002","journal-title":"Phys. Rev. Lett."},{"key":"ref_40","doi-asserted-by":"crossref","unstructured":"Buet, E., Braun, J., and Sauder, C. (2022). Influence of Texture and Thickness of Pyrocarbon Coatings as Interphase on the Mechanical Behavior of Specific 2.5D SiC\/SiC Composites Reinforced with Hi-Nicalon S Fibers. Coatings, 12.","DOI":"10.3390\/coatings12050573"}],"container-title":["Polymers"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/www.mdpi.com\/2073-4360\/18\/6\/702\/pdf","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2026,3,15]],"date-time":"2026-03-15T05:29:14Z","timestamp":1773552554000},"score":1,"resource":{"primary":{"URL":"https:\/\/www.mdpi.com\/2073-4360\/18\/6\/702"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2026,3,13]]},"references-count":40,"journal-issue":{"issue":"6","published-online":{"date-parts":[[2026,3]]}},"alternative-id":["polym18060702"],"URL":"https:\/\/doi.org\/10.3390\/polym18060702","relation":{},"ISSN":["2073-4360"],"issn-type":[{"value":"2073-4360","type":"electronic"}],"subject":[],"published":{"date-parts":[[2026,3,13]]}}}