A New Fluorinated Polysiloxane with Good Optical Properties and Low Dielectric Constant at High Frequency Based on Easily Available Tetraethoxysilane (TEOS)
A novel fluorinated macromonomer (TFVE-Si) with four functional groups derived from easily available tetraethoxysilane (TEOS) has been successfully synthesized through the Piers–Rubinsztajn reaction using B(C6F5)3 as a catalyst. This procedure efficiently avoids the generation of Si–OH and −Si–CH2–...
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Veröffentlicht in: | Macromolecules 2017-12, Vol.50 (23), p.9394-9402 |
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description | A novel fluorinated macromonomer (TFVE-Si) with four functional groups derived from easily available tetraethoxysilane (TEOS) has been successfully synthesized through the Piers–Rubinsztajn reaction using B(C6F5)3 as a catalyst. This procedure efficiently avoids the generation of Si–OH and −Si–CH2–CH2– groups, which greatly affect the properties of the organosiloxanes. Prepolymerizing the macromonomer in mesitylene solution gives an oligomer which can form a flexible and highly transparent free-standing cross-linked polysiloxane film followed by a postpolymerization procedure at high temperature. The cross-linked polysiloxane (thickness = 2 mm) shows a transmittance of higher than 91% in the visible region and an absorbance of near 100% in the UV region (3.0). Moreover, D–E loop tests illustrate that the cross-linked polysiloxane possesses excellent linear dielectric properties, further suggesting its good insulating properties. Furthermore, the prepared polysiloxane exhibits high thermostability with a 5 wt % loss temperature of 476 °C and a glass transition temperature (T g) of 110 °C as well as good mechanical strength (with an elastic modulus of 1.1 GPa). Because of the existence of fluoro-containing groups, the polysiloxane also shows high hydrophobicity. Furthermore, TFVE-Si can efficiently improve the T g of linear polysiloxane prepared from dimethylsiloxane with two functional groups. These indicate that the fluorinated TEOS has potential application in the microelectronics industry; especially, it can meet the requirement of the high-frequency communication fields for the materials with both low D k and D f . |
doi_str_mv | 10.1021/acs.macromol.7b02000 |
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This procedure efficiently avoids the generation of Si–OH and −Si–CH2–CH2– groups, which greatly affect the properties of the organosiloxanes. Prepolymerizing the macromonomer in mesitylene solution gives an oligomer which can form a flexible and highly transparent free-standing cross-linked polysiloxane film followed by a postpolymerization procedure at high temperature. The cross-linked polysiloxane (thickness = 2 mm) shows a transmittance of higher than 91% in the visible region and an absorbance of near 100% in the UV region (<350 nm), exhibiting its potential application as a transparent coating for blocking ultraviolet rays in both household and industrial uses. In particular, the cross-linked film shows low dielectric constant (D k ) of 2.50 and low dissipation factor (D f ) of 4.0 × 10–3 at an ultrahigh frequency of 10 GHz. This is the first example of nonporous polysiloxane having both low D k and D f while conventional TEOS-based polymers exhibit higher D k (>3.0). Moreover, D–E loop tests illustrate that the cross-linked polysiloxane possesses excellent linear dielectric properties, further suggesting its good insulating properties. Furthermore, the prepared polysiloxane exhibits high thermostability with a 5 wt % loss temperature of 476 °C and a glass transition temperature (T g) of 110 °C as well as good mechanical strength (with an elastic modulus of 1.1 GPa). Because of the existence of fluoro-containing groups, the polysiloxane also shows high hydrophobicity. Furthermore, TFVE-Si can efficiently improve the T g of linear polysiloxane prepared from dimethylsiloxane with two functional groups. These indicate that the fluorinated TEOS has potential application in the microelectronics industry; especially, it can meet the requirement of the high-frequency communication fields for the materials with both low D k and D f .</description><identifier>ISSN: 0024-9297</identifier><identifier>EISSN: 1520-5835</identifier><identifier>DOI: 10.1021/acs.macromol.7b02000</identifier><language>eng</language><publisher>American Chemical Society</publisher><ispartof>Macromolecules, 2017-12, Vol.50 (23), p.9394-9402</ispartof><rights>Copyright © 2017 American Chemical Society</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a292t-6057ed73865dd01f04d25d70f1aa613bc75b79f02134ce9de70e89746eb98c113</citedby><cites>FETCH-LOGICAL-a292t-6057ed73865dd01f04d25d70f1aa613bc75b79f02134ce9de70e89746eb98c113</cites><orcidid>0000-0002-3549-5600 ; 0000-0002-1714-0283</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://pubs.acs.org/doi/pdf/10.1021/acs.macromol.7b02000$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/acs.macromol.7b02000$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>314,780,784,2765,27076,27924,27925,56738,56788</link.rule.ids></links><search><creatorcontrib>Wang, Jiajia</creatorcontrib><creatorcontrib>Zhou, Junfeng</creatorcontrib><creatorcontrib>Jin, Kaikai</creatorcontrib><creatorcontrib>Wang, Liang</creatorcontrib><creatorcontrib>Sun, Jing</creatorcontrib><creatorcontrib>Fang, Qiang</creatorcontrib><title>A New Fluorinated Polysiloxane with Good Optical Properties and Low Dielectric Constant at High Frequency Based on Easily Available Tetraethoxysilane (TEOS)</title><title>Macromolecules</title><addtitle>Macromolecules</addtitle><description>A novel fluorinated macromonomer (TFVE-Si) with four functional groups derived from easily available tetraethoxysilane (TEOS) has been successfully synthesized through the Piers–Rubinsztajn reaction using B(C6F5)3 as a catalyst. This procedure efficiently avoids the generation of Si–OH and −Si–CH2–CH2– groups, which greatly affect the properties of the organosiloxanes. Prepolymerizing the macromonomer in mesitylene solution gives an oligomer which can form a flexible and highly transparent free-standing cross-linked polysiloxane film followed by a postpolymerization procedure at high temperature. The cross-linked polysiloxane (thickness = 2 mm) shows a transmittance of higher than 91% in the visible region and an absorbance of near 100% in the UV region (<350 nm), exhibiting its potential application as a transparent coating for blocking ultraviolet rays in both household and industrial uses. In particular, the cross-linked film shows low dielectric constant (D k ) of 2.50 and low dissipation factor (D f ) of 4.0 × 10–3 at an ultrahigh frequency of 10 GHz. This is the first example of nonporous polysiloxane having both low D k and D f while conventional TEOS-based polymers exhibit higher D k (>3.0). Moreover, D–E loop tests illustrate that the cross-linked polysiloxane possesses excellent linear dielectric properties, further suggesting its good insulating properties. Furthermore, the prepared polysiloxane exhibits high thermostability with a 5 wt % loss temperature of 476 °C and a glass transition temperature (T g) of 110 °C as well as good mechanical strength (with an elastic modulus of 1.1 GPa). Because of the existence of fluoro-containing groups, the polysiloxane also shows high hydrophobicity. Furthermore, TFVE-Si can efficiently improve the T g of linear polysiloxane prepared from dimethylsiloxane with two functional groups. These indicate that the fluorinated TEOS has potential application in the microelectronics industry; especially, it can meet the requirement of the high-frequency communication fields for the materials with both low D k and D f .</description><issn>0024-9297</issn><issn>1520-5835</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2017</creationdate><recordtype>article</recordtype><recordid>eNp9kM1uGjEUha2qkUqTvkEXd9kshlzPD2aWhEJSCZVIpevRHftOcWTG1DYhvEseNoOSbru6i6PznatPiK8SxxJzeUM6jnekg995N1Yt5oj4QYxklWNWTYvqoxgh5mVW57X6JD7H-IgoZVUWI_Eyg598hKU7-GB7SmzgwbtTtM4_U89wtGkLd94bWO-T1eTgIfg9h2Q5AvUGVv4I3y071ilYDXPfx0R9Akpwb_9sYRn474F7fYJbigPd97CgAX-C2RNZR61j2HAKxGnrn8_D59lvm8X61_WVuOjIRf7yfi_F7-ViM7_PVuu7H_PZKqO8zlM2wUqxUcV0UhmDssPS5JVR2EmiiSxarapW1d1gqig114YV8rRW5YTbeqqlLC5F-cYdFMYYuGv2we4onBqJzdlwMxhu_hlu3g0PNXyrndNHfwj98OT_K6_ZwYU-</recordid><startdate>20171212</startdate><enddate>20171212</enddate><creator>Wang, Jiajia</creator><creator>Zhou, Junfeng</creator><creator>Jin, Kaikai</creator><creator>Wang, Liang</creator><creator>Sun, Jing</creator><creator>Fang, Qiang</creator><general>American Chemical Society</general><scope>AAYXX</scope><scope>CITATION</scope><orcidid>https://orcid.org/0000-0002-3549-5600</orcidid><orcidid>https://orcid.org/0000-0002-1714-0283</orcidid></search><sort><creationdate>20171212</creationdate><title>A New Fluorinated Polysiloxane with Good Optical Properties and Low Dielectric Constant at High Frequency Based on Easily Available Tetraethoxysilane (TEOS)</title><author>Wang, Jiajia ; Zhou, Junfeng ; Jin, Kaikai ; Wang, Liang ; Sun, Jing ; Fang, Qiang</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a292t-6057ed73865dd01f04d25d70f1aa613bc75b79f02134ce9de70e89746eb98c113</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2017</creationdate><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Wang, Jiajia</creatorcontrib><creatorcontrib>Zhou, Junfeng</creatorcontrib><creatorcontrib>Jin, Kaikai</creatorcontrib><creatorcontrib>Wang, Liang</creatorcontrib><creatorcontrib>Sun, Jing</creatorcontrib><creatorcontrib>Fang, Qiang</creatorcontrib><collection>CrossRef</collection><jtitle>Macromolecules</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Wang, Jiajia</au><au>Zhou, Junfeng</au><au>Jin, Kaikai</au><au>Wang, Liang</au><au>Sun, Jing</au><au>Fang, Qiang</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>A New Fluorinated Polysiloxane with Good Optical Properties and Low Dielectric Constant at High Frequency Based on Easily Available Tetraethoxysilane (TEOS)</atitle><jtitle>Macromolecules</jtitle><addtitle>Macromolecules</addtitle><date>2017-12-12</date><risdate>2017</risdate><volume>50</volume><issue>23</issue><spage>9394</spage><epage>9402</epage><pages>9394-9402</pages><issn>0024-9297</issn><eissn>1520-5835</eissn><abstract>A novel fluorinated macromonomer (TFVE-Si) with four functional groups derived from easily available tetraethoxysilane (TEOS) has been successfully synthesized through the Piers–Rubinsztajn reaction using B(C6F5)3 as a catalyst. This procedure efficiently avoids the generation of Si–OH and −Si–CH2–CH2– groups, which greatly affect the properties of the organosiloxanes. Prepolymerizing the macromonomer in mesitylene solution gives an oligomer which can form a flexible and highly transparent free-standing cross-linked polysiloxane film followed by a postpolymerization procedure at high temperature. The cross-linked polysiloxane (thickness = 2 mm) shows a transmittance of higher than 91% in the visible region and an absorbance of near 100% in the UV region (<350 nm), exhibiting its potential application as a transparent coating for blocking ultraviolet rays in both household and industrial uses. In particular, the cross-linked film shows low dielectric constant (D k ) of 2.50 and low dissipation factor (D f ) of 4.0 × 10–3 at an ultrahigh frequency of 10 GHz. This is the first example of nonporous polysiloxane having both low D k and D f while conventional TEOS-based polymers exhibit higher D k (>3.0). Moreover, D–E loop tests illustrate that the cross-linked polysiloxane possesses excellent linear dielectric properties, further suggesting its good insulating properties. Furthermore, the prepared polysiloxane exhibits high thermostability with a 5 wt % loss temperature of 476 °C and a glass transition temperature (T g) of 110 °C as well as good mechanical strength (with an elastic modulus of 1.1 GPa). Because of the existence of fluoro-containing groups, the polysiloxane also shows high hydrophobicity. Furthermore, TFVE-Si can efficiently improve the T g of linear polysiloxane prepared from dimethylsiloxane with two functional groups. These indicate that the fluorinated TEOS has potential application in the microelectronics industry; especially, it can meet the requirement of the high-frequency communication fields for the materials with both low D k and D f .</abstract><pub>American Chemical Society</pub><doi>10.1021/acs.macromol.7b02000</doi><tpages>9</tpages><orcidid>https://orcid.org/0000-0002-3549-5600</orcidid><orcidid>https://orcid.org/0000-0002-1714-0283</orcidid></addata></record> |
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title | A New Fluorinated Polysiloxane with Good Optical Properties and Low Dielectric Constant at High Frequency Based on Easily Available Tetraethoxysilane (TEOS) |
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