具有rGO三维导热网络结构聚酰亚胺复合薄膜的制备及性能
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摘要
为了使还原氧化石墨烯(rGO)的面内导热方向与复合物材料散热方向一致,提高rGO在复合材料中的导热效率,更大程度地释放rGO的导热潜力,采用冷冻干燥的方法处理rGO的聚酰胺酸(PAA)分散液,得到PAA黏结的rGO三维网络结构,热酰亚胺化之后得到聚酰亚胺(PI)加固的rGO三维网络结构模板(3DrGO-PI).使用10 wt%的PAA胶液浇铸上述3DrGO-PI模板,制备得到含有rGO三维导热网络结构的3DrGO/PI复合薄膜.结果表明,所得到的复合薄膜具有良好的导热性能,当rGO的含量为8 wt%时,3DrGO/PI复合薄膜导热系数达到1.57 W·m-1·K-1,为纯PI导热系数的8.72倍.同时复合薄膜具有较好的热稳定性,随着rGO含量的增加,薄膜的Tg上升,热膨胀系数(CTE)下降,热性能更稳定.
In this work, high thermal conductive polyimide(PI) composites with reduced graphene oxide(rGO)as filler were prepared. In order to improve the thermal conductivity of rGO in the PI composites, rGO should form heat conductive paths in PI matrix, and the in-plane direction of rGO should be consistent with the heat dissipation direction of composite materials. Therefore, three-dimensional rGO networks(3 DrGO) were prepared by freeze-drying technology to construct an effective thermal conductive path in PI matrix. In order to stabilize3 DrGO networks during the preparation process of PI composites, the 3 DrGO networks were adhered and reinforced by PI. The process includes:(1) the rGO dispersion containing 3 wt% polyamide acid(PAA) was freeze-dried to prepare the PAA-reinforced 3 DrGO network(3 DrGO-PAA);(2) the 3 DrGO-PAA was treated by thermal imidization to obtain the PI-reinforced 3 DrGO network(3 DrGO-PI);(3) 10 wt% PAA was cast onto the3 DrGO-PI template and imidized at 100, 200, and 350 °C for 1 h, respectively, at each temperature to obtain the3 DrGO-PI/PI composite films. The 3 DrGO-PI/PI composite film exhibits the thermal conductivity of1.57 W·m-1·K-1 with 8 wt% rGO(772% enhancement compared to that of neat PI film). Whereas the PI composite films with random distributed rGO(rGO/PI composite film) or unreinforced 3 DrGO(3 DrGO-water/PI composite film) only exhibit the thermal conductivity of 0.51 W·m-1·K-1(183% enhancement compared to that of neat PI film) or 1.02 W·m-1·K-1(467% enhancement compared to that of neat PI film), respectively. All the composite films maintain very good thermal stabilities. The Td5%(thermal decomposition temperature at 5 wt%weight loss) values of the composite films are higher than that at 540 °C. Compared with that of neat PI, the Tgs of the composite films are slightly enhanced and relatively higher(higher than 390 °C). The coefficient of thermal expansion(CTE) of the composite films can be greatly decreased by the addition of 3 DrGO. The CTE of 3 DrGOPI/PI composite film is as low as 2.16 × 10–5/°C when loading 8 wt% 3 DrGO.
In this work, high thermal conductive polyimide(PI) composites with reduced graphene oxide(rGO)as filler were prepared. In order to improve the thermal conductivity of rGO in the PI composites, rGO should form heat conductive paths in PI matrix, and the in-plane direction of rGO should be consistent with the heat dissipation direction of composite materials. Therefore, three-dimensional rGO networks(3 DrGO) were prepared by freeze-drying technology to construct an effective thermal conductive path in PI matrix. In order to stabilize3 DrGO networks during the preparation process of PI composites, the 3 DrGO networks were adhered and reinforced by PI. The process includes:(1) the rGO dispersion containing 3 wt% polyamide acid(PAA) was freeze-dried to prepare the PAA-reinforced 3 DrGO network(3 DrGO-PAA);(2) the 3 DrGO-PAA was treated by thermal imidization to obtain the PI-reinforced 3 DrGO network(3 DrGO-PI);(3) 10 wt% PAA was cast onto the3 DrGO-PI template and imidized at 100, 200, and 350 °C for 1 h, respectively, at each temperature to obtain the3 DrGO-PI/PI composite films. The 3 DrGO-PI/PI composite film exhibits the thermal conductivity of1.57 W·m-1·K-1 with 8 wt% rGO(772% enhancement compared to that of neat PI film). Whereas the PI composite films with random distributed rGO(rGO/PI composite film) or unreinforced 3 DrGO(3 DrGO-water/PI composite film) only exhibit the thermal conductivity of 0.51 W·m-1·K-1(183% enhancement compared to that of neat PI film) or 1.02 W·m-1·K-1(467% enhancement compared to that of neat PI film), respectively. All the composite films maintain very good thermal stabilities. The Td5%(thermal decomposition temperature at 5 wt%weight loss) values of the composite films are higher than that at 540 °C. Compared with that of neat PI, the Tgs of the composite films are slightly enhanced and relatively higher(higher than 390 °C). The coefficient of thermal expansion(CTE) of the composite films can be greatly decreased by the addition of 3 DrGO. The CTE of 3 DrGOPI/PI composite film is as low as 2.16 × 10–5/°C when loading 8 wt% 3 DrGO.
引文
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17 Sun R H,Yao H,Zhang H B,Li Y,Mai Y W,Yu Z Z.Compos Sci Technol,2016,137:16-23
18 Xia J W,Zhang G P,Deng L B,Yang H P,Sun R,Wong C P.RSC Adv,2015,5:19315-19320
19 Shahil K M F,Balandin A A.Nano Lett,2012,12:861-867
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21 Xie Dan(谢丹),Teng Chao(滕超),Jiang Lei(江雷).Acta Polymerica Sinica(高分子学报),2018,(11):1460-1466
22 Lian G,Tuan C C,Li L Y,Jiao S L,Wang Q L,Moon K S,Cui D L,Wong C P.Chem Mater,2016,28:6096-6104
23 Hummers J W S,Offeman R E.J Am Chem Soc,1958,80:1339
24 Wang J Y,Yang S Y,Huang Y L,Tien H W,Chin W K,Ma C C M.J Mater Chem,2011,21:13569-13575
25 Zhang Libin(张立斌),Wang Jinqing(王金清),Yang Shengrong(杨生荣),Kong Xiangzheng(孔祥正).Acta Polymerica Sinica(高分子学报),2014,(11):1472-1478
26 Dong X C,Chen J,Ma Y W,Wang J,Chan-Park M B,Liu X M,Wang L H,Huang W,Chen P.Chem Commun,2012,48:10660
27 McAllister M J,Li J L,Adamson D H.Chem Mater,2007,18:4396-4404
28 Li D,Mueller M B,Gilje S.Nat Nanotechnol,2008,2:101-105
29 Erickson K,Erni R,Lee Z.Adv Mater,2010,40:4467-4472
30 Gilje S,Han S,Wang M.Nano Lett,2007,11:3394-3398
31 Tung V C,Allen M J,Yang Y.Nat Nanotechnol,2009,1:25-29
32 Wei S Y,Yu Q X,Fan Z G,Liu S W,Chi Z G,Chen X D,Zhang Y,Xu J R.RSC Adv,2018,8:22169-22176
2 Lim H,Cho W J,Ha C S,Ando S,Kim Y K,Park C H,Lee K.Adv Mater,2002,14:1275-1279
3 Yang Tingting(杨婷婷),Zhou Zhuxin(周竹欣),Zhang Yi(张艺),Liu Siwei(刘四委),Chi Zhenguo(池振国),Xu Jiarui(许家瑞).Acta Polymerica Sinica(高分子学报),2017,(3):411-428
4 Zu Mengyi(祖梦祎),Ke Ying(柯颖),Qi Shengli(齐胜利),Yang Huichuan(杨汇川),Tian Guofeng(田国峰),Wu Dezhen(武德珍).Acta Polymerica Sinica(高分子学报),2018,(5):617-623
5 Prasher R.Phys Rev B,2008,77:075424
6 Derue L,Dautel O,Tournebize A,Drees M,Pan H,Berthumeyrie S,Pavageau B,Cloutet E,Chambon S,Hirsch L,Rivaton A,Hudhomme P,Facchetti A,Wantz G.Adv Mater,2014,26:5831-5838
7 Moore A L,Shi L.Mater Today,2014,17:163-174
8 Yan W,Zhang Y,Sun H W,Liu S W,Chi Z G,Chen X C,Xu J R.J Mater Chem A,2014,2:20958-20965
9 Xu L B,Chen G F,Wang W,Li L,Fang X Z.Composites Part A,2016,84:472-481
10 Ren P G,Hou S Y,Ren F,Zhang Z P,Sun Z F,Xu L.Composites Part A,2016,90:13-21
11 Han W F,Bai Y F,Liu S C,Ge C H,Wang L X,Ma Z Y,Yang Y X,Zhang X D.Composites Part A,2017,102:218-227
12 Kim K,Yoo M,Ahn K,Kim J.Ceram Int,2015,41:179-187
13 Kim K,Kim J.Composites Part B,2016,93:67-74
14 Yin L Y,Zhou X G,Yu J S,Wang H L,Ran C C.Composites Part A,2016,90:626-632
15 Ramdani N,Derradji M,Feng T T,Tong Z,Wang J,Mokhnache E O,Liu W B.Mater Lett,2015,155:34-37
16 Xu R J,Chen M Y,Zhang F,Huang X R,Luo X G,Lei C H,Lu S G,Zhang X Q.Compos Sci Technol,2016,133:111-118
17 Sun R H,Yao H,Zhang H B,Li Y,Mai Y W,Yu Z Z.Compos Sci Technol,2016,137:16-23
18 Xia J W,Zhang G P,Deng L B,Yang H P,Sun R,Wong C P.RSC Adv,2015,5:19315-19320
19 Shahil K M F,Balandin A A.Nano Lett,2012,12:861-867
20 Pop E,Varshney V,Roy A K.MRS Bull,2012,37:1273
21 Xie Dan(谢丹),Teng Chao(滕超),Jiang Lei(江雷).Acta Polymerica Sinica(高分子学报),2018,(11):1460-1466
22 Lian G,Tuan C C,Li L Y,Jiao S L,Wang Q L,Moon K S,Cui D L,Wong C P.Chem Mater,2016,28:6096-6104
23 Hummers J W S,Offeman R E.J Am Chem Soc,1958,80:1339
24 Wang J Y,Yang S Y,Huang Y L,Tien H W,Chin W K,Ma C C M.J Mater Chem,2011,21:13569-13575
25 Zhang Libin(张立斌),Wang Jinqing(王金清),Yang Shengrong(杨生荣),Kong Xiangzheng(孔祥正).Acta Polymerica Sinica(高分子学报),2014,(11):1472-1478
26 Dong X C,Chen J,Ma Y W,Wang J,Chan-Park M B,Liu X M,Wang L H,Huang W,Chen P.Chem Commun,2012,48:10660
27 McAllister M J,Li J L,Adamson D H.Chem Mater,2007,18:4396-4404
28 Li D,Mueller M B,Gilje S.Nat Nanotechnol,2008,2:101-105
29 Erickson K,Erni R,Lee Z.Adv Mater,2010,40:4467-4472
30 Gilje S,Han S,Wang M.Nano Lett,2007,11:3394-3398
31 Tung V C,Allen M J,Yang Y.Nat Nanotechnol,2009,1:25-29
32 Wei S Y,Yu Q X,Fan Z G,Liu S W,Chi Z G,Chen X D,Zhang Y,Xu J R.RSC Adv,2018,8:22169-22176