利用化学浸渍法将蔗糖负载到SBA-15介孔材料孔道内部,高温炭化形成的多聚苯环经发烟硫酸气相磺化处理后,得到磺酸基团功能化的新型碳-硅介孔复合材料.发烟硫酸气相磺化处理是该材料合成的关键步骤.X射线衍射、扫描电镜和氮气吸附结果表明,碳-硅介孔复合材料经磺酸化处理保持了高度有序的介孔结构.热重、傅里叶变换的红外光谱及吡啶吸附红外光谱结果证明,磺酸功能基团成功的嫁接于碳-硅介孔复合材料孔道的内表面,反应活性中心为Brφnsted酸,酸密度在0.09~0.70mmol/g可以有效调变.当碳负载量为35%时,该复合材料在生物柴油的绿色合成中显示出最优的催化性能,且可重复使用3次以上.
A carbon-mesoporous silica (CS) composite functionalized with sulfonic acid (-SO3H) groups was prepared by controlled carbonization of sucrose impregnated in SBA-15 mesoporous silica and its subsequent sulfonation.The moderate vapor phase sulfonation of the CS composite with fuming sulfuric acid (H2SO4·20%SO3) was the key step in preparing the strong acid solid material (CS-SO3H).Structural analysis and reaction data revealed that sulfonic acid groups were successfully incorporated into the mesoporous CS composite,and the Brφnsted acid site density was tunable from 0.09 to 0.70 mmol/g by tuning the carbon loading.The sample with 35 wt% carbon exhibited a remarkable catalytic activity for biodiesel production by the esterification of palmitic acid and the transesterification of soybean oil with methanol.
参考文献
[1] | Hara M .[J].Energy Environ Sci,2010,3:601. |
[2] | Yang P F;Kobayashi H;Fukuoka A .[J].催化学报,2011,32:716. |
[3] | Shibasaki-Kitakawa N;Honda H;Kuribayashi H;Toda T;Fukumura T;Yonemoto T .Biodiesel production using anionic ion-exchange resin as heterogeneous catalyst[J].Bioresource Technology: Biomass, Bioenergy, Biowastes, Conversion Technologies, Biotransformations, Production Technologies,2007(2):416-421. |
[4] | Serio M D;Tesser R;Dimiccoli M;Cammarota F Nastasi M Santacesaria E .[J].Journal of Molecular Catalysis A:Chemical,2005,239:111. |
[5] | Liu K S .[J].Journal of the American Oil Chemists'Society,1994,71:1179. |
[6] | Shu Q;Yang B;Yuan H;Qing S Zhu G .[J].Catalysis Communications,2007,8:2159. |
[7] | Nakagaki S;Bail A;Cristina dos Santos V;Rodrigues de Souza V H Vrubel H Nunes F S Ramos L P .[J].Applied Catalysis A:General,2008,351:267. |
[8] | Ghesti G F;Lemos de Macedo J;Parente V C I;Dias J A Dias S C L .[J].Applied Catalysis A:General,2008,355:139. |
[9] | Jacobson K;Gopinath R;Meher L C;Dalai A K .[J].Applied Catalysis B:Environmental,2008,85:86. |
[10] | Kresge C T;Leonowicz M E;Roth W J;Vartuli J C Beck J S .[J].Nature,1992,359:710. |
[11] | Zhao D;Feng J;Huo Q;Melosh N Fredrickson G H Chmelka B F Stucky G D .[J].Science,1998,279:548. |
[12] | Margolese D;Melero J A;Christiansen S C;Chmelka B F Stucky G D .[J].Chemistry of Materials,2000,12:2448. |
[13] | Shen J G C;Herman R G;Klier K .[J].Journal of Physical Chemistry B,2002,106:9975. |
[14] | Bossaert W D;De Vos D E;Van Rhijn W M;Bullen J Grobet P J Jacobs P A .[J].Journal of Catalysis,1999,182:156. |
[15] | Díaz I;Mohino F;Blasco T;Sastre E Pérez-Pariente J .[J].Microporous and Mesoporous Materials,2005,80:33. |
[16] | Toda M;Takagaki A;Okamura M;Kondo J N Hayashi S Domen K Hara M .[J].Nature,2005,438:178. |
[17] | Xing R;Liu N;Liu YM;Wu HW;Jiang YW;Chen L;He MY;Wu P .Novel solid acid catalysts: Sulfonic acid group-functionalized mesostructured polymers[J].Advanced functional materials,2007(14):2455-2461. |
[18] | Xing R;Liu Y M;Wang Y;Chen L Wu H H Jiang Y W He M Y Wu P .[J].Microporous and Mesoporous Materials,2007,105:41. |
[19] | Nakajima K;Okamura M;Kondo J N;Domen K Tatsumi T Hayashi S Hara M .[J].Chemistry of Materials,2009,21:186. |
[20] | Suganuma S;Nakajima K;Kitano M;Kato H Tamura A Kondo H Yanagawa S Hayashi S Hara M .[J].Microporous and Mesoporous Materials,2011,143:443. |
[21] | Ryoo R;Joo S H;Jun S .[J].Journal of Physical Chemistry B,1999,103:7743. |
[22] | Van Der Voort P;Ravikovitch P I;De Jong K P;Neimark A V,Janssen A H,Benjelloun M,Van Bavel E,Cool P,Weckhuysen B M,Vansant E F.[J].Chemical Communications,2002:1010. |
[23] | Wang, Y.;Liu, Y.;Li, X.;Wu, H.;He, M.;Wu, P. .Intermolecular condensation of ethylenediamine to 1,4-diazabicyclo[2,2,2]octane over TS-1 catalysts[J].Journal of Catalysis,2009(2):258-267. |
[24] | Furuta S;Matsuhashi H;Arata K .[J].Catalysis Communications,2004,5:721. |
[25] | Zong M H;Duan Z Q;Lou W Y;Smith T J Wu H .[J].Green Chemistry,2007,9:434. |
- 下载量()
- 访问量()
- 您的评分:
-
10%
-
20%
-
30%
-
40%
-
50%