欢迎登录材料期刊网

材料期刊网

高级检索

Inexpensive γ-alumina-based nickel-copper bimetallic catalysts were studied for the hydrogenolysis of levulinic acid, a key platform molecule for biomass conversion to biofuels and other valued chemicals, into γ-valerolactone as a first step towards the production of 2-methyltetrahydrofurane. The activities of both monometallic and bimetallic catalysts were tested. Their textural and chemical characteristics were determined by nitrogen physisorption, elemental analysis, temperature-pro-grammed ammonia desorption, and temperature-programmed reduction. The monometallic nickel catalyst showed high activity but the highest by-product production and significant amounts of carbon deposited on the catalyst surface. The copper monometallic catalyst showed the lowest activity but the lowest carbon deposition. The incorporation of the two metals generated a bimetal-lic catalyst that displayed a similar activity to that of the Ni monometallic catalyst and significantly low by-product and carbon contents, indicating the occurrence of important synergetic effects. The influence of the preparation method was also examined by studying impregnated- and sol-gel-derived bimetallic catalysts. A strong dependency on the preparation procedure and calcina-tion temperature was observed. The highest activity per metal atom was achieved using the sol-gel-derived catalyst that was calcined at 450 °C. High reaction rates were achieved;the total levulinic acid conversion was obtained in less than 2 h of reaction time, yielding up to 96%γ-valerolactone, at operating temperature and pressure of 250 °C and 6.5 MPa hydrogen, respec-tively.

参考文献

[1] Serrano-Ruiz J C;Dumesic J A .[J].Energy Environ Sci,2011,4:83.
[2] British Petroleum.BP Statistical Review of World Energy June 2013[M].London:BP,2013
[3] Sorrell S;Speirs J;Bentley R;Brandt A,Miller R.Global Oil Deple-tion,An Assessment of the Evidence for a Near-Term Peak in Global Oil Production[M].London:UK ENERGY RESEARCH CENTRE,2009
[4] IPCC .Climate Change 2001:The Scientific Basis.Contribu-tion of Working Group I to the Third Assessment Report of the In-tergovernmental Panel on Climate Change[R].Cambridge:Cambridge University Press,2001.
[5] Alonso D M;Bond J Q;Dumesic J A .[J].Green Chemistry,2010,12:1493.
[6] Hayes D J .[J].Catalysis Today,2009,145:138.
[7] Mascal M;Nikitin E B .[J].Green Chemistry,2010,12:370.
[8] Mascal M;Nikitin E B .[J].ChemSusChem,2009,2:859.
[9] Hayes D J;Fitzpatrick S W;Hayes M H B;Ross J R H.:Kamm B,Gruber P R eds.Biorefineries-Industrial Processes and Products[M].Weinheim:Wiley-VCH Verlag GmbH,2006:139.
[10] Bozell J J;Moens L;Elliott D C;Wang Y Neuenscwander G G Fitz-patrick S W Bilski R J Jarnefeld J L .[J].RESOURCES CONSERVATION AND RECYCLING,2000,28:227.
[11] Horváth I T;Mehdi H;Fabos V;Boda L Mika L T .[J].Green Chemistry,2008,10:238.
[12] Huber G W;Iborra S;Corma A .[J].CHEMICAL REVIEWS,2006,106:4044.
[13] Paul S F .[P].US Patent 6309430B1,2001.
[14] US Department of Energy.Federal Register ed.Alternative Fuel Transportation Programe;P-Series Fuels;Final Rule[M].Washington,NW:U.S.Government Printing Office,1999:26822.
[15] Elliott D C;Frye J G .[P].US Patent 5883266A,1999.
[16] Upare P P;Lee J M;Hwang Y K;Hwang D W Lee J H Halligudi S B Hwang J S Chang J S .[J].ChemSusChem,2011,4:1749.
[17] Manzer L E .[P].US Patent 6617464 B2,2003.
[18] Yan Z P;Lin L;Liu S J .[J].Energy and Fuels,2009,23:3853.
[19] Gong Y;Lin L;Yan Z P .[J].BioResources,2011,6:686.
[20] Al-Shaal M G;Wright W R H;Palkovits R .[J].Green Chemistry,2012,14:1260.
[21] Galletti A M R;Antonetti C;De Luise V;Martinelli M .[J].Green Chemistry,2012,14:688.
[22] Serrano-Ruiz J C;Braden D J;West R M;Dumesic J A .[J].Applied Catalysis B:Environmental,2010,100:184.
[23] Serrano-Ruiz J C;Wang D;Dumesic J A .[J].Green Chemistry,2010,12:574.
[24] Ayoub P M;Lange J P .[P].WO Patent 2008142127A1,2008.
[25] Lange J P;Price R;Ayoub P M;Louis J Petrus L Clarke L Gosselink H .[J].ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2010,49:4479.
[26] Haan R J;Lange J P .[P].WO Patent 2011015645A2,2011.
[27] Du X L;He L;Zhao S;Liu Y M Cao Y He H Y Fan K N .[J].ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2011,50:7815.
[28] 杜贤龙,刘永梅,王建强,曹勇,范康年.碳纳米管担载纳米Ir催化生物质基乙酰丙酸合成γ-戊内酯[J].催化学报,2013(05):993-1001.
[29] Hengne A M;Rode C V .[J].Green Chemistry,2012,14:1064.
[30] Yan K;Liao J Y;Wu X;Xie X M .[J].RSC Adv,2013,3:3853.
[31] Gandarias, I.;Requies, J.;Arias, P.L.;Armbruster, U.;Martin, A..Liquid-phase glycerol hydrogenolysis by formic acid over Ni-Cu/Al _2O _3 catalysts[J].Journal of Catalysis,2012:79-89.
[32] Salagre P;Fierro J L G;Medina F;Sueiras J E .[J].Journal of Molecular Catalysis A:Chemical,1996,106:125.
[33] Priya G K;Padmaja P;Warrier K G K;Damodaran A D Aruldhas G .[J].Journal of Materials Science Letters,1997,16:1584.
[34] Ashok J;Subrahmanyam M;Venugopal A .[J].International Journal of Hydrogen Energy,2008,33:2704.
[35] Luo W H;Deka U;Beale A M;van Eck E R H Bruijnincx P C A Weckhuysen B M .[J].Journal of Catalysis,2013,301:175.
[36] El Doukkali M;Iriondo A;Arias P L;Cambra J F Gandarias I Barrio V L .[J].International Journal of Hydrogen Energy,2012,37:8298.
[37] Shamsi A;Baltrus J P;Spivey J J .[J].Applied Catalysis A:General,2005,293:145.
上一张 下一张
上一张 下一张
计量
  • 下载量()
  • 访问量()
文章评分
  • 您的评分:
  • 1
    0%
  • 2
    0%
  • 3
    0%
  • 4
    0%
  • 5
    0%