Pd/Ni-MCM-41制备及其对苯甲醛加氢的催化性能
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摘要
以十六烷基三甲基溴化铵为模板剂,正硅酸乙酯为硅源,MCM-41为载体,碱性条件下,合成Pd/Ni-MCM-41。通过XRD、HR-TEM、FT-IR和BET等对Pd/Ni-MCM-41进行表征。Pd/Ni-MCM-41的比表面积为(444.32～621.69) m~2·g(-1),孔容为(0.54～0.69) cm~3·g~(-1),孔径分布均匀,主要集中在(2～4) nm。将Pd/Ni-MCM-41用于苯甲醛加氢制备苯甲醇反应中,Ni质量分数6%时,在反应温度100℃和反应压力0.20 MPa条件下反应2 h,苯甲醛转化率65.1%,苯甲醇选择性为100%。
Pd/Ni-MCM-41 was synthesized under alkaline conditions with cetyltrimethylammonium bromide as template,ethyl orthosilicate as silicon source and MCM-41 as carrier,and characterized by XRD,HR-TEM,FT-IR,BET and so on.Results showed that specific surface area of Pd/Ni-MCM-41 was(444.32-621.69) m~2·g~(-1),pore volume was(0.54-0.69) cm~3·g~(-1),and pore size was(2-4) nm.When Pd/Ni-MCM-41 with Ni mass fraction of 6% was used in hydrogenation of benzaldehyde to benzyl alcohol,conversion of benzaldehyde was 65.1% and selectivity was 100% in 2 h under 100 ℃ and 0.20 MPa.
Pd/Ni-MCM-41 was synthesized under alkaline conditions with cetyltrimethylammonium bromide as template,ethyl orthosilicate as silicon source and MCM-41 as carrier,and characterized by XRD,HR-TEM,FT-IR,BET and so on.Results showed that specific surface area of Pd/Ni-MCM-41 was(444.32-621.69) m~2·g~(-1),pore volume was(0.54-0.69) cm~3·g~(-1),and pore size was(2-4) nm.When Pd/Ni-MCM-41 with Ni mass fraction of 6% was used in hydrogenation of benzaldehyde to benzyl alcohol,conversion of benzaldehyde was 65.1% and selectivity was 100% in 2 h under 100 ℃ and 0.20 MPa.
引文
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[2]李金志.相转移催化水解法制备苯甲醇的研究[J].化工矿物与加工,2000,29(12):8-9.Li Jinzhi. Study on benzene methanol preparation with phase transfer hydrolysis catalytic method[J]. Industrial Minerals&Processing,2000,29(12):8-9.
[3]邓莹,袁佩,袁霞,等.疏水性Cosalen/SBA-15的制备及在甲苯选择性氧化中的应用[J].高等学校化学学报,2013,34(11):2617-2622.Deng Ying,Yuan Pei,Yuan Xia,et al. Preparation of hydrophobic Cosalen/SBA-15 and its application in the selective oxidation of toluene[J]. Chemical Journal of Chinese Universities,2013,34(11):2617-2622.
[4]冯秋菊,李峰,肖永来,等.离子液体BMIMBF4溶液中电化学还原苯甲醛合成苯甲醇[J].吉首大学学报(自然科学版),2016,37(2):47-50.Feng Qiuju,Li Feng,Xiao Yonglai,et al. Electrochemical reduction of benzaldehyde to phenylmethanol in ionic liquid BMIMBF4[J]. Journal of Jishou University(Natural Science Edition),2016,37(2):47-50.
[5]Yan F,Zhao C,Yi L,et al. Effect of the degree of dispersion of Pt over MgAl2O4on the catalytic hydrogenation of benzaldehyde[J]. Chinese Journal of Catalysis,2017,38(9):1613-1620.
[6]钟春龙,梅乐和,胡方敏,等.有机介质中固定化面包酵母催化苯甲醛加氢反应[J].功能材料,2007,38(8):1342-1344.Zhong Chunlong,Mei Lehe,Hu Fanmin,et al. Studies on catalytic hydrogenation of benzaldehyde with immobilized baker's yeast in organic solvents[J]. Journal of Functional Materials,2007,38(8):1342-1344.
[7]吴鑫干,李陵岚.苯甲醇制造方法[J].工业催化,2002,10(2):26-32.Wu Xingan,Li Linlan. Process and catalysts for manufacture of benzyl alcohol[J]. Industrial Catalysis,2002,10(2):26-32.
[8]邱显清,朱起明,Fischer W.等.离子束技术改性苯甲醛加氢反应Pd/Al2O3催化剂[J].自然科学进展,1998,8(5):545-549.
[9]鄢峰,赵才贤,易兰花,等. Pt在MgAl2O4载体上的分散程度对催化苯甲醛加氢反应影响[J].催化学报,2017,38(9):1613-1620.Yan Feng,Zhao Caixian,Yi Lanhua,et al. Effect of the degree of dispersion of Pt over MgAl2O4on the catalytic hydrogenation of benzaldehyde[J]. Chinese Journal of Catalysis,2017,38(9):1613-1620.
[10]Haddad N,Saadi A,L9fberg A,et al. Benzaldehyde reduction over Cu-Al-O bimetallic oxide catalyst. Influence of p H during hydrothermal synthesis on the structural and catalytic properties[J]. Journal of Molecular Catalysis A:Chemical,2015,396:207-215.
[11]Agrawal A,Habibi H R,Agrawal R K,et al. Effect of deposition pressure on the microstructure and electrochromic properties of electron-beam-evaporated nickel oxide films[J]. Thin Solid Films,1992,221(1/2):239-253.
[12]吴乃瑾.过渡金属在介孔分子筛中的高度分散及催化性能研究[D].北京:北京化工大学,2015.
[13]张燕,李湘祁,汤德平.微波法合成有序介孔分子筛的研究进展[J].化工时刊,2007,21(11):71-75.Zhang Yan,Li Xiangqi,Tang Deping. Advances in the microwave synthesis of ordered mesoporous material[J].Chemical Industry Times,2007,21(11):71-75.
[14]Yang S L,Yao H B,Gao M R,et al. Monodisperse cubic pyrite Ni S2 dodecahedrons and microspheres synthesized by a solvothermal process in a mixed solvent:thermal stability and magnetic properties[J]. Crystengcomm,2009,11(7):1383-1390.
[15]Stefanis A D,Kaciulis S,Pandolfi L. Preparation and characterization of Fe-MCM-41 catalysts employed in the degradation of plastic materials[J]. Microporous&Mesoporous Materials,2007,99(1):140-148.
[16]Bhosale R,Kelkar S,Parte G,et al. Ni S1. 97:a new efficient water oxidation catalyst for photoelectrochemical hydrogen generation[J]. Acs Applied Materials&Interfaces,2015,7(36):20053-20060.