活性炭负载磷钨酸催化聚酰胺6水解反应的研究
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摘要
以活性炭为载体,磷钨酸(HPW)为活性组分,通过浸渍法制备活性炭负载磷钨酸(HPW/C)催化剂,研究其对聚酰胺6(PA6)水解反应的影响。通过FT-IR、XRD、BET、GCMS和UV等对催化剂和水解产物进行表征分析。结果表明,当HPW负载量小于55%时,能均匀分散在活性炭的表面和孔隙;固相剩余物为未完全分解的PA6;液相产物的主要成分为己内酰胺(CPL); HPW/C催化PA6水解的优化条件为:HPW负载量为45%、催化剂质量分数为10%、反应温度为260℃、反应时间为1 h,此时,PA6降解率和CPL产率可分别达83%与56%。
HPW/C,an activated carbon supported phosphotungstic acid catalyst,is prepared by impregnation method with activated carbon as support and phosphotungstic acid( HPW) as active component. Its effects on the hydrolysis reaction of polyamide 6( PA6) are also studied.The catalyst and hydrolysis products are characterized by test methods like FT-IR,XRD,BET,GCMS and UV.It is shown that HPW disperses highly on the surface and in the pores of activated carbon when the loading amount of HPW is lower than 55%; the solid phase residue contains incompletely decomposed PA6 and the main component of the liquid phase product is ε-caprolactam( CPL).The optimum conditions of hydrolysis reaction are proved as follows: the loading amount of HPW is 45%,the dosage of the catalyst is 10%,the reaction temperature and time are 260℃ and 1 hour,respectively.Under optimum conditions,PA6 degradation rate and CPL yield can reach 83% and 56% respectively.
HPW/C,an activated carbon supported phosphotungstic acid catalyst,is prepared by impregnation method with activated carbon as support and phosphotungstic acid( HPW) as active component. Its effects on the hydrolysis reaction of polyamide 6( PA6) are also studied.The catalyst and hydrolysis products are characterized by test methods like FT-IR,XRD,BET,GCMS and UV.It is shown that HPW disperses highly on the surface and in the pores of activated carbon when the loading amount of HPW is lower than 55%; the solid phase residue contains incompletely decomposed PA6 and the main component of the liquid phase product is ε-caprolactam( CPL).The optimum conditions of hydrolysis reaction are proved as follows: the loading amount of HPW is 45%,the dosage of the catalyst is 10%,the reaction temperature and time are 260℃ and 1 hour,respectively.Under optimum conditions,PA6 degradation rate and CPL yield can reach 83% and 56% respectively.
引文
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[3]詹世平,何友宝,王晓宁,等.亚超临界水技术在废旧尼龙6解聚中的应用[J].环境污染与防治,2008,30(1):68-71.
[4]Hocker S,Rhudy A K,Ginsburg G,et al.Polyamide hydrolysis accelerated by small weak organic acids[J].Polymer,2014,55(20):5057-5064.
[5]Shukla S R,Harad A M,Mahato D.Depolymerization of nylon 6waste fibers[J].Journal of Applied Polymer Science,2010,100(1):186-190.
[6]于荟.负载型杂多酸催化剂的研究进展[J].广州化工,2010,38(10):52-54.
[7]李谦定,张亮,徐海升.负载型磷钨钼杂多酸催化剂研究进展[J].石化技术与应用,2011,29(2):179-185.
[8]Chen J,Li Z,Jin L,et al.Catalytic hydrothermal depolymerization of nylon 6[J].Journal of Material Cycles and Waste Management,2010,12(4):321-325.
[9]金鹿江,陈晋阳,刘桂洋,等.尼龙6的催化水热解聚工艺与动力学[J].高分子材料科学与工程,2010,26(5):65-68.
[10]陈晋阳,金鹿江,褚燕萍,等.杂多酸催化废尼龙水解再资源化的研究[J].现代化工,2007,(s2):243-244.
[11]Bajuk-Bogdanovi'c D,Popa A,Uskokovi'c-Markovi'c S,et al.Vibrational study of interaction between 12-tungstophosphoric acid and microporous/mesoporous supports[J].Vibrational Spectroscopy,2017,92:151-161.
[12]Nakamura E.ChemInform Abstract:New acyl anion equivalent.a short route to the enol lactam intermediate in cytochalasin synthesis[J].Chemischer Informationsdienst,1981,12(23):663-666.
[13]张太顺.活性炭负载磷钨酸催化蒎烯与苯乙烯阳离子共聚合研究[D].南宁:广西民族大学,2012.
[14]Almohalla M,Rodriguez-Ramos I,Guerrero-Ruiz A.Comparative study of three heteropolyacids supported on carbon materials as catalysts for ethylene production from bioethanol[J].Catal Sci Technol,2017,7(9):1892-1901.
[15]Vasanthan N,Salem D R.FT-IR spectroscopic characterization of structural changes in polyamide-6 fibers during annealing and drawing[J].Journal of Polymer Science Part B Polymer Physics,2015,39(5):536-547.
[16]Eren E,Guney M,Eren B,et al.Performance of layered birnessitetype manganese oxide in the thermal-catalytic degradation of polyamide 6[J].Applied Catalysis B-Environmental,2013,(132):370-378.
[17]Wang W,Meng L,Yu J,et al.Enhanced hydrothermal conversion of caprolactam from waste monomer casting polyamide over H-Beta zeolite and its mechanism[J].Journal of Analytical and Applied Pyrolysis,2017,(125):218-226.