技術(shù)領(lǐng)域

本發(fā)明涉及一種利用亞甲基自轉(zhuǎn)移反應(yīng)制備N-甲基烏洛托品鹽的方法，屬于高氮雜環(huán)化合物制備化學(xué)領(lǐng)域。

背景技術(shù)

眾所周知，烏洛托品(六次甲基四胺，hexamethylenetetraamine,hexamine)是一種價廉易得的高氮雜環(huán)化工原料，它及它的鹽在藥物、殺菌劑(近年的評論：Paranjape,S.G.；Turankar,A.V.；Sontakke,S.D.Medical?Hypotheses?2013,80,507.Yao,Joseph?D.C.；Moellering,Robert?C.,Jr.Edited?by?Versalovic,James,Manual?of?Clinical?Microbiology,10th?Edition,2011,1,1043-1081.Bendewald,Margo?J.；Farmer,Sara?A.；Davis,Mark?D.P.Dermatitis?2010,21,33-40.Dowling,Patricia?M.Edited?by?Giguere,Steeve?Antimicrobial?Therapy?in?Veterinary?Medicine4th?Edition,2006,285-300.Mitscher,Lester?A.；Lemke,Thomas?L.；Gentry,Elmer?J.Edited?by?Lemke,Thomas?L.；Williams,David?A?Foye's?Principles?of?Medicinal?Chemistry?6th?Edition,2008,1028-1083)，高分子材料(Kirillov,Alexander?M.Coord.Chem.Rev.2011,255(15-16),1603-1622)，高孔材料(Candelaria,Stephanie?L.；Chen,Rong；Jeong,Yoon-Ha；Cao,Guozhong?Energy&Env.Sci.2012,5,5619-5637),高能密度材料(Angew.Chem,2006,45,3584-3601.Singh,Rajendra?P.；Gao,Haixiang；Meshri,Dayal?T.；Shreeve,Jean'ne?M.Structure?and?Bonding?Berlin,Ger.2007,125(High?Energy?Density?Materials),35-83)等制備中有重要意義，并在有機和無機合成中被廣泛用作甲?；?Rajadhyaksha,Mangesh?Narayan；Jadhav,Vidyadhar?Kashinath；Shrigadi,Nilesh?Balkrishna；Panandikar,Aditi?Milind?PCT?Int.Appl.WO?2012073259.Chawla,H.M.；Pant,N.；Srivastava,Bindu；Upreti,Shailesh?Org.Lett.2006,8,2237-2240.Balalaie,Saeed；Golizeh,Makan?Chemistry:India.J.2005,2,171-173.Hagiya,Kazutake；Sato,Yasuhiro?PCT?Int.Appl.2005,WO?2005012267.Horizoe,Tatsuo；Shinoda,Masanobu；Emori,Eita；Matsuura,Fumiyoshi；Kaneko,Toshihiko；Ohi,Norihito；Kasai,Shunji；Yoshitomi,Hideki；Yamazaki,Kazuto；Miyashita,Sadakazu；et?al?PCT?Int.Appl.2002,WO?2002080899.Komissarova,N.L.；Belostotskaya,I.S.；Shubina,O.V.；Grishina,E.A.；Ershov,V.V.Zhu.Org.khim.1992,28,188-91.Papenfuhs,Theodor；Volk,Heinrich?1977,DE?2533960.Naik,R.M.；Thakor,V.M.J.Org.Chem.1957,22,1626-9)、甲基源(Kilenyi,S.Nicholas?e-EROS?Encyclopedia?of?Reagents?for?Organic?Synthesis?2001.Barrault,J.；Pouilloux,Y.Catalysis?Today?1997,37(2)137-153.Caillault,Xavier；Chupin,Jerome；Pouilloux,Yannick；Barrault,Joel，Chem.Ind.(Dekker)1996,68(Catalysis?of?Organic?Reactions),231-240；Caillault,X.；Pouilloux,Y.；Barrault,J.J.Mol.Catal.A:Chem.1995,103(2),117-23.X.Caillault,J.Chupin,Y.Pouilloux,J.Barranlt,in:M.Dekker(Ed.),Catal.Org.Reactions,Atlanta,1996,p.231_.Fouquay,Stephane?1993,EP?550307；Bogdanov,V.I.；Morgunova,E.S.；Sakson,O.F.；Khazanov,M.Ya.1986,SU?1271863)和氮源(Sun,Qi；Li,Yan；Sun,Huiying?2015,CN?104300140.Vuorinen,Tapani；Paeaekkoenen,Timo；Nuopponen,Markus?PCT?Int.Appl.2012,WO?2012168562.Wang,Li-Jun；Xie,Li-Li；Li,Yong-Lun；Yuan,Hao；Li,Qing-Hua；Li,Quan-Zhi?Huaxue?Xuebao?2007,65,913-916.He,Binglin；Sun,Juntan；Li,Hong；Jin,Xiaonong；Zhao,Weijun；Zhang,Shuji；Fang,Yanquan?Cuihua?Xuebao,1985,6,168-71_.Warmus,Joseph?S.；Dilley,Garrett?J.；Meyers,A.I.J.Org.Chem.1993,58,270-271.Fuellbier,Harry；Jabs,Gisela；Feistel,Lothar；Schwachula,Gerhard；Wagnitz,Petra?1991,Ger.(East)DD?293595.1971,DE?2016602.1965,FR?1409087)。