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1、组会汇报文献汇报李满04/15/2016文献汇报1Inorg.Chem.,2015,54,5043-5052文献汇报2R.A.BaillieandP.Legzdins,Acc.Chem.Res.,2014,47,330−340L.Queetal.,J.Am.Chem.Soc.,2003,126,472−473M.J.BurkandR.H.Crabtree,J.Am.Chem.Soc.,1987,109,8025−8032S.Kraftetal.,J.Am.Chem.Soc.,2011,133,1832−1848文献汇报3(1)thecombinationofacatalystres
2、ponsibleforC−Hactivationwithacocatalystresponsiblefordioxygenactivation,(2)transition-metalcatalysts,whichreactwithbothhydrocarbonsandmolecularoxygen,(3)theintroductionofveryrobustmain-groupelementcatalystsforC−Hfunctionalizationchemistry.D.MunzandT.Strassner,Inorg.Chem.,2015,54,5043-5052Three
3、strategies:Strategy14D.MunzandT.Strassner,Inorg.Chem.,2015,54,5043-5052Strategy15M.Muehlhofer,T.Strassner,W.A.Herrmann,Angew.Chem.Int.Ed.,2002,41,1745−1747Strategy16D.MunzandT.Strassner,Angew.Chem.Int.Ed.,2014,53,2485−2488D.MunzandT.Strassner,Chem.Eur.J.,2014,20,14872−14879D.Munz,D.Meyer,T.Str
4、assner,Organometallics,2013,32,3469−3480HalogenslikechlorineorbromineappeartobegoodcandidatesforefficientredoxcatalystsbecausetheyarestrongenoughoxidantsforC−Hfunctionalizationchemistryandarewell-knowntobecapableofgeneratingtransition-metalcomplexesinhighoxidationstateslikepalladium(IV)orcoppe
5、r(III)byanonradicaltwo-electronprocess(Scheme3).Strategy17D.Munz,D.Meyer,T.Strassner,Organometallics,2013,32,3469−3480Strategy18D.MeyerandT.Strassner,J.Organomet.Chem.,2015,784,84−87Strategy19D.MeyerandT.Strassner,J.Organomet.Chem.,2015,784,84−87T.Strassneretal.,Organometallics,2006,25,5409-54
6、15If11isanintermediateinthecatalyticcycleitshouldbeasactiveas8inthemethaneactivation(Scheme1).Wethereforetested11underourstandardconditions(seeMethaneactivationforexperimentaldetails)andfoundacomparableactivity(TON22)asinthecaseof8(TON24)[19].Strategy110D.MeyerandT.Strassner,J.Organomet.Chem.,
7、2015,784,84−87Strategy111D.Meyer,A.ZellerandT.Strassner,J.Organomet.Chem.,2012,701,56−61Strategy112R.A.Perianaetal.,Science,1998,280,560−564Becauseoleumisproducedbytheaerobicoxidationofsulfurdioxideinthepresenceofavanadium(V)catalyst(co
