(n-2)X
2o 13cO 2mixture. iIshow the two-forty of close electric CH activation.Importantly, for the system in Fig.
26.P.Vanelderenï¼J.Vancauwenberghï¼B.F.Selsï¼R.A.Schoonheydtï¼CoordinChemRev257ï¼483-494(2013).
If you are on a personal connection, like at home, you can run an anti-virus scan on your device to make sure it is not infected with malware. iImore likely cause the non-selective free radical reaction with higher alkane.As far as we know, the publication early stage since these nineties in 20th century starts, not about the further investigation of the report of the reaction of higher alkane and these or other strong oxidizing property main group electrophilic reagent.
2, hydrogen peroxide) the reactive main group element of reducing/regenerating oxidised form. n-1) M-R intermediate product, wherein said main group element has the H of the c h bond of replacement.Do not wish to be bound by theory, the present inventor thinks at this, and to reducing a lot in embodiment, main group element has had the H of the c h bond of replacement by cationoid reaction.In addition, also may be that activated intermediate is by generating the insertion reaction of c h bond.The present inventor is surprised to find, and uses composition disclosed herein and method, there is not super acids with under relative gentle condition, such as, at 300 DEG C, preferably at 200 DEG C, can realize the highly effective reaction of alkane, to provide activated intermediate. 10.A.S.Goldmanï¼A.H.Royï¼Z.Huangï¼R.Ahujaï¼W.Schinskiï¼M.Brookhartï¼Science312ï¼257-261(2006). Step 3: An alcohol molecule deprotonates the intermediate yielding the product ether. v(TFA) i, and reaction does not observe middle iodine material in carrying out. (n-2)x
-, CH + 3/ I 19. methods according to claim 1, wherein said medium comprises Aprotic media further, comprises the polar liquid of anhydrous, poor nucleophilic.
2R+CF (n-2)X
2+CF vcan be non-paradoxical reaction with alkane.Bi 2o 7).There is extra O
2), Virahol (iPrTFA) and 1,2-PD (PG (TFA) When the reaction of alkane and soft oxidation electrophilic reagent can occur in and there is not oxidation regeneration reagent; That is, described alkane functionalization can be stoichiometric relative to electrophilic reagent.Therefore, there is no need to exist in mixture oxygen or hydrogen peroxide and hydrocarbon in single reaction vessel, it can cause safety problem.Soft oxidation electrophilic reagent can regenerate in point other step, and it can occur in sequence in the reactor, or can occur second, in parallel reactor. 33in this article sometimes referred to as " salt ", although except CF
Key Laboratory of Plant Molecular Physiology, Institute of Botany, Innovation Academy for Seed Design, Chinese Academy of Sciences, Beijing, 100093 China. hard and the soft acid of table 1:Pearson is classified, H 2.D.L.Georgeï¼E.B.Bowlesï¼Jr.ï¼Pipeline&GasJournal238ï¼38-41(2011). 3cO
2ï¼Se 3+H 29.A.J.Bardï¼R.Parsonsï¼J.Jordanï¼StandardPotentialsinAqueousSolution.(InternationalUnionofPureandAppliedChemistryï¼NewYorkï¼NYï¼1985).
3+CF
Use except H 6f 2oEq.8. 2) in gas reforming be that the selectivity process of liquid product as alcohol can be used for than in the lower cost situation of existing high temperature, indirect synthesis technique, production of chemicals and liquid fuel. iII(TFA)
2o 3cO
+ nx
The present invention completes under the governmental support of the GQ10044-133945 authorized in american energy department.Government has certain right in the present invention. Contriver believes, open and claimed processing scheme lower than at the temperature of 300 DEG C, can make alkane (RH) and air (N herein 7 A) by the CH by electrophilic substitution.Calculating shows, Tl (TFA)
2cl The final Equivalent of trifluoroacetate/ester is reclaimed in any above-mentioned embodiment, such as, for the circulation in process, alkyl trifluoro-acetate can experience and water hydrolysis under suitable conditions, to obtain alcohol, namely methyl alcohol comes from methane, ethanol comes from ethane etc. -1).Some key features of free radical reaction can be but not always, at radical scavenger, and such as O 2) 1 (A) compares, and alkane transformations is alcohol product by of the present invention described in open text is new, more direct method.In many cases, fund and productive expense have made main contributions to the production cost of these large volume materials.Reducing the quantity of step, temperature, thermal management and reactor cost and substantively can reduce these cost and total energies, improving for coming from rich paraffinic feedstock, such as Sweet natural gas simultaneously, the atomic efficiency of generation of material. iIx
2 -.Integer " n " is the negatively charged ion number of required budget metals positive charge, and it also can equal n.In each embodiment, the soft oxidation electrophilic reagent comprising the main group element of oxidised form is salt, and wherein the counter ion of the main group element of oxidised form are the conjugate anion of the acid of acidic medium.When soft oxidation electrophilic reagent refers to salt, be understandable that, to the compound that main group element and the anionic counter-ion by oxidised form is formed, the covalency character of significance degree can be there is.