Process for the benign direct fixation and conversion of nitrogen oxides
AssigneeUniversity of Houston System
InventorsRamiro Sanchez, Graciela Lubertino
Life of this patent
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Abstract
A direct fixation of NO.sub.2 and N.sub.2 O.sub.4 at room temperature and atmospheric pressure is described using bis(diorganoamino)magnesium compounds formed from reactions between donor-solvent free diorganomagnesium compounds and primary or secondary amines, yielding new compositions of matter having the general formulas [(R.sub.2 N).sub.i (R.sub.2 NN.sub.x O.sub.y)jMg].sub.m and [(R.sub.2 N).sub.i (R.sub.2 NN.sub.x O.sub.y).sub.j (N.sub.x O.sub.y).sub.k Mg].sub.m. Methods are also described to convert these new compositions of matter into useful organic compounds and nitrogen gas.
Claims20
An organoaminomagnesium complex comprising a composition of formula (III):
- [(R.sub.2 N).sub.i (R.sub.2 NN.sub.x O.sub.y).sub.j Mg].sub.m(III)
- where:
- the R groups are the same or different and are hydrogen atoms, carbon containing groups or silicon containing groups;
- i is a number having a value less than 2.0 (i<2.0);
- j is a number having a value greater than 0.0 and less than or equal to 2.0 (0.0<j.ltoreq.2.0);
- m is an integer having a value between 1 and infinity (1.ltoreq.m.ltoreq..infin.);
- x is an integer having a value between 1 and about 8;
- and
- y is an integer having a value between 1 and about 16.
An organoaminomagnesium complex comprising compounds of formula (IIIa):
- [(R.sub.2 N).sub.i (R.sub.2 NNO.sub.2).sub.ja (R.sub.2 NN.sub.2 O.sub.4).sub.jb Mg].sub.m (IIIa)
- where:
- the R groups are the same or different and are hydrogen atoms, carbon containing groups or silicon containing groups;
- i is a number having a value less than 2.0 (i<2.0);
- ja and jb are numbers, the sum of which is greater than 0.0 and less than or equal to 2.0 (0.0<ja+jb.ltoreq.2.0);
- and
- m is an integer having a value between 1 and infinity (1.ltoreq.m.ltoreq..infin.).
An organoaminomagnesium complex comprising compounds of formula (IIIb):
- [(R.sub.2 N).sub.i (R.sub.2 NNO.sub.2).sub.j Mg].sub.m (IIIb)
- where:
- the R groups are the same or different and are hydrogen atoms, carbon containing groups or silicon containing groups;
- i is a number having a value less than 2.0 (i<2.0);
- j is a number having a value greater than 0.0 and less than or equal to 2.0 (0.0<j.ltoreq.2.0);
- and
- m is an integer having a value between 1 and infinity (1.ltoreq.m.ltoreq..infin.).
An organoaminomagnesium complex comprising compounds of formula (IIIc):
- [(R.sub.2 N).sub.i (R.sub.2 NN.sub.2 O.sub.4).sub.j Mg].sub.m(IIIc)
- where:
- the R groups are the same or different and are hydrogen atoms, carbon containing groups or silicon containing groups;
- i is a number having a value less than 2.0 (i<2.0);
- j is a number having a value greater than 0.0 and less than or equal to 2.0 (0.0<j.ltoreq.2.0);
- and
- m is an integer having a value between 1 and infinity (1.ltoreq.m.ltoreq..infin.).
An organoaminomagnesium complex comprising compounds of formula (IV):
- [(R.sub.2 N).sub.i (R.sub.2 NN.sub.x O.sub.y).sub.j (N.sub.x O.sub.y).sub.k Mg].sub.m (IV)
- where:
- the R groups are the same or different and are hydrogen atoms, carbon containing groups or silicon containing groups;
- i is a number having a value less than 2.0 (i<2.0);
- j is a number having a value greater than or equal to 0.0 and less than or equal to 2.0 (0.0.ltoreq.j.ltoreq.2.0);
- k is a number having a value less than 2.0 (k<2.0);
- m is an integer having a value between 1 and infinity (1.ltoreq.m.ltoreq..infin.);
- x is an integer having a value between 1 and about 8;
- and
- y is an integer having a value between 1 and about 16.
A process comprising the step of:
- contacting a compound of formula (I):
- [(R.sub.2 N).sub.2 Mg].sub.n (I)
- with a compound of formula (II):
- N.sub.x O.sub.y (II)
- to form a reaction mixture comprising intermediates of formulas (III) and (IV):
- [(R.sub.2 N).sub.i (R.sub.2 NN.sub.x O.sub.y).sub.j Mg].sub.m(III)
- [(R.sub.2 N).sub.i (R.sub.2 NN.sub.x O.sub.y).sub.j (N.sub.x O.sub.y).sub.k Mg].sub.m (IV)
- under reaction conditions sufficient to facilitate the formation of the intermediates of formulas (III) and (IV), where:
- the R groups are the same or different and are a hydrogen atom, a linear or branched carbon containing group or a linear or branched silicon containing group;
- i is a number having a value less than 2.0 (i<2.0);
- j is a number having a value greater than 0.0 and less than or equal to 2.0 (0.0<j.ltoreq.2.0) for compounds of formula (III) and a value greater than or equal to 0.0 and less than or equal to 2.0 (0.0.ltoreq.j.ltoreq.2.0) for compounds of formula (IV);
- k is a number having a value less than 2.0 (k<2.0);
- n is an integer having a value between 1 and infinity (1.ltoreq.n.ltoreq..infin.);
- m is an integer having a value between 1 and infinity (1.ltoreq.m.ltoreq..infin.);
- x is an integer having a value between 1 and about 8;
- and
- y is an integer having a value between 1 and about 16.
A process comprising the steps of:
- (a) contacting a scavenger comprising compounds of formula (I):
- [(R.sub.2 N).sub.2 Mg].sub.n (I)
- with a waste stream comprising compounds of formula (II):
- N.sub.x O.sub.y (II)
- to form a reaction mixture comprising intermediates of formulas (III) and (IV):
- [(R.sub.2 N).sub.i (R.sub.2 NN.sub.x O.sub.y).sub.j Mg].sub.m(III)
- [(R.sub.2 N).sub.i (R.sub.2 NN.sub.x O.sub.y).sub.j (N.sub.x O.sub.y).sub.k Mg].sub.m (IV)
- and an unreacted portion of the compounds of formula (I) under reaction conditions sufficient to facilitate the formation of the intermediates of formulas (III) and (IV);
- and
- (b) separating the reaction mixture into an intermediate product comprising the compounds of formulas (III) and (IV) and unreacted compounds of formula (I);
- where:
- the R groups are the same or different and are a hydrogen atom, a linear or branched carbon containing group or a linear or branched silicon containing group;
- i is a number having a value less than 2.0 (i<2.0);
- j is a number having a value greater than 0.0 and less than or equal to 2.0 (0.0<j.ltoreq.2.0) for compounds of formula (III) and a value greater than or equal to 0.0 and less than or equal to 2.0 (0.0.ltoreq.j.ltoreq.2.0) for compounds of formula (IV);
- k is a number having a value less than 2.0 (k<2.0);
- n is an integer having a value between 1 and infinity (1.ltoreq.n.ltoreq..infin.);
- m is an integer having a value between 1 and infinity (1.ltoreq.m.ltoreq..infin.);
- x is an integer having a value between 1 and about 8;
- and
- y is an integer having a value between 1 and about 16.
Dependencies are inferred from the claim text.