Discussion:
Azides from Hydrazine Salts GB128014
(too old to reply)
Rosco P. Coaltrain
2004-02-05 06:17:36 UTC
Permalink
A simplified method for producing azides was described
in two old British patents issued in 1919 , and this
subject became the topic for a lengthy thread in this
news group . In order to simplify readers access to
the text for the main patent GB128014 , without having
to sort through the presently eighty-six messages
in the original thread , it seems fitting to repost
that patent text as a separate topic here .


GB128014 , Complete Specification ,
Improvements in and relating to the Production of Azides
application date: June 17 , 1918 No. 9952 / 18
complete accepted : June 17 , 1919

I , William Richard Hodgkinson , C.B.E. , of Ordnance College ,
Woolwich , London , S.E. 18 , Professor of Chemistry and Metallurgy ,
do hereby declare the nature of this invention and in what manner
the same is to be performed , to be particularly described and
ascertained in and by the following statement :

This invention relates to the production of azides .

The object of the invention is to provide a process of producing
azides from salts of hydrazine without the employment of
ethyl benzoate or the like , and the formation of benzoyl hydrazine .
According to the invention , salts of hydrazine are diazotised
by means of a suitable nitrite under such conditions that the
reaction mass is at no time so distinctly acid as to redden
litmus paper , but appears on the border line of acidity and
alkalinity . The conditions of acidity under which the reaction
is carried out according to the invention , are preferably
comparable with the conditions of acidity as indicated by
litmus paper , of , for instance a solution of boric acid .
Thus in accordance with the invention , the nitrite solution
is brought together with a salt of hydrazine in approximately
the proportions required on the basis of theory to diazotise
the hydrazine , under such conditions that the acidity never
exceeds the degree of acidity indicated above , and an
acidified salt of the metal of which the azide is required ,
is introduced into the mixture , or alternatively the mixture
is added to the solution of the salt of the metal .

For example , silver azide is formed by adding a neutral solution
of hydrazine sulphate and sodium nitrite in molecular proportions
to a solution of silver nitrate of a degree of acidity with
nitric acid enabling the conditions in regard to acidity
set forth above to be realised , while avoiding the precipitation
of silver sulphate . Thus,for example 130 grams of hydrazine sulphate
is converted to the neutral hydrazine ammonium sulphate , which is
more soluble in water than is the simple hydrazine sulphate ,
by the addition of ammonia solution , the mixture being made up
to about 500 ccs . To this solution contained in a vessel in which
it can be violently agitated , the calculated amount of sodium nitrite
dissolved in 500 ccs. of water is added slowly so that the temperature
does not rise much above 30 degrees Centigrade .

The reaction resulting in the formation of sodium azide may be
represented by the following equation :

N2H4-H-NH3-H-SO4 + NaNO2 -----> NH4HSO4 + NaN3 + 2 H2O

From this equation it will be seen that the solution would
become acid as the result of the reaction were it not for
the fact that sodium nitrite is never pure but is alkaline ,
the alkali in the nitrite ordinarily being sufficient to maintain
the solution on the border line of acidity and alkalinity ,
and addition of a small quantity of alkali being made
should such not be the case . The solution thus made contains
sodium azide , some unchanged reagents , and the by-products
of the reaction .

The sodium sulphate and sodium azide contained in the solution
may be separated by crystallisation but preferably the solution
is added gradually to an acidified solution of silver nitrate
produced by adding 1.0 cc. of 70% of nitric acid to 1000 ccs.
of a normal solution of silver nitrate which is violently agitated
during such adding , the temperature of the reaction mass being
prevented from rising much higher than 30 - 40 degrees Centigrade .
With adequate cooling and agitation the yield of silver azide may
be obtained equivalent to 85 % of the calculated possible amount .
Instead of adding the diazotised solution to the acidifed
silver nitrate solution , the latter may be added to the former .

When starting from hydrazine nitrate which is also an acid salt ,
a solution of ammonia should be added in order to form the
neutral hydrazine ammonium salt or , if desired ,
the neutral hydrazine sodium salt may be produced ,
the remaining steps of the process being then carried out
as above described .

In producing lead azide , a solution of a hydrazine salt
of an acid which will not result in the precipitation
of an insoluble lead salt of the acid in question ,
for instance hydrazine nitrate , is employed , and
the reaction mass in this case should be only just acid ,
as lead azide is particularly easily acted on by acids ,
while in producing silver azide the acidity of the
reaction mass may be greater in order to avoid the precipitation
of silver sulphate and agitation indicated in the foregoing example .

The azides produced in accordance with the invention are
usually amorphous , and in this state they are safer to handle
than when crystalline .

Having now particularly described and ascertained the nature
of my said invention and in what manner the same is to be performed ,
I declare that what I claim is :

1. The process of producing azides from salts of hydrazine
in which salts of hydrazine are diazotised by means of a
suitable nitrite under such conditions that the reaction mass
is at no time so distinctly acid as to redden litmus paper ,
but appears on the border line of acidity and alkalinity .

2. The process as claimed in Claim 1 in which the conditions
of acidity under which the reaction is carried out according
to the invention are preferably comparable with conditions
of acidity as indicated by litmus paper , of , for instance ,
a solution of boric acid .

3. The process of producing azides from salts of hydrazine ,
substantially as hereinbefore described .

Dated this 10th day of December , 1918
Rosco P. Coaltrain
2004-02-12 18:09:26 UTC
Permalink
***@yahoo.com (Rosco P. Coaltrain) wrote in message news:<***@posting.google.com>...

Louis ,

Please share your thoughts on this .

I have two significant , ( yet reconcilable ) issues
concerning the Hodgkinson patent .

In the above patent there is information which I must
legitimately question , regarding both the mechanism
of the reaction and the pH .

According to Hodgkinsons description of the reaction ,
[QUOTE]
The reaction resulting in the formation of sodium azide may be
represented by the following equation :

N2H4-H-NH3-H-SO4 + NaNO2 -----> NH4HSO4 + NaN3 + 2 H2O

From this equation it will be seen that the solution would
become acid as the result of the reaction were it not for
the fact that sodium nitrite is never pure but is alkaline ,
the alkali in the nitrite ordinarily being sufficient to maintain
the solution on the border line of acidity and alkalinity ,
and addition of a small quantity of alkali being made
should such not be the case . The solution thus made contains
sodium azide , some unchanged reagents , and the by-products
of the reaction .
[END QUOTE]

The observation I can make is that even *if* the Sodium Nitrite
used by Hodgkinson was alkaline due to the presence of an
"impurity" of an *added* equimolar amount of Sodium Hydroxide ,
( which is certainly a great deal more than a "small quantity"
of added alkali like Hodgkinson describes ) ......
the reaction product would still be so acid as to be more than
sufficient to redden litmus . Let us consider the reaction
equation for the situation I describe and this will be evident .

N2H4-H-NH3-H-SO4 + NaNO2 + NaOH -----> NaNH4SO4 + NaN3 + 3 H2O

The NaNH4SO4 is a "stipulated compound" to illustrate acidity ,
but in reality would probably be an indeterminate mixture of
normal and acid sulfates of Sodium and Ammonia .

There is a ( possible ? ) way of reconciling this descrepancy .
Where Hodgkinson describes preparing a solution of
*neutral* hydrazine ammonium sulfate , no particular quantity
of ammonia is specified as being added to achieve that *neutral*
solution . There may be actually present in such a "neutral"
solution an "excess" of alkali not accurately reflected by
the simplified equation for the reaction as written by Hodgkinson .
This excess alkali , together with the unspecified amount of alkali
described as being present in Hodgkinsons "impure nitrite" ,
may satisfy the accounting for some of the missing amount of
additional alkali not detailed by Hodgkinson .

The second issue regarding pH as described by Hodgkinson relates
to the comparison of the pH required for the reaction as being
comparable to the pH for a solution of Boric Acid .
The pH for a .1 M solution of Boric Acid is pH 5.2 .
The color change range for Litmus is pH 6 to pH 8 ,
so at pH 5.2 , the reaction mixture would already be
quite red to litmus .....in direct contradiction with
Hodgkinsons description .

In spite of these discrepancies which seem most obvious
and somewhat perplexing , I believe that Hodgkinsons
process probably does indeed work , although not all
of the finer details are disclosed completely by the patent .

It would be nice to have a more detailed and modern description
of the process after the subtleties are worked out from
experiments . Only from experiments shall we know
"the rest of the story" about Hodgkinsons patent process
for producing azides from hydrazine salts .

Rosco
LOUIS
2004-02-14 09:40:40 UTC
Permalink
Sorry Rosco for the late reply but I'm working hard on my mother's appartement restoring and rebuilding.
Right now I'm at innerwall building and ending electricity...water supply is almost done....then I still have to do the
ground, place commodities and ... all that you can think of.


Yes indeed some uncertainities lay in that modus operandi.
Since:
-to make mixed sulfate of (N2H5)NH4SO4 they must have used exces NH3 introduced into N2H5HSO4
This exces must be present inthere.
-Depending on the process used to make NaNO2, it may contain traces of NaOH (if made from NaNO2 and NOx) but then also of
NaNO3 (another process involves heating of NaNO3 eventually with lead to get NaNO2 and PbO)...then NaNO3 will always be in
depending on the number of recristallisations used at that time.
-If exces mixed sulfate is present and that acidic N2H5HSO4 is formed you get a buffer couple but this will make a triming
of the solution between pH 4,8-5,8
-If there is excess NH3 and/or excess NaOH due to the origins of the reactants; then pH will be higher than 6 no doubt but
will never exceed 5,8 in all the course of the reaction.
-About the boric acid yes, it should produce red litmus, but when we mix boric acid to ammonia or NaOH...you have triming
effect but arround pH 4,6 (3,6-5,6) but since the amount of NaOH /NH3 is unknown, you might go to the second pKa2/2 triming
and most likely never to the pKa3/2
H3BO3 --> H(+) + H2BO3(-) pKa1 = 9,14 --> pKa1/2= 4,6 approx and triming 3,6-5,6
H2BO3(-) --> H(+) + HBO3(-) pKa2 = ??? 12 or more --> pKa/2 > or = 6 and triming 5 (or more) to 7 (or more).


Ph Z
Post by Rosco P. Coaltrain
Louis ,
Please share your thoughts on this .
I have two significant , ( yet reconcilable ) issues
concerning the Hodgkinson patent .
In the above patent there is information which I must
legitimately question , regarding both the mechanism
of the reaction and the pH .
According to Hodgkinsons description of the reaction ,
[QUOTE]
The reaction resulting in the formation of sodium azide may be
N2H4-H-NH3-H-SO4 + NaNO2 -----> NH4HSO4 + NaN3 + 2 H2O
From this equation it will be seen that the solution would
become acid as the result of the reaction were it not for
the fact that sodium nitrite is never pure but is alkaline ,
the alkali in the nitrite ordinarily being sufficient to maintain
the solution on the border line of acidity and alkalinity ,
and addition of a small quantity of alkali being made
should such not be the case . The solution thus made contains
sodium azide , some unchanged reagents , and the by-products
of the reaction .
[END QUOTE]
The observation I can make is that even *if* the Sodium Nitrite
used by Hodgkinson was alkaline due to the presence of an
"impurity" of an *added* equimolar amount of Sodium Hydroxide ,
( which is certainly a great deal more than a "small quantity"
of added alkali like Hodgkinson describes ) ......
the reaction product would still be so acid as to be more than
sufficient to redden litmus . Let us consider the reaction
equation for the situation I describe and this will be evident .
N2H4-H-NH3-H-SO4 + NaNO2 + NaOH -----> NaNH4SO4 + NaN3 + 3 H2O
The NaNH4SO4 is a "stipulated compound" to illustrate acidity ,
but in reality would probably be an indeterminate mixture of
normal and acid sulfates of Sodium and Ammonia .
There is a ( possible ? ) way of reconciling this descrepancy .
Where Hodgkinson describes preparing a solution of
*neutral* hydrazine ammonium sulfate , no particular quantity
of ammonia is specified as being added to achieve that *neutral*
solution . There may be actually present in such a "neutral"
solution an "excess" of alkali not accurately reflected by
the simplified equation for the reaction as written by Hodgkinson .
This excess alkali , together with the unspecified amount of alkali
described as being present in Hodgkinsons "impure nitrite" ,
may satisfy the accounting for some of the missing amount of
additional alkali not detailed by Hodgkinson .
The second issue regarding pH as described by Hodgkinson relates
to the comparison of the pH required for the reaction as being
comparable to the pH for a solution of Boric Acid .
The pH for a .1 M solution of Boric Acid is pH 5.2 .
The color change range for Litmus is pH 6 to pH 8 ,
so at pH 5.2 , the reaction mixture would already be
quite red to litmus .....in direct contradiction with
Hodgkinsons description .
In spite of these discrepancies which seem most obvious
and somewhat perplexing , I believe that Hodgkinsons
process probably does indeed work , although not all
of the finer details are disclosed completely by the patent .
It would be nice to have a more detailed and modern description
of the process after the subtleties are worked out from
experiments . Only from experiments shall we know
"the rest of the story" about Hodgkinsons patent process
for producing azides from hydrazine salts .
Rosco
Rosco P. Coaltrain
2004-02-15 06:52:50 UTC
Permalink
Post by LOUIS
Sorry Rosco for the late reply but I'm working hard
on my mother's appartement restoring and rebuilding.
Right now I'm at innerwall building and ending electricity...
water supply is almost done....then I still have to do the
ground, place commodities and ... all that you can think of.
Yes indeed some uncertainities lay in that modus operandi.
-to make mixed sulfate of (N2H5)NH4SO4 they must have used exces NH3
introduced into N2H5HSO4
This exces must be present inthere.
-Depending on the process used to make NaNO2, it may contain traces
of NaOH (if made from NaNO2 and NOx) but then also of
NaNO3 (another process involves heating of NaNO3 eventually with lead
to get NaNO2 and PbO)...then NaNO3 will always be in
depending on the number of recristallisations used at that time.
-If exces mixed sulfate is present and that acidic N2H5HSO4 is formed
you get a buffer couple but this will make a triming
of the solution between pH 4,8-5,8
-If there is excess NH3 and/or excess NaOH due to the origins of the
reactants; then pH will be higher than 6 no doubt but
will never exceed 5,8 in all the course of the reaction.
-About the boric acid yes, it should produce red litmus, but when we mix
boric acid to ammonia or NaOH...you have triming
effect but arround pH 4,6 (3,6-5,6) but since the amount of NaOH /NH3
is unknown, you might go to the second pKa2/2 triming
and most likely never to the pKa3/2
H3BO3 --> H(+) + H2BO3(-) pKa1 = 9,14 --> pKa1/2= 4,6 approx and triming 3,6-5,6
H2BO3(-) --> H(+) + HBO3(-) pKa2 = ??? 12 or more --> pKa/2 > or = 6 and
triming 5 (or more) to 7 (or more).
Ph Z
Louis ,

Part of the uncertainty is resolved by an additional detail in
the companion patent GB129152 filed a few weeks later by the same
inventor . In that later patent GB129152 , Hodgkinson makes
reference to the same method as described by the earlier patent ,
[QUOTE]
According to the preferred manner of carrying the invention into
effect , a solution of hydrazine as,for instance,hydrazine sulphate,
neutralized *and* RENDERED FAINTLY ALKALINE with ammonia or soda ,
and an equivalent proportion of sodium nitrite , is prepared and
this mixed solution is then added to a solution of silver nitrate
rendered slightly acid with nitric acid , under conditions
of violent agitation , the temperature being regulated so as
not to exceed 30 degrees C .
Silver azide will thus be formed and will separate out under favorable
conditions in quantity equivalent to 85% of the theoretical .
The silver azide is washed with cold water and suspended or agitated
with a proportion of common salt slightly less than is required
according to the equation : AgN3 + NaCl -----> AgCl + NaN3
The reaction in these conditions is completed in a few minutes ,
and the silver chloride may then be filtered off and the solution
of sodium azide concentrated on a steam bath . In this way sodium azide
in an approximately pure state will be obtained and this sodium azide
may in accordance with the invention be employed for the formation of
lead azide or other azides by double decomposition with lead or
other salts .
[END QUOTE]

Since litmus is the pH indicator which Hodgkinson has mentioned ,
it is probably a safe guess that the pH of the solution of the
hydrazine salt which is neutralized and "rendered faintly alkaline"
is a pH in the range of pH 7.1 to pH 8 , probably nearer pH 8 .
I need to check what pH exactly is where red litmus just begins to
go blue to more accurately guess what Hodgkinson would call
"faintly alkaline" .

This detail confirms that there is indeed free alkali present on
the left side of the equation , as I expected there should be .
Since the reaction only goes to about 85% completion , the
unreacted alkali on the left side of the equation prevents the
acidity of the system from rising too high from the acidic
product on the right side of the equation . This is the region
where the presence of a buffer in the system might possibly
allow the reaction to go to completion , instead of quenching
at 85% due to the decreasing pH . Deliberately basifying the
sodium nitrite solution in advance to a favorable alkalinity ,
and performing the reaction with more concentrated solutions
may also result in increased yields . This is quite interesting
because even at 85% yield , Hodgkinsons process is more efficient
and economical than the modern synthetic methods which are used
for current production of azides .

From a few test runs , it should be possible to optimize the
concentrations of solutions and added alkali requirement .

From studying these patents , I now realize that some of my
past failed experiments would have actually worked fine , *IF*
the pH of the reactions being attempted had been very carefully
controlled . Evidently pH is absolutely the critical factor in
making these type reactions work .

This has been a very interesting and enlightening discussion :-)
I feel much more confident now about the potential for
success with any future experiments with this type of reaction ,
knowing in advance that it is a very pH critical reaction .

I know you have done some experiments already before the text
of these patents was available and we were trying to make
educated guesses concerning the parameters of this reaction .

But now that we have this information that the reaction proceeds
to 85% completion , would you venture a guess as to the amount
of added NaOH (on a molar basis) to the NaNO2 which would be
a good approximation of Hodgkinsons "impure nitrite" . The
nitrite which I have on hand is exceptionally pure , so I will
have to add some alkali to it and/or use a buffer for pH control .

Rosco
Rosco P. Coaltrain
2004-02-15 14:37:30 UTC
Permalink
***@yahoo.com (Rosco P. Coaltrain) wrote in message news:<***@posting.google.com>...

Louis ,

Please amend my last question regarding added NaOH .

I meant to ask how much added Na2CO3 (on a molar basis)
with regards to the NaNO2 *NOT* NaOH .... I was thinking "soda" ,
but mistakenly wrote the formula for "caustic soda" instead .
Since the idea is to buffer the reaction without greatly disturbing the pH ,
then obviously NaOH would not be a good choice of added alkali . I have
even wondered if Hodgkinsons reference to "soda" may not be bicarbonate ,
(baking soda) which would be an even milder base perhaps most suitable
as the added alkali . And according to the same reasoning , even
better still as an added alkali may be sodium acetate or sodium citrate .
Using an alkaline salt of a weak acid in this way should allow for
more leeway in the amount of added alkali which would be useful to add
to the nitrite solution without adversely affecting the pH of the system .
If NaOH was used , even a slight error in the quantity of NaOH used
could effectively "poison" the reaction system by driving the pH too high .
The same undesired effect could occur even with the correctly calculated
amount of NaOH , if the dynamic of the reaction did not follow the rate of
addition of the NaNO2 solution including such a strong base as NaOH .

Rosco

[SNIP]
Post by Rosco P. Coaltrain
But now that we have this information that the reaction proceeds
to 85% completion , would you venture a guess as to the amount
of added NaOH (on a molar basis) to the NaNO2 which would be
a good approximation of Hodgkinsons "impure nitrite" . The
nitrite which I have on hand is exceptionally pure , so I will
have to add some alkali to it and/or use a buffer for pH control .
Rosco
Don T
2004-02-15 20:19:24 UTC
Permalink
It is standard lab practice to make up a NaOH or KOH "standard" solution
when titration's are done. Why use Na2CO3 or even NaHCO3? other than they
are relatively less basic and you can "fudge" a bit on amounts added?
--
Don Thompson

"The only stupid questions are those that should have been asked, but
weren't, or those that have been asked and answered over and over, but the
answers not listened to." Peter Rowe
Post by Rosco P. Coaltrain
Louis ,
Please amend my last question regarding added NaOH .
I meant to ask how much added Na2CO3 (on a molar basis)
with regards to the NaNO2 *NOT* NaOH .... I was thinking "soda" ,
but mistakenly wrote the formula for "caustic soda" instead .
Since the idea is to buffer the reaction without greatly disturbing the pH ,
then obviously NaOH would not be a good choice of added alkali . I have
even wondered if Hodgkinsons reference to "soda" may not be bicarbonate ,
(baking soda) which would be an even milder base perhaps most suitable
as the added alkali . And according to the same reasoning , even
better still as an added alkali may be sodium acetate or sodium citrate .
Using an alkaline salt of a weak acid in this way should allow for
more leeway in the amount of added alkali which would be useful to add
to the nitrite solution without adversely affecting the pH of the system .
If NaOH was used , even a slight error in the quantity of NaOH used
could effectively "poison" the reaction system by driving the pH too high .
The same undesired effect could occur even with the correctly calculated
amount of NaOH , if the dynamic of the reaction did not follow the rate of
addition of the NaNO2 solution including such a strong base as NaOH .
Rosco
[SNIP]
Post by Rosco P. Coaltrain
But now that we have this information that the reaction proceeds
to 85% completion , would you venture a guess as to the amount
of added NaOH (on a molar basis) to the NaNO2 which would be
a good approximation of Hodgkinsons "impure nitrite" . The
nitrite which I have on hand is exceptionally pure , so I will
have to add some alkali to it and/or use a buffer for pH control .
Rosco
Rosco P. Coaltrain
2004-02-16 10:40:17 UTC
Permalink
Don T ,

Being able to "fudge" the quantity of the buffering alkali
without upsetting the delicately balanced pH of the reaction
system is precisely the reason for not choosing NaOH as the alkali .
When you have a reaction system like this which involves several
buffer relationships between the reactants themselves , in a delicate
balance very near a neutral pH , it is a system so very close
to a delicate equilibrium that any adjustment has to be gently done
or the delicate balance will be upset by the reagent used to
make the adjustment to the pH . The dynamic for this reaction
is possibly not a linear slope either , so an alkali that can
be present in excess without upsetting the pH of the system
would be desirable for its reserve capacity to accomodate
fluctuations in pH that may not coincide with the rate of addition
of the nitrite solution . The use of a carbonate has the advantage
also that the acidic component of its molecule can escape
the system as effervescing carbon dioxide .

If NaOH was being used as the alkali , there would probably need to be
constant sampling and measurement of the pH by an automated reaction
monitoring system , an "automatic demand-type titrator/pH regulator" .
On an industrial scale this would not be any difficulty . Such
equipment is even used to regulate the pH of nutrient solutions
that are used in large hydroponic gardening operations .

For economy and expediency in working up an experimental lab scale
synthesis like this , it is just more practical to use a calculated
amount of a buffer which should regulate the pH .

Trying to calculate the exact amount of NaOH which would be needed
and at what rate it should be added is a more error prone task
for this type reaction , than "guess-timating" a ball park figure
for a buffer .

The intuitive figure that I have been thinking may be a good starting
point is using a buffer at about 20% the molar basis of the nitrite .
That is just a guess , because honestly the calculations and projections
concerning this deceptively "simple" reaction give me a headache .

There is probably some chemical engineering software that could run
the analysis of all the parameters for this narrow pH range reaction
and specify the optimum amount of which alkali is recommended .

Beyond this point for me await experiments involving trial and error ,
charting results and determining the details by observation .
Post by Don T
It is standard lab practice to make up a NaOH or KOH "standard" solution
when titration's are done. Why use Na2CO3 or even NaHCO3? other than they
are relatively less basic and you can "fudge" a bit on amounts added?
--
Don Thompson
"The only stupid questions are those that should have been asked, but
weren't, or those that have been asked and answered over and over, but the
answers not listened to." Peter Rowe
Post by Rosco P. Coaltrain
Louis ,
Please amend my last question regarding added NaOH .
I meant to ask how much added Na2CO3 (on a molar basis)
with regards to the NaNO2 *NOT* NaOH .... I was thinking "soda" ,
but mistakenly wrote the formula for "caustic soda" instead .
Since the idea is to buffer the reaction without greatly disturbing the pH
,
Post by Rosco P. Coaltrain
then obviously NaOH would not be a good choice of added alkali . I have
even wondered if Hodgkinsons reference to "soda" may not be bicarbonate ,
(baking soda) which would be an even milder base perhaps most suitable
as the added alkali . And according to the same reasoning , even
better still as an added alkali may be sodium acetate or sodium citrate .
Using an alkaline salt of a weak acid in this way should allow for
more leeway in the amount of added alkali which would be useful to add
to the nitrite solution without adversely affecting the pH of the system .
If NaOH was used , even a slight error in the quantity of NaOH used
could effectively "poison" the reaction system by driving the pH too high
.
Post by Rosco P. Coaltrain
The same undesired effect could occur even with the correctly calculated
amount of NaOH , if the dynamic of the reaction did not follow the rate of
addition of the NaNO2 solution including such a strong base as NaOH .
Rosco
[SNIP]
Post by Rosco P. Coaltrain
But now that we have this information that the reaction proceeds
to 85% completion , would you venture a guess as to the amount
of added NaOH (on a molar basis) to the NaNO2 which would be
a good approximation of Hodgkinsons "impure nitrite" . The
nitrite which I have on hand is exceptionally pure , so I will
have to add some alkali to it and/or use a buffer for pH control .
Rosco
LOUIS
2004-02-22 09:28:47 UTC
Permalink
Buffer effect will help get the pH right much easier than with NaOH wich
catches CO2 from the air to form the very same buffer upon time ;-)

Ph Z
Post by Don T
It is standard lab practice to make up a NaOH or KOH "standard" solution
when titration's are done. Why use Na2CO3 or even NaHCO3? other than they
are relatively less basic and you can "fudge" a bit on amounts added?
--
Don Thompson
"The only stupid questions are those that should have been asked, but
weren't, or those that have been asked and answered over and over, but the
answers not listened to." Peter Rowe
Post by Rosco P. Coaltrain
Louis ,
Please amend my last question regarding added NaOH .
I meant to ask how much added Na2CO3 (on a molar basis)
with regards to the NaNO2 *NOT* NaOH .... I was thinking "soda" ,
but mistakenly wrote the formula for "caustic soda" instead .
Since the idea is to buffer the reaction without greatly disturbing the pH
,
Post by Rosco P. Coaltrain
then obviously NaOH would not be a good choice of added alkali . I have
even wondered if Hodgkinsons reference to "soda" may not be bicarbonate ,
(baking soda) which would be an even milder base perhaps most suitable
as the added alkali . And according to the same reasoning , even
better still as an added alkali may be sodium acetate or sodium citrate .
Using an alkaline salt of a weak acid in this way should allow for
more leeway in the amount of added alkali which would be useful to add
to the nitrite solution without adversely affecting the pH of the system .
If NaOH was used , even a slight error in the quantity of NaOH used
could effectively "poison" the reaction system by driving the pH too high
.
Post by Rosco P. Coaltrain
The same undesired effect could occur even with the correctly calculated
amount of NaOH , if the dynamic of the reaction did not follow the rate of
addition of the NaNO2 solution including such a strong base as NaOH .
Rosco
[SNIP]
Post by Rosco P. Coaltrain
But now that we have this information that the reaction proceeds
to 85% completion , would you venture a guess as to the amount
of added NaOH (on a molar basis) to the NaNO2 which would be
a good approximation of Hodgkinsons "impure nitrite" . The
nitrite which I have on hand is exceptionally pure , so I will
have to add some alkali to it and/or use a buffer for pH control .
Rosco
LOUIS
2004-02-22 09:27:35 UTC
Permalink
If you have Na2CO3 and NaHCO3 then it will buffer the media no mather there is little NaOH or HNO3 in it.
The best is to work with a 1/2 molar amount of the buffer.

Ph Z
Post by Rosco P. Coaltrain
Louis ,
Please amend my last question regarding added NaOH .
I meant to ask how much added Na2CO3 (on a molar basis)
with regards to the NaNO2 *NOT* NaOH .... I was thinking "soda" ,
but mistakenly wrote the formula for "caustic soda" instead .
Since the idea is to buffer the reaction without greatly disturbing the pH ,
then obviously NaOH would not be a good choice of added alkali . I have
even wondered if Hodgkinsons reference to "soda" may not be bicarbonate ,
(baking soda) which would be an even milder base perhaps most suitable
as the added alkali . And according to the same reasoning , even
better still as an added alkali may be sodium acetate or sodium citrate .
Using an alkaline salt of a weak acid in this way should allow for
more leeway in the amount of added alkali which would be useful to add
to the nitrite solution without adversely affecting the pH of the system .
If NaOH was used , even a slight error in the quantity of NaOH used
could effectively "poison" the reaction system by driving the pH too high .
The same undesired effect could occur even with the correctly calculated
amount of NaOH , if the dynamic of the reaction did not follow the rate of
addition of the NaNO2 solution including such a strong base as NaOH .
Rosco
[SNIP]
Post by Rosco P. Coaltrain
But now that we have this information that the reaction proceeds
to 85% completion , would you venture a guess as to the amount
of added NaOH (on a molar basis) to the NaNO2 which would be
a good approximation of Hodgkinsons "impure nitrite" . The
nitrite which I have on hand is exceptionally pure , so I will
have to add some alkali to it and/or use a buffer for pH control .
Rosco
LOUIS
2004-02-22 09:24:54 UTC
Permalink
Post by Rosco P. Coaltrain
Louis ,
Part of the uncertainty is resolved by an additional detail in
the companion patent GB129152 filed a few weeks later by the same
inventor . In that later patent GB129152 , Hodgkinson makes
reference to the same method as described by the earlier patent ,
[QUOTE]
According to the preferred manner of carrying the invention into
effect , a solution of hydrazine as,for instance,hydrazine sulphate,
neutralized *and* RENDERED FAINTLY ALKALINE with ammonia or soda ,
and an equivalent proportion of sodium nitrite , is prepared and
this mixed solution is then added to a solution of silver nitrate
rendered slightly acid with nitric acid , under conditions
of violent agitation , the temperature being regulated so as
not to exceed 30 degrees C .
-Funny thing is that silver nitrate upon exposure to NaOH forms little soluble and
mild alkaline AgOH (Ag2O + H2O).
AgNO3 upon contact with NH4OH forms explosive silver mirror (AgNH2 + Ag3N (silver
nitride)) but also complexes of silver and ammonia...but owing to the mild acidic
amount of HNO3 all this is prevented.
Post by Rosco P. Coaltrain
Silver azide will thus be formed and will separate out under favorable
conditions in quantity equivalent to 85% of the theoretical .
The silver azide is washed with cold water and suspended or agitated
with a proportion of common salt slightly less than is required
according to the equation : AgN3 + NaCl -----> AgCl + NaN3
The reaction in these conditions is completed in a few minutes ,
and the silver chloride may then be filtered off and the solution
of sodium azide concentrated on a steam bath . In this way sodium azide
in an approximately pure state will be obtained and this sodium azide
may in accordance with the invention be employed for the formation of
lead azide or other azides by double decomposition with lead or
other salts .
[END QUOTE]
-Great.
Post by Rosco P. Coaltrain
Since litmus is the pH indicator which Hodgkinson has mentioned ,
it is probably a safe guess that the pH of the solution of the
hydrazine salt which is neutralized and "rendered faintly alkaline"
is a pH in the range of pH 7.1 to pH 8 , probably nearer pH 8 .
I need to check what pH exactly is where red litmus just begins to
go blue to more accurately guess what Hodgkinson would call
"faintly alkaline" .
-Actually litmus is mustard yellow at pH 7 turns orange and then red and finally
deep purple when in acidic media (it doesn't resist long oxydising acids); on the
contrary when it goes alkaline it passes from yellow green to green to emerald green
and then to green blue.Mild alkaline will thus be green!
Post by Rosco P. Coaltrain
This detail confirms that there is indeed free alkali present on
the left side of the equation , as I expected there should be .
Since the reaction only goes to about 85% completion , the
unreacted alkali on the left side of the equation prevents the
acidity of the system from rising too high from the acidic
product on the right side of the equation . This is the region
where the presence of a buffer in the system might possibly
allow the reaction to go to completion , instead of quenching
at 85% due to the decreasing pH . Deliberately basifying the
sodium nitrite solution in advance to a favorable alkalinity ,
and performing the reaction with more concentrated solutions
may also result in increased yields . This is quite interesting
because even at 85% yield , Hodgkinsons process is more efficient
and economical than the modern synthetic methods which are used
for current production of azides .
Economical?
NaNO3 + 3NaNH2 --> NaN3 + 3NaOH + NH3 (in solid state at 175°C)
N2O + 2NaNH2 --> NaN3 + NaOH + NH3 (in milten state stream of N2O at 190°C)
3N2O + 4Na + NH3 --> NaN3 + 3NaOH + 2N2 (in liquid NH3).

N2O is formed by heating NH4NO3.
Post by Rosco P. Coaltrain
From a few test runs , it should be possible to optimize the
concentrations of solutions and added alkali requirement .
From studying these patents , I now realize that some of my
past failed experiments would have actually worked fine , *IF*
the pH of the reactions being attempted had been very carefully
controlled . Evidently pH is absolutely the critical factor in
making these type reactions work .
This has been a very interesting and enlightening discussion :-)
I feel much more confident now about the potential for
success with any future experiments with this type of reaction ,
knowing in advance that it is a very pH critical reaction .
I know you have done some experiments already before the text
of these patents was available and we were trying to make
educated guesses concerning the parameters of this reaction .
But now that we have this information that the reaction proceeds
to 85% completion , would you venture a guess as to the amount
of added NaOH (on a molar basis) to the NaNO2 which would be
a good approximation of Hodgkinsons "impure nitrite" . The
nitrite which I have on hand is exceptionally pure , so I will
have to add some alkali to it and/or use a buffer for pH control .
-Yes even if more concise, still uncertainities...and research to do ;-).
But a 85% yield is a good base to look further .

Ph Z
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