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US3959342A Expired / Lapsed US ⏱️ 0.0 years remaining

Process for the preparation of nitrilotriacetonitrile (NTN)

Assignee: Bethlehem Steel Corp
•
Filing: 1974-12-10
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Granted: 1976-05-25
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Expires: 1994-12-10
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Abstract

Abstract Nitrilotriacetonitrile (NTN) is produced in high yeilds from hydrogen cyanide, formaldehyde and ammonia, or its equivalent as an ammonium salt of a strong acid, by utilization of a critical two-stage reaction sequence within a narrow dilution ratio and temperature range. The reaction sequence steps provide for a first mixture to be prepared comprising a mixture of the formaldehyde and ammonia. No external adjustment of the pH of this mixture is permitted. A second mixture is prepared comprised of the HCN in an aqueous solution and a strong mineral acid such as sulfuric acid for adjusting the pH of the mixture to about 1 or less. NTN is produced by combining the mixtures at a temperature of from about 55° C. to about 70° C. either by adding the formaldehyde/ammonia solution to the HCN/acid solution or vice versa. The ratios and dilution of the reactants is critical for good yields. The aqueous solution of formaldehyde and ammonia or ammonium salt (calculated as ammonia) may have a ratio of total solute weight to solution weight within a range of about 25 to 60%, and an optimum mole ratio of formaldehyde to ammonia of no more than 3 to 1. In the combined mixtures a mole ratio of hydrogen cyanide to formaldehyde of 1.1 or greater and a concentration factor of total reactant weight to solution weight of from about 30 to about 40% is required. The nitrilotriacetonitrile produced may be converted by hydrolysis to the carboxylic acid, nitrilotriacetic acid (NTA) or a carboxylic acid salt such as the sodium salt, known as SNTA. NTA and its salt are useful as detergent builders.

Inventors

  • 👤 Otto A. Homberg
  • 👤 Alan H. Singleton

Bibliographic Details

Application Number —
Jurisdiction US
Data Source google_patents
Last Synchronized 2026-11-04 20:52
CPC Classifications
C; C07; C07C; C07C255/00; Y; Y02; Y02P; Y02P20/00; Y02P20/50; Y02P20/582

Claims Analysis

Total Claims: 8
Claim 1
Independent Claim 125 words
A process for the preparation of nitrilotriacetonitrile comprising: a. preparing a first aqueous solution of formaldehyde and at least one member selected from the group consisting of ammonia and ammonium salts of strong mineral acids, which solution contains no other components which would affect the pH of said solution; b. preparing a second aqueous solution of hydrogen cyanide and a strong mineral acid wherein the strong mineral acid is present in an amount precalculated to maintain the pH of the reaction of sub-paragraph (c) at a pH of about one or less; c. reacting said first aqueous solution with said second aqueous solution by combining said first aqueous solution and said second aqueous solution at a temperature from about 35° C to about 70° C.
Claim 2
Dependent Claim 125 words
A process for the preparation of nitrilotriacetonitrile comprising: a. preparing a first aqueous solution of formaldehyde and at least one member selected from the group consisting of ammonia and ammonium salts of strong mineral acids, which solution contains no other components which would affect the pH of said solution; b. preparing a second aqueous solution of hydrogen cyanide and a strong mineral acid wherein the strong mineral acid is present in an amount precalculated to maintain the pH of the reaction of sub-paragraph (c) at a pH of about one or less; c. reacting said first aqueous solution with said second aqueous solution by combining said first aqueous solution and said second aqueous solution at a temperature from about 35° C to about 70° C.
Claim 3
Dependent Claim 42 words
The process according to claim 1 wherein in step (a) the mole ratio of formaldehyde to ammonia is 3:1 or less, and the ratio of total solute weight to total solution weight is within the range of about 25 to about 60%.
Claim 4
Dependent Claim 47 words
The process according to claim 1 wherein in step (c) the reaction mixture has a concentration factor of total reactant weight to total solution weight within the range of about 30 to about 40% and a mole ratio of hydrogen cyanide to formaldehyde of 1.1 or greater.
Claim 5
Dependent Claim 200 words
A process for the preparation of nitrilotriacetonitrile comprising: a. preparing a first aqueous solution of formaldehyde and at least one member selected from the group consisting of ammonia and ammonium salts of strong mineral acids, which solution contains no other components which would affect the pH of said solution, wherein the mole ratio of formaldehyde to ammonia is less than about 3 to 1, and the ratio of total solute weight to total solution weight is within the range of about 25 to 60%; b. preparing a second aqueous solution of hydrogen cyanide and a strong mineral acid wherein the strong mineral acid is present in an amount precalculated to maintain the pH of the reaction of sub-paragraph (c) at a pH of about 1 or less; c. reacting said first aqueous solution with said second aqueous solution by combining said first aqueous solution and said second aqueous solution at a temperature of from about 35° C to about 70° C and wherein the reaction mixture has a concentration factor of total reactant weight to total solution weight within the range of about 30 to about 40% and a mole ratio of hydrogen cyanide to formaldehyde of 1.1 or greater.
Claim 6
Dependent Claim 200 words
A process for the preparation of nitrilotriacetonitrile comprising: a. preparing a first aqueous solution of formaldehyde and at least one member selected from the group consisting of ammonia and ammonium salts of strong mineral acids, which solution contains no other components which would affect the pH of said solution, wherein the mole ratio of formaldehyde to ammonia is less than about 3 to 1, and the ratio of total solute weight to total solution weight is within the range of about 25 to 60%; b. preparing a second aqueous solution of hydrogen cyanide and a strong mineral acid wherein the strong mineral acid is present in an amount precalculated to maintain the pH of the reaction of sub-paragraph (c) at a pH of about 1 or less; c. reacting said first aqueous solution with said second aqueous solution by combining said first aqueous solution and said second aqueous solution at a temperature of from about 35° C to about 70° C and wherein the reaction mixture has a concentration factor of total reactant weight to total solution weight within the range of about 30 to about 40% and a mole ratio of hydrogen cyanide to formaldehyde of 1.1 or greater.
Claim 7
Dependent Claim 54 words
A process according to claim 4 wherein a portion of the mother liquor centrifugate from the nitrilotriacetonitrile product slurry derived from the reaction of paragraph 4(c) is recycled to the reaction vessel such that said mother liquor represents a portion of the weight of the reaction medium solvent for said reaction of paragraph 4(c).
Claim 8
Dependent Claim 28 words
A process according to claim 5 wherein the recycled mother liquor represents at least 30% of the weight of the reaction medium solvent for the reaction paragraph 4(c).

References Cited (Backward Citations)

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USPTO Annuity & Maintenance Windows

Annuity Stage Window Opens Payment Deadline Surcharge Period Until Estimated Fee Status
3.5 Years (Year 4) 1979-05-25 1979-11-24 1980-05-25 $2000.00 Window Closed / Lapsed
7.5 Years (Year 8) 1983-05-25 1983-11-24 1984-05-25 $3760.00 Window Closed / Lapsed
11.5 Years (Year 12) 1987-05-25 1987-11-24 1988-05-25 $7700.00 Window Closed / Lapsed

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