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AU1035601A - A process for producing bismuth dithiocarbamates and dithiophosphorates - Google Patents

A process for producing bismuth dithiocarbamates and dithiophosphorates Download PDF

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Publication number
AU1035601A
AU1035601A AU10356/01A AU1035601A AU1035601A AU 1035601 A AU1035601 A AU 1035601A AU 10356/01 A AU10356/01 A AU 10356/01A AU 1035601 A AU1035601 A AU 1035601A AU 1035601 A AU1035601 A AU 1035601A
Authority
AU
Australia
Prior art keywords
bismuth
represented
dithiocarbamate
dithiophosphorate
reaction
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Abandoned
Application number
AU10356/01A
Inventor
Robert Cisler
Hocine Faci
Shih-Ying Hsu
Randall Krinker
Curtis Lege
Bill Pastore
Andrew Phillips
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Castrol Ltd
Original Assignee
Castrol Ltd
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Priority claimed from GBGB0002524.7A external-priority patent/GB0002524D0/en
Application filed by Castrol Ltd filed Critical Castrol Ltd
Publication of AU1035601A publication Critical patent/AU1035601A/en
Abandoned legal-status Critical Current

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Classifications

    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10MLUBRICATING COMPOSITIONS; USE OF CHEMICAL SUBSTANCES EITHER ALONE OR AS LUBRICATING INGREDIENTS IN A LUBRICATING COMPOSITION
    • C10M135/00Lubricating compositions characterised by the additive being an organic non-macromolecular compound containing sulfur, selenium or tellurium
    • C10M135/12Thio-acids; Thiocyanates; Derivatives thereof
    • C10M135/14Thio-acids; Thiocyanates; Derivatives thereof having a carbon-to-sulfur double bond
    • C10M135/18Thio-acids; Thiocyanates; Derivatives thereof having a carbon-to-sulfur double bond thiocarbamic type, e.g. containing the groups
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C333/00Derivatives of thiocarbamic acids, i.e. compounds containing any of the groups, the nitrogen atom not being part of nitro or nitroso groups
    • C07C333/14Dithiocarbamic acids; Derivatives thereof
    • C07C333/18Esters of dithiocarbamic acids
    • C07C333/20Esters of dithiocarbamic acids having nitrogen atoms of dithiocarbamate groups bound to hydrogen atoms or to acyclic carbon atoms
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07FACYCLIC, CARBOCYCLIC OR HETEROCYCLIC COMPOUNDS CONTAINING ELEMENTS OTHER THAN CARBON, HYDROGEN, HALOGEN, OXYGEN, NITROGEN, SULFUR, SELENIUM OR TELLURIUM
    • C07F9/00Compounds containing elements of Groups 5 or 15 of the Periodic Table
    • C07F9/02Phosphorus compounds
    • C07F9/06Phosphorus compounds without P—C bonds
    • C07F9/16Esters of thiophosphoric acids or thiophosphorous acids
    • C07F9/165Esters of thiophosphoric acids
    • C07F9/17Esters of thiophosphoric acids with hydroxyalkyl compounds without further substituents on alkyl
    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10MLUBRICATING COMPOSITIONS; USE OF CHEMICAL SUBSTANCES EITHER ALONE OR AS LUBRICATING INGREDIENTS IN A LUBRICATING COMPOSITION
    • C10M137/00Lubricating compositions characterised by the additive being an organic non-macromolecular compound containing phosphorus
    • C10M137/02Lubricating compositions characterised by the additive being an organic non-macromolecular compound containing phosphorus having no phosphorus-to-carbon bond
    • C10M137/04Phosphate esters
    • C10M137/10Thio derivatives
    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10MLUBRICATING COMPOSITIONS; USE OF CHEMICAL SUBSTANCES EITHER ALONE OR AS LUBRICATING INGREDIENTS IN A LUBRICATING COMPOSITION
    • C10M2219/00Organic non-macromolecular compounds containing sulfur, selenium or tellurium as ingredients in lubricant compositions
    • C10M2219/06Thio-acids; Thiocyanates; Derivatives thereof
    • C10M2219/062Thio-acids; Thiocyanates; Derivatives thereof having carbon-to-sulfur double bonds
    • C10M2219/066Thiocarbamic type compounds
    • C10M2219/068Thiocarbamate metal salts
    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10MLUBRICATING COMPOSITIONS; USE OF CHEMICAL SUBSTANCES EITHER ALONE OR AS LUBRICATING INGREDIENTS IN A LUBRICATING COMPOSITION
    • C10M2223/00Organic non-macromolecular compounds containing phosphorus as ingredients in lubricant compositions
    • C10M2223/02Organic non-macromolecular compounds containing phosphorus as ingredients in lubricant compositions having no phosphorus-to-carbon bonds
    • C10M2223/04Phosphate esters
    • C10M2223/045Metal containing thio derivatives

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Health & Medical Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Biochemistry (AREA)
  • General Health & Medical Sciences (AREA)
  • Molecular Biology (AREA)
  • Lubricants (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)

Description

WO 01/32612 PCT/GBOO/03909 1 A PROCESS FOR PRODUCING BISMUTH DITHIOCARBAMATES AND DITHIOPHOSPHORATES The present invention concerns a process for producing oil-soluble bismuth dithiocarbamates and dithiophosphorates. In the past, bismuth dithiocarbamates have been prepared by reacting bismuth halide such as bismuth trichloride with a dithiocarbamate. The reaction is a displacement reaction which produces hydrogen chloride as a by-product. One drawback of this reaction is that undesirable residues of chloride can remain in the product. These residues can be from partially reacted by-products, unreacted bismuth trihalide or metal halides generated in situ. Even small amounts of these residues are considered to be undesirable. US-A-5,631,214 discloses a process for producing bismuth dithiocarbamates using an exchange reaction between a bismuth carboxylate and a metal dithiocarbamate. Although the product produced in this reaction is not contaminated with a residue of chloride, it is contaminated with metal carboxylate (see lines 62-64 in column 2) An aim of this invention is to provide an improved method for producing oil-soluble bismuth dithiocarbamates and dithiophosphorates. A further aim of this invention is to provide a method for producing bismuth dithiocarbamates and dithiophosphorates in which the product is not contaminated with residues of chloride or metal carboxylate. In accordance with the present invention there is provided a process for producing a bismuth dithiocarbamate or dithiophosphorate by the reaction of a bismuth hydroxide, bismuth oxide or bismuth oxynitrate with either a dithiocarbamate or dithiophosphoric acid.
WO 01/32612 PCT/GBOO/03909 2 In the reaction, water is produced as a by-product, which can be easily removed from the reaction. The bismuth dithiocarbamate or dithiophosphorate produced in this process is free from the contaminants contained in the organometallic dithio-compounds produced by the prior art methods. The bismuth dithiocarbamate or dithiophosphorate produced by this process is also structurally different from the organometallic dithio-compounds produced in the above mentioned prior art methods. The bismuth dithiocarbamate or dithiophosphorate produced in this process is a very good extreme pressure agent. It also exhibits very good anti-wear properties. These properties make the product useful and unique in lubricant formulations. The bismuth oxide, bismuth hydroxide or bismuth oxynitrate may be represented by the following formulas: Bi 2
O
3 , Bi(OH) 3 , or BiO(OH) 9
(NO
3
)
4 respectively. The dithiocarbamate or dithiophosphorate used as the starting material in the process of the present invention is preferably prepared prior to use, freshly distilled or generated in situ. A solvent can be used in the reaction, but is not essential. Suitable solvents are, for example, dimethyl sulfoxide, N,N-dimethylformamide, tetrahydrofuran, acetonitrile, benzonitrile, or commonly used polar or aprotic solvents, including any viscosity grade of paraffinic and naphthanic basestocks. The preferred solvent is acetonitrile or a 100 SUS base oil. The reaction is preferably conducted at a temperature between 50 to 200 "C. The reaction is more preferably conducted at a temperature between 60 and 130 OC. The reaction is preferably conducted under pressure of 10-1000 psi of nitrogen, air or hydrogen sulfide. The most preferred pressure is between 60-250 psi of nitrogen.
WO 01/32612 PCT/GBOO/03909 3 The dithiocarbamate is preferably represented by the following formula:
R
3 S C -SH R 4 wherein R 3 and R 4 may be the same or different, or one of them is a H. R 3 and R 4 are preferably selected from the following groups: alkyl, alkenyl, cycloalkyl, cycloalkenyl, aryl, arylalkyl or hydrocarbyl groups, optionally incorporated with hetero atoms such as nitrogen, oxygen or sulfur atoms.
R
3 and R 4 are preferably represented by the following formula:
CH
3
(CH
2 )m-X-(CH 2 )n wherein: m is 1-30, preferably 1-20, and n ranges from 1-10, preferably from 1-5. X can be oxygen, nitrogen or sulfur. When bismuth oxide, hydroxide or oxynitrate is reacted with dithiocarbamate (commonly referred to as 'DTC') in accordance with the present invention, the product can be represented by the following formula: Bi(OH),(DTC)y(NO 3 ), wherein x+y+z=3, and z is zero when the bismuth oxide or hydroxide is used as one of the starting materials. The dithiophosphoric acid is preferably represented by the following formula
R
5 0 S P- SH
R
5 0 wherein R 5 is a hydrocarbyl group having a carbon chain length of 1-20, preferably of 1-10. The dithiophosphoric acid can be prepared by reaction of the an alcohol having the R 5 group with a phosphorous pentasulfide, which is well-known to persons skilled in the art. The reaction temperature and time for the reaction of the WO 01/32612 PCT/GBOO/03909 4 bismuth oxide, hydroxide or oxynitrate with the dithiophosphoric acid are the same as mentioned above for the reaction of the bismuth hydroxide or oxide with the dithiocarbamate. The bismuth dithiophosphorate produced in accordance with the present invention is preferably represented by the following general formula: Bi(OH)m(DTP)n(NO 3 )o wherein m+n+o=3, and o is zero when Bi 2 0 3 or Bi(OH) 3 is used in the process. The product may appear as a brown-red oil or a yellow solid which is very soluble in non-polar solvents such as pentane or hexane. The product exhibits excellent solubility in paraffinic or naphthanic base stocks. The bismuth dithiocarbamates and dithiophosphorates produced in the process of the present invention exhibit load-carrying and antiwear characteristics. The bismuth dithiocarbamates and dithiophosphorates may, for example, be incorporated into a standard grease formulation. The present invention will now be described, by way of example only, with reference to the following examples: Example 1 Preparation of Bismuth (1ll) diamyldithiocarbamate using Bismuth Oxide A suspension of bismuth (Ill) oxide (9.2g, 0.0198 mol) and diamyldithiocarbamate (27.9g, 0.119 mol) was prepared in acetonitrile (200 ml). The suspension was brought to reflux and then maintained at that temperature for 5 hours. A brown suspension was produced. The brown suspension was filtered, and the solvent was evaporated under reduced pressure to produce a viscous brown liquid (13.0g).
WO 01/32612 PCT/GBOO/03909 5 Example 2 Preparation of Bismuth (111) Dioctyldithiocarbamate using Bismuth Oxide A suspension of bismuth (111) oxide (34.3g, 0.0736 mol) and di-n-octylamine (106g, 0.4416 mol) was prepared in acetonitrile (200 ml). The suspension was cooled to 15 'C, followed by a slow addition of carbon disulfide (27 ml, 0.4416 mol) over a 30 minute period. The mixture was then refluxed for 5 hours during which the colour of the mixture changed from yellow to a brownish colour. The resultant mixture was filtered and the solvent was evaporated under reduced pressure to produce a viscous brown oil (120g). Example 3 Preparation of Bismuth (111) Diamyldithiocarbamate Using Bismuth Oxynitrate A suspension of bismuth (Ill) oxynitrate (20.5g, 0.0789 mol) and diamylamine (37.2g, 0.2367 mol) was prepared in acetonitrile (200 ml). Carbon disulfide (15mI, 0.2367 mol) was slowly added at ambient temperature. A slight exotherm occurred which took the reaction temperature up by 10 0 C. A yellow mixture was produced which was refluxed for 5 hours to produce a brown liquid. The brown liquid was filtered and the solvent was evaporated to produce a brown liquid (40g). Example 4 Preparation of Bismuth (Ill) Diisononyldithiocarbamate Using Bismuth Oxynitrate A suspension of bismuth (111) oxynitrate (24.4g, 0.0936 mol) and diisononylamine (75.5g, 0.2808 mol) was prepared in acetonitrile (200 ml). Carbon disulfide (17ml, 0.2367 mol) was added slowly at ambient temperature. A slight exotherm took place on addition of the carbon disulfide which brought the temperature up by 10 *C. A yellow mixture was produced which was refluxed for 5 hours. After filtration and WO 01/32612 PCT/GBOO/03909 6 solvent removal, the product produced was a brown paste (47g). Further purification was conducted by dissolving the brown paste in hexane (300 ml), followed by cooling at 40 OF overnight to effect recrystallization and produce a bright yellow solid. Example 5 Preparation of Bismuth (Ill) 2-Ethylhexyldithiophosphorate Using Bismuth Hydroxide A suspension of bismuth (ll) hydroxide (27.0g, 0.1036 mol) and 2,6-di-t-butyl-4-methyl phenol (BHT, 500mg) was prepared in acetonitrile (200ml). 2-ethylhexyldithiophosphoric acid (109g, 0.3108 mol) was added over a 15 minute period. The resultant suspension was heated under reflux for 8 hours to produce a yellow liquid. The yellow liquid was filtered and the solvent was evaporated under reduced pressure to produce a reddish oil (131g). The performance of the bismuth dithiocarbamate and bismuth dithiophosphorate prepared above in Examples 3 and 5 respectively were compared to a commercial EP additive. The results are given below: TEST ASTM Grease with Grease with Grease with METHOD Commercial BiDADTC BiDIODTP EP Additive prepared in prepared in Example 3 Example 5 Four-ball EP D-2596 400 500 400 Weld Load, Kg Four-ball D2265 0.54 0.83 0.51 Wear mm Scar The grease used in the above test was lithium 12-hydroxystearate. The commercial EP additive was antimony dithiocarbamate. As shown above, the oil-soluble bismuth dithiocarbamate prepared in Example 3 exhibited better EP results than the commercial EP additive.
WO 01/32612 PCT/GBOO/03909 7 As also shown above, the bismuth dithiophosphorate prepared in Example 5 exhibited better wear results than the commercial EP additive. The oil-soluble bismuth dithiophosphorates produced in the above Examples also exhibited an improved reduction in the coefficient of friction and enhanced thermo-oxidative stability.

Claims (15)

1. A process for producing a bismuth dithiocarbamate or dithiphosphorate by the reaction of bismuth hydroxide, bismuth oxide or bismuth oxynitrate with a dithiocarbamate or dithiophosphoric acid.
2. The process claimed in claim 1, wherein the bismuth oxide, bismuth hydroxide or bismuth oxynitrate is represented by the following formulas: Bi 2 0 3 , Bi(OH) 3 , or BiO(OH) 9 (NO 3 ) 4 respectively.
3. The process claimed in claims 1 or 2, wherein a solvent is not used in the process.
4. The process claimed in claim 3, wherein the solvent is selected from: dimethyl sulfoxide, N,N-dimethylformamide, tetrahydrofuran, acetonitrile, benzonitrile, or commonly used polar or aprotic solvents including paraffinic and naphthanic basestocks.
5. The process claimed in claims 3 or 4, wherein the solvent is acetonitrile or a 100 SUS base oil.
6. The process claimed in any one of the preceding claims, wherein the reaction is conducted at a temperature between 50 to 200 "C, preferably at a temperature between 60 and 130 "C.
7. The process claimed in any one of the preceding claims, wherein the reaction is conducted under pressure between 10-1000 psi of nitrogen, air or hydrogen sulfide; preferably 6-250 psi of nitrogen.
8. The process claimed in any one of the preceding claims, wherein the dithiophosphoric acid is represented by the following formula: WO 01/32612 PCT/GBOO/03909 9 R 3 S C -SH R 4 wherein R 3 and R 4 may be the same or different, and only one of them is a H; R 3 and R 4 are selected from the following groups: alkyl, alkenyl, cycloalkyl, cycloalkenyl, aryl, arylalkyl or hydrocarbyl groups, optionally with hetero atoms such as nitrogen or oxygen atoms; and R 3 and R 4 are preferably represented by the following formula: CH 3 (CH 2 )m-X-(CH 2 )n wherein: m is 1-30, preferably 1-20, and n ranges from 1-10, preferably from 1-5. X can be oxygen or nitrogen.
9. The process claimed in any one of the preceding claims, wherein the process produces a bismuth dithiocarbamate represented by the following formula: Bi(OH),((DTC)y(NO3), wherein x+y+z=3, and z is zero when the bismuth oxide or hydroxide is represented by Bi 2 0 3 or Bi(OH) 3 .
10. The process claimed in any one of the preceding claims, wherein the dithiophosphoric acid is represented by the following formula: R 5 0 S \| P- SH R 5 0 wherein R 5 is a hydrocarbyl group having a carbon chain length of 1-20, preferably of 1-10.
11. The process claimed in claim 10, wherein the process produces a bismuth dithiophosphorate represented by the following general formula: Bi(OH)m(DTP)n(NO 3 )o wherein m+n+o=3, and o is zero when Bi 2 0 3 or Bi(OH) 3 is used. WO 01/32612 PCT/GBOO/03909 10
12. Use of the bismuth dithiocarbamate or dithiophosphorate produced by any one of the processes claimed in claims 1-11, as an extreme pressure agent and/or an antiwear agent.
13. A lubricant or a grease comprising the bismuth dithiocarbamate or dithiophosphorate produced in any one of claims 1-11.
14. A bismuth dithiocarbamate represented by the following general formula: Bi(OH),(DTC)y(NO3), wherein x+y+z=3.
15. A bismuth dithiophosphorate represented by the following general formula: Bi(OH).(DTP)n(NO 3 )o wherein m+n+o=3.
AU10356/01A 1999-11-05 2000-10-12 A process for producing bismuth dithiocarbamates and dithiophosphorates Abandoned AU1035601A (en)

Applications Claiming Priority (5)

Application Number Priority Date Filing Date Title
US16356999P 1999-11-05 1999-11-05
US60163569 1999-11-05
GB0002524 2000-02-04
GBGB0002524.7A GB0002524D0 (en) 2000-02-04 2000-02-04 A process for producing organometallic dithio-compounds and the orgenometallic dithio-compounds produced therefrom
PCT/GB2000/003909 WO2001032612A1 (en) 1999-11-05 2000-10-12 A process for producing bismuth dithiocarbamates and dithiophosphorates

Publications (1)

Publication Number Publication Date
AU1035601A true AU1035601A (en) 2001-05-14

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Country Status (7)

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EP (1) EP1226117A1 (en)
JP (1) JP2003513067A (en)
CN (1) CN1387510A (en)
AU (1) AU1035601A (en)
BR (1) BR0015134A (en)
CA (1) CA2389296A1 (en)
WO (1) WO2001032612A1 (en)

Families Citing this family (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP1498472B1 (en) 2003-07-04 2016-11-16 JTEKT Corporation Use of a Grease Composition in a Rolling Bearing
DE102012014395B3 (en) * 2012-07-13 2013-08-22 Oxea Gmbh Isononylamines starting from 2-ethylhexanol, process for their preparation and their use
CN105056986B (en) * 2015-08-10 2017-04-05 南京信息工程大学 A kind of method and catalyst applications for preparing lamellar hydroxyl bismuth subnitrate photocatalyst

Family Cites Families (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4632950A (en) * 1985-09-09 1986-12-30 Pennwalt Corporation Scorch resistant, crosslinkable composition containing mixture of copper and metal dithiocarbamates
US5631214A (en) * 1995-07-31 1997-05-20 R.T. Vanderbilt Company, Inc. Preparation of bismuth dithiocarbamates

Also Published As

Publication number Publication date
BR0015134A (en) 2002-06-25
EP1226117A1 (en) 2002-07-31
CA2389296A1 (en) 2001-05-10
CN1387510A (en) 2002-12-25
JP2003513067A (en) 2003-04-08
WO2001032612A1 (en) 2001-05-10

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