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US4268415A Expired / Lapsed US ⏱️ 0.0 years remaining

Regeneration of spent hydrodesulfurization catalysts with heteropoly acids and hydrogen peroxide

Assignee: ExxonMobil Technology and Engineering Co
•
Filing: 1979-07-19
•
Granted: 1981-05-19
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Expires: 1999-07-19
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Abstract

Abstract Contacting deactivated hydrodesulfurization catalyst, such as Co-Mo supported on alumina, with a heteropoly acid, such as molybdophosphoric acid or tungstosilicic acid, to which dilute hydrogen peroxide is added, results in a significant enhancement in the rate and extent of carbon and metals removal. Forms of deposited vanadium intractable by other treatments are also removed. The process results in substantially complete regeneration of catalytic activity.

Inventors

  • 👤 Raam R. Mohan
  • 👤 Bernard G. Silbernagel
  • 👤 Gopal H. Singhal

Bibliographic Details

Application Number —
Jurisdiction US
Data Source google_patents
Last Synchronized 2026-11-08 19:20
CPC Classifications
B; B01; B01J; B01J23/00; B01J23/90; B01J23/94; C; C10; C10G; C10G45/00; C10G45/02; C10G45/04; C10G45/06; C10G45/08; Y; Y10; Y10S; Y10S502/00; Y10S502/515; Y10S502/516

Claims Analysis

Total Claims: 20
Claim 1
Independent Claim 54 words
An improved process for regenerating spent hydrofining catalysts which comprises contacting spent catalyst with an aqueous solution of a heteropoly acid containing about 1 to 50 wt.% hydrogen peroxide, based on the amount of heteropolyacid, impregnating with a water soluble cobalt or nickel salt and calcining at a maximum temperature of about 450° C.
Claim 2
Dependent Claim 54 words
An improved process for regenerating spent hydrofining catalysts which comprises contacting spent catalyst with an aqueous solution of a heteropoly acid containing about 1 to 50 wt.% hydrogen peroxide, based on the amount of heteropolyacid, impregnating with a water soluble cobalt or nickel salt and calcining at a maximum temperature of about 450° C.
Claim 3
Dependent Claim 15 words
The process of claim 1 in which spent catalyst is pre-cleaned with an organic solvent.
Claim 4
Dependent Claim 17 words
The process of claim 1 in which the catalyst is impregnated with a water soluble cobalt salt.
Claim 5
Dependent Claim 16 words
The process of claim 1 in which the impregnation and calcination are repeated at least once.
Claim 6
Dependent Claim 16 words
The process of claim 1 in which the hydrofining catalyst comprises a cobalt-molybdenum loaded alumina support.
Claim 7
Dependent Claim 76 words
The process of claim 1 in which the heteropoly acid is represented by the general formula H x (YM 12 O 40 ), where Y is at least one element selected from the group consisting of phosphorus, silicon, titanium, germanium, arsenic zirconium, thorium and cerium, M is at least one element selected from the group consisting of molybdenum, tungsten, niobium and tantalum and x is 3 when Y is pentavalent and 4 when y is tetravalent.
Claim 8
Dependent Claim 26 words
The process of claim 6 in which Y is at least one of phosphorus and silicon and M is at least one of molybdenum and tungsten.
Claim 9
Dependent Claim 14 words
The process of claim 7 in which Y is phosphorus and M is molybdenum.
Claim 10
Dependent Claim 29 words
The process of claim 6 in which up to one-half of M is replaced by at least one element selected from the group consisting of nickel, cobalt and vanadium.
Claim 11
Dependent Claim 27 words
The process of claim 1 in which the spent catalyst is contacted with the heteropoly acid/hydrogen peroxide solution at a temperature between ambient and about 80° C.
Claim 12
Dependent Claim 16 words
The process of claim 10 in which the temperature ranges from about 30° to 60° C.
Claim 13
Dependent Claim 20 words
The process of claim 1 in which the heteropoly acid in solution ranges from about 0.1 to 25 wt. %.
Claim 14
Dependent Claim 17 words
The process of claim 12 in which the concentration ranges from about 0.2 to 6 wt. %.
Claim 15
Dependent Claim 18 words
The process of claim 12 in which the solution has a pH ranging from about 1 to 3.
Claim 16
Dependent Claim 15 words
The process of claim 13 in which the pH ranges from about 1.5 to 2.5.
Claim 17
Dependent Claim 20 words
The process of claim 1 in which the concentration of hydrogen peroxide ranges from about 3 to 15 wt. %.
Claim 18
Dependent Claim 17 words
The process of claim 16 in which the concentration of hydrogen peroxide is about 15 wt. %.
Claim 19
Dependent Claim 30 words
The process of claim 1 in which the spent catalyst is contacted by the heteropoly acid/hydrogen peroxide solution for a period of time of between about 4 and 200 hours.
Claim 20
Dependent Claim 18 words
The process of claim 18 in which the period of contact ranges from about 10 to 50 hours.

References Cited (Backward Citations)

US2547380A Cited
GB644239A Cited
US3259588A Cited
US3403111A Cited
US3562150A Cited
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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) 1984-05-18 1984-11-17 1985-05-19 $2000.00 Window Closed / Lapsed
7.5 Years (Year 8) 1988-05-18 1988-11-17 1989-05-19 $3760.00 Window Closed / Lapsed
11.5 Years (Year 12) 1992-05-18 1992-11-17 1993-05-19 $7700.00 Window Closed / Lapsed

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