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US3987146A Expired / Lapsed US ⏱️ 0.0 years remaining

Simultaneous removal of nitrogen oxides and sulfur oxides from combustion gases

Assignee: Energy Research and Development Administration ERDA
•
Filing: 1975-08-07
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Granted: 1976-10-19
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Expires: 1995-08-07
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Abstract

Abstract A process for the simultaneous removal of sulfur oxides and nitrogen oxides from power plant stack gases comprising contacting the stack gases with a supported iron oxide catalyst/absorbent in the presence of sufficient reducing agent selected from the group consisting of carbon monoxide, hydrogen, and mixtures thereof, to provide a net reducing atmosphere in the SO x /NO x removal zone. The sulfur oxides are removed by absorption substantially as iron sulfide, and nitrogen oxides are removed by catalytic reduction to nitrogen and ammonia. The spent iron oxide catalyst/absorbent is regenerated by oxidation and is recycled to the contacting zone. Sulfur dioxide is also produced during regeneration and can be utilized in the production of sulfuric acid and/or sulfur.

Inventors

  • 👤 David T. Clay
  • 👤 Scott Lynn

Bibliographic Details

Application Number —
Jurisdiction US
Data Source google_patents
Last Synchronized 2026-10-31 13:00
CPC Classifications
B; B01; B01D; B01D53/00; B01D53/34; B01D53/46; B01D53/60; Y; Y02; Y02A; Y02A50/00; Y02A50/20

Claims Analysis

Total Claims: 16
Claim 1
Independent Claim 149 words
A dry solids process for the simultaneous removal of SO x and NO x from diluent gases containing them wherein So x is removed by absorption substantially as a sulfide and NO x is removed by reduction which comprises: a. contacting the diluent gases in an SO x and NO x removal zone with a solid catalyst/absorbent comprising partially reduced iron oxide and ferric oxide at a temperature of at least about 370° C in the presence of an amount of a reducing agent selected from carbon monoxide, hydrogen, and a mixture thereof sufficient to provide a net reducing atmosphere in the SO x and NO x removal zone, thereby removing SO x by absorption on the catalyst/absorbent substantially as ferrous sulfide and removing NO x by reduction; and b. separating the resulting ferrous sulfide containing catalyst/absorbent from the diluent gases reduced in SO x and NO x content.
Claim 2
Dependent Claim 149 words
A dry solids process for the simultaneous removal of SO x and NO x from diluent gases containing them wherein So x is removed by absorption substantially as a sulfide and NO x is removed by reduction which comprises: a. contacting the diluent gases in an SO x and NO x removal zone with a solid catalyst/absorbent comprising partially reduced iron oxide and ferric oxide at a temperature of at least about 370° C in the presence of an amount of a reducing agent selected from carbon monoxide, hydrogen, and a mixture thereof sufficient to provide a net reducing atmosphere in the SO x and NO x removal zone, thereby removing SO x by absorption on the catalyst/absorbent substantially as ferrous sulfide and removing NO x by reduction; and b. separating the resulting ferrous sulfide containing catalyst/absorbent from the diluent gases reduced in SO x and NO x content.
Claim 3
Dependent Claim 27 words
A process according to claim 1 further defined by maintaining an amount of ferric oxide in the catalyst/absorbent at least sufficient to oxidize the excess reducing agent.
Claim 4
Dependent Claim 15 words
A process according to claim 1 wherein the catalyst/absorbent is supported on a particulate matrix.
Claim 5
Dependent Claim 23 words
A process according to claim 3 wherein the particulate matrix is a substance selected from alumina and a mixture of alumina and silica.
Claim 6
Dependent Claim 18 words
A process according to claim 1 wherein the reducing agent is a mixture comprising carbon monoxide and hydrogen.
Claim 7
Dependent Claim 32 words
A process according to claim 1 wherein SO x is SO 2 , NO x is NO, and the gases containing them are effluent gases produced by combustion of a fossil fuel.
Claim 8
Dependent Claim 31 words
A process according to claim 1 wherein the temperature in the SO x and NO x removal zone is in the range of from about 370° C to about 540° C.
Claim 9
Dependent Claim 68 words
A process according to claim 1 further defined by contacting at least a portion of the separated ferrous sulfide containing catalyst/absorbent with an oxidizing gas in a regeneration zone at a temperature of at least about 650° C, thereby regenerating the catalyst/absorbent by conversion of the iron compounds contained therein substantially to ferric oxide, and recycling the regenerated catalyst/absorbent to the SO x and NO x removal zone.
Claim 10
Dependent Claim 12 words
A process according to claim 8 wherein the oxidizing gas is air.
Claim 11
Dependent Claim 26 words
A process according to claim 8 wherein the temperature in the regeneration zone is in the range of from about 650° C to about 760° C.
Claim 12
Dependent Claim 27 words
A process according to claim 8 further defined by maintaining an amount of ferric oxide in the catalyst/absorbent at least sufficient to oxidize the excess reducing agent.
Claim 13
Dependent Claim 271 words
A dry solids process for the simultaneous removal of SO x and NO x from diluent gases containing them to provide a gas suitable for discharge into the atmosphere and wherein SO x is removed substantially as a sulfide and NO x is removed by reduction, which process comprises: a. contacting the diluent gases in an SO x and NO x removal zone with a dispersed bed of a solid catalyst/absorbent comprising partially reduced iron oxide and ferric oxide supported on a particulate matrix at a temperature of at least about 370° C in the presence of a reducing agent selected from carbon monoxide, hydrogen, and mixtures thereof in an amount sufficient to provide a net reducing atmosphere in said removal zone, thereby simultaneously removing from said diluent gases SO x by absorption on the catalyst/absorbent substantially as ferrous sulfide and NO x by reduction; b. separating the resulting ferrous sulfide containing catalyst/absorbent from the diluent gases reduced in SO x and NO x content; c. recycling a first portion of the separated ferrous sulfide containing catalyst/absorbent to the SO x and NO x removal zone; d. contacting a second portion of the separated ferrous sulfide containing catalyst/absorbent with an oxidizing gas in a regeneration zone at a temperature of at least about 650° C, thereby converting the iron compounds contained therein to ferric oxide; e. recycling regenerated catalyst/absorbent from step (d) to the SO x and NO x removal zone; and f. maintaining an amount of ferric oxide in the catalyst/absorbent recycle stream at least sufficient to oxidize excess reducing agent in the SO x and NO x removal zone.
Claim 14
Dependent Claim 271 words
A dry solids process for the simultaneous removal of SO x and NO x from diluent gases containing them to provide a gas suitable for discharge into the atmosphere and wherein SO x is removed substantially as a sulfide and NO x is removed by reduction, which process comprises: a. contacting the diluent gases in an SO x and NO x removal zone with a dispersed bed of a solid catalyst/absorbent comprising partially reduced iron oxide and ferric oxide supported on a particulate matrix at a temperature of at least about 370° C in the presence of a reducing agent selected from carbon monoxide, hydrogen, and mixtures thereof in an amount sufficient to provide a net reducing atmosphere in said removal zone, thereby simultaneously removing from said diluent gases SO x by absorption on the catalyst/absorbent substantially as ferrous sulfide and NO x by reduction; b. separating the resulting ferrous sulfide containing catalyst/absorbent from the diluent gases reduced in SO x and NO x content; c. recycling a first portion of the separated ferrous sulfide containing catalyst/absorbent to the SO x and NO x removal zone; d. contacting a second portion of the separated ferrous sulfide containing catalyst/absorbent with an oxidizing gas in a regeneration zone at a temperature of at least about 650° C, thereby converting the iron compounds contained therein to ferric oxide; e. recycling regenerated catalyst/absorbent from step (d) to the SO x and NO x removal zone; and f. maintaining an amount of ferric oxide in the catalyst/absorbent recycle stream at least sufficient to oxidize excess reducing agent in the SO x and NO x removal zone.
Claim 15
Dependent Claim 51 words
A process according to claim 12 wherein the temperature in the SO x and NO x removal zone is in the range of from about 370° C to about 540° C and the temperature in the regeneration zone is in the range of from about 650° C to about 760° C.
Claim 16
Dependent Claim 38 words
A process according to claim 12 further defined by maintaining an amount of ferrous sulfide in the catalyst/absorbent in the SO x and NO x removal zone to provide a net exothermic reaction in the subsequent regeneration step.

References Cited (Backward Citations)

US2189250A Cited
US3454355A Cited
US3695828A Cited
US3795730A Cited
US3888970A Cited
US3917800A Cited

USPTO Annuity & Maintenance Windows

Annuity Stage Window Opens Payment Deadline Surcharge Period Until Estimated Fee Status
3.5 Years (Year 4) 1979-10-19 1980-04-19 1980-10-19 $2000.00 Window Closed / Lapsed
7.5 Years (Year 8) 1983-10-19 1984-04-19 1984-10-19 $3760.00 Window Closed / Lapsed
11.5 Years (Year 12) 1987-10-19 1988-04-19 1988-10-19 $7700.00 Window Closed / Lapsed

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