Method and apparatus for the initiation of chemical reactions

• US 4,012,301 A
• Filed: 07/28/1975
• Issued: 03/15/1977
• Est. Priority Date: 07/28/1975
• Status: Expired due to Term

• Current Assignee: Calpine Corporation
• Original Assignee: Calpine Corporation
• Inventors: Rich, Joseph W., Raymonda, John W.
• Primary Examiner(s): Williams, Howars S.
• Application Number:
  US05/599,512
• Time in Patent Office: 596 Days
• Field of Search: 204/DIG. 11, 204/157.1 R, 204/158 R, 204/162 R, 250/527
• US Class Current: 204/157.41
• CPC Class Codes: B01J 19/121 Coherent waves, e.g. laser beams lasers per se H01S3/00

Abstract

Laser radiation is employed to initiate and promote chemical reactions by creating states of molecular vibrational mode excitation exceeding those appropriate to the translational temperature of the medium in one or more of the reactants. In favorable cases, vibrational excitation in a certain vibrational normal mode of a reactant will act to accelerate the rate of a desired chemical reaction. The reactants can be pressurized so that their vibration-rotation spectrum can be broadened to the point that laser radiation can be absorbed without the need for exact coincidence between a line or lines of the spectrum of the reactant and that of available lasers. Provision can be made for isolation and analysis of products, recycling of unused reactants, temperature control of reactants and real-time monitoring of the state of vibrational excitation of the reactants.

Claims

1. A method for initiating and accelerating vapor phase chemical reactions in a mixture of reactant species including the steps of:

supplying a plurality of reactant species to a reaction chamber;

continuously flowing the reactant species through the reaction chamber;

maintaining the reaction chamber at a pressure such that the vibration-rotation spectra of the reactant species are pressure-broadened to enhance the efficiency of absorption of laser radiation;

selectively exciting vibrational modes of at least one of the continuously flowing reactant species with a continuous wave laser which emits radiation that is absorbed by the vibrational mode of at least one reactant species to achieve a condition of high molecular vibrational excitations and low translational temperature to create a nonequilibrium mixture of the reactant species whereby the rate of vapor phase chemical reactions is accelerated while the translational and rotational modes of the mixture of reactant species is maintained relatively cold; and

withdrawing the reaction products from the reaction chamber.

2. The method of claim 1 further including the step of supplying diluent at a pressure in the range of 20 to 100 atmospheres so that the vibration-rotation spectrum of the reactant species to be excited is pressure-broadened.

3. The method of claim 1 wherein hydrogen and nitrogen are the reactant species.

4. The method of claim 1 wherein carbon monoxide and hydrogen are the reactant species.

5. The method of claim 1 wherein a mixture of reactant species is supplied to a reaction chamber.

6. The method of claim 1 wherein the step of supplying a plurality of reactant species to a reaction chamber includes controlling the temperature of the reactant species supplied to the reaction chamber.

7. The method of claim 1 further including the steps of:

recovering the reaction product;

sampling withdrawn reaction products and reaction products at selected locations in the reaction chamber;

recovering reaction products; and

recovering and recycling unreacted reaction species.

8. A method for initiating and accelerating vapor phase chemical reactions in a mixture of reactant species including the steps of:

supplying a plurality of reactant species to a reaction chamber;

continuously flowing the reactant species through the reaction chamber;

maintaining the reaction chamber at a pressure such that the vibration-rotation spectra of the reactant species are pressure-broadened to enhance the efficiency of absorption of laser radiation;

selectively exciting vibrational modes of at least one of the continuously flowing reactant species by using a transfer gas which absorbs radiation energy emitted by a continuous wave pumping laser and transfers the absorbed energy to the reactant species by inelastic molecular collisions to achieve a condition of high molecular vibrational excitations and low translational temperature to create a nonequilibrium mixture of the reactant species whereby the rate of vapor phase chemical reactions is accelerated while the translational and rotational modes of the mixture of reactant species is maintained relatively cold; and

withdrawing the reaction products from the reaction chamber.

9. Apparatus for initiating and accelerating vapor phase chemical reactions in a mixture of reactant species including:

reaction vessel means defining a flow-through high-pressure cell having inlet means for supplying a plurality of reactant species, outlet means for withdrawing reaction products and a pair of optically aligned windows which are transparent to laser radiation; and

means including a continuous wave, high power, short wavelength, electrically excited supersonic flow laser for selectively creating a state of vibrational excitation of at least one of the reactant species whereby the vibrational degree of freedom of said at least one reactant species is much higher than is appropriate to the translational temperature of the mixture of reactant species so that vapor phase chemical reactions are promoted.

10. The apparatus of claim 9 further including:

reactant species storage means and diluent storage means;

means connecting said reactant species storage means and said diluent storage means to said inlet means for supplying said reactant species and diluent to said reaction vessel means; and

means for controlling the relative amounts and pressures of the reactant species and diluent supplied to said reaction vessel means.

11. The apparatus of claim 10 further including means for controlling the temperature of the reactant species and diluent supplied to said reaction vessel means.

12. The apparatus of claim 9 further including means for supplying inert diluent to said reaction vessel means at a pressure in the range of 20 to 100 atmospheres whereby the vibration-rotation spectrum of the mixture of reactant species is pressure broadened.

13. The apparatus of claim 9 wherein said reaction vessel means is provided with means for monitoring the chemical reactions in said reaction vessel means.

14. The apparatus of claim 9 wherein said reaction vessel means is provided with means for withdrawing samples from said reaction vessel means.

15. The apparatus of claim 9 further including:

reactant species storage means;

means connecting said reactant species storage means to said inlet means and including means controlling the relative amounts, pressures and temperatures of said reactant species supplied to said reaction vessel means.

16. The apparatus of claim 15 further including:

reaction product recovery means connected to said outlet means; and

reactant recovery and recycling means connected to said reaction product recovery means and said means connecting said reactant species storage means to said inlet means.