Gas separation: processes – Solid sorption – Including reduction of pressure
Reexamination Certificate
2001-04-30
2003-01-07
Simmons, David A. (Department: 1724)
Gas separation: processes
Solid sorption
Including reduction of pressure
C095S056000, C095S106000, C095S116000
Reexamination Certificate
active
06503298
ABSTRACT:
FIELD OF THE INVENTION
The present invention relates to hydrogen separation by thermally cycled sorption and desorption. The invention also relates to apparatus containing hydrogen sorbents.
INTRODUCTION
Purified hydrogen has long been and continues to be used in a variety of industrial processes. For example, petroleum refineries are using increasing quantities of hydrogen to meet regulatory requirements on diesel, gasoline, and other petroleum products. Hydrogen-based treating processes are expected to grow substantially because fuel regulations in North America, Europe, and other regions are becoming increasing stringent. For example, the sulfur levels in U.S. diesel fuels must decrease from the current level of 250 ppm to 15 ppm by 2007. While several options exist for lowering sulfur levels, all of commercially available processes require a hydrogen input stream.
Another major use of hydrogen is in upgrading crude oil to make gasoline. To meet the world's increasing demand for gasoline, it has been necessary to develop poorer grades of crude oil that are denser and require hydrogenation for upgrading to gasoline.
Additionally, for more than 10 years there have been intense research and development efforts directed toward hydrogen as a clean power source for fuel cells. Compared to conventional power systems, hydrogen-powered fuel cells are more energy efficient, more robust, and less polluting. Fuel cells can totally eliminate ozone and nitrogen oxides, the most noxious precusors of smog. However, problems such as excessive cost, equipment size, and process complexity have prevented hydrogen-based fuel cell technology from replacing most conventional power sources.
The present invention provides apparatus and methods for separating hydrogen. The invention can be used, for example, to purify hydrogen formed in a steam-reforming reaction (typically a gas containing hydrogen, carbon monoxide and carbon dioxide). Compared to conventional hydrogen separation technology, many of the configurations and procedures of this invention are relatively simple, scaleable over a broad range, including small, and are amenable to cost-effective mass production.
SUMMARY OF THE INVENTION
In a first aspect, the invention provides a method of separating hydrogen gas. In this method, a hydrogen-containing gas mixture passes into a channel at a first temperature. This channel includes a sorbent within the channel that has a surface exposed to the gas. Flow through the channel is constrained such that in at least one cross-sectional area of the channel, the furthest distance to a channel wall is 0.5 cm or less. The sorption, at this first temperature, occurs at a rate of at least 0.1 mol of H
2
/(second)(cm
3
of sorbent), where the volume of sorbent is the volume of sorbent used in the method and where the rate is averaged over the sorption phase of each cycle and the “first temperature” is the average temperature of the sorbent (measured, for a film, at the interface of the sorbent film and the surface of the flow channel or, for a porous sorbent, within a porous sorbent) during the sorption phase. Then, energy is added to the sorbent to increase temperature of the sorbent to a second temperature that is higher than the first temperature. At the second temperature, hydrogen is desorbed and hydrogen gas is obtained. The “second temperature” is the average temperature of the sorbent (measured as above) during the desorption phase.
In a second aspect, the invention provides a method of separating hydrogen gas that includes a first step of sorbing hydrogen gas. In this first step, a hydrogen-containing gas mixture is passed into a channel at a first temperature. This channel includes a sorbent within the channel that has a surface exposed to the gas. In a second step, energy is added to the sorbent to increase temperature of the sorbent to a temperature that is higher than the first temperature. Then, in a third step hydrogen gas desorbs at a second temperature that is higher than the first temperature and hydrogen gas is obtained. In this method, the second and third steps, combined, take 10 seconds or less and at least 20% of the hydrogen sorbed in the first step is desorbed from the sorbent.
In a third aspect, the invention provides a method of separating hydrogen gas from a gas mixture, in which, in a first step, at a first temperature, a hydrogen-containing gas mixture contacts a sorbent that sorbs hydrogen. This sorbent includes a layer of Pd or Pd alloy overlying a hydrogen sorbent. Then subsequently, in a second step, energy is added to the sorbent, thus bringing the sorbent to a second temperature that is at least 5° C. higher than the first temperature and hydrogen desorbs from the sorbent. The desorbed hydrogen obtained is in a higher purity form than the feed gas mixture.
In a fourth aspect, the invention provides a method for separating hydrogen from a gas mixture, wherein a hydrogen-containing gas mixture is passed into a first sorption region at a first temperature and first pressure, wherein the first sorption region comprises a first sorbent and wherein the sorbent temperature and pressure in the first sorption region are selected to favor sorption of hydrogen into the first sorbent in the first sorption region. Hydrogen is selectively removed from the gas mixture resulting in sorbed hydrogen in the first sorbent and a relatively hydrogen-depleted gas mixture. The relatively hydrogen-depleted gas mixture passes into a second sorption region at a second temperature and second pressure. The second sorption region comprises a second sorbent, and the temperature and pressure in the second sorption region are selected to favor sorption of hydrogen into the sorbent in the second sorption region. Hydrogen is selectively removed from the relatively hydrogen-depleted gas mixture resulting in sorbed hydrogen in the second sorbent and a relatively more hydrogen-depleted gas mixture. The second temperature is different than the first temperature. Heat is added to the first sorbent, through a distance of about 1 cm or less to substantially the entire first sorbent, to raise the first sorbent to a third temperature and hydrogen desorbs from the first sorbent. Heat is added to the second sorbent, through a distance of about 1 cm or less to substantially the entire second sorbent, to raise the second sorbent to a fourth temperature, and hydrogen desorbs from the second sorbent. Hydrogen desorbed from the first and second sorbents is obtained. The amount of hydrogen obtained from the first and second sorbents is greater than the amount that would have been obtained by operating the first and second sorbents at the same temperature, given the same total amount of added heat. Although this fourth aspect of the invention is generally applicable, it is preferred to locate the sorbent in a channel having a dimension of one cm or less that is in thermal contact with a heat exchanger to achieve rapid and efficient thermal transport.
The invention also provides an hydrogen separation apparatus in which a flow channel having an internal surface that comprises palladium (which includes a palladium alloy) on at least a portion of the internal surface. The flow channel has at least one dimension of 1 cm or less, and a heat exchanger is in thermal contact with the flow channel.
The invention further provides an hydrogen separation apparatus in which a flow channel includes an inlet, an outlet and a sorbent disposed between the inlet and the outlet. The sorbent comprises a hydrogen sorbent having a surface coating over more than 90% of the surface of the hydrogen sorbent, wherein the surface coating comprises palladium. A heat exchanger is in thermal contact with the sorbent.
In yet another aspect, the invention provides an hydrogen separation apparatus containing a flow channel with a thin film of a hydrogen sorbent. Because the film is so thin, it adheres to the apparatus even after multiple sorption/desorption cycles—conditions in which conventional hydrogen sorbents (such as nickel) would crumble.
Any
Cucksey Chad M.
Fitzgerald Sean P.
McDaniel Jeffrey S.
Monzyk Bruce F.
Perry Steven T.
Battelle (Memorial Institute)
Lawrence Frank M.
Rosenberg Frank
Simmons David A.
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