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02.05.2014
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Kirk-Othmer: “Encyclopedia of Chemical Technology 4th edition” 1995, John Wiley & Sons, New York (US) XP002226757, p.
FIELD OF THE INVENTIONThis invention relates to a method of methanol production having reduced emission of carbon dioxide.BACKGROUND OF THE INVENTIONMethanol is a synthetic fuel which is produced from reactants which provide carbon, hydrogen and oxygen. Dilwale Full Movie Watch Online Free Known as the most romantic pair of Bollywood, Shah Rukh Khan & Kajol will reunite in this film after a long time. Daayre Lyrics from Dilwale: The song is sung by Arijit Singh and composed by Pritam with lyrics penned by Amitabh Bhattacharya featuring Shahrukh Khan and Kajol.
Janam Janam Lyrics from Dilwale A romantic song sung by Arijit Singh and Antara Mitra featuring Shahrukh Khan and Kajol. Manma Emotion Jaage Lyrics from Dilwale A peppy dance number featuring Varun Dhawan and Kriti Sanon. Gerua Full Song Lyrics from Dilwale Full movie Watch Online (2015) sung by Antara Mitra, Arijit Singh. Ghayal Once Again Full Movie (previously titled as Ghayal Returns) is an upcoming Indian action drama film directed by Sunny Deol [1] and produced by Dharmendra.
Daayre Lyrics from Dilwale: Arijit Singh sings this song composed by Pritam starring SRK, Kajol with lyrics penned by Amitabh Bhattacharya.
Janam Janam Lyrics from Dilwale A romantic song sung by Arijit Singh and Antara Mitra featuring Shahrukh Khan and Kajol. Janam Janam Lyrics from Dilwale (2015) sung by Antara Mitra, Arijit Singh. Mera desi typical saiyanPeepal ki thandi chhaiyamein naache ta ta thaiyathaiya saiyan saiyan thaiya. Ghayal Once Again Full Movie (previously titled as Ghayal Returns) is an upcoming Indian action drama film directed by Sunny Deol [1] and produced by Dharmendra. It is the sequel to 1990 super-hit film Ghayal. We have combined here Hindi movie Dilwale links from dailymotion, YouTube, vimeo, putlocker, cloudy, videoweed, Movshare, Vevo etc.
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The process as claimed in claim 1 further comprising the step of recovering at least a portion of the oxygen produced by electrolyzing water to produce at least a portion of the oxygen feedstock.
The process as claimed in claim 2 wherein essentially all of the hydrogen and the oxygen is obtained by electrolysis. The process as claimed in claim 2 wherein at least a portion of electricity used to electrolyze the water is valley power. The process as claimed in claim 1 further comprising the step of adjusting the amount of the oxygen feedstock to the amount of the hydrocarbon feed stock fed to the partial oxidation reactor such that the partial oxidation reactor effluent contains some unoxidized hydrocarbon feedstock.
The process as claimed in claim 5 wherein the partial oxidation reactor effluent contains less than about 10 wt % of the unoxidized hydrocarbon feedstock based on the weight of the partial oxidation reactor effluent. The process as claimed in claim 5 wherein the synthesis gas contains less than about 4 wt % of the unoxidized hydrocarbon feedstock based on the weight of the partial oxidation reactor effluent. The process as claimed in claim 5 further comprising the step of adjusting the amount of the oxygen feedstock to the amount of the hydrocarbon feed stock fed to the partial oxidation reactor such that the partial oxidation reactor effluent is essentially free of oxygen.
The process as claimed in claim 1 wherein the synthesis gas, which is subjected to methanol synthesis has a ratio of hydrogen minus carbon dioxide mole fraction to carbon dioxide plus carbon monoxide mole fraction is about 2:1.
The process as claimed in claim 1 wherein the tail gas stream contains nitrogen and the tail gas stream is treated in step(e) such that the purge stream is nitrogen rich and the recycle stream is a nitrogen reduced waste gas stream. The process as claimed in claim 11 wherein a membrane separator is used to separate the tail gas stream into the nitrogen reduced waste gas stream and the nitrogen rich purge stream.
The process as claimed in claim 12 further comprising combusting the nitrogen rich purge stream to produce energy. The process as claimed in claim 13 wherein the combustion of the purge stream produces heat that is used to preheat at least one of the feedstocks of the partial oxidation reactor. The process as claimed in claim 13 wherein the combustion of the purge stream produces electricity. The process as claimed in claim 1 wherein the partial oxidation reactor produces waste heat and the waste heat is used to generate electricity. The process as claimed in claim 1 wherein the electrolysis is conducted by running a fuel cell in reverse.
The process as claimed in claim 1 further comprising recovering oxygen from electrolysis step (b) to produce the oxygen feedstock.
The process as claimed in claim 19 further comprising combusting the purge stream to produce energy.
The process as claimed in claim 20 wherein the combustion of the purge stream produces heat that is used to preheat at least one of the feedstocks of the partial oxidation reactor. The process as claimed in claim 20 wherein the combustion of the purge stream produces electricity.
The process as claimed in claim 19 wherein the partial oxidation reactor produces waste heat and the waste heat is used to generate electricity.
The process as claimed in claim 19 wherein the electrolysis is conducted by running a fuel cell in reverse.
The process as claimed in claim 19 wherein all of the oxygen feedstock is obtained from the oxygen stream. The duo worked together in blockbusters like Baazigar, Diwale Dulhaniya Le Jayenge, Karan Arjun, Kuch Kuch Hota Hai & Kabhi Khushi Kabhi Gham.
Starring Shah Rukh Khan, Kajol, Kriti Sanon, Varun Dhawan, Kabir Bedi, Boman Irani, Sanjay Mishra, Mukesh Tiwari, Johnny Lever , Varun Sharma, Vinod Khanna, Murli Sharma, Chetan Pandit, Chetna Pande.
Daayre Lyrics - One more love song from Dilwale movie sung by Arijit Singh, is composed by Pritam, written by Amitabh Bhattacharya. Manma Emotion Jaage song from Dilwale is sung by Amit Mishra, Anushka Manchanda & Antara Mitra and composed by Pritam.
Gerua Lyrics song is composed by Pritam Chakraborty with lyrics penned by Amitabh Bhattacharya. This couple is so many time work together like baazigar, dilwale dulhania le jayenge, kuch kuch hota hai, kabhi khushi kabhie gham. But his role was scrapped from the film. Dilwale 2015 Full Movie Watch Online Rohit Shetty had earlier expressed interest to work with SRK on a remake of the 1982 comedy Angoor, before working on Chennai Express. Starring Shah Rukh Khan, Kajol, Kriti Sanon, Varun Dhawan, Kabir Bedi, Boman Irani, Sanjay Mishra, Mukesh Tiwari, Johnny Lever , Varun Sharma, Vinod Khanna, Murli Sharma, Chetan Pandit, Chetna Pande. This song is composed by Pritam Chakraborty with lyrics penned by Amitabh Bhattacharya. Dilwale Full Movie Watch Online.


This couple is so many time work together like baazigar, dilwale dulhania le jayenge, kuch kuch hota hai, kabhi khushi kabhie gham. Gerua Full Song Lyrics from Dilwale is sung by Arijit Singh & Antara Mitra and featuring Shah Rukh Khan and Kajol.
Dilwale releases on 18 December 2015. Daayre Lyrics from Dilwale (2015) sung by Arijit Singh.
Dilwale Full Movie Kajol was in Varun’s first movie Student of the Year, but she just had a cameo. However, for the ease of reading, we have just written pink here in the song’s translation.
Ghayal Once Again Full Movie Download promo was released along with salman khan’s ready (2011 film). 5,496,589 Fong et al.) and heavy hydrocarbons such as pitch and atmospheric and vacuum residues (see for example Canadian Patent Application No. Similarly, the oxygen and hydrogen which are combined with the carbon during the synthesis step to form methanol may be obtained from various sources. 5,416,245 (McGregor et al.) disclosed the use of electrolysis to provide hydrogen and oxygen. The reduced emissions associated with methanol will not favor its production unless methanol can be produced in a cost effective manner.
In the retail marketplace, methanol must be priced competitively with gasoline and diesel fuel to be a commercial alternative fuel.The advantage of methanol being a low polluting fuel will be reduced, or potentially lost, if the process for producing methanol has substantial emissions of greenhouse gases.
Typical commercial processes which are in operation to date produce about 600 to 1200 pounds of carbon dioxide per ton of methanol produced. Therefore, while the methanol produced by these processes may be relatively non-polluting compared to gasoline and diesel fuel when it is combusted, when considered with the manufacturing process, the production and use of methanol may in fact be a substantial source of greenhouse gases.SUMMARY OF THE INVENTIONIn accordance with the instant invention, a process for the production of methanol is provided which has a reduced emission of carbon dioxide as a by-product of the manufacturing process. In particular, in accordance with the instant invention, a process for the production of methanol may result in the emission of only 240 pounds of carbon dioxide per ton of methanol produced and, preferably, 120 pounds or less of carbon dioxide per ton of methanol produced.
For example, the process may consume up to about 650 pounds of CO2 per ton of methanol produced.In accordance with one aspect of this invention, a partial oxidation reactor is utilized to produce the synthesis gas which is then subjected to methanol synthesis to produce methanol and a tail gas stream. The remainder of the stream, or essentially all of the remainder of the stream, is recycled to the partial oxidation reactor. In this way, carbon dioxide, as well as carbon monoxide and methane, may be recycled through the system essentially to extinction except for the purge stream.
The amount of greenhouse gases emitted by the process effectively depends upon the relative size of the purge gas stream to the recycle stream.
The recycle stream may comprise up to 95 weight percent, and preferably from 50 to 95 weight percent of the tail gas stream, based on the weight of the tail gas stream.In order to reduce the size of the purge stream, the introduction of inert gases into the system is reduced. To this end, the oxygen which is used in the partial oxidation reactor preferably comprises essentially pure oxygen. Not only does this result in the need to increase the size of the process equipment to have the same through put of methanol, but it also requires a larger purge stream and the consequential emission of additional greenhouse gases.Typically, methanol production processes utilize reformers to provide additional hydrogen to the synthesis gas to obtain the desired stoichiometric of hydrogen to CO and CO2. Reformers, such as steam reformers, require the introduction of substantial quantities of water into the process and may result in the production of additional carbon dioxide at the expense of carbon monoxide formation. However, in one embodiment of the instant invention, a reformer is used to consume hydrogen in the conversion of CO2 to CO. In accordance with another aspect of the instant invention, a hydrogen source other than reformers is utilized to adjust the hydrogen balance of the synthesis gas just ahead of the methanol reactor. Preferably, at least some of the hydrogen is obtained by electrolysis and more preferably essentially all of the hydrogen is obtained by electrolysis.In a further preferred aspect of the instant invention, at least some of the electricity which is utilized in operating the electrolysis step is obtained as off-peak or valley power from a power grid. Typically, the power demand of a power grid varies throughout the day with the power demand from the grid being reduced at night when commercial and residential requirements are reduced. Not only may off-peak or valley power be obtainable at a reduced rate compared to peak demand time, but, in addition, the use of valley power may result in more efficient operation of power generating plants.
For example, if it is necessary to reduce the electrical output of a power generation plant, then the efficiency of the plant may be reduced. Alternately, it may not be possible to reduce the power output of a generating plant thus resulting in the emission of greenhouse gases to produce power which is not required. Therefore, the use of valley power to run at least a portion of the electrolysis step may be highly beneficial.
In fact, the oxygen and hydrogen produced by electrolysis such as at night may be stored in storage tanks so as to ensure a continuous supply of hydrogen and oxygen.
In this way, the feed of raw materials to produce a synthesis gas may be leveled to ensure a uniform continuous supply. In a further alternate embodiment, the electricity may be generated by running a fuel cell in reverse (i.e.
2 is a schematic drawing of an alternate preferred embodiment in accordance with the instant invention;FIG. 3 is a schematic drawing of a further alternate preferred embodiment in accordance with the instant invention; and,FIG. 4 is a schematic drawing of a further alternate preferred embodiment in accordance with the instant invention.DETAILED DESCRIPTION OF THE INVENTIONAs shown in FIG. 1, according to a preferred embodiment of the instant invention, the process comprises partial oxidation reactor 10 and methanol synthesis reactor 12. Hydrocarbon feedstock 14 and oxygen feedstock 16 are fed to partial oxidation reactor 10 to produce synthesis gas 18. Hydrogen feedstock 20 is combined with synthesis gas 18 to produce synthesis gas 22 wherein the stoichiometric balance has been adjusted.
The adjusted synthesis gas 22 is fed to methanol synthesis reactor 12 to produce tail gas 24 and methanol 26.In steam reformation processes, steam is added to a reformer. Further, the hydrocarbon feedstock fed to the stream reformer may be humidified (which provides a further source of water). Overall, the process gas streams contain substantial quantities of water and the methanol produced typically is treated such as by distillation to reduce the water content of the methanol. In accordance with one embodiment of the instant process a hydrogen gas stream which is relatively pure (e.g.
In accordance with this embodiment, water need not be added to the process and is preferably not added to the process (except in so far as some quantities may be contained with the hydrocarbon feedstock such as may be contained for example in natural gas). Accordingly, the amount of water traveling through the process and accordingly exiting methanol synthesis reactor 12 is substantially reduced compared to steam reformation processes. Accordingly, methanol 26 may have a relatively low level of water.Methanol which contains as much as 10 weight percent water may be burned in convention combustion devices such as an internal combustion engine. In accordance with this embodiment of the instant invention, by avoiding the use of reformation in the process, methanol 26 (which is the product produced directly from methanol synthesis reactor 12 without distillation) may contain less than this amount of water and accordingly, may be a commercial product without further processing.


In one particular embodiment, hydrocarbon feedstock 14 preferably comprises and, more preferably, consists essentially of natural gas or methane.As shown in FIG.
In particular, water 32 is feed to electrolysis unit 28 to produce oxygen stream 16 and hydrogen stream 34. Some or all of oxygen stream 16 may be fed directly to partial oxidation reactor 10 as oxygen stream 16? (as shown by the broken feed line shown in FIG. Similarly, some or all of hydrogen stream 34 may be fed directly to synthesis gas 18 as hydrogen stream 20 (as shown by the broken feed line shown in FIG. Preferably, storage tanks are utilized to produce a generally continuous flow of hydrogen and oxygen to streams 16? and 20. To this end, one or more oxygen storage tanks 36 and one or more hydrogen storage tanks 38 may be provided.In operation, electricity for electrolysis unit 28 may be obtained from a power grid. During peak periods, when the cost of electricity is greater or, in some cases, when the requisite amount of electricity may not be available, the production of hydrogen and oxygen by electrolysis unit 28 may be reduced. In such cases, the amount of hydrogen and oxygen delivered to storage tanks 36 and 38 is reduced. However, depending upon the capacity of storage tanks 36 and 38, the process may be supplied with hydrogen and oxygen via streams 42 and 40 at about the same rate regardless of the flow rate of hydrogen and oxygen into tanks 36 and 38 via streams 32 and 34. In this way, tanks 36 and 38 may be utilized to produce a continuous flow of hydrogen and oxygen to the process.In another embodiment of the instant invention, electrolysis unit 28 may produce excess hydrogen and oxygen then are required for the operation of partial oxidation and methanol synthesis reactors 10 and 12. To achieve these ratios, particularly if hydrocarbon feedstock 14 substantially comprises or consists essentially of methane, a greater proportion of the oxygen produced by electrolysis unit 28 will be required then the hydrogen produced by electrolysis unit 28.
Accordingly, then in one embodiment of operation, electrolysis unit 28 may be operated to produce essentially the requisite amount of oxygen to produce this ratio resulting in essentially no product oxygen stream 44. However, as less hydrogen will be required to produce the desired ratio, only a portion of the hydrogen produced by electrolysis unit 28 need be combined with synthesis gas 18 via stream 20.
If the oxygen content of the synthesis gas is too high, then oxygen will react with methanol in methanol synthesis reactor 12 to form carbon dioxide and water.
To reduce the amount of oxygen in the synthesis gas, the amount of hydrocarbon feedstock 14 fed to partial oxidation reactor 10 is preferably adjusted, based upon the flow rate of oxygen stream 16 to partial oxidation reactor 10 such that the effluent from partial oxidation reactor 10 contains at least some unoxidized hydrocarbon feedstock.
Preferably, the effluent contains from less than about 10 weight percent of the unoxidized hydrocarbon feedstock and, more preferably, less than about 4 weight percent of the unoxidized hydrocarbon feedstock, based on the weight of the effluent stream. At these levels, essentially all of the oxygen will be utilized in partial oxidation reactor 10.
It will be appreciated by those skilled in the art that the actual amount of unoxidized hydrocarbon which is required will vary in part depending upon the efficiency of partial oxidation reactor 10.Referring to FIG. 3, in a further embodiment of the instant invention, tail gas stream 24 is subjected to gas separation unit 48 to produce tail gas recycle stream 50 and purge stream 52. Preferably, gas separation unit 48 utilizes cryogenic separation or a membrane separator and, more preferably, a membrane separator. The inert material that is to be removed will vary depending upon the contaminants in the feedstocks. For example, if hydrocarbon feedstock stream 14 is natural gas, purge stream 52 is utilized to remove, for example, nitrogen that is present with the natural gas. In particular, recycle stream 50 may comprise up to about 95 weight percent and, more preferably from about 50 to about 95 weight percent of tail gas stream 24. Accordingly, a substantial portion of an unreacted synthesis gas is recycled into the system.
3, recycle stream 50 is preferably combined with hydrocarbon feedstock stream 14 to produce blended hydrocarbon stream 54 which is then fed to partial oxidation reactor 10. In either case, the unreacted synthesis gases, which include carbon dioxide, is recycled through the partial oxidation reactor wherein some of the carbon dioxide may be converted to carbon monoxide which is then combined with hydrogen in the methanol synthesis reactor 12 to produce methanol.Purge stream 52 may be fed to a combustion unit 56, such as a gas turbine, to produce power 58 and stack gases 60. Power 58 may be in the form of mechanical power or electricity if combustion unit 56 is drivingly connected to a generator.Stack gases will be at an elevated temperature. Accordingly, excess heat from stack gases 60 may be recovered by means of heat exchanger 62. For example, water 64 may be fed to heat exchanger 62 to indirectly heat the water to produce steam 66 and cooled stack gases 68. In such a case, purge stream 52 may be fed directly to indirect exchanger 62 or it may first be fed to combustion unit 56 to further increase the temperature of the purge stream prior to the heat exchange step.In a further alternate embodiment shown in FIG. 2, the excess heat generated by partial oxidation reactor 10 may be recovered to produce steam and, more preferably electricity. The water may be heated by its passage through jacket 70 to such an extent that it produces stream 74 which may be steam. Pursuant to this embodiment, reformer 86 is provided downstream from partial oxidation reactor 10.
As discussed previously, the instant process may be conducted to produce product hydrogen stream 46.
According to this embodiment, at least a portion of the product hydrogen stream could effectively be used by reformer 86. In this way, the amount of product hydrogen stream 46 may be reduced or eliminated depending on the amount of hydrogen required for reformer 86.
By operating a reformer effectively in reverse, the product of the reformer (reformed synthesis gas stream 84) will contain water. Typically, reformer 86 will be operated at a pressure less than methanol synthesis reactor 12 and at a higher temperature. As the temperature of reformed synthesis gas stream 84 is reduced and the pressure is increased so that reformed synthesis gas stream 84 is suitable for feeding to methanol synthesis reactor 12, water may be removed from reformed synthesis gas stream 84.The carbon dioxide for reformer 86 may be supplied from synthesis stream 18.
Carbon dioxide feedstock stream 82 may be obtained from various sources and is preferably relatively pure since any contaminants will have to be purged from the system or will contaminate the methanol produced by the process. Carbon dioxide feedstock stream 82 may be obtained as excess carbon dioxide from a bottling plant or as exhaust gas produced by combustion. In the later case, the exhaust gas is preferably subjected to cleaning steps to remove undesirable contaminants.
The carbon dioxide is preferably obtained as a by product of another process so that the instant process becomes effectively a temporary carbon sink to convert carbon dioxide, which would otherwise be released to the atmosphere, to a stored carbon source.Reformed synthesis gas stream 84 may be treated as discussed previously. Alternately, hydrogen may be added to the process upstream of reformer 86 (as shown by the dashed line in FIG.
4).It will be appreciated by those skilled in the art that each of the embodiments of the instant invention may be utilized individually or combined to produce an improved process for the production of methanol.



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