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[*] posted on 23-6-2008 at 09:22
Fuel from atmospheric CO2


A project that interests me is the variation on the classic Fischer-Tropsch reaction that catalytically converts atmospheric CO2 into methane, methanol or higher chain length hydrocarbons. There appears to be an extensive literature on this topic. Given the current energy situation & concerns about CO2 contributing to global warming, this project should interest a number of subscribers here.

This chemistry can be broken down into 2 modules:

1. Sequestration of atmospheric CO2.
2. Catalytic conversion (reduction) of the CO2 into fuel.

Regarding sequestration of CO2, rather than build & power a gas separation plant to remove it from the atmosphere, I think that pumping air into aqueous caustic soda to form aqueous sodium carbonate or bicarbonate might have a lot going for it. That could be the starting point for continuous operation, which is nearly always desirable from an economic POV.

Here is one recent paper's abstract on the catalytic conversion of aqueous sodium carbonate into methane. Note that they hypothesize sodium formate being an intermediate. Formate esters can be reduced to methanol.

Quote:
In the presence of Raney alloy, the direct reaction of alkali or alkali-earth metal carbonates with water resulted in reduction of the carbonates to give methane in high selectivity at a temperature near the critical point of water (∼ 380°C). Raney Ni showed an efficient activity to promote the methanation. On the contrary, Raney Fe did not cause the methanation, but the addition of catalytic amount of a carbon-supported ruthenium (Ru/C) to the Raney Fe brought about a highly selective reduction of the carbonates to methane. The reaction was also controlled by the reaction temperatures, i.e., the selectivity and yield of methane increased with increasing temperature suppressing the formation of metal formate. One characteristic in the present reaction is a rapid formation of a considerable amount of metal formate at an initial stage. It is proposed that the formation of methane from metal carbonate occurs via the formation of metal formate and its subsequent hydrogenation by nascent hydrogen which is produced from water by action of Raney alloy. The apparent activation energy for the methanation of Na2CO3 on Raney Fe-Ru/C mixed catalyst was estimated to be 14 kcal mol-1.

Revue / Journal Title
Journal of molecular catalysis. A, Chemical ISSN 1381-1169
Source
1999, vol. 145, no1-2, pp. 159-167 (26 ref.)


[Edited on 23-6-2008 by Ritter]




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[*] posted on 23-6-2008 at 09:50


Here is another interesting report on similar chemistry:

Quote:
Originally published in Science Express on 1 April 2004
Science 14 May 2004:
Vol. 304. no. 5673, pp. 1002 - 1005
DOI: 10.1126/science.1096033

Reports

Hydrocarbons in Hydrothermal Vent Fluids: The Role of Chromium-Bearing Catalysts

Dionysis I. Foustoukos* and William E. Seyfried, Jr.

Fischer-Tropsch type (FTT) synthesis has long been proposed to account for the existence of hydrocarbons in hydrothermal fluids. We show that iron- and chromium-bearing minerals catalyze the abiotic formation of hydrocarbons. In addition to production of methane (CH4aq), we report abiotic generation of ethane (C2H6aq) and propane (C3H8aq) by mineral-catalyzed hydrothermal reactions at 390°Cand 400 bars. Results suggest that the chromium component in ultramafic rocks could be an important factor for FTT synthesis during water-rock interaction in mid-ocean ridge hydrothermal systems. This in turn could help to support microbial communities now recognized in the subsurface at deep-sea vents.

Department of Geology and Geophysics, University of Minnesota, Minneapolis, MN 55455, USA.


* To whom correspondence should be addressed. E-mail: fous0009@umn.edu





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[*] posted on 23-6-2008 at 09:56


Here is a comprehensive review article on the electrochemical reduction of CO2, carbonate & bicarbonate to obtain methane, higher hydrocarbons, formic acid, methanol, etc.

http://www.uctm.edu/journal/j2007-4/1_Jitaru_333-344.pdf




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[*] posted on 23-6-2008 at 10:12


Here is another report of abiogenic CH4 production from bicarbonate ion under hydrothermal vent conditions:

Quote:
Science 13 August 1999:
Vol. 285. no. 5430, pp. 1055 - 1057
DOI: 10.1126/science.285.5430.1055

Reports

Abiogenic Methane Formation and Isotopic Fractionation Under Hydrothermal Conditions

Juske Horita, 1* Michael E. Berndt 2

Recently, methane (CH4) of possible abiogenic origin has been reported from many localities within Earth's crust. However, little is known about the mechanisms of abiogenic methane formation, or about isotopic fractionation during such processes. Here, a hydrothermally formed nickel-iron alloy was shown to catalyze the otherwise prohibitively slow formation of abiogenic CH4 from dissolved bicarbonate (HCO3) under hydrothermal conditions. Isotopic fractionation by the catalyst resulted in 13C values of the CH4 formed that are as low as those typically observed for microbial methane, with similarly high CH4/(C2H6 + C3H8) ratios. These results, combined with the increasing recognition of nickel-iron alloy occurrence in oceanic crusts, suggest that abiogenic methane may be more widespread than previously thought.

1 Chemical and Analytical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA.
2 Department of Geology and Geophysics, University of Minnesota, Minneapolis, MN 55455, USA.
* To whom correspondence should be addressed. E-mail: horitaj@ornl.gov







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[*] posted on 23-6-2008 at 10:12


Here is another report of abiogenic CH4 production from bicarbonate ion under hydrothermal vent conditions:

Quote:
Science 13 August 1999:
Vol. 285. no. 5430, pp. 1055 - 1057
DOI: 10.1126/science.285.5430.1055

Reports

Abiogenic Methane Formation and Isotopic Fractionation Under Hydrothermal Conditions

Juske Horita, 1* Michael E. Berndt 2

Recently, methane (CH4) of possible abiogenic origin has been reported from many localities within Earth's crust. However, little is known about the mechanisms of abiogenic methane formation, or about isotopic fractionation during such processes. Here, a hydrothermally formed nickel-iron alloy was shown to catalyze the otherwise prohibitively slow formation of abiogenic CH4 from dissolved bicarbonate (HCO3) under hydrothermal conditions. Isotopic fractionation by the catalyst resulted in 13C values of the CH4 formed that are as low as those typically observed for microbial methane, with similarly high CH4/(C2H6 + C3H8) ratios. These results, combined with the increasing recognition of nickel-iron alloy occurrence in oceanic crusts, suggest that abiogenic methane may be more widespread than previously thought.

1 Chemical and Analytical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA.
2 Department of Geology and Geophysics, University of Minnesota, Minneapolis, MN 55455, USA.
* To whom correspondence should be addressed. E-mail: horitaj@ornl.gov







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[*] posted on 23-6-2008 at 10:24


Very interesting topic indeed. I wonder if copper catalysts can effect that kind of reduction, and how re-useable the catalyst employed would be.
Adapting a small scale setup doesn't seem to a easy thing, especially if pressure is required for the reduction.

BTW, please use the edit function to avoid multiple posts like this....




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[*] posted on 23-6-2008 at 10:54


Quote:
Originally posted by Klute
Very interesting topic indeed. I wonder if copper catalysts can effect that kind of reduction, and how re-useable the catalyst employed would be.
Adapting a small scale setup doesn't seem to a easy thing, especially if pressure is required for the reduction.



A small-scale pilot unit could be built of coiled thick-walled metal tubing set inside a heat-resistant structure made of something like fire brick. I think standard gauges could be used to monitor pressure & I don't think thermocouples with digital readouts are very expensive. You would need to cool & then compress the output gas & store it in standard propane tanks such as are used to fuel gas grills. Your input stream of aqueous carbonate or bicarbonate solution would also have to be pumped to get to the needed pressures, which I think are in the range of 400 bar.

Of course you don't get something for nothing. You are hydrogenating the CO2 or bicarbonate or carbonate ions, so you need a source of hydrogen (water is preferred I think). You are also adding a tremendous amount of energy, which would be one of your major cost elements. But as the cost of fuels keeps rising, at some point this kind of 'do it yourself' CO2 recycling could become economically attractive.

As far as catalysts are concerned, they seem to be restricted to the transition metals, so Cu might work.

One other point: if your target is methane, you would have to be careful not to vent this to the atmosphere as it has many times the potency of CO2 in terms of a greenhouse gas.

[Edited on 23-6-2008 by Ritter]

[Edited on 23-6-2008 by Ritter]




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[*] posted on 23-6-2008 at 10:59


Here is a recent U.S. patent to a major university that claims the use of dehydrogenase enzymes coupled to spinach chloroplasts for NADH cofactor regeneration. CO2 goes in & methanol comes out in (claimed) high yield at room temperature & standard pressure:

http://tinyurl.com/4tb28m




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[*] posted on 23-6-2008 at 13:24


Quote:
Journal of Photochemistry and Photobiology A: Chemistry
Volume 182, Issue 3, 10 September 2006, Pages 306-309
Proceedings of 7th AIST International Symposium on Photoreaction Control and Photofunctional Materials

Half-sandwich complexes with dihydroxy polypyridine: Water-soluble, highly efficient catalysts for hydrogenation of bicarbonate attributable to electron-donating ability of oxyanion on catalyst ligand

Studies in Surface Science and Catalysis, Volume 153, 2004, Pages 263-266

Yuichiro Himeda, Nobuko Onozawa-Komatsuzaki, Hideki Sugihara, Hironori Arakawa, Kazuyuki Kasuga

Abstract
Half-sandwich Ru(II), Ir(III), and Rh(III) complexes with 4,7-dihydroxy-1,10- phenanthroline or 4,4′-dihydroxy-2,2′-bipyridine are highly efficient catalysts for hydrogenation of bicarbonate in alkaline aqueous solution without an amine additive. The generation of an oxyanion by deprotonation of the hydroxy substituents on the catalyst ligand caused a dramatic enhancement of catalytic activity due to its strong electron-donating ability of the oxyanionas well as imparting water solubility. Turnover frequencies (TOF) up to 42,000 h−1 and turnover numbers (TON) up to 222,000 have been obtained by using iridium catalysts under 6 MPa at 120 °C. The production of formate (TOF = 3.5 h−1) was observed even under ambient conditions (0.1 MPa, 30 °C).




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[*] posted on 23-6-2008 at 18:24


Quote:

so you need a source of hydrogen



http://sciencelinks.jp/j-east/article/200415/000020041504A04...

...Pure hydrogen was formed by the reaction between biomass and NaOH at > 473 K in the absence of water vapor as well...

theres your hydrogen, but you need lots of economical NaOH

Is recycleing Na2CO3 back to NaOH tough?
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[*] posted on 23-6-2008 at 19:04


Not too long ago I stumbled across a few articles relevant to this.

Ultrasonics Sonochemistry
Volume 5, Issue 2, June 1998, Pages 73-77

Involves sonication of CO2 solutions, producing CO, H2, and trace O2.

Another referred to bicarbonate reduction (to H2 and/or formaldehyde, depending on conditions) by iron salts under UV radiation.

They could be worth looking into.

edit: heres the latter article I mentioned: http://www.jstor.org/pss/32422

[Edited on by stygian]
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[*] posted on 23-6-2008 at 19:12


Quote:
Is recycleing Na2CO3 back to NaOH tough?


Well, yes and no.

Na2CO3 (aq) + CaO is the old way of making lye. The CaO is made from CaCO3 by eating, which dumps the CO2 right back in the atmosphere. There are several other ways, all of which have the problem of cranking out CO2 and taking a fair amount of energy.

If you want to convert CO2 to more reduced forms, it's best not to start with the 380 ppm in the atmosphere, but rather to go for concentrated sources from big producers such as power plants.

Note that plants, which been in the CO2 fixing business for about a billion years, generally don't do much better than converting 1% of their energy input into fixed CO2 (mostly as carbohydrates). There's serious problems with the lifespan of synthetic systems, sensitivity to poisoning, and so on. Non-trival work remains to be done.
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[*] posted on 24-6-2008 at 09:56


Quote:
Originally posted by not_important
Quote:
If you want to convert CO2 to more reduced forms, it's best not to start with the 380 ppm in the atmosphere, but rather to go for concentrated sources from big producers such as power plants.



The classic Fischer-Tropsch process:

1. H2O (superheated steam) + C (powdered coal) > CO + H2
(synthesis gas, or syngas)

2. CO + H2 > Hydrocarbons + CO2

has not been implemented on a large scale yet in this country because the waste CO2 is vented to the atmosphere, adding to the greenhouse problem. Using the CO2 conversion options discussed above you could eliminate that waste problem with a 2-stage F-T plant.

FWIW, the U.S. has coal reserves that rival Saudi Arabia's oil reserves. And F-T technology is available off-the-shelf. You could build F-T plants near the coal mines.

The Germans ran WWII on F-T fuel and the South Africans are independent of imported oil because of their Sasol F-T initiative. And the U.S. Air Force is going F-T for avgas.

Conveniently, the usual output of a F-T plant is primarily linear hydrocarbons that are more suited for avgas & diesel applications, just what is needed for the trains, planes & trucks. I believe diesels are significantly more efficient than gasoline also.




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[*] posted on 24-6-2008 at 21:32


Quote:
Originally posted by roamingnome
Is recycleing Na2CO3 back to NaOH tough?


Think about it. The process turns CO3(2-) (or HCO3-) into CH3OH. Thus, NaOH is left in solution.

Tim




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[*] posted on 25-6-2008 at 07:50


Quote:
Think about it. The process turns CO3(2-) (or HCO3-) into CH3OH. Thus, NaOH is left in solution.

Tim


I believe that the only other thing that gets consumed in this reaction is some of the water, so the aqueous NaOH could be reused after adjusting the concentration.




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[*] posted on 1-7-2008 at 06:10


Quote:
Originally posted by Ritter

Regarding sequestration of CO2, rather than build & power a gas separation plant to remove it from the atmosphere, I think that pumping air into aqueous caustic soda to form aqueous sodium carbonate or bicarbonate might have a lot going for it. That could be the starting point for continuous operation, which is nearly always desirable from an economic POV.


This process, when applied industrially is known as 'Spent Caustic Carbonation' and is in use. Plants originally adopted it because it was a fairly cheap method of dealing with caustic waste. A college's father had developed and patented a mobile version on a semi that could trounce around from plant to plant on a rostered basis, but he died of cancer before he managed to attract enough investment to build it. That was in the early nineties. I am sure that these days, for plants producing (and having to dispose of) caustic waste, this process is very high on their list of 'pieces of kit to buy before the Co2 footprint audit' list.




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[*] posted on 1-7-2008 at 14:05


Never will happen. The problem is the energy losses. It's an uphill battle the entire way. At BEST (which will never happen), we are talking 0% energy loss (i.e. the amount of energy in the product = the amount of energy it took to make the product).

This is why hydrogen is such a silly idea. People think that it's a great SOURCE of energy, but what it really is is a crappy way to STORE and TRANSPORT energy.
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[*] posted on 1-7-2008 at 14:07


What, exactly, will never happen?

You should notice no one mentioned hydrogen.




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[*] posted on 2-7-2008 at 05:07


Quote:
Originally posted by 12AX7
What, exactly, will never happen?

You should notice no one mentioned hydrogen.


Hydrogen currently comes from petrochemical plants, which generate it as a result of cracking ethane & propane to ethylene & propylene. But the amounts of hydrogen required to make a significant impact on domestic hydrocarbon fuel consumption would be huge & most likely would have to come from electrolysis of water, which would require equally huge amounts of electric energy.

Beyond the basic economics of producing hydrogen, you would have to transport it & we currently have a bulk fuel transport infrastructure that is dedicated to hydrocarbon fuels. How are you going to transport hydrogen & do it safely?

The most significant problem with hydrogen comes at the consumer level. Forty-nine of the 50 states have filling stations designed for pump-it-yourself service. Just imagine the chaos as millions of untrained people try to fill their tanks with a pressurized & highly flammable gas! And a car with a tank of pressurized hydrogen becomes a fuel-air bomb just waiting for an accident to trigger it.

I still feel that the most feasible fuel source is F-T conversion of coal to diesel & avgas. The technology exists now. The Germans & the South Africans proved that it works. And our current distribution infrastructure would not have to be either enhanced or modified. The price of oil is getting close to where the economics of F-T fuel will be both competitive & a lot cheaper than an endless series of Middle Eastern wars fought for oil.

[Edited on 2-7-2008 by Ritter]

[Edited on 2-7-2008 by Ritter]




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[*] posted on 2-7-2008 at 08:39


Quote:
Originally posted by 12AX7
What, exactly, will never happen?

You should notice no one mentioned hydrogen.


Since the post was fuel from CO2, that may be what I was speaking of. Also, I was using hydrogen as a SIMILAR example.
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[*] posted on 2-7-2008 at 10:29


Quote:
Originally posted by Ritter
I still feel that the most feasible fuel source is F-T conversion of coal to diesel & avgas. The technology exists now. The Germans & the South Africans proved that it works. And our current distribution infrastructure would not have to be either enhanced or modified. The price of oil is getting close to where the economics of F-T fuel will be both competitive & a lot cheaper than an endless series of Middle Eastern wars fought for oil.

I think the amortized costs of production for F-T already make coal-to-liquids cheaper than imported crude for the US. There are at least two problems, though. The first is that building a new CTL plant, at least one like those Sasol uses, is extremely capital intensive. The second is that not everyone is confident that the current high and rising price of oil reflects a "fundamental" valuation. Some think that oil is currently experiencing a price bubble. It's very doubtful that oil would ever be as cheap again as it was in the late 1990s, but if the current price is speculation-driven it could drop 30-50 dollars a barrel even faster than it gained the last 30-50 dollars per barrel. Even if it's not speculation driven, an economic slowdown or recession could drop the price of oil due to decreased demand. The very high current price of crude oil is good news for purveyors of alternatives, but a stable price (even if somewhat lower than it is now) would be better yet. Even in an era of $140/barrel oil, a 7 billion dollar CTL plant needs some time to show a profit.

Governments and other large investors got burned on energy investments during the fuel crisis of the 1970s. By the late 1970s, early 1980s there had been a lot of R&D on crude oil alternatives and energy efficiency measures (oil shale, coal to liquids, solar heated buildings, MHD generators...) and a number of pilot scale programs. Then oil prices dropped in the mid 1980s and most of the fruits of investment became uncompetitive with business-as-usual. Investors may be more cautious this time around, even though there are strong signs that oil prices are not going to collapse again.

[Edited on 7-2-2008 by Polverone]




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[*] posted on 2-7-2008 at 11:10


Quote:
Originally posted by Polverone
I think the amortized costs of production for F-T already make coal-to-liquids cheaper than imported crude for the US. There are at least two problems, though. The first is that building a new CTL plant, at least one like those Sasol uses, is extremely capital intensive. The second is that not everyone is confident that the current high and rising price of oil reflects a "fundamental" valuation. Some think that oil is currently experiencing a price bubble. It's very doubtful that oil would ever be as cheap again as it was in the late 1990s, but if the current price is speculation-driven it could drop 30-50 dollars a barrel even faster than it gained the last 30-50 dollars per barrel. Even if it's not speculation driven, an economic slowdown or recession could drop the price of oil due to decreased demand. The very high current price of crude oil is good news for purveyors of alternatives, but a stable price (even if somewhat lower than it is now) would be better yet. Even in an era of $140/barrel oil, a 7 billion dollar CTL plant needs some time to show a profit.



Here is a somewhat dated cost analysis of building & operating a F-T plant: http://www.netl.doe.gov/publications/proceedings/97/97cl/cho.... Even taking inflation into consideration, actual cost is likely closer to a billion $ than to $7B.

My information is that the oil supply rate has peaked while the demand rate is increasing at over 2%/year, compounded. All the cheap oil has been consumed & what is left should be reserved for applications where there are no feasible alternative, such as petrochemical feedstocks for chemical raw materials that can be made in no other way.

The situation with oil is a serious matter involving national security. It is a similar situation to the situation the Germans faced in the World Wars, that South Africa faced with oil embargoes, and the situation that the U.S. found itself in when WWII started & supplies of natural rubber were cut off. A major effort in all these cases relieved the fuel & rubber shortages through the application of organic chemistry.

The true irony of the current situation is the fact that the major oil companies all led the research effort in the U.S. on F-T technology. Since they own most of the distribution infrastructure, tax credits to Big Oil should be tied to capital investment in F-T plants located near major coal producing areas.

In the near term, if the current trend in oil cost is not brought under control, I predict we will see 1973-style rationing, with the bulk of the oil products being shifted to the trains, trucks & planes in order to prop up our national transportation infrastructure.

Hopefully this country will soon lose its oil baron leadership & put someone with broad vision in their place.

Here is a typical F-T pilot plant:

[img]http://f9g.yahoofs.com/groups/g_17454011/.HomePage/__sr_/becf.jpg?grAgWbIBCSg8xts2[/img]

[Edited on 2-7-2008 by Ritter]




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[*] posted on 2-7-2008 at 12:27


Unfortunately, we need an "oil baron". Right now (or even within the next 20 years) if oil becomes too expensive/unavailable we are screwed. VERY screwed. What we need is someone who can be an "oil baron" while, at the same time, actively searching for other alternatives. I almost got ahead of myself there. What many people seem to have forgotten is that the president doesn't (or SHOULDn't anyway) have much control over those types of things. His main purpose is to enforce the laws and help in the "3-way" govt. process. I feel that sometimes we rely on him to be a dictator that can control directly what the nation spends its money on.

In some ways that would help. But we don't want that now do we?

I think the future is in fusion. Once we figure out how to get more energy out of it than we spend... Well, we'll have all the hydrogen we want. And once we have that setting up infrastructure for it will just be a minor issue (since we'll basically have "free" energy... yes I know it's not really "free").

You guys know what I mean... gotta go laksdhf;asdhf




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[*] posted on 2-7-2008 at 13:08


My money for the future is on hot dry rock geothermal energy. Basically it involves drilling a REALLY deep hole, pumping water down there and using the steam generated to power turbines. Problems with it right now are keeping the hole stable (we're talking 3-5 km holes).

If that doesn't work, maybe a global war/plague, elimating two thirds of the world population will.
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Registered: 20-6-2008
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[*] posted on 2-7-2008 at 13:39


Quote:
Originally posted by MagicJigPipe
I think the future is in fusion. Once we figure out how to get more energy out of it than we spend... Well, we'll have all the hydrogen we want.


You can't run trains, planes & trucks on hydrogen, which is a nightmare to make, transport & handle safely at the consumer level in the kinds of quantities required. And fusion is 10+ years away...maybe.




Ritter
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\"The production of too many useful things results in too many useless people.\"

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