Thorium fuel cycle

The thorium fuel cycle is a nuclear fuel cycle that uses the naturally abundant isotope of thorium, 232
Th, as the fertile material. In the reactor, 232
Th is transmuted into the fissile artificial uranium isotope 233
U which is the nuclear fuel. Unlike natural uranium, natural thorium contains only trace amounts of fissile material (such as 231
Th), which are insufficient to initiate a nuclear chain reaction. Additional fissile material or another neutron source are necessary to initiate the fuel cycle. In a thorium-fueled reactor, 232
Th absorbs neutrons eventually to produce 233
U. This parallels the process in uranium reactors whereby fertile 238
U absorbs neutrons to form fissile 239
Pu. Depending on the design of the reactor and fuel cycle, the 233
U generated either fissions in situ or is chemically separated from the used nuclear fuel and formed into new nuclear fuel.

The thorium fuel cycle claims several potential advantages over a uranium fuel cycle, including thorium's greater abundance, superior physical and nuclear properties, better resistance to nuclear weapons proliferation, and reduced plutonium and actinide production.

1 History
2 Nuclear reactions with thorium
3 Advantages as a nuclear fuel
4 Disadvantages as nuclear fuel
5 Reactors
- 5.1 List of thorium-fueled reactors
6 References and links

History

Concerns about the limits of worldwide uranium resources motivated initial interest in the thorium fuel cycle.^[1] It was envisioned that as uranium reserves were depleted, thorium would supplement uranium as a fertile material. However, for most countries, uranium was relatively abundant, and research in thorium fuel cycles waned. A notable exception was India's three stage nuclear power programme. In the twenty-first century thorium's potential for improving proliferation resistance and waste characteristics led to renewed interest in the mineral.^[2]^[3]^[4]

At Oak Ridge National Laboratory in the 1960s, the Molten-Salt Reactor Experiment used 233
U as the fissile fuel as an experiment to demonstrate a part of the Molten Salt Breeder Reactor that was designed to operate on the thorium fuel cycle. Molten Salt Reactor (MSR) experiments assessed thorium's feasibility, using thorium(IV) fluoride dissolved in a molten salt fluid which eliminated the need to fabricate fuel elements. The MSR program was defunded in 1976.

In 2006, Carlo Rubbia proposed the concept of an energy amplifier or "accelerator driven system" (ADS), which he saw as a novel and safe way to produce nuclear energy that exploited existing accelerator technologies. Rubbia's proposal offered the potential to incinerate high-activity nuclear waste and produce energy from natural thorium and depleted uranium.^[5]^[6]

Kirk Sorensen, former NASA scientist and Chief Nuclear Technologist at Teledyne Brown Engineering, has been a long time promoter of thorium fuel cycle and particularly liquid fluoride thorium reactors. He first researched thorium reactors while working at NASA, while evaluating power plant designs suitable for lunar colonies. In 2006 Sorensen started "energyfromthorium.com" to promote and make information available about this technology.^[7]^[8]^[9]^[10]

Nuclear reactions with thorium

Actinides				Half-life	Fission products
²⁴⁴Cm	²⁴¹Pu ^f	²⁵⁰Cf	²⁴³Cm^f	10–30 y	¹³⁷Cs	⁹⁰Sr	⁸⁵Kr
²³²U ^f		²³⁸Pu	f is for fissile	69–90 y			¹⁵¹Sm nc➔
4n	²⁴⁹Cf ^f	²⁴²Am^f	f is for fissile	141–351	No fission product has half-life 10² to 2×10⁵ years
4n	²⁴¹Am		²⁵¹Cf ^f	431–898
²⁴⁰Pu	²²⁹Th	²⁴⁶Cm	²⁴³Am	5–7 ky
4n	²⁴⁵Cm^f	²⁵⁰Cm	²³⁹Pu ^f	8–24 ky
	²³³U ^f	²³⁰Th	²³¹Pa	32–160
	4n+1	²³⁴U	4n+3	211–290	⁹⁹Tc		¹²⁶Sn	⁷⁹Se
²⁴⁸Cm	4n+1	²⁴²Pu		340–373	Long-lived fission products
	²³⁷Np	4n+2		1–2 My	⁹³Zr	¹³⁵Cs nc➔
²³⁶U	4n+1		²⁴⁷Cm^f	6–23 My		¹⁰⁷Pd	¹²⁹I
²⁴⁴Pu				80 My	>7%	>5%	>1%	>.1%
²³²Th		²³⁸U	²³⁵U ^f	0.7–12 Gy	fission product yield

In the thorium cycle, fuel is formed when 232
Th captures a neutron (whether in a fast reactor or thermal reactor) to become 233
Th. This normally emits an electron and an anti-neutrino (ν) by β−
decay to become 233
Pa. This then emits another electron and anti-neutrino by a second β−
decay to become 233
U, the fuel:

$\mathrm{n}%2B{}_{\ 90}^{232}\mathrm{Th}\rightarrow {}_{\ 90}^{233} \mathrm{Th} \xrightarrow{\beta^-} {}_{\ 91}^{233}\mathrm{Pa} \xrightarrow{\beta^-} {}_{\ 92}^{233}\mathrm{U}$

Fission product wastes

Nuclear fission produces radioactive fission products which can have half-lives from days to greater than 200,000 years. According to some toxicity studies,^[11] the thorium cycle can fully recycle actinide wastes and only emit fission product wastes, and after a few hundred years, the waste from a thorium reactor can be less toxic than the uranium ore that would have been used to produce low enriched uranium fuel for a light water reactor of the same power. Other studies assume some actinide losses and find that actinide wastes dominate thorium cycle waste radioactivity at some future periods.^[12]

Actinide wastes

In a reactor, when a neutron hits a fissile atom (such as certain isotopes of uranium), it either splits the nucleus or is captured and transmutes the atom. In the case of 233
U, the transmutations tend to produce useful nuclear fuels rather than transuranic wastes. When 233
U absorbs a neutron, it either fissions or becomes 234
U. The chance of fissioning on absorption of a thermal neutron is about 92%; the capture-to-fission ratio of 233
U, therefore, is about 1:10 — which is better than the corresponding capture vs. fission ratios of 235
U (about 1:6), or 239
Pu (about 1:2), or 241
Pu (about 1:4).^[1] The result is shorter-lived transuranic waste than in a reactor using the uranium-plutonium fuel cycle.

Transmutation in the thorium fuel cycle
²³⁰Th	→	²³¹Th	←	²³²Th	→	²³³Th		(White actinides: t_½<27d)
		↓				↓
		²³¹Pa	→	²³²Pa	←	²³³Pa	→	²³⁴Pa		(Colored : t_½>68y)
		↑		↓		↓		↓
		²³¹U	←	²³²U	↔	²³³U	↔	²³⁴U	↔	²³⁵U	↔	²³⁶U	→	²³⁷U
				↓		↓				↓				↓
		(Fission products with t_½<90y or t_½>200ky)												²³⁷Np

234
U, like most actinides with an even number of neutrons, is not fissile, but neutron capture produces fissile 235
U. If the fissile isotope fails to fission on neutron capture, it produces 236
U, 237
Np, 238
Pu, and eventually fissile 239
Pu and heavier isotopes of plutonium. The 237
Np can be removed and stored as waste or retained and transmuted to plutonium, where more of it fissions, while the remainder becomes 242
Pu, then americium and curium, which in turn can be removed as waste or returned to reactors for further transmutation and fission.

However, the 231
Pa (with a half-life of 3.27×10⁴ yr) formed via (n,2n) reactions with 232
Th (yielding 231
Th that decays to 231
Pa), while not a transuranic waste, is a major contributor to the long term radiotoxicity of spent nuclear fuel.

Uranium-232 contamination

Uranium-232 is also formed in this process, via (n,2n) reactions between fast neutrons and 233
U, 233
Pa, and 232
Th:

$\mathrm{n}%2B{}_{\ 90}^{232}\mathrm{Th}\rightarrow {}_{\ 90}^{233} \mathrm{Th} \xrightarrow{\beta^-} {}_{\ 91}^{233}\mathrm{Pa} \xrightarrow{\beta^-} {}_{\ 92}^{233}\mathrm{U}%2B\mathrm{n}\rightarrow {}_{\ 92}^{232} \mathrm{U}%2B2\mathrm{n}$

$\mathrm{n}%2B{}_{\ 90}^{232}\mathrm{Th}\rightarrow {}_{\ 90}^{233} \mathrm{Th} \xrightarrow{\beta^-} {}_{\ 91}^{233}\mathrm{Pa}%2B\mathrm{n} \rightarrow {}_{\ 91}^{232}\mathrm{Pa}%2B2\mathrm{n} \xrightarrow{\beta^-} {}_{\ 92}^{232}\mathrm{U}$

$\mathrm{n}%2B{}_{\ 90}^{232}\mathrm{Th}\rightarrow {}_{\ 90}^{231} \mathrm{Th} %2B 2\mathrm{n} \xrightarrow{\beta^-} {}_{\ 91}^{231}\mathrm{Pa}%2B\mathrm{n} \rightarrow {}_{\ 91}^{232}\mathrm{Pa} \xrightarrow{\beta^-}{}_{\ 92}^{232}\mathrm{U}$

Uranium-232 has a relatively short half-life (68.9 yr), and some decay products emit high energy gamma radiation, such as 224
Rn, 212
Bi and particularly 208
Tl. The full decay chain, along with half-lives and relevant gamma energies, is: 232
U decays to 228
Th where it joins decay chain of 232
Th

${}_{\ 92}^{232}\mathrm{U} \xrightarrow{\ \alpha\ } {}_{\ 90}^{228}\mathrm{Th}\ \mathrm{(68.9\ a)}$

${}_{\ 90}^{228}\mathrm{Th} \xrightarrow{\ \alpha\ } {}_{\ 88}^{224}\mathrm{Ra}\ \mathrm{(1.9\ a)}$

${}_{\ 88}^{224}\mathrm{Ra} \xrightarrow{\ \alpha\ } {}_{\ 86}^{220}\mathrm{Rn}\ \mathrm{(3.6\ d,\ 0.24\ MeV)}$

${}_{\ 86}^{220}\mathrm{Rn} \xrightarrow{\ \alpha\ } {}_{\ 84}^{216}\mathrm{Po}\ \mathrm{(55\ s,\ 0.54\ MeV)}$

${}_{\ 84}^{216}\mathrm{Po} \xrightarrow{\ \alpha\ } {}_{\ 82}^{212}\mathrm{Pb}\ \mathrm{(0.15\ s)}$

${}_{\ 82}^{212}\mathrm{Pb} \xrightarrow{\beta^-\ } {}_{\ 83}^{212}\mathrm{Bi}\ \mathrm{(10.64\ h)}$

${}_{\ 83}^{212}\mathrm{Bi} \xrightarrow{\ \alpha\ } {}_{\ 81}^{208}\mathrm{Tl}\ \mathrm{(61\ m,\ 0.78\ MeV)}$

${}_{\ 81}^{208}\mathrm{Tl} \xrightarrow{\beta^-\ } {}_{\ 82}^{208}\mathrm{Pb}\ \mathrm{(3\ m,\ 2.6\ MeV)}$

Thorium-cycle fuels produce hard gamma emissions, which damage electronics, limiting their use in military bomb triggers. 232
U cannot be chemically separated from 233
U from used nuclear fuel; however, chemical separation of thorium from uranium removes the decay product 228
Th and the radiation from the rest of the decay chain, which gradually build up as 228
Th reaccumulates. The hard gamma emissions also create a radiological hazard which requires remote handling during reprocessing.

Advantages as a nuclear fuel

Thorium is estimated to be about three to four times more abundant than uranium in the Earth's crust,^[13] although present knowledge of reserves is limited. Current demand for thorium has been satisfied as a by-product of rare-earth extraction from monazite sands. Also, unlike uranium, mined thorium consists of a single isotope (232
Th). Consequently, it is useful in thermal reactors without the need for isotope separation.

Thorium-based fuels exhibit several attractive properties relative to uranium-based fuels. The thermal neutron absorption cross section (σ_a) and resonance integral (average of neutron cross sections over intermediate neutron energies) for 232
Th are about three times and one third of the respective values for 238
U; consequently, fertile conversion of thorium is more efficient in a thermal reactor. Also, although the thermal neutron fission cross section (σ_f) of the resulting 233
U is comparable to 235
U and 239
Pu, it has a much lower capture cross section (σ_γ) than the latter two fissile isotopes, providing fewer non-fissile neutron absorptions and improved neutron economy. Finally, the ratio of neutrons released per neutron absorbed (η) in 233
U is greater than two over a wide range of energies, including the thermal spectrum; as a result, thorium-based fuels can be the basis for a thermal breeder reactor.^[1]

Thorium-based fuels also display favorable physical and chemical properties which improve reactor and repository performance. Compared to the predominant reactor fuel, uranium dioxide (UO₂), thorium dioxide (ThO₂) has a higher melting point, higher thermal conductivity, and lower coefficient of thermal expansion. Thorium dioxide also exhibits greater chemical stability and, unlike uranium dioxide, does not further oxidize.^[1]

Because the 233
U produced in thorium fuels is inevitably contaminated with 232
U, thorium-based used nuclear fuel possesses inherent proliferation resistance. 232
U can not be chemically separated from 233
U and has several decay products which emit high energy gamma radiation. These high energy photons are a radiological hazard that necessitate the use of remote handling of separated uranium and aid in the passive detection of such materials.

The long term (on the order of roughly 10³ to 10⁶ yr) radiological hazard of conventional uranium-based used nuclear fuel is dominated by plutonium and other minor actinides, after which long-lived fission products become significant contributors again. A single neutron capture in 238
U is sufficient to produce transuranic elements, whereas six captures are generally necessary to do so from 232
Th. 98–99% of thorium-cycle fuel nuclei would fission at either 233
U or 235
U, so fewer long-lived transuranics are produced. Because of this, thorium is a potentially attractive alternative to uranium in mixed oxide (MOX) fuels to minimize the generation of transuranics and maximize the destruction of plutonium.

Disadvantages as nuclear fuel

There are several challenges to the application of thorium as a nuclear fuel, particularly for solid fuel reactors.

Unlike uranium, natural thorium contains no fissile isotopes; fissile material, generally 233
U, 235
U, or plutonium, must be added to achieve criticality. This, along with the high sintering temperature necessary to make thorium-dioxide fuel, complicates fuel fabrication. Oak Ridge National Laboratory experimented with thorium tetrafluoride as fuel in a molten salt reactor from 1964–1969, which was far easier to both process and separate from contaminants that slow or stop the chain reaction.

In an open fuel cycle (i.e. utilizing 233
U in situ), higher burnup is necessary to achieve a favorable neutron economy. Although thorium dioxide performed well at burnups of 170,000 MWd/t and 150,000 MWd/t at Fort St. Vrain Generating Station and AVR respectively,^[1] challenges complicate achieving this in light water reactors (LWR), which compose the vast majority of existing power reactors.

Another challenge associated with a once-through thorium fuel cycle is the comparatively long interval over which 232
Th breeds to 233
U. The half-life of 233
Pa is about 27 days, which is an order of magnitude longer than the half-life of 239
Np. As a result, substantial 233
Pa develops in thorium-based fuels. 233
Pa is a significant neutron absorber, and although it eventually breeds into fissile 235
U, this requires two more neutron absorptions, which degrades neutron economy and increases the likelihood of transuranic production.

Alternatively, if solid thorium is used in a closed fuel cycle in which 233
U is recycled, remote handling is necessary for fuel fabrication because of the high radiation levels resulting from the decay products of 232
U. This is also true of recycled thorium because of the presence of 228
Th, which is part of the 232
U decay sequence. Further, unlike proven uranium fuel recycling technology (e.g. PUREX), recycling technology for thorium (e.g. THOREX) is only under development.

Although the presence of 232
U complicates matters, 233
U has occasionally been used to produce fission weapons. The United States first tested 233
U as part of a bomb core in Operation Teapot in 1955.^[14] However, unlike plutonium, 233
U can be easily denatured by mixing it with natural or depleted uranium. Another option is to mix thorium fuels with small amounts of natural or depleted uranium during fabrication to ensure that 233
U concentrations at cycle end are acceptably low.

Though thorium-based fuels produce far less long-lived transuranics than uranium-based fuels,^[11] some long-lived actinide products constitute a long term radiological impact, especially 231
Pa.^[12]

Advocates for liquid core and molten salt reactors claim that these technologies negate thorium's disadvantages. Since only one liquid core reactor using thorium has been built, it is hard to validate the exact benefits. The lack of relevance to the nuclear weapon industry can be seen as a disadvantage to the development of Thorium usage in power generation, but a worldwide resurgence of nuclear power use could provide enough incentives and funding to negate this disadvantage.

Reactors

Thorium fuels have fueled several different reactor types, including light water reactors, heavy water reactors, high temperature gas reactors, sodium-cooled fast reactors, and molten salt reactors.^[15]

List of thorium-fueled reactors

From IAEA TECDOC-1450 "Thorium Fuel Cycle - Potential Benefits and Challenges", Table 1: Thorium utilization in different experimental and power reactors.^[1]

Name	Country	Type	Power	Fuel	Operation period
AVR	Germany	HTGR, Experimental (Pebble bed reactor)	015000 15 MW(e)	Th+235 U Driver Fuel, Coated fuel particles, Oxide & dicarbides	1967–1988
THTR-300	Germany	HTGR, Power (Pebble Type)	300000 300 MW(e)	Th+235 U, Driver Fuel, Coated fuel particles, Oxide & dicarbides	1985–1989
Lingen	Germany	BWR Irradiation-testing	060000 60 MW(e)	Test Fuel (Th,Pu)O₂ pellets	1968; terminated in 1973
Dragon (OECD-Euratom)	UK (also Sweden, Norway & Switzerland)	HTGR, Experimental (Pin-in-Block Design)	020000 20 MWt	Th+235 U Driver Fuel, Coated fuel particles, Oxide & Dicarbides	1966–1973
Peach Bottom	USA	HTGR, Experimental (Prismatic Block)	040000 40 MW(e)	Th+235 U Driver Fuel, Coated fuel particles, Oxide & dicarbides	1966–1972
Fort St Vrain	USA	HTGR, Power (Prismatic Block)	330000 330 MW(e)	Th+235 U Driver Fuel, Coated fuel particles, Dicarbide	1976–1989
MSRE ORNL	USA	MSBR	007500 7.5 MWt	233 U Molten Fluorides	1964–1969
BORAX-IV & Elk River Station	USA	BWR (Pin Assemblies)	002400 2.4 MW(e); 24 MW(e)	Th+235U Driver Fuel Oxide Pellets	1963 - 1968
Shippingport	USA	LWBR PWR, (Pin Assemblies)	100000 100 MW(e)	Th+233 U Driver Fuel, Oxide Pellets	1977–1982
Indian Point 1	USA	LWBR PWR, (Pin Assemblies)	285000 285 MW(e)	Th+233 U Driver Fuel, Oxide Pellets	1962–1980
SUSPOP/KSTR KEMA	Netherlands	Aqueous Homogenous Suspension (Pin Assemblies)	001000 1 MWt	Th+HEU, Oxide Pellets	1974–1977
NRX & NRU	Canada	MTR (Pin Assemblies)	020000 20MW; 200MW (see)	Th+235 U, Test Fuel	1947 (NRX) + 1957 (NRU); Irradiation–testing of few fuel elements
CIRUS; DHRUVA; & KAMINI	India	MTR Thermal	040000 40 MWt; 100 MWt; 30 kWt (low power, research)	Al+233 U Driver Fuel, ‘J’ rod of Th & ThO2, ‘J’ rod of ThO₂	1960-2010 (CIRUS); others in operation
KAPS 1 &2; KGS 1 & 2; RAPS 2, 3 & 4	India	PHWR, (Pin Assemblies)	220000 220 MW(e)	ThO₂ Pellets (For neutron flux flattening of initial core after start-up)	1980 (RAPS 2) +; continuing in all new PHWRs
FBTR	India	LMFBR, (Pin Assemblies)	040000 40 MWt	ThO₂ blanket	1985; in operation

References and links

References

^ ^a ^b ^c ^d ^e ^f "IAEA-TECDOC-1450 Thorium Fuel Cycle-Potential Benefits and Challenges" (PDF). International Atomic Energy Agency. May 2005. http://www-pub.iaea.org/MTCD/publications/PDF/TE_1450_web.pdf. Retrieved 2009-03-23.
^ "IAEA-TECDOC-1349 Potential of thorium-based fuel cycles to constrain plutonium and to reduce the long-lived waste toxicity". International Atomic Energy Agency. 2002. http://www.iaea.org/inisnkm/nkm/aws/fnss/fulltext/tdi33008.pdf. Retrieved 2009-03-24.
^ Evans, Brett (April 14, 2006). "Scientist urges switch to thorium". ABC News. Archived from the original on 2010-03-28. http://web.archive.org/web/20100328211103/http://www.abc.net.au/news/newsitems/200604/s1616391.htm. Retrieved 2011-09-17.
^ Martin, Richard (December 21, 2009). "Uranium Is So Last Century — Enter Thorium, the New Green Nuke". Wired. http://www.wired.com/magazine/2009/12/ff_new_nukes/. Retrieved 2010-06-19.
^ Dean, Tim (April 2006). "New age nuclear". Cosmos. http://www.cosmosmagazine.com/features/print/348/new-age-nuclear?page=0%2C3. Retrieved 2010-06-19.
^ MacKay, David J. C. (February 20, 2009). Sustainable Energy - without the hot air. UIT Cambridge Ltd.. p. 166. http://www.inference.phy.cam.ac.uk/withouthotair/c24/page_166.shtml. Retrieved 2010-06-19.
^ http://flibe-energy.com/
^ http://nextbigfuture.com/2011/05/kirk-sorensen-has-started-thorium-power.html
^ http://www.guardian.co.uk/environment/blog/2011/sep/07/live-web-chat-nuclear-kirk-sorensen
^ http://www.huntsvillenewswire.com/2011/09/27/huntsville-company-build-thoriumbased-nuclear-reactors/
^ ^a ^b Le Brun, C.; L. Mathieu, D. Heuer and A. Nuttin. "Impact of the MSBR concept technology on long-lived radio-toxicity and proliferation resistance" (PDF). Technical Meeting on Fissile Material Management Strategies for Sustainable Nuclear Energy, Vienna 2005. http://hal.archives-ouvertes.fr/docs/00/04/14/97/PDF/document_IAEA.pdf. Retrieved 2010-06-20.
^ ^a ^b Brissot R.; Heuer D.; Huffer E.; Le Brun, C.; Loiseaux, J-M; Nifenecker H.; Nuttin A. (July 2001). "Nuclear Energy With (Almost) No Radioactive Waste?". Laboratoire de Physique Subatomique et de Cosmologie (LPSC). http://lpsc.in2p3.fr/gpr/english/NEWNRW/NEWNRW.html#foot284. "according to computer simulations done at ISN, this Protactinium dominates the residual toxicity of losses at 10,000 yr"
^ "The Use of Thorium as Nuclear Fuel" (PDF). American Nuclear Society. November 2006. http://www.ans.org/pi/ps/docs/ps78.pdf. Retrieved 2009-03-24.
^ "Operation Teapot". Nuclear Weapon Archive. 15 October 1997. http://nuclearweaponarchive.org/Usa/Tests/Teapot.html. Retrieved 2008-12-09.
^ "IAEA-TECDOC-1319 Thorium Fuel Utilization: Options and trends". International Atomic Energy Agency. November 2002. http://www.iaea.org/inisnkm/nkm/aws/fnss/fulltext/te_1319_f.pdf. Retrieved 2009-03-24.