Katana VentraIP

Nuclear reprocessing

Nuclear reprocessing is the chemical separation of fission products and actinides from spent nuclear fuel.[1] Originally, reprocessing was used solely to extract plutonium for producing nuclear weapons. With commercialization of nuclear power, the reprocessed plutonium was recycled back into MOX nuclear fuel for thermal reactors.[2] The reprocessed uranium, also known as the spent fuel material, can in principle also be re-used as fuel, but that is only economical when uranium supply is low and prices are high. Nuclear reprocessing may extend beyond fuel and include the reprocessing of other nuclear reactor material, such as Zircaloy cladding.

The high radioactivity of spent nuclear material means that reprocessing must be highly controlled and carefully executed in advanced facilities by specialized personnel. Numerous processes exist, with the chemical based PUREX process dominating. Alternatives include heating to drive off volatile elements, burning via oxidation, and fluoride volatility (which uses extremely reactive Fluorine). Each process results in some form of refined nuclear product, with radioactive waste as a byproduct. Because this could allow for weapons grade nuclear material, nuclear reprocessing is a concern for nuclear proliferation and is thus tightly regulated.


Relatively high cost is associated with spent fuel reprocessing compared to the once-through fuel cycle, but fuel use can be increased and waste volumes decreased.[3] Nuclear fuel reprocessing is performed routinely in Europe, Russia, and Japan. In the United States, the Obama administration stepped back from President Bush's plans for commercial-scale reprocessing and reverted to a program focused on reprocessing-related scientific research.[4] Not all nuclear fuel requires reprocessing; a breeder reactor is not restricted to using recycled plutonium and uranium. It can employ all the actinides, closing the nuclear fuel cycle and potentially multiplying the energy extracted from natural uranium by about 60 times.[5][6]

History[edit]

The first large-scale nuclear reactors were built during World War II. These reactors were designed for the production of plutonium for use in nuclear weapons. The only reprocessing required, therefore, was the extraction of the plutonium (free of fission-product contamination) from the spent natural uranium fuel. In 1943, several methods were proposed for separating the relatively small quantity of plutonium from the uranium and fission products. The first method selected, a precipitation process called the bismuth phosphate process, was developed and tested at the Oak Ridge National Laboratory (ORNL) between 1943 and 1945 to produce quantities of plutonium for evaluation and use in the US weapons programs. ORNL produced the first macroscopic quantities (grams) of separated plutonium with these processes.


The bismuth phosphate process was first operated on a large scale at the Hanford Site, in the later part of 1944. It was successful for plutonium separation in the emergency situation existing then, but it had a significant weakness: the inability to recover uranium.


The first successful solvent extraction process for the recovery of pure uranium and plutonium was developed at ORNL in 1949.[7] The PUREX process is the current method of extraction. Separation plants were also constructed at Savannah River Site and a smaller plant at West Valley Reprocessing Plant which closed by 1972 because of its inability to meet new regulatory requirements.[8]


Reprocessing of civilian fuel has long been employed at the COGEMA La Hague site in France, the Sellafield site in the United Kingdom, the Mayak Chemical Combine in Russia, and at sites such as the Tokai plant in Japan, the Tarapur plant in India, and briefly at the West Valley Reprocessing Plant in the United States.


In October 1976,[9] concern of nuclear weapons proliferation (especially after India demonstrated nuclear weapons capabilities using reprocessing technology) led President Gerald Ford to issue a Presidential directive to indefinitely suspend the commercial reprocessing and recycling of plutonium in the U.S. On 7 April 1977, President Jimmy Carter banned the reprocessing of commercial reactor spent nuclear fuel. The key issue driving this policy was the risk of nuclear weapons proliferation by diversion of plutonium from the civilian fuel cycle, and to encourage other nations to follow the US lead.[10][11][12] After that, only countries that already had large investments in reprocessing infrastructure continued to reprocess spent nuclear fuel. President Reagan lifted the ban in 1981, but did not provide the substantial subsidy that would have been necessary to start up commercial reprocessing.[13]


In March 1999, the U.S. Department of Energy (DOE) reversed its policy and signed a contract with a consortium of Duke Energy, COGEMA, and Stone & Webster (DCS) to design and operate a mixed oxide (MOX) fuel fabrication facility. Site preparation at the Savannah River Site (South Carolina) began in October 2005.[14] In 2011 the New York Times reported "...11 years after the government awarded a construction contract, the cost of the project has soared to nearly $5 billion. The vast concrete and steel structure is a half-finished hulk, and the government has yet to find a single customer, despite offers of lucrative subsidies." TVA (currently the most likely customer) said in April 2011 that it would delay a decision until it could see how MOX fuel performed in the nuclear accident at Fukushima Daiichi.[15]

The principles behind it are well understood, and no significant technical barriers exist to their adoption.

[43]

Readily applied to high- spent fuel and requires little cooling time, since the operating temperatures are high already.

burnup

[44]

More compact than aqueous methods, allowing on-site reprocessing at the reactor site, which avoids transportation of spent fuel and its security issues, instead storing a much smaller volume of on site as high-level waste until decommissioning. For example, the Integral Fast Reactor and Molten Salt Reactor fuel cycles are based on on-site pyroprocessing.

fission products

It can separate many or even all at once and produce highly radioactive fuel which is harder to manipulate for theft or making nuclear weapons. (However, the difficulty has been questioned.[45]) In contrast the PUREX process was designed to separate plutonium only for weapons, and it also leaves the minor actinides (americium and curium) behind, producing waste with more long-lived radioactivity.

actinides

Most of the radioactivity in roughly 102 to 105 years after the use of the nuclear fuel is produced by the actinides, since there are no fission products with half-lives in this range. These actinides can fuel , so extracting and reusing (fissioning) them increases energy production per kg of fuel, as well as reducing the long-term radioactivity of the wastes.

fast reactors

(see below) produces salts that can readily be used in molten salt reprocessing such as pyroprocessing

Fluoride volatility

The ability to process "fresh" spent fuel reduces the needs for (even if the recovered short lived radionuclides are "only" sent to storage, that still requires less space as the bulk of the mass, uranium, can be stored separately from them). Uranium – even higher specific activity reprocessed uranium – does not need cooling for safe storage.

spent fuel pools

Short lived radionuclides can be recovered from "fresh" spent fuel allowing either their direct use in industry science or medicine or the recovery of their decay products without contamination by other isotopes (for example: ruthenium in spent fuel decays to rhodium all isotopes of which other than 103
Rh
further decay to stable . Palladium derived from the decay of fission ruthenium and rhodium will be nonradioactive, but fission Palladium contains significant contamination with long-lived 107
Pd
. Ruthenium-107 and rhodium-107 both have half lives on the order of minutes and decay to palladium-107 before reprocessing under most circumstances)

isotopes of palladium

Possible fuels for (RTGs) that are mostly decayed in spent fuel, that has significantly aged, can be recovered in sufficient quantities to make their use worthwhile. Examples include materials with half lives around two years such as 134
Cs
, 125
Sb
, 147
Pm
. While those would perhaps not be suitable for lengthy space missions, they can be used to replace diesel generators in off-grid locations where refueling is possible once a year.[a] Antimony would be particularly interesting because it forms a stable alloy with lead and can thus be transformed relatively easily into a partially self-shielding and chemically inert form. Shorter lived RTG fuels present the further benefit of reducing the risk of orphan sources as the activity will decline relatively quickly if no refueling is undertaken.

radioisotope thermoelectric generators

Economics[edit]

The relative economics of reprocessing-waste disposal and interim storage-direct disposal was the focus of much debate over the first decade of the 2000s. Studies[60] have modeled the total fuel cycle costs of a reprocessing-recycling system based on one-time recycling of plutonium in existing thermal reactors (as opposed to the proposed breeder reactor cycle) and compare this to the total costs of an open fuel cycle with direct disposal. The range of results produced by these studies is very wide, but all agreed that under then-current economic conditions the reprocessing-recycle option is the more costly one.[61] While the uranium market - particularly its short term fluctuations - has only a minor impact on the cost of electricity from nuclear power, long-term trends in the uranium market do significantly affect the economics of nuclear reprocessing. If uranium prices were to rise and remain consistently high, "stretching the fuel supply" via MOX fuel, breeder reactors or even the thorium fuel cycle could become more attractive. However, if uranium prices remain low, reprocessing will remain less attractive.


If reprocessing is undertaken only to reduce the radioactivity level of spent fuel it should be taken into account that spent nuclear fuel becomes less radioactive over time. After 40 years its radioactivity drops by 99.9%,[62] though it still takes over a thousand years for the level of radioactivity to approach that of natural uranium.[63] However the level of transuranic elements, including plutonium-239, remains high for over 100,000 years, so if not reused as nuclear fuel, then those elements need secure disposal because of nuclear proliferation reasons as well as radiation hazard.


On 25 October 2011 a commission of the Japanese Atomic Energy Commission revealed during a meeting calculations about the costs of recycling nuclear fuel for power generation. These costs could be twice the costs of direct geological disposal of spent fuel: the cost of extracting plutonium and handling spent fuel was estimated at 1.98 to 2.14 yen per kilowatt-hour of electricity generated. Discarding the spent fuel as waste would cost only 1 to 1.35 yen per kilowatt-hour.[64][65]


In July 2004 Japanese newspapers reported that the Japanese Government had estimated the costs of disposing radioactive waste, contradicting claims four months earlier that no such estimates had been made. The cost of non-reprocessing options was estimated to be between a quarter and a third ($5.5–7.9 billion) of the cost of reprocessing ($24.7 billion). At the end of the year 2011 it became clear that Masaya Yasui, who had been director of the Nuclear Power Policy Planning Division in 2004, had instructed his subordinate in April 2004 to conceal the data. The fact that the data were deliberately concealed obliged the ministry to re-investigate the case and to reconsider whether to punish the officials involved.[66][67]

Nuclear fuel cycle

Breeder reactor

Nuclear fusion-fission hybrid

Spent nuclear fuel shipping cask

Taylor Wilson's nuclear waste-fired small reactor

announced February 2006

Global Nuclear Energy Partnership

Williamson, M.A.; Willit, J.L. (2011). (PDF). Nuclear Engineering and Technology. 43 (4): 329–334. doi:10.5516/NET.2011.43.4.329.

"Pyroprocessing Flowsheets for Recycling Used Nuclear Fuel"

Till, C.E.; Chang, Y.I; Hannum, W.H. (1997). "The integral fast reactor-an overview". Progress in Nuclear Energy. 31 (1–2): 3–11. :10.1016/0149-1970(96)00001-7.

doi

OECD Nuclear Energy Agency, , Paris, 1994

The Economics of the Nuclear Fuel Cycle

I. Hensing and W Schultz, Economic Comparison of Nuclear Fuel Cycle Options, Energiewirtschaftlichen Instituts, Cologne, 1995.

Cogema, Reprocessing-Recycling: the Industrial Stakes, presentation to the Konrad-Adenauer-Stiftung, Bonn, 9 May 1995.

OECD Nuclear Energy Agency, Plutonium Fuel: An Assessment, Paris, 1989.

National Research Council, "Nuclear Wastes: Technologies for Separation and Transmutation", National Academy Press, Washington D.C. 1996.

World Nuclear Association

Processing of Used Nuclear Fuel

PUREX Process, European Nuclear Society

– World Nuclear Association

Mixed Oxide Fuel (MOX)

– Congressional Research Service Report for Congress

Disposal Options for Surplus Weapons-Usable Plutonium

Brief History of Fuel Reprocessing

Annotated bibliography for reprocessing spent nuclear fuel from the Alsos Digital Library for Nuclear Issues