Showing posts with label uranium. Show all posts
Showing posts with label uranium. Show all posts

Wednesday, 22 September 2021

Plutonium

 Plutonium

 

In 1952, the Periodic Table that covered our exam questions had plutonium, atomic number 94, on it. It also had americium, curium, berkelium and californium but all these were faint, made of dots, faded as though they were ghosts of elements rather than the elements themselves.

 

It was exciting to know that scientists were still “discovering” new elements. They described what they were doing as “discovering”; I had no idea that they were actually manufacturing them nor that they existed for mere seconds or milliseconds. To my eight-year-old mind, their “discovery” meant that they were part of the basic building blocks of the universe. I was now primed for more elements, for more atomic “discoveries”!

 

In fact, uranium is the last element natural to our environment; all elements with atomic numbers greater than 92 were or would be created, would be artificial, transient, and radioactive.  

 

Uranium was first isolated in 1789. A German chemist, Martin Klaproth, isolated it from pitchblende ore. He named it “uran” in honour of a recently discovered seventh planet from the sun, Uranus. 

 

Martin had no knowledge of nuclear physics; he did not know that uranium had an atomic number of 92 for the 92 protons in its nucleus and the 92 electrons flying around it. A hundred and fifty years later when Manhattan project scientists created an element with 93 protons in its nucleus, they named it “neptunium” (Np) after the eighth planet from the sun. It was natural for them to name element number 94 “plutonium” after then-ninth-planet Pluto[1].

 

Planet Pluto itself was named for the god of the underworld, and of the afterlife. Pluto was also the god of wealth because gold and silver came from the ground. It was an apt name for a long-lived and entirely manufactured element that would become the sought-after explosive for atomic bombs.

 

Both neptunium and plutonium[i] were formed by bombarding uranium-238 with neutrons in a cyclotron. 

 

Scientists knew that uranium-235 was fissile bomb-making material; its disadvantage for this purpose was that nearly 50 kg were required to make an explosive device. Furthermore, natural uranium was mostly U238. Being less than 5% of natural uranium, it required time-consuming processes to be enriched to a bomb-making concentration greater than 90%. Scientists didn’t feel that they had “lots of time”. They also knew that a heavier element was theoretically possible.

 

Element 93, neptunium, was not fissile, but it spontaneously and quickly (two days half-life) decayed by beta emission into element 94, plutonium, which proved to be fissile. Only eleven kilograms, a 4-inch diameter sphere of plutonium-239 would be needed to make a bomb. 

 

The race was on to isolate it, characterize it and weaponize it. Scientists at Los Almos, New Mexico, worked with quantities so small that they could not see them. They could only trace them by following their radioactivity. The history of the “radium girls” was in their minds so they watched contamination rigorously. They worked in a highly ventilated and filtered atmosphere, submitted to “nose wipes” that were checked for radioactivity, and tried to recover every spilled atom of plutonium. 

 

It is clear from the records kept by Dr. Hempelmann, the medical doctor in charge of the health team, that measures to protect the staff were not taken for simple humanitarian reasons – he, Oppenheimer and another physician, Stafford Warren, were concerned about lawsuits. Studies with plutonium in rats indicated that the element was a “bone-seeker” like radium and also that it accumulated in the liver. Compared to radium, it was excreted much more slowly which meant that it stayed in the body longer. Having a longer biological half-life meant greater exposure to radioactivity.

 

One of their other early discoveries was the difficulty in keeping it contained. They couldn’t even see the element, but it got onto their shirt cuffs, soles of shoes, laboratory doorknobs and their own faces. 

 

On August 1, 1944, a chemist, Don Mastick, had an accident that illustrates the concern that the laboratory had about their plutonium samples.

 

Don’s equipment was miniature – his test tubes were the size of darning needles. He was working with microscopic quantities when he opened a tiny vial containing 10 mg of plutonium[2] dissolved in acid. Because gas had accumulated in the vial, it exploded onto the wall, his face and his clothing. He tasted the acid.

 

He immediately went to the medical clinic across the road. His face was washed and the water saved. His mouth was swished and the spittle saved. His stomach was pumped twice and the contents saved. In fact, as the only chemist working in isolation of plutonium, after these decontamination procedures, Don was given all the washings to return to the laboratory and retrieve the plutonium. All but 1 microgram (one thousandth of a milligram) was recovered. That one microgram in his body was enough to blow the ionization chamber off-scale for days after the accident with his breath and, thirty years later, still be detectable in his urine!

 

Plutonium is an unusual element. When pure plutonium is exposed to air it quickly forms hydrides and oxides and can expand massively to 70% more that its original volume. The flakes are pyrophoric meaning that they can spontaneously ignite. It reacted chemically in such different ways that it was easy to separate from its parent element, uranium-238.

 

John Gofman had isolated 1.2 milligrams of plutonium from 2 tons of uranium in a cyclotron in autumn, 1942. It took six weeks of neutron bombardment[3] and a further three weeks to chemically isolate it (at this time, every step had to be invented; they were just beginning to learn about its characteristics). In liquid form, the 1.2 mg had a volume equal to ¼ of a teaspoon.

 

Clearly, for bomb construction, they need a faster process. Enrico Fermi created a primitive nuclear reactor in Chicago, the Chicago Pile 1, to demonstrate that a sustained reaction could be obtained. An Oak Ridge reactor was in construction and would be functioning by November 1943 to deliver plutonium to Los Almos the following year.  

 

By this time, the uranium bomb had been designed as a “gun-type” device. A half sphere of uranium was “shot” using a conventional explosive into another half-sphere to create a critical mass which would explode. Scientists needed to work on a different device because the desired plutonium isotope, Pu239, was contaminated with another isotope, Pu240, which just fizzles along and interfers with the explosive quality of Pu239. 

 

They came up with a different device, an implosion bomb that brought the bits of plutonium forcibly together by a circle of explosive charges. Once united, they reached criticality and would explode.

 

They weren’t entirely sure that it would work as planned and arranged to test it. The Trinity Test was secretive, allegedly done “where there were no people or animals”. In the highly secretive wartime atmosphere, General Groves’ pre-prepared press release lied about the detonation, seen and felt up to 100 miles away like this: “A remotely located ammunition magazine containing a considerable amount of high explosives and pyrotechnics exploded.” 

 

Thirty miles away farm animals and cattle lost the hair on their backs – it regrew white. The army purchased these animals and allegedly took them to Los Almos and Oak Ridge to follow their health. Some researchers claim that there may have been human fetal loss of up to 52% using state statistics. It was not, in fact, an unpopulated location and many of the rural people in the area consider themselves to be the first victims of nuclear weapons.

 

One thousand miles away, the Eastman Kodak officials reported furiously that their unexposed film had been contaminated by radioactive particles, presumably from Wabash River water. Any delusions about limited radioactive fallout were dashed from the first atomic bomb blast.

 

When the Manhattan project scientists were working with it, plutonium was code-named as “the Product”. Dogs, cats, rats and rabbits were injected, forced to breath plutonium-contaminated air or fed plutonium. Those that received the largest doses sickened and died. Pregnant animals aborted or eventually delivered small or deformed babies. Large numbers of lab animals were sacrificed in numerous studies. This was not enough to establish plutonium’s toxicity.

 

They wanted human subjects to test “the product”. They didn’t know how quickly people could excrete it, whether through urine or feces. They knew that radioactivity caused a decline in blood cells but they didn’t know how quickly it might happen with plutonium. They explained that human experiments “were needed to see how to apply the animal data to human problems”[ii].

 

At this point, the story of plutonium slips into the bizarre.

 

While they determined that the human subjects sought needed to be suffering from incurable diseases but have close to normal kidney function in order to study excretion of plutonium in urine and feces, their first victim was a "well developed...well nourished" "colored male"[iii] who had been involved in a motor-vehicle accident. He was employed as a construction worker from the Oak Ridge site of the Manhattan project.

 

It is very unclear why he was chosen because he was noted to have “somewhat diminished”[iv] kidney function. Perhaps he was only a victim of opportunity. His motor-vehicle accident occurred on the Oak Ridge site. 

 

Ebb Cade was 55 years old. He had multiple broken bones which left untreated for three weeks in order prepare for the experiment. The bones were surgically reduced five days after the plutonium was given an opportunity to “settle” in and on them. During the surgery, physicians were able to determine that plutonium did indeed go to bones. 

Their study was badly flawed because they failed to keep the pre-injection urine and feces separate from the post-injection products

 

When describing the experiment in a classified talk, perhaps in an attempt to assuage his guilt, one of the researchers described Ebb as “an elderly male whose age and general health was such that there is little or no possibility that the injection can have any effect on the normal course of his life”[v]. No mention was made of his employment or of his broken bones. No mention is made of his subsequent health until his death in 1953 from “ventricular fibrillation following heart failure”[vi] at the age of 63. No consent for the experiment was ever sought and no information was given by the researchers to his wife or family.

 

The next patient was Arthur Hubbard, a retired businessman with an aggressive squamous cell cancer. He received 6.5 micrograms of plutonium intravenously and his urine and stool samples were collected thereafter. Arthur’s cancer was well advanced so he fit their criteria.

 

The third patient was Albert Stevens, a fifty-eight-year-old house painter. He was presumed to have a limited lifespan with stomach cancer. He had normal kidney function, an “ideal candidate for the experiment”. He was injected with Pu238, a more radiotoxic isotope of plutonium but more readily measured than Pu239 with the instruments of the 1940’s.

 

Four days after the injection, with plutonium coursing throughout his body, Albert went to surgery for removal of his “carcinomatous mass”[vii]. When the pathologist could not find any evidence of cancer, the entire team was shocked. Albert lived for another 21 years; there seems to be no comment about his general health although he had received one of the largest test doses of plutonium.

 

Neither Arthur nor Albert nor their families were sought for permission nor were they ever told about the experimental nature of their injections. Arthur died shortly after the injection; Albert died of heart failure at age 79.[viii]

 

There were a total of eighteen victims of plutonium injections. They received poor follow-up, their initial health conditions were so varied that it was impossible to establish a baseline, and of course, none of them were informed or asked to sign releases. 

 

Lying, obfuscation and secrecy kept the experimenters connected and established the foundation for denial of health effects of ionizing radiation. This was true for both scientists and politicians who supported research and continuing development of nuclear bombs.

 

There have been and will continue to be many more victims of Trinity, Hiroshima[ix] and Nagasaki.

 

Minute traces of plutonium are now found in every human body on earth. More than 550 atmospheric and underwater nuclear tests have been carried out and some dozen or more major nuclear accidents have contaminated the globe. 

 

While scientists with the Manhattan Project were unable to establish the health effects of relatively small exposures to plutonium, they certainly knew the effects of large exposures through some of the criticality accidents in their research labs. 

 

A critical reaction is one that is self-sustaining, a reaction that only needs “moderating” to continue, a reaction where the numbers of neutrons produced effect the further release of the same numbers of neutrons. A nuclear power plant is said to go “critical” when it is “turned on” to create the heat necessary to boil water.

 

A “criticality accident” occurs when an accidental uncontrolled, unmoderated chain reaction occurs. According to Wikipedia, there have been sixty criticality accidents recorded since 1945[x]. 

 

In order to determine the exact amount of plutonium required to explode, scientists experimented by bringing pieces of plutonium into close proximity to one another. They also tried various means to increase the number of neutrons released from the plutonium core by using various elements as “reflectors”. The experiments were called “tickling the dragon’s tail”. 

 

On two well known occasions, scientists received fatal doses of radiation when their experiments went critical. Since both men were using the same plutonium core and running trials less than a year apart, that core gained the name, “the demon core”. It was later melted down for use in other bomb tests.

 

Both men, Harry Daghlian and Louis Slotin, received estimated radiation doses greater than 5 Sv. Both men received the best possible medical care, specialists flown to the site hospital from across the United States. Their families were also notified and flown to their bedside knowing that they would not live. Both died painful prolonged deaths, their bodies bloating and edematous as cell walls broke apart, their minds disordered, excruciating diarrhea as the linings of their guts became part of their feces. 

 

Harry’s accident occurred less than three weeks after the bombs were dropped on Hiroshima and Nagasaki. His agonizing death took 25 days. All the scientists and highest-ranking military men could not avoid knowing that some people would die this way when bombed in an atomic war.

 

Louis actually moved closer to the reaction, possibly to protect the other people in the room. He died nine days later.

 

We heard nothing about these experiments in 1952; the information was classified.

 

Later, in 1958, Cecil Kelley’s death was also classified. Cecil was a chemist, a technician working in a plutonium-separation laboratory. He received an estimated 36 Seiverts exposure when a plutonium acid bath that he was mixing went critical. Since exposure to 5 Sv was considered a universally fatal dose for humans, medical staff knew that Cecil would die and considered him an “experiment of opportunity”. Repeated blood samples, catherization of his bladder and even a bone marrow biopsy of his sternum were done without permission. Every moment of his life was recorded.

 

The blood samples taken six hours after the accident showed that he no longer had white blood cells; a bone marrow examination produced only acellular red watery substance. He had been knocked unconscious initially, had a very brief period of lucidity before he slipped into a coma and died 35 hours later. He was autopsied and more than eight pounds of body parts and tissues were removed from his body. His wife was not informed of the accident until after his death, nor was her permission sought for either the autopsy or removal of organs. His cause of death was recorded as “congestive heart failure”.

 

Plutonium, like its namesake, the god of the underworld, afterlife, and wealth, was powerful. Dangerous to handle, it grabbed the hearts and minds of countless brilliant people. Even as it continues to leak poisonously into the environment, more is constantly being created. Like heroin, it has become an addiction.

 

 



[1] Pluto was demoted from planetary status to “dwarf planet” in August 2006.

[2] Plutonium is very dense. Twenty mg of plutonium occupies 1 cubic mm.

 

[3] Deuteron was used for bombardment. It is the nucleus of a deuterium atom, one proton and one neutron.



[i] There is argument that plutonium may have been a primordial element because infinitesimal amounts have been found in nature. The counterargument is that they are the result of natural bombardment of uranium-238 by neutrons. Neptunium is entirely of human manufacture.

[ii] Plutonium files p89, from Russell & Nickson, p2 Distribution and Excretion of Plutonium”

[iv] The Plutonium Files P83

[v] Ibid, p86

[vii] “Description of Operation” June 6, 1945, Stevens m.r. Quoted in Plutonium Files P92

[ix] “Little Boy”, the bomb that was dropped on Hiroshima, was a uranium-235 bomb. “Fat Man” on Nagasaki was a plutonium-239 bomb.

Monday, 6 November 2017

Uranium Mining: Human and Environmental Health Effects


 Uranium is a common element in the earth’s crust, more abundant than gold, silver and mercury and found everywhere. Being chemically reactive, it is never found in its elemental form; most commonly it is bound as uranium oxide, U308. Mining can be cost effective wherever ore concentrations reach 0.02%. One of the highest concentrations was Saskatchewan’s mine at Key Lake at 15.9% U308. Saskatchewan also boasts the world’s largest mine at McArthur River (concentration of 9.6% U308).

From 1990 to 1996, I worked with Northern Medical Services in Saskatchewan. In 1991, our clinic diagnosed three miners with Systemic Lupus Erythematosus, a disease rarely found in men and, at that time, unknown among the Dene. We were told by specialists that there was no connection between the disease and the exposure of these men to uranium. The dearth of research on environmental contamination from mining and the lack of baseline health information on Northerners left me with questions.

The Process of Mining, Milling and Refining:

Wherever mining occurs, the earth’s mantle is disrupted and mining waste (tailings) remain on the surface or placed back into the mines in its pulverized form. On the surface, to prevent wind erosion and spread of toxicity, they are usually covered with water creating tailings ponds. Placed back into the mines, the previously bound material is now loose aggregate.

What does the ore contain? Besides uranium, a host of common elements are found including arsenic, iron, magnesium, titanium, calcium, sodium, potassium, sulfur and silicon. The heavy metal and toxic content is the real concern; the tailings contain all the progeny of uranium’s radioactive decay - thorium, protactinium, radium, radon, polonium, bismuth, francium, astatine, thallium and lead. 85% of the radioactivity remains in the tailings and, over time, the waste actually becomes more radioactive as the elements with very long half-lives[1] decay[2] into the elements with shorter half-lives.

Of special concern is radon, a gas considered responsible for 20% of the lung cancers in Canada. It is heavier than air and can be spread over 1000 km by a stiff wind. Furthermore, as it decays in its 3.8 day half-life, it becomes polonium, a solid which eventually settles out of the air and may be taken up by plants and lichens. Polonium is the most toxic substance known to human kind. An alpha emitter and therefore undetectable by normal Geiger counters, the amount of polonium equivalent to the ink in a period in this sentence is 200 times a lethal dose for humans. (That amount was used to kill the double Russian spy, Litvinenko, in 2006 in the U.K.)

Milling occurs close to the mine sites. The ore is pulverized into a dust, the uranium oxide extracted using ammonia or sodium bicarbonate. The resulting “yellowcake” which is 70% uranium, is trucked to a refinery at Blind River in Ontario where it is further purified to uranium trioxide. Further processing occurs at a conversion plant in Port Hope which changes the trioxide into either a dioxide powder for CANDU-type reactors or to uranium hexafluoride. The uranium hexafluoride is transported to enrichment plants in the United States. Both refinement and conversion leave waste products with radioactive content.

Environmental Effects:

Uranium has been mined in Canada for over seventy years. Little research has been done on the direct effect of the mines and their tailings upon the environment. Mining, processing, and reclamation have the potential to affect soils, air quality, and biota through surface water quality and groundwater quality and quantity[3].

Any mine is physically disruptive to the environment, displacing plant and wild life kilometers away, separating animals from their food sources and affecting migration patterns. In Ontario, the mining act permits a company to clear-cut and surface-strip removing up to 1000 tonnes of rock without any restoration. Open Pit mines may occupy hectares of land surface, release radon and other elemental dust particles to the atmosphere; underground and leach mining continue the same releases during the milling process. The tailings from both mining and milling remain toxic for thousands of years.

The potential to affect surface and ground water quality is evident in Nero Lake, a small lake west of Uranium City used as a dump for tailings prior to the closure of the Lorado mine site in 1961. When assessed in 2013, 52 years later, Nero Lake had very little biological activity in its waters or rocky bed. “Even if the entire set of mine sites are cleaned-up around Uranium City, four watersheds will have levels of selenium and uranium in excess of Saskatchewan Surface Water Quality Objectives.”[4]

The potential to affect much wider areas was realized when the Church Rock Dam in New Mexico was breached by its tailing pond in 1979. The amount of radiation released to the water and the atmosphere was three times that of the Three Mile Island power plant disaster. A swath of land following the overflowed creek continues to be heavily contaminated, its water unsafe for cattle. Clean-up, 38 years later, continues to await resolution of federal/facility law suits.[5]

In summary, to date there have been little substantive research upon the exact impact to the environment of uranium mining. With the known toxicity of both the ore mined and the tailings remaining exposed or remediated, the potential for environmental contamination exists for millennia.  Tailings ponds (as at Elliot Lake) may dry up and the protected toxins lifted into the atmosphere by the wind; wastes buried in mine pits (as in Cluff Lake) can be absorbed by plants which in turn are ingested by animals.[6] Long term risks are poorly defined.

It is human hubris to assume that any attempt at restoration can stand the test of time for these wastes.

Human Health Effects:

Studies of workers at all of the mining and processing stages has established some of the human health effects of uranium. Uranium and its progeny are heavy metals and would be expected to have effects on human growth and development similar to the two most extensively studied heavy metals, mercury and lead. These include renal failure and brain damage, DNA damage and fertility problems, high blood pressure and atherosclerosis, muscle and joint pain without arthritic changes, behavioural and developmental challenges in children and hearing damage.

However, these potential risks have been very poorly researched. While the CNSC (Canadian Nuclear Safety Commission) Synopsis report[7]concluded that “no adverse health effects have occurred or are likely to occur in Port Hope as a result of the operations of the nuclear industry in the town” they actually ignored some the research they quoted in the paper. The same organization claimed that the report was “peer-reviewed” when, in fact, a single Harvard researcher was paid to review the document. The document itself admits to statistically higher incidences of circulatory disease, and pneumonia; some of the research quoted as non-significant showed increases in incidence of the target health concern up to the end of the period of time allotted to the study which leads to the question of why that particular “cut-off” date or why the need for longer term research was not recommended? Other objections to the quality of research include: an increase in Down’s syndrome amongst the children of male workers at the refinement plant in spite of the short length of time and small population studied, mixing rare and relatively common cancers so that the effect of the common cancer (leukemia) is lost in the data, excusing the elevated incidences of circulatory disease and pneumonia on poorly matched mortality data – all suggestive of CNSC’s collusion with the industry itself. 


New data is arising as more and more researchers focus on uranium as a chemically reactive heavy metal. Besides its effect as a heavy metal, it mimics estrogen. Rat studies indicate fertility problems but while this conclusion requires human studies to confirm the effect on human populations, the estrogenic effects may be responsible for the increase in a female-dominated disease, Systemic Lupus Erythematosis.[8]
The radioactivity cannot be discounted; the increase in cancer deaths amongst Eldorado miners who worked unprotected from 1930’s to 1960 is never contested but attributed solely to radon exposure by the CNSC; the SENES study reviewed the health of miners from 1975 onwards and concluded that miners would experience 1:100 increase lung cancer over non-miners[9]. Because it is an alpha-particle producer, uranium has the potential to be extremely carcinogenic and genotoxic but it might take generations to document the effect in humans.
As Brugge and Buchner point out in their review paper of 2011, “As much damage is irreversible, and possibly cumulative, present efforts must be vigorous to limit environmental uranium contamination and exposure[10].”
Conclusion:
Uranium has two uses, nuclear bombs and nuclear power.
Nuclear Bombs are an indiscriminate weapon. The Non-Proliferation Treaty was established in 1967 to disarm the nuclear powers and prevent the spread of nuclear bombs to other countries. It has failed on both counts so a Nuclear Weapons Ban Treaty has been proposed by 122 countries. Clearly, the majority global citizenry want disarmament.
Nuclear power was developed initially in order to provide material for nuclear weapons. It has created enormous amounts of waste for which, after 70 years and billions of dollars, no long-term storage facility has been found. In addition to the failure to deal with its waste, the industry has priced itself out of the market. It cannot compete with solar, wind or other sustainable energy technology. Currently responsible for only 3% of the worlds energy, it is unlikely that there is a future for nuclear power.
Since there is no other purpose for uranium, a moratorium on the mining of uranium (as exists in the provinces of British Columbia and Quebec) should become global.
                                                                                   









[1] A “half-life is the length of time that a radioactive element takes to change one half of its atoms into another element. Half-lives of uranium-238 and uranium-235 are 4.5 billion and 703.8 million years while those of thallium-206 and polonium-210 (at the other end of the series of decaying elements) are 4.2 minutes and 138.3 days.
[2] “Decay” occurs when the element releases energy in the form of an alpha or beta particle and changes into the next element of its decay chain. This length of time required for a decay is specific to each element – it cannot be stopped.
[3] https://www.nap.edu/read/13266/chapter/9
[4] Ann Coxworth, PhD, The Environmental Resource, Saskatchewan Environmental Society, Jan-Feb 2014, p13.
[5] Dale Dewar & Florian Oelck, From Hiroshima to Fukushima You, Between the Lines, Toronto, 2014
[6] Local hunters claim that moose have already disturbed the overlaying protection in search of salt. (Personal communication).
[7] CNSC Synopsis Report, April, 2009. “Understanding Health Studies and Risk Assessments Conducted in the Port Hope Community from the 1950’s to the Present”
[8] Lu-Fritts, et al, “Systemi Lupus Erythematosus is Associationed with Uranium Exposure in a Community Living Near a Uranium Processing Plant: A Nested Case-Control Study”, Arthritis Rheummatol, 2014 Novemember, 66(11): 3105-3112
[9] Jointly reviewed by CNSC in this paper: http://nuclearsafety.gc.ca/eng/pdfs/health-studies/Opportunity-North-Vol13-Issue4-P21-The-Health-of-Uranium-Miners_e.pdf. It is interesting to compare the jump to conclusions reported here with the quandary where the entire nuclear industry tried to discount the findings of the KiKK study, a Germany study which concluded that there was a distance-related increase in leukemia in children living close to nuclear power plants.
[10] Brugge D, Buchner V, “Health Effects of uranium: new research findings”, Rev Environ Health. 2011;26(4):231-49