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Spontaneous separation of californium and curium.

The environmental tragedy now commencing in the United States means that future generations will be even more challenged to address severe environmental issues than they would have been had the United States constitution prevented the installation of an insane administration.

The insanity exists however, and those of us who can in the United States should not abandon our pursuit of knowledge, however much science may be threatened by the anti-intellectual bent of the mob that has seized control of the United States in defiance of Democracy.

If we have learned nothing in the last two decades about addressing climate change, it is that so called "renewable energy" cannot stabilize the atmosphere. This is demonstrated by the incontrovertible fact that the expenditure of trillion dollar sums on this failed technology has had no effect whatsoever on the unrelenting increase in climate change forcing gases.

We're at 406,14 ppm this week, 3.52 ppm higher than last year.

Although we have left a great mess for all future generations, one thing that they may not appreciate is that we have left them is sufficient fully isolated uranium to provide for all of the world's energy demands for many generations to come, as well as technology that can make access to uranium inexhaustible beyond several centuries, with rather less than dire environmental impact. A relatively small amount of uranium is capable of eliminating all the world's energy mines, all of the coal fields, all of the gas fields, fracked and traditional, and all of the world's oil fields.

For the overwhelming bulk of this uranium to be utilized, it will need to be converted to plutonium, utilizing, among other things, existing plutonium inventories (including weapons grade plutonium which must be denatured and rendered impossible to use in nuclear weapons.)

Right now, and for the immediate forseeable future, most of the world's nuclear reactors utilize the thermal neutron spectrum which is many ways undesirable, but it's what we have for now, at least until the fine upcoming generation of nuclear, chemical, and materials science engineers can apply their intellects to change this state of affairs, as we must hope they will.

Continuously recycled plutonium in a thermal cycle, according to one reference, (Ref: Nuclear Reactor Physics, William E. Stacy, Wiley and Sons 2001. pg.234) will consist of an isotopic mixture having roughly 8.17% 238Pu, 45.10% 239Pu,
20.54% 240Pu, 18.57%, 241Pu, and 7.62% 242Pu. These figures show - they are probably only valid as a first approximation - that plutonium can be readily transformed into a form totally unsuitable for weapons use, owing to the heat load associated with 238Pu and 241Pu which decays in situ to 241Am.

However the transuranium isotope distribution will not be limited to plutonium in this state of affairs (which is less sustainable than fast spectrum fission reactors, which can supply all human energy needs indefinitely.) Among the transuranium elements, working from the same reference, only 51% will be represented by plutonium. Roughly 5% will be neptunium, 9% will be americium, 34% will be curium, with smaller amounts being represented by californium and berkelium.

As I noted earlier in a post here, the accessibility of high oxidation states makes the separation of plutonium, neptunium, and americium from traditional used nuclear fuels, almost all of which are based on oxides of the actinides. Neptunium and americium are the key to generating 238Pu to eliminate the value of plutonium for weapons diversion.

In the case of americium, however, an intermediate in the production of 238Pu is 242Cm. The other curium isotopes will also be present, and what's more, inevitably, this curium will also be contaminated with californium. Because of californium's high rate of neutron production, it is desirable to separate it from other elements both to utilize this spontaneous flux, and to simplify the handling of curium for the recovery of its heat.

Neither californium nor curium however exhibit stable higher oxidation states. This means that while they are easily separated from the lower actinides, they are more challenging to separate from one another; in general (especially since in general only small amounts are produced today), one must resort to procedures like chromatography.

All of this is why I read with interest today a paper detailing a spontaneous separation of curium and californium.

The paper is here: Inorg. Chem., 2015, 54 (23), pp 11399–11404 "Spontaneous Partitioning of Californium from Curium: Curious Cases from the Crystallization of Curium Coordination Complexes"

Some text from the paper:

Curium plays a central role in actinide chemistry in that it is isoelectronic with gadolinium, and both trivalent ions possess half-filled f7 shells. This allows curium(III) compounds and complexes to be used as benchmarks for comparisons with gadolinium and other lanthanide analogues as well as with both earlier and later actinides.(1) Given the spherical symmetry of the f7 configuration and the general perception that both 4f and 5f orbitals are nonbonding, one might expect that gadolinium(III) would be an excellent analogue of curium(III) if the difference in their ionic radii is excluded. In fact, the electronic characteristics of curium(III) diverge from those of gadolinium(III) in a number of respects...

Actually the "general perception" of 5f is not really valid, but no matter.

A little more on uses for curium:

Curium(III) is perhaps the most luminescent of all 5f-element ions and emits characteristic orange light centered near 600 nm.(7) This property is extraordinarily useful in a wide variety of applications that range from solution complexation studies to the environmental behavior of trivalent actinides to biological probes to understanding energy-transfer processes in f-block materials.(7) Changes in the coordination of curium(III) can cause substantial shifts in the photoluminescence peak position and spectral shape.(7) In contrast, gadolinium(III) compounds, while capable of emitting at visible wavelengths, have low quantum yields even when antennas are utilized for energy transfer and are often used as nonemitting hosts in europium(III)- and terbium(III)-doped materials.(8)

Some remarks on separations:

The separation of middle-to-late actinides from one another has been a key challenge for decades in the development of the chemistry of these elements, their use as targets for the production of super heavy elements (i.e., transactinides), and advanced nuclear fuel cycles for separating lanthanides from actinides. Studies of the stability constants of trivalent lanthanides and actinides with α-hydroxyisobutyrate show that a monotonic trend exists with lanthanides.(14) However, with diethylenetriamine-N,N,N′,N″,N″-pentaacetic acid, this trend is not preserved; curium binds more weakly, and californium more strongly, than expected.(14, 15) These early studies were already suggestive of a change in chemistry occurring at californium that continues through mendelevium.(14, 15)

We recently communicated a few features of the curium(III) tris-chelate, 2,6-pyridinedicarboxylate (dipicolinic acid, DPA) complex, Cm(HDPA)3, as a part of a comprehensive study that compared middle actinides with californium.(16-18) Herein, we substantially expand on our analysis of this complex as well as elucidate the structure and properties of the bis-chelate complex 2Cl]+.

They ran some crystallizations and to their surprise found that the crystallization process lead to the separation of tiny amounts of californium complexes from curium complexes.

The collection of photoluminescence spectra from groups of crystals revealed that the colorless crystals of DPA that cocrystallize with the bis-chelate luminesce green, as shown in Figure 4. Collection of this luminescence spectrum showed that the green luminescence is superimposable with that of Cf(HDPA)3, including the fine vibronic structure (see the Supporting Information).(16) Single-crystal X-ray diffraction studies demonstrate that these crystals are ostensibly just DPA. However, it must be kept in mind that crystal structures are averages of the total composition of the crystal and are largely insensitive to trace doping.(31) However, they are clearly doped with low levels of Cf(HDPA)3, . Dissolution of the crystals followed by energy-resolved liquid scintillation counting of californium in the crystals reveals doping levels of 37(5) ppm. The error on this number represents the deviation in the dopant levels between crystals and supports essentially constant doping levels from crystal to crystal. Crystals were also cut and broken, and the lack of significant variation in the photoluminescence intensity of the interior versus exterior of the crystals reveals a relatively uniform distribution of californium throughout the samples. This level also indicates that californium is concentrated within the DPA crystals because the californium levels in typical 248Cm samples are ∼1 ppm (or less).

Here's the picture of the crystals:

Esoteric, I know, but cool. They'll need to know these sort of things in the future if they wish to save themselves from what our irresponsibility has done.

Enjoy the coming week.

My personal favorite protest picture today: Antarctica.

CNN's photos of protests around the world.

We have one running on every damned continent.

We may have a large subset of sexist racists in the USA who have managed to subvert the will of the majority, but it's very, very, very, very clear that humanity is not going to stand aside while the United States is pillaged by thugs.

The orange thug may find his 1930's style "America First" fascism may lead to severe economic sanctions, a pariah status, and a vast retreat by his Quisling collaborators.

We'll be watching horror movies to avoid listening to the Trump crap. What about you?

We figure that the scariest horror movie can't equate to the horror in the White House, a zombie with a paint on off color tan and a comb over that glows in the dark.

What you gonna do?

A remarkable advance in actinide separations in used nuclear fuel has been discovered.

I'm not shy about offering my opinion, irrespective of public hostility that is very dangerous to the future of humanity, that nuclear energy is the last best environmental approach to producing a sustainable world, given that uranium is inexhaustible, and that when converted to plutonium, the uranium already mined can supply all of humanity's energy needs for centuries to come.

The key to obtaining this plutonium is however, involved in separating it from used nuclear fuel.

Continuous recycling of used nuclear fuel in thermal reactors, however - and I'm not a thermal reactor kind of guy, I'm a fast reactor kind of guy - leads to the accumulation of the minor actinides neptunium (Np), americium (Am), and curium (Cm).

Of these three, two can be oxidized to the +6 oxidation state, (as can uranium (U) and plutonium (Pu)). They are Am and Np. This facilitates their separation from lanthanides (rare earths) that are fission products.

Am and Np are important tools in denaturing plutonium to make it unsuitable for use in nuclear weapons. I discussed this in some detail elsewhere: On Plutonium, Nuclear War, and Nuclear Peace

The stability of the +6 oxidation state is in the following order U > Np > Pu > Am. The oxidation to Am is challenging, but can be accomplished.

Generally using current technology, which is based around the dubious idea of constructing "nuclear waste" dumps, which in my view are completely unnecessary, these separations rely on very old chemistry, solvent extraction, notably in the commercial "Purex" process. Purex processing involves the generation of considerable quantities of chemical waste, in particular because of the instability of extraction agents to high radiation doses. Therefore better processes are advisable, and I've been following these advances for many years.

A very interesting one showed up last year in the literature. Here is a few excerpts from a paper published last year. The reference is Inorg. Chem., 2016, 55 (17), pp 8913–8919 "Group Hexavalent Actinide Separations: A New Approach to Used Nuclear Fuel Recycling"

Some excerpts:

For nuclear power to become a major component in the future of a sustainable energy strategy, several barriers have to be overcome to leverage its inherent carbon-free power generation, which has the possibility of curtailing global greenhouse gas emissions.(1-3) One major barrier is the complexity of implementing the separations involved in the recycle of used fuel to recover the actinides (Ans), maximize energy utilization of the fuel, minimize the waste going to geologic storage, and additionally serve the needs of nonproliferation.(1-3) This will require a technology to recover not only the U and Pu, which are most important in energy generation, but also the minor Ans (MAs, i.e., Np, Am, and Cm), major contributors to the heat load and long-term hazard of geologic storage.(4-8) Currently, the most advantageous technological practices employ solvent extraction as a means to separate U and Pu,(9) yet these technologies haven proven to be challenging to apply to the MAs in a similar manner. This weakness in dealing with the MAs has spawned a large international research effort.(10) Many new technologies are developing in the area of solvent extraction to meet deficiencies; however, the added cost of these advances to separate the MAs is a major limitation and has stifled implementation on a large scale.(11) An innovative solution would be to have a technology achieve a single-step separation for all the Ans, known as a group actinide extraction (GANEX) process.(12, 13)...

Some experimental details of the crystallization, which assumes nitric acid dissolution of the nuclear fuel (which is not necessarily the best approach):

Small batch crystallization experiments with volumes of 1–2 mL were performed with UO2(NO3)2·6H2O as the carrier species. The starting was 1–2 M, with other An species (Np, Pu, and Am) spiked in at concentrations of 0.12–3.0 mM, and an acidity of 5.7–6.7 N. The An concentrations selected were designed to balance achieving actual U:An ratios seen in used nuclear fuel while ensuring the safety of the experimenter and keeping the radiation exposure ALARA. In experiments that included multiple TRU species, an aliquot of a Pu(VI) solution was first combined with an aliquot of a U(VI) solution, followed by the addition of an aliquot of a Np(VI) solution, and finally addition of an aliquot of Am(III). In the case of Am(VI), the mixture of U(VI), Np(VI), and Pu(VI) was added to the Am(VI) solution, which contained an excess of NaBiO3, as mentioned above.

Conclusions from the paper:

The group An(VI) (U–Am) cocrystallization in nitric acid by a simple adjustment of temperature has been investigated as a new elegant approach for actinide separation in an economical nuclear fuel recycle. Removal of single hexavalent TRUs with UNH was demonstrated to occur in near proportion with a reduction of the system’s temperature, while the lower-valent ions, Am(III) and Pu(IV), were only slightly removed. A group cocrystallization was then achieved with all four An(VI) ions being removed in near proportion to one another. A separation of U(VI), Np(VI), and Pu(VI) from Am(III) was performed with a separation factor of 12–14. It was also seen that, within the crystalline phase, the stability of Am(VI) is significantly increased, showing almost no reduction observed over a period of 13 days, while more than half of the Am(VI) autoreduced to Am(III) in solution in only 10 days. This makes our concept for a single-technology cocrystallization approach much more appealing, as the difficult oxidation may need to be achieved only once to perform multiple recrystallizations and thereby significantly increase the separation factor of the An(VI) species. An effective separation of An(VI) dioxo cations from key fission products was observed, with decontamination factors ranging from 6.5 to 71 in a mildly oxidizing system without Am(VI)

It is interesting that Am (VI) can be separated from Pu (VI), Np (VI) and U (VI) simply be leaving the solution standing for a few weeks, during which time the Am (VI) is reduced to Am (III).

I personally think however that it may not be necessary, or even desirable in many cases, to effect this separation. The presence of Am and Np in nuclear fuels necessarily results in the formation of the heat generating plutonium isotope Pu-238, which is the key to making plutonium unsuitable for use in weapons. It is necessary to do this since as our recent election in this country shows, it is possible for weapons grade plutonium to fall into the hands of psychopathological fools.

Esoteric I know, but interesting.

Have a nice day tomorrow.

You Can Actually See It For A Short Time: Beckmann's "Hell of Birds."

In an age of encroaching fascism around the world, I have had cause to reflect on the life of the Painter Max Beckmann, who is not as widely known as he should be.

Happily the Metropolitan Museum of Art, ("The Met") in New York City is now featuring an exhibition of his work entitled "Beckmann in New York."

After becoming a successful artist in the 1920's in Weimar Germany, his works were banned and confiscated by the Nazis as "Degenerate Art."

Beckmann fled to Holland in 1938 after producing powerful works to protest fascism, and lived and worked in Amsterdam - which he viewed as a way station - and lived through the Nazi occupation of the Netherlands before finally being granted a visa to the United States. He refused to return to Germany and called his life in the United States which began in 1948 the "end" of his "exile."

He taught at Washington College in Saint Louis, and at the Brooklyn Academy of Art. He died of a heart attack at Central Park West and 69th Street in New York City in 1950 while walking on his way to see one of his works which was being exhibited at The Met.

It is in an unbelievable exhibition of his work there right now; I spent several hours yesterday, and frankly, I wept, because of what is happening to my country.

My son - an artist in his own right - had only a mild criticism of the show, this being that they used the words "National Socialism" to describe Nazism, and that the show did not focus heavily enough on Beckmann's politics. This said, when asked by an art dealer to explain the symbolism of his powerful triptych "Departure" Beckmann is said to have responded, "If you need me to tell you that, send it back. "Departure," which is owned by the Museum of Modern Art in New York and is regrettably not continuously on display is also available for viewing at the Met show.

Here is a link to the show: Max Beckmann in New York

The show runs through February 20, and if you're in New York, and want to see some powerful art, I strongly recommend this show.

The "Hell of Birds" - sometimes called "Hell's Birds" is in a private collection and is thus not available for public viewing very often. Thus, you may never have a chance to see it live again, and no Art book or photograph or web page can do it justice.

WHO has caught up with the scientific literature on air pollution deaths.

For many years, until I came across the paper reporting on the comprehensive study of the causes of human mortality funded by the Gates Foundation, this one (Lancet 2012, 380, 2224–60), I used the figure of 3.3 million deaths per year from air pollution, a figure that was conveniently available on a web page of the World Health Organization.

This was, of course, an impressive figure, but it is too low by a factor of 2. The actual figure as reported in the Lancet paper is 7 million people year. This means that every decade, air pollution kills more people than died in all of World War II from combat, aerial bombings, genocide, etc.

I use these figures to support my contention that opposition to nuclear power is at best stupid, at worst criminal, since in its entire history, commercial nuclear power operations have not lead to more deaths than will take place in the next 48 hours from air pollution.

Recently, in one of my periodic posts on the subject of how everything humanity has done to fight climate change - which consists mainly of investing huge sums of money in so called "renewable energy" - has failed miserably, an anti-nuke showed up in the most to complain that the new figure that I've been using, roughly seven million deaths per year was wrong, and, in the spectacular logic of anti-nukes, therefore everything I say about nuclear power was wrong. I dismissed this silliness by reference to the Lancet paper, although I doubt that there are any anti-nukes anywhere who are bright enough to get it.

This exchange is here: At 3.37 ppm over November of 2015, November 2016 is the worst November for new carbon dioxide...

Apparently the anti-nuke googled his way to the old WHO website - which is by the way unreferenced sort of like an Amory Lovins "paper" - to find the 3.3 million figure.

I was stumbling around the internet today, doing a little lazy Googling myself, to discover that WHO has updated their web page.

It appears that WHO has caught up with the scientific literature on the subject:

7 million premature deaths annually linked to air pollution

The opening text from the (still unreferenced) web page:

25 MARCH 2014 | GENEVA - In new estimates released today, WHO reports that in 2012 around 7 million people died - one in eight of total global deaths – as a result of air pollution exposure. This finding more than doubles previous estimates and confirms that air pollution is now the world’s largest single environmental health risk. Reducing air pollution could save millions of lives.

New estimates

In particular, the new data reveal a stronger link between both indoor and outdoor air pollution exposure and cardiovascular diseases, such as strokes and ischaemic heart disease, as well as between air pollution and cancer. This is in addition to air pollution’s role in the development of respiratory diseases, including acute respiratory infections and chronic obstructive pulmonary diseases.

The new estimates are not only based on more knowledge about the diseases caused by air pollution, but also upon better assessment of human exposure to air pollutants through the use of improved measurements and technology. This has enabled scientists to make a more detailed analysis of health risks from a wider demographic spread that now includes rural as well as urban areas.

The bold is mine.

I hope you're enjoying the holiday season.

At 3.37 ppm over November of 2015, November 2016 is the worst November for new carbon dioxide...

...accumulations observed since record keeping at the Mauna Loa Carbon Dioxide Observatory began recording its measurements.

This follows the 3.03 ppm increase recorded last November, which contributed to the fact that 2015 was the worst year ever observed, 2015 being the first year that the annual increase exceeded 3.00 ppm.

January 2016 (2.56 ppm) was the 4th worst January in recorded history.

February 2016 (3.75) was the worst February in recorded history.

March 2016 (3.31 ppm) was the worst March in recorded history.

April 2016 (4.16 ppm) was the worst April in recorded history - and, in fact, the worst month of any month in history.

May 2016 (3.76 ppm) was the worst May in recorded history - and, in fact, the third worst month of any month in history.

June 2016 (4.01 ppm) was the worst June in recorded history - and, in fact, the second worst month of any month in history.

July 2016 (3.09 ppm) was the third worst July in recorded history.

August 2016 (3.09 ppm) was the second worst August in recorded history.

September 2016 (3.39 ppm) was the second worst September in recorded history.

October 2016 (3.28 ppm) was the second worst October in recorded history.

And then, returning to the fold of "worst ever" months, we have November of 2016, as mentioned in the opening paragraph.

2015 was recorded as the worst year ever, coming in at 3.05 ppm over 2014. With the exception of January, every single month this year has exceeded, and in some cases dwarfed that doleful figure.

If any of this troubles you, don't worry, be happy. Dipshits, I mean, um, "experts" in Wisconsin, a Trump/Walker state with a once great state university system in research and intellectual free fall owing to decreased funding has experts who have announced that so called "renewable energy" will do just fine under Trump: Wisconsin Experts Confident About Renewable Energy's Future, Even Under Trump.

You read it right here at Democratic Underground.

We may be amused that voters in Wisconsin are so pleased with their ability to lie to themselves, but the fact is that we on the left are also lying to ourselves.

So called "renewable energy" has not worked. It is not working. It will not work, this because of the laws of physics, which no state legislature, no congress, no dictator can repeal.

If we on the left were anywhere as nearly concerned with the 7 million people who die each year from air pollution as we were and are with a few atoms of cesium-137 and cesium-134 found in a tuna fish, things might have been different.

Look, in the next 4 years, for more "don't worry, be happy." The new thought police will probably defund the Mauna Loa observatory, pushing the wax deeper into their ear canals with their fingers and screaming, "La...la...la, live for today and don't worry about tomorrow."

History will not forgive the generation now living for what it has done, should history survive.

Have a nice weekend.

Gridded National Inventory of U.S. Methane Emissions.

Methane emissions in the United States as a gridded map:

Source: Environ. Sci. Technol., 2016, 50 (23), pp 13123–13133

It dates from 2012.

I'm sure things are much better now, now that so called "renewable energy" has saved the day with a series of "world's largest," "breakthroughs" and "coulds."

Of course, now that the United States has "President-Electoral College Trump" on the way, we can improve on our vast capability to lie to ourselves. We were good it previously, but now we'll be even "great again."

And there is hope in the world: Rwanda: From killing fields to technopolis.

In these rotten times, it may be useful to learn how a great positive emerged from a humanitarian disaster on an unimaginable scale:

First-time visitors to Kigali, Rwanda's capital, usually remark that they cannot believe they are in a country that a little over 20 years was in the midst of a civil war. The 1994 genocide against the Tutsi resulted in the slaughter of up to one million people — around 15% of the population. But the landlocked country is developing rapidly. Where gravel roads once dominated, paved streets are now the rule. Internet connections are fast and stable. Buildings are constructed at breakneck speed, and airy, reliably scheduled public buses and shuttles have replaced cramped, unpredictable minivans.

For Jimmy Gasore, a Rwandan physics graduate who left the country in 2011 to pursue a PhD at the Massachusetts Institute of Technology in Cambridge, each trip home throws up new advances. For instance, the year he left, he had to spend ten hours on a bus to Uganda's capital, Kampala, to register for the standardized tests needed for his MIT application, but these exams can now be taken all over Rwanda — an indication of the central role that the government has given to science and education in the country's development strategy.

Rwanda has used investment in science, technology and innovation as a springboard to grow and diversify its economy. Between 1996 and 2015, its per capita gross domestic product (GDP) more than tripled to US$1,756 — outpacing some bigger and more resource-rich African countries with fast-growing economies, such as Kenya, whose per capita GDP merely doubled over the same period. As a result, Rwanda is often held up as a model of what can be achieved if clear ambitions are backed up with strong political leadership...

Rwanda's remarkable journey started after the genocide, when stitching the war-torn nation back together seemed like an insurmountable task. The country's economy, which was small and agriculture-based to begin with, was in tatters. Farm workers had fled their homes and abandoned their fields. Worse, the social fabric of the country had unravelled: schools, health centres, and water and transport infrastructure were in ruins, and survivors had to live alongside perpetrators.

Rwanda's new leaders realized that education, including science education, would be essential to the nation's rebirth...

...Rwandan President Paul Kagame, who will seek re-election for his third term in 2017, has driven the science push. After becoming president in 2000, one of his first moves was to appoint Romain Murenzi as science minister. The Rwandan mathematical physicist had been working on multidimensional continuous wavelet transforms — which can be used in image compression — at Clark Atlanta University in Georgia...

Nature 537, S4–S5 (01 September 2016)

It's something to keep in mind while we enter a period of rule by racist fools working to stir up hatred.

Without Buchanan, no Lincoln. Without Coolidge/Hoover, no FDR. And without Trump, sure to be even worse than those two...well what... (We don't know.)

Without Bagosora, no Kagame...

If Rwanda can be reborn, so can anyone, and we have much farther to fall, fall as we do, to be Rwanda.

Trump was "elected" by a white mob with pitchforks. From history let's look at Robespierre...

...also chosen by a white mob with pitchforks.

He was, um, beheaded in short order.

The First White Terror

Trump should start to think about saving his cowardly ass.

He fully intends to screw the idiot white mob with pitchforks who "elected" him - it wasn't a real "election" since he did not get the majority of votes, but relied on an accession owing to what proved to be a historical artifact, the electoral college.

This is obvious to educated people with brains, but the problem is that Trump got votes by appealing to the ignorant and fearful.

I absolutely could see his mob - and a violent set they are - turning on him in a big way, a way that could end up with him and his fellow idiots being dragged around by their comb overs.

I oppose violence at all junctures, but I'm just saying...

I don't want a second or third "White Terror" in this country, but we are all learning how fragile a democracy can be if not respected and nutured.

This mob will need to live without healthcare, without social security, without any safety net, and they're about to learn that one should be extremely careful about one wishes for, since one may get it.

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