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Did Failure to Understand Fuel Rod Chemical Properties Lead to the

Release of Most of the Radiation at Fukushima? ( Version Written 212-15 by Mark Kelly. )
The NHK World January 29,2015 report "New Findings on Fallout" contains
remarkable information about how attempts by Fukushima accident
responders to cool nuclear fuel rods unexpectedly increased temperatures,
leading to the release of three times the amounts of radiation that were
released by the explosions of the containment buildings.
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/nhkworld/english/news/nuclearwatch/20150130.html- Note link is disrupted
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Investigation into why radiation releases peaked in the weeks after the
accident rather than days after containment building explosions led to studies
of water- nuclear fuel rod cladding reactions at elevated temperatures. Their
findings indicate that heat generated by the zirconium alloy cladding raised
fuel pellet temperatures causing more of the volatile and soluble
radioisotopes to be "baked" out of the fuel pellets.

Figure. Left: Nuclear Fuel Rod Cut-away view showing fuel pellets in
zirconium cladding. Center: Diagram showing how radioisotopes can escape
breached cladding. Right: Photo of section of breached fuel rod cladding
with fuel pellets. Source: Nuclear Regulatory Commission.
Although chemists have known that high temperature water-- metal reactions
produce a lot of heat, the nuclear engineers and operators responsible for
designing the plant and planning accident responses appear to have been
taken by surprise by some of the consequences of the zirconium reactions
with coolant water under accident conditions.

Zirconium reactions with water and steam at high temperatures produce


hydrogen gas, zirconium oxides, zirconium hydrides, and heat. The
consequences of the formation of these reaction products are generally bad.
Hydrogen gas can explode and destroy buildings and equipment, as
happened at Fukushima. Zirconium oxides can form as hard brittle coatings
on fuel rod cladding, which can cause cladding intended to contain
radioisotopes to leak and break. Formation of zirconium hydrides can make
cladding brittle, cause components to "warp" or change shape, and can store
energy which, when released, can increase the temperatures and severity of
zirconium fires and reactions with emergency coolant water.
The nuclear industry and regulatory agencies have known of the hazards of
hydrogen explosions, cladding embrittlement, cladding failures, and
zirconium fires for years. They have designed materials and systems to
prevent, minimize, or mitigate these failures, many of which failed
spectacularly at Fukushima.
The NHK report exposes an aspect of cladding reactions that designers,
operators, and accident responders apparently failed to anticipate:
temperature increases triggered by accident responders, apparently leading
to the highest nuclear accident radiation releases in history.
Responders were ordered to take actions that made the accident worse,
which leads to some questions. Why were the releases unexpected? Why
didn't those directing accident responders know to that their attempts to cool
cladding would lead to temperature increases that would "bake off" more
radioisotopes?
Why was the public put at risk? If TEPCO and regulators
had known that they could occur, could evacuations and other measures
intended to protect the public been more effective? What should be done if
(when) the same situation recurs during a future nuclear accident?
Failures to anticipate the consequences of zirconium-water reactions leads
more fundamental and systemic technical questions. For over a decade, the
US NRC has steadfastly resisted correction of known inaccurate technical
information and records concerning properties of zirconium cladding that
influence chemical reactivity, citing industry sources whose focus was on
mechanical properties.
Could responders have been trained to take actions that to control cladding
temperatures so as to better control radiation releases? Boron solutions are
stored at nuclear plants for emergency quenching of nuclear reactions. Are
there chemicals that could have been added to the coolant that would
quench or allow control of the water-cladding reaction time-temperature
behavior? Some alloys react more vigorously than others. Were
opportunities to make cladding that is less reactive under accident conditions

missed by designers?
Zirconium alloys are regarded as the best practical cladding materials for
current nuclear technology. Zirconium alloys are aso used in other safetycritical core components, such as control rod systems. Nuclear operators
apparently failed to design safety systems that could withstand the products
of zirconium chemical reactions. Explosions and unexpected radiation
releases caused by chemical reactions of zirconium at Fukushima
demonstrate that the best was not good enough under real-world accident
conditions. What should be done with a technology when the "best" is not
good enough?

Background: Mark Kelly Ph. D. in Chemistry. Experience includes: Fuel rod


cladding analysis by x-ray diffraction. Materials analysis. Electrochemistry.
Water chemistry. Quality Assurance.

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