Degradation mechanism of UN and UN- U3Si2 …...Degradation mechanism of UN and UN-U 3 Si 2 pellets...

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Degradation mechanism of UN and UN- U 3 Si 2 pellets of varying microstructure by comparative steam oxidation experiments Selim Uygur Ongoing MSc. Thesis Kyle Johnson, Denise Adorno Lopes, PhD, KTH Reactor Physics Nuclear Fuel Laboratory

Transcript of Degradation mechanism of UN and UN- U3Si2 …...Degradation mechanism of UN and UN-U 3 Si 2 pellets...

Page 1: Degradation mechanism of UN and UN- U3Si2 …...Degradation mechanism of UN and UN-U 3 Si 2 pellets of varying microstructure by comparative steam oxidation experiments Selim Uygur

Degradation mechanism of UN and UN-U3Si2 pellets of varying microstructure by

comparative steam oxidation experiments

Selim Uygur – Ongoing MSc. ThesisKyle Johnson, Denise Adorno Lopes, PhD,

KTH Reactor Physics –Nuclear Fuel Laboratory

Page 2: Degradation mechanism of UN and UN- U3Si2 …...Degradation mechanism of UN and UN-U 3 Si 2 pellets of varying microstructure by comparative steam oxidation experiments Selim Uygur

UN: An Accident Tolerant Fuel candidate

High thermal conductivity:

Less thermal inertia after reactor shut down

Much lower peak centerline temperature

Higher U-density enable different cladding options

Performance in contact with water/steam

Little literature on high quality (SP-Sintered) pellets

Ongoing R&D on behavior in high pressure steam

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Steam exposure experiments at KTH

1. High pressure batch autoclave @300 °C ,9MPa

Air+Steam

2. Digerator @ 400°C ,1atm

Ar+Steam

N2+Steam

Basic chemistry of UN-Hydrolysis:

𝑈𝑁 + 2𝐻2𝑂∆ 𝑈𝑂2 + 𝑁𝐻3 + ½𝐻2

2𝑈𝑁 + 2𝐻2𝑂∆ 𝑈𝑂2 𝑁 + 𝑈𝑁𝑥 + 𝐻2 with 1.68 < 𝑥 < 1.74 ≡ 𝑈2𝑁3

𝑈2𝑁3 + 4𝐻2𝑂∆ 2𝑈𝑂2 + 8/3𝑁𝐻3 + 1/6𝐻2

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Influence of NH3 and N2-partial pressure

Higher NH3 / N2 causes higher inter-granular

U2N3 deposition

EDS /SEM: Precipitation of U2N3, UO2 phases in a

“sandwich” structure at GB

Where does the Nitrogen go to?

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Influence of density and grain size

Higher density higher hydrolysis tolerance

Smaller grains higher hydrolysis tolerance

TD: 94-96%, grain size:a)23,8µm (x50) b)6,7µm (x500)

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Very high TD(99.88%), large grain sample

As fabricated: a) x500 After 90min 300°C: b) x100, c) x200, d)x1000

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Influence of grain size – Findings

UN-hydrolysis rate is controlled by specific

surface available to exposure

Large grain samples crack more easily

Cracking increases the specific inter-granular

surface exposed to hydrolysis

Inter-granular cracking is the main driver of

UN-pellet collapse

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Hydrolysis of a UN-10U3Si2 sample

UN-10U3Si2 |TD:98.01, GS:10.8µm As fabricated a)x500, After 30min 300°C: b)x1000, c)x1000

The degradation in the UN-

10U3Si2 sample is almost

exclusively intra-granular

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Behavior UN-10U3Si2 vs. pure UN pellets

The degradation mechanism in the UN-U3Si2sample is almost exclusively intra-granular

Current results show also lower degradation

than most UN samples

The role of the U3Si2 phase has yet to be

investigated.