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Author:Loukusa, Henri
Title:Computational module for the calculation of thermochemical equilibria in nuclear fuel
Laskennallinen moduuli termokemiallisten tasapainojen laskentaan ydinpolttoaineessa
Publication type:Master's thesis
Publication year:2014
Pages:xii + 123 s. + liitt. 11      Language:   eng
Department/School:Kemian tekniikan korkeakoulu
Main subject:Fysikaalinen kemia   (Kem-31)
Supervisor:Laasonen, Kari
Instructor:Ikonen, Timo
Electronic version URL: http://urn.fi/URN:NBN:fi:aalto-201410212835
OEVS:
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Location:P1 Ark Aalto  1842   | Archive
Keywords:nuclear fuel
thermochemistry
Gibbs energy minimization
nuclear safety
ydinpolttoaine
termodynamiikka
Gibbsin energian minimointi
ydinturvallisuus
Abstract (eng):A computational module was developed in this work for the calculation of thermochemical equilibria bearing in mind the application of the module to chemical phenomena in nuclear fuel.
Gibbs energy minimization principles set forth by Gunnar Eriksson in the SOLGASMIX program were applied for the calculation of thermochemical equilibria along with some improvements published in the literature.
The underlying theory behind Gibbs energy minimization is presented, and the program applying this theory developed in this work is described in detail.

To increase understanding of the chemical phenomena to be modelled with the program, chemistry of nuclear fuel in operation was reviewed.
In the review, the chemistry of the actinides uranium and plutonium along with the fission products formed in irradiated nuclear fuel were explored.

Published thermochemical treatments of irradiated nuclear fuel and the applications of thermochemical modelling to nuclear fuel were reviewed to gain knowledge of state of research in this matter.
Thermodynamic data for this system in the form of the Royal Military College of Canada Fuel Thermochemical Treatment was found to be publicly available, and this data was applied in this work.

The program developed in this work was tested and in many cases was found to calculate results comparable to other, established programs.
Even difficult cases possible in the application of irradiated nuclear fuel were evaluated with the new program.
Finally, a simulation of oxygen potential in a nuclear fuel rod under irradiation was performed with the new program with fission product amounts generated by the point depletion code ORIGEN and temperatures and pressures in the fuel rod calculated with the fuel performance code FRAPCON.
Abstract (fin):Työssä kehitettiin laskennallinen moduuli termokemiallisten tasapainojen laskentaan käytettäväksi ydinpolttoainesovelluksissa.
Termokemiallisten tasapainojen laskennassa käytetyssä Gibbsin energian minimoinnissa sovellettiin Gunnar Erikssonin kehittämän SOLGASMIX-ohjelman sisältämiä periaatteita, ja lisäksi sovellettiin joitakin kirjallisuudessa esitettyjä parannuksia.
Gibbsin energian minimoinnin teoreettinen pohja ja tätä teoriaa soveltava ohjelma esitellään työssä seikkaperäisesti.

Ydinpolttoaineessa tapahtuvien kemiallisten ilmiöiden mallintamiseksi työssä tehtiin kirjallisuuskatsaus ydinpolttoaineen kemiaan.
Katsauksessa syvennyttiin erityisesti uraanin, plutoniumin ja säteilytyksen aikana syntyvien fissiotuotteiden kemiaan.
Lisäksi tarkasteltiin kirjallisuudesta löytyviä ydinpolttoaineen termokemiallisia malleja ja tietokantoja.
Royal Military College of Canada Fuel Thermochemical Treatment on vapaasti saatavilla oleva termokemiallinen tietokanta ydinpolttoainesovelluksiin, ja tätä tietokantaa sovellettiin tässä työssä.

Työssä kehitettyä ohjelmaa testattiin ja sen todettiin laskevan ideaalisissa tapauksissa vertailukelpoisia tuloksia vakiintuneisiin ohjelmiin verrattuna.
Myös haasteellisia ydinpolttoainesovelluksissa usein kohdattavia tapauksia oli mahdollista laskea tässä työssä kehitettyä ohjelmaa käyttäen.
Lopuksi ohjelmalla simuloitiin säteilytyksessä olevan ydinpolttoainesauvan happipotentiaali käyttäen ORIGEN-ohjelmalla laskettuja fissiotuotteiden määriä ja FRAPCON-polttoainekoodilla laskettuja lämpötiloja ja paineita sauvan sisällä.
ED:2014-10-26
INSSI record number: 49917
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