Abstract
We utilize first principles density functional theory (DFT) calculations and ab-initio molecular dynamic (AIMD) simulations to identify underlying mechanisms elucidating the initial stage of electrocrystallization process of U on Mo(110) surface in a eutectic LiCl–KCl molten salt at T = 773 K. Our results clearly unveil surprisingly different principles on the nucleation of U in the media from that under vacuum conditions. U nanoclusters exposed to vacuum completely collapse into flat atomic layers on Mo(110) surface similar to an electrodeposition process. On the other hand, Cl ions in eutectic molten salt thermodynamically drive crystallite formation consisting of UCln(n = 3–6) through agglomeration of U atoms. Those crystallite gradually grows into bigger nuclei by adsorbing on Mo(110) surface. We propose that those behaviors are understandable only with revised conventional theories and that atomic level interactions among U, LiCl–KCl molten salt and Mo(110) surface play a key role to describe the atomic-scale dendrite formation of U in the electrorefining process. Our study can be one of the basic steps to design efficient electrorefining systems by identifying the fundamental cause of the experimentally observed uranium nucleation phenomena.
| Original language | English |
|---|---|
| Pages (from-to) | 1381-1388 |
| Number of pages | 8 |
| Journal | International Journal of Energy Research |
| Volume | 40 |
| Issue number | 10 |
| DOIs | |
| Publication status | Published - 2016 Aug 1 |
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All Science Journal Classification (ASJC) codes
- Renewable Energy, Sustainability and the Environment
- Nuclear Energy and Engineering
- Fuel Technology
- Energy Engineering and Power Technology
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First-principles based computational study on nucleation and growth mechanisms of U on Mo(110) surface solvated in an eutectic LiCl–KCl molten salt. / Kwon, Choah; Kang, Joonhee; Han, Byungchan.
In: International Journal of Energy Research, Vol. 40, No. 10, 01.08.2016, p. 1381-1388.Research output: Contribution to journal › Article
TY - JOUR
T1 - First-principles based computational study on nucleation and growth mechanisms of U on Mo(110) surface solvated in an eutectic LiCl–KCl molten salt
AU - Kwon, Choah
AU - Kang, Joonhee
AU - Han, Byungchan
PY - 2016/8/1
Y1 - 2016/8/1
N2 - We utilize first principles density functional theory (DFT) calculations and ab-initio molecular dynamic (AIMD) simulations to identify underlying mechanisms elucidating the initial stage of electrocrystallization process of U on Mo(110) surface in a eutectic LiCl–KCl molten salt at T = 773 K. Our results clearly unveil surprisingly different principles on the nucleation of U in the media from that under vacuum conditions. U nanoclusters exposed to vacuum completely collapse into flat atomic layers on Mo(110) surface similar to an electrodeposition process. On the other hand, Cl ions in eutectic molten salt thermodynamically drive crystallite formation consisting of UCln(n = 3–6) through agglomeration of U atoms. Those crystallite gradually grows into bigger nuclei by adsorbing on Mo(110) surface. We propose that those behaviors are understandable only with revised conventional theories and that atomic level interactions among U, LiCl–KCl molten salt and Mo(110) surface play a key role to describe the atomic-scale dendrite formation of U in the electrorefining process. Our study can be one of the basic steps to design efficient electrorefining systems by identifying the fundamental cause of the experimentally observed uranium nucleation phenomena.
AB - We utilize first principles density functional theory (DFT) calculations and ab-initio molecular dynamic (AIMD) simulations to identify underlying mechanisms elucidating the initial stage of electrocrystallization process of U on Mo(110) surface in a eutectic LiCl–KCl molten salt at T = 773 K. Our results clearly unveil surprisingly different principles on the nucleation of U in the media from that under vacuum conditions. U nanoclusters exposed to vacuum completely collapse into flat atomic layers on Mo(110) surface similar to an electrodeposition process. On the other hand, Cl ions in eutectic molten salt thermodynamically drive crystallite formation consisting of UCln(n = 3–6) through agglomeration of U atoms. Those crystallite gradually grows into bigger nuclei by adsorbing on Mo(110) surface. We propose that those behaviors are understandable only with revised conventional theories and that atomic level interactions among U, LiCl–KCl molten salt and Mo(110) surface play a key role to describe the atomic-scale dendrite formation of U in the electrorefining process. Our study can be one of the basic steps to design efficient electrorefining systems by identifying the fundamental cause of the experimentally observed uranium nucleation phenomena.
UR - http://www.scopus.com/inward/record.url?scp=84962468725&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=84962468725&partnerID=8YFLogxK
U2 - 10.1002/er.3527
DO - 10.1002/er.3527
M3 - Article
AN - SCOPUS:84962468725
VL - 40
SP - 1381
EP - 1388
JO - International Journal of Energy Research
JF - International Journal of Energy Research
SN - 0363-907X
IS - 10
ER -