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Adsorption of Chlorine on Zr(0001) Surface: First-Principles Predictions

Journal Article · · Transactions of the American Nuclear Society
OSTI ID:23047348
; ;  [1];  [2]
  1. Department of Physics, University of Nevada Las Vegas, Las Vegas, NV 89154 (United States)
  2. Sandia National Laboratories, Albuquerque, NM 87185 (United States)

The adsorption of atomic and gaseous chlorine on Zr (0001) surface has been investigated using state-of-the-art density functional theory calculations as part of an effort to gain fundamental understanding of chlorination processes occurring in fuel cladding materials. Zirconium alloys, including Zircaloy-4, Zircaloy-2 and Zr-Nb alloys (Zirlo{sup TM} and Zr-2.5Nb) are the most common fuel cladding materials in nuclear light water reactors (LWRs) due to their favorable mechanical properties, corrosion resistance, low thermal-neutron capture cross section and criticality. The United States produces a large amount of cladding material from used nuclear fuel, which could approach 1,000 MT/year in the next 50 years. In nuclear fuel recycling, spent nuclear fuel assemblies are disassembled and the cladding hulls are separated from the U oxide spent fuel. Zr can be recovered from Zr cladding using the chlorination method. However the presence of impurities in the recovered ZrCl{sub 4} was reported, including Sn, Cr and Fe. Thus, further efforts are necessary to improve the purification process significantly. This requires fundamental understanding of chlorination processes in cladding materials. Most of the material properties are expected to be similar between the pure zirconium and its alloys due to the fact that the alloy composition consists of more than 95 weight-percent zirconium and less than 2% of tin, niobium, iron, chromium, nickel and other metals. Therefore, while the overarching goal is to understand the chlorination process occurring in complex fuel cladding materials, chlorination of pure zirconium was used as an initial system for the modeling and simulation efforts in this study.

OSTI ID:
23047348
Journal Information:
Transactions of the American Nuclear Society, Journal Name: Transactions of the American Nuclear Society Vol. 116; ISSN 0003-018X
Country of Publication:
United States
Language:
English