IHEP OpenIR  > 院士
Adsorption and dissociation of H2O on the (001) surface of uranium mononitride: energetics and mechanism from first-principles investigation
Bo T(薄涛); Lan JH(蓝建慧); Chai ZF(柴之芳); Shi WQ(石伟群); Bo, T; Lan, JH; Zhang, YJ; Zhao, YL; He, CH; Chai, ZF; Shi, WQ
2016
Source PublicationPHYSICAL CHEMISTRY CHEMICAL PHYSICS
ISSN1463-9076
EISSN1463-9084
Volume18Issue:19Pages:13255-13266
SubtypeArticle
AbstractThe interfacial interaction of uranium mononitride (UN) with water from the environment unavoidably leads to corrosion of nuclear fuels, which affects a lot of processes in the nuclear fuel cycle. In this work, the microscopic adsorption behaviors of water on the UN(001) surface as well as water dissociation and accompanying H-2 formation mechanisms have been investigated on the basis of DFT+U calculations and ab initio atomistic thermodynamics. For adsorption of one H2O monomer, the predicted adsorption energies are -0.88, -2.07, and -2.07 eV for the most stable molecular, partially dissociative, and completely dissociative adsorption, respectively. According to our calculations, a water molecule dissociates into OH and H species via three pathways with small energy barriers of 0.78, 0.72, and 0.85 eV, respectively. With the aid of the neighboring H atom, H-2 formation through the reaction of H* + OH* can easily occur via two pathways with energy barriers of 0.61 and 0.36 eV, respectively. The molecular adsorption of water shows a slight coverage dependence on the surface while this dependence becomes obvious for partially dissociative adsorption as the water coverage increases from 1/4 to 1 ML. In addition, based on the "ab initio atomistic thermodynamic'' simulations, increasing H2O partial pressure will enhance the stability of the adsorbed system and water coverage, while increasing temperature will decrease the H2O coverage. We found that the UN(001) surface reacts easily with H2O at room temperature, leading to dissolution and corrosion of the UN fuel materials.
DOI10.1039/c6cp01175f
Indexed BySCI ; ADS
Language英语
WOS IDWOS:000376138000015
ADS Bibcode2016PCCP...1813255B
ADS URLhttps://ui.adsabs.harvard.edu/abs/2016PCCP...1813255B
ADS CITATIONShttps://ui.adsabs.harvard.edu/abs/2016PCCP...1813255B/citations
Citation statistics
Cited Times:5 [ADS]
Document Type期刊论文
Identifierhttp://ir.ihep.ac.cn/handle/311005/247850
Collection院士
多学科研究中心
Recommended Citation
GB/T 7714
Bo T,Lan JH,Chai ZF,et al. Adsorption and dissociation of H2O on the (001) surface of uranium mononitride: energetics and mechanism from first-principles investigation[J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS,2016,18(19):13255-13266.
APA 薄涛.,蓝建慧.,柴之芳.,石伟群.,Bo, T.,...&Shi, WQ.(2016).Adsorption and dissociation of H2O on the (001) surface of uranium mononitride: energetics and mechanism from first-principles investigation.PHYSICAL CHEMISTRY CHEMICAL PHYSICS,18(19),13255-13266.
MLA 薄涛,et al."Adsorption and dissociation of H2O on the (001) surface of uranium mononitride: energetics and mechanism from first-principles investigation".PHYSICAL CHEMISTRY CHEMICAL PHYSICS 18.19(2016):13255-13266.
Files in This Item:
File Name/Size DocType Version Access License
377.pdf(3837KB)期刊论文作者接受稿限制开放CC BY-NC-SAApplication Full Text
Related Services
Recommend this item
Bookmark
Usage statistics
Export to Endnote
Google Scholar
Similar articles in Google Scholar
[薄涛]'s Articles
[蓝建慧]'s Articles
[柴之芳]'s Articles
Baidu academic
Similar articles in Baidu academic
[薄涛]'s Articles
[蓝建慧]'s Articles
[柴之芳]'s Articles
Bing Scholar
Similar articles in Bing Scholar
[薄涛]'s Articles
[蓝建慧]'s Articles
[柴之芳]'s Articles
Terms of Use
No data!
Social Bookmark/Share
All comments (0)
No comment.
 

Items in the repository are protected by copyright, with all rights reserved, unless otherwise indicated.