IGGCAS OpenIR  > 地球与行星物理院重点实验室
Density functional theory calculations of nitrogen and oxygen equilibrium isotope fractionations in NO3--NO2--H2O aqueous system reveal inverse kinetic isotope effects during nitrite oxidation
He, Yuyang1,2; Li, Long3
2022-04-01
Source PublicationAPPLIED GEOCHEMISTRY
ISSN0883-2927
Volume139Pages:11
AbstractNitrate and nitrite play key roles in the nitrogen cycle on Earth's surface. The isotope fractionation during nitrate reduction on enzymatic level involves multiple steps, including transfer of free NO3- to the activate site on nitrate reductase and NO2 equilibration with ambient water. However, the isotope fractionation factors of 15N and O-18 among NO3-, NO2-, and H2O molecules in aqueous phases are poorly constrained. It strongly impedes the understanding of the involved processes and using stable isotopes to quantitatively examine the biogeochemical nitrogen cycle. In this contribution, we employ the density functional theory method with the UreyBigeleisen-Goeppert-Mayer model to predict the nitrogen and oxygen equilibrium isotope fractionation factors of NO3-, NO2-, and H2O molecules in gaseous and aqueous phases. Our calculation results show that the solvent effect has a large influence on equilibrium isotope fractionation for oxygen in water (+10.1 parts per thousand between liquid and vapor water at 25 degrees C), which is different to the little solvent effects on both oxygen and nitrogen in nitrate and nitrite. The calculated temperature-dependent equilibrium isotope fractionations between nitrogen of NO3- and NO2, and oxygen of H2O and NO2 are consistent with previous laboratory experiments. Our results confirm that the oxygen equilibrium isotope fractionations between NO3 and NO2 should be +9.4 parts per thousand at 25 degrees C. Integrating the new results and previously reported kinetic isotope effects of nitrate reduction, we demonstrate inverse kinetic isotope effects for both nitrogen (+15.4 parts per thousand) and oxygen (+5.2 parts per thousand) during nitrite oxidation, which falls in the range of previous experiments. The new results enable us to use both nitrogen and oxygen isotopes as a bonded isotope tool to quantitatively assess the nitrogen cycle in low-temperature environments.
KeywordReduced partition function ratio Nitrate reduction Water-droplet model Solvent effect Inverse kinetic isotope effect
DOI10.1016/j.apgeochem.2022.105265
Funding OrganizationNational Science Foundation of China ; National Science Foundation of China ; National Science Foundation of China ; National Science Foundation of China ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; pre-research project on Civil Aerospace Technologies of China National Space Administration ; pre-research project on Civil Aerospace Technologies of China National Space Administration ; pre-research project on Civil Aerospace Technologies of China National Space Administration ; pre-research project on Civil Aerospace Technologies of China National Space Administration ; National Science Foundation of China ; National Science Foundation of China ; National Science Foundation of China ; National Science Foundation of China ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; pre-research project on Civil Aerospace Technologies of China National Space Administration ; pre-research project on Civil Aerospace Technologies of China National Space Administration ; pre-research project on Civil Aerospace Technologies of China National Space Administration ; pre-research project on Civil Aerospace Technologies of China National Space Administration ; National Science Foundation of China ; National Science Foundation of China ; National Science Foundation of China ; National Science Foundation of China ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; pre-research project on Civil Aerospace Technologies of China National Space Administration ; pre-research project on Civil Aerospace Technologies of China National Space Administration ; pre-research project on Civil Aerospace Technologies of China National Space Administration ; pre-research project on Civil Aerospace Technologies of China National Space Administration ; National Science Foundation of China ; National Science Foundation of China ; National Science Foundation of China ; National Science Foundation of China ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; pre-research project on Civil Aerospace Technologies of China National Space Administration ; pre-research project on Civil Aerospace Technologies of China National Space Administration ; pre-research project on Civil Aerospace Technologies of China National Space Administration ; pre-research project on Civil Aerospace Technologies of China National Space Administration
WOS KeywordTHEORETICAL CALCULATION ; NITRATE REDUCTION ; WATER MOLECULE ; CARBON-DIOXIDE ; LIQUID WATER ; AB-INITIO ; EXCHANGE ; DIFFRACTION ; MECHANISMS ; RATIOS
Language英语
Funding ProjectNational Science Foundation of China[4217030170] ; National Science Foundation of China[42150202] ; China Postdoctoral Science Foundation[2019M660811] ; pre-research project on Civil Aerospace Technologies of China National Space Administration[D020203]
Funding OrganizationNational Science Foundation of China ; National Science Foundation of China ; National Science Foundation of China ; National Science Foundation of China ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; pre-research project on Civil Aerospace Technologies of China National Space Administration ; pre-research project on Civil Aerospace Technologies of China National Space Administration ; pre-research project on Civil Aerospace Technologies of China National Space Administration ; pre-research project on Civil Aerospace Technologies of China National Space Administration ; National Science Foundation of China ; National Science Foundation of China ; National Science Foundation of China ; National Science Foundation of China ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; pre-research project on Civil Aerospace Technologies of China National Space Administration ; pre-research project on Civil Aerospace Technologies of China National Space Administration ; pre-research project on Civil Aerospace Technologies of China National Space Administration ; pre-research project on Civil Aerospace Technologies of China National Space Administration ; National Science Foundation of China ; National Science Foundation of China ; National Science Foundation of China ; National Science Foundation of China ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; pre-research project on Civil Aerospace Technologies of China National Space Administration ; pre-research project on Civil Aerospace Technologies of China National Space Administration ; pre-research project on Civil Aerospace Technologies of China National Space Administration ; pre-research project on Civil Aerospace Technologies of China National Space Administration ; National Science Foundation of China ; National Science Foundation of China ; National Science Foundation of China ; National Science Foundation of China ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; China Postdoctoral Science Foundation ; pre-research project on Civil Aerospace Technologies of China National Space Administration ; pre-research project on Civil Aerospace Technologies of China National Space Administration ; pre-research project on Civil Aerospace Technologies of China National Space Administration ; pre-research project on Civil Aerospace Technologies of China National Space Administration
WOS Research AreaGeochemistry & Geophysics
WOS SubjectGeochemistry & Geophysics
WOS IDWOS:000799844300006
PublisherPERGAMON-ELSEVIER SCIENCE LTD
Citation statistics
Document Type期刊论文
Identifierhttp://ir.iggcas.ac.cn/handle/132A11/106042
Collection地球与行星物理院重点实验室
Corresponding AuthorHe, Yuyang
Affiliation1.Chinese Acad Sci, Inst Geol & Geophys, Key Lab Earth & Planetary Phys, Beijing, Peoples R China
2.Chinese Acad Sci, Inst Mech, State Key Lab High Temp Gas Dynam, Beijing, Peoples R China
3.Univ Alberta, Dept Earth & Atmospher Sci, Edmonton, AB T6G 2E3, Canada
First Author AffilicationKey Laboratory of Earth and Planetary Physics, Chinese Academy of Sciences
Corresponding Author AffilicationKey Laboratory of Earth and Planetary Physics, Chinese Academy of Sciences
Recommended Citation
GB/T 7714
He, Yuyang,Li, Long. Density functional theory calculations of nitrogen and oxygen equilibrium isotope fractionations in NO3--NO2--H2O aqueous system reveal inverse kinetic isotope effects during nitrite oxidation[J]. APPLIED GEOCHEMISTRY,2022,139:11.
APA He, Yuyang,&Li, Long.(2022).Density functional theory calculations of nitrogen and oxygen equilibrium isotope fractionations in NO3--NO2--H2O aqueous system reveal inverse kinetic isotope effects during nitrite oxidation.APPLIED GEOCHEMISTRY,139,11.
MLA He, Yuyang,et al."Density functional theory calculations of nitrogen and oxygen equilibrium isotope fractionations in NO3--NO2--H2O aqueous system reveal inverse kinetic isotope effects during nitrite oxidation".APPLIED GEOCHEMISTRY 139(2022):11.
Files in This Item:
There are no files associated with this item.
Related Services
Recommend this item
Bookmark
Usage statistics
Export to Endnote
Google Scholar
Similar articles in Google Scholar
[He, Yuyang]'s Articles
[Li, Long]'s Articles
Baidu academic
Similar articles in Baidu academic
[He, Yuyang]'s Articles
[Li, Long]'s Articles
Bing Scholar
Similar articles in Bing Scholar
[He, Yuyang]'s Articles
[Li, Long]'s Articles
Terms of Use
No data!
Social Bookmark/Share
Add to CiteULike Add to Connotea Add to Del.icio.us Add to Digg Add to Reddit Add to Technorati
All comments (0)
No comment.
 

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