title: Substitutional Disorder of SeO32-/IO3-in the Crystalline Solid Matrix: Insights into the Fate of Radionuclides79Se and129I in the Environment.
abstract: As the crucial soluble species of long-lived radionuclides129I and79Se, iodate and selenite anions commonly share similar geometry of the trigonal pyramid XO3(X = I, Se) but in different valence states. Although large amounts of investigations have been performed aiming at understanding the environmental behavior of these two anions individually, studies on cases when they coexist are extremely scarce. Structurally well-characterized natural/synthetic crystalline solids simultaneously incorporating these two anions as potential solubility-limiting products at the nuclear waste geological depository remain elusive. We report here a crystalline solid Th(IO3)2(SeO3) representing the first example of aliovalent substitution between IO3-and SeO32-sharing the same structural site, as demonstrated by single crystal X-ray diffraction, laser-ablation inductively coupled plasma mass spectrometry analysis, and spectroscopic techniques including infrared, Raman, and X-ray absorption spectroscopies. Sequentially, in the Eu(IO3)3solid matrix, we demonstrated that the IO3-site can be sufficiently substituted by SeO32-in the presence of Th4+via simultaneous incorporation of Th4+and SeO32-in a charge-balancing mechanism. The obtained results provide insights into the environmental behavior of fission products79Se and129I: they may cocrystallize in one solid matrix and may be efficiently immobilized by incorporation into each other's solid phase through solid solution.
authors.affiliation: School for Radiological and Interdisciplinary Sciences (RAD-X), Soochow University , 215123 Suzhou, P. R. China.|Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions , 215123 Suzhou, P. R. China.|Key Laboratory of Radiation Physics and Technology, Ministry of Education, Institute of Nuclear Science and Technology, Sichuan University , Chengdu 610064, P. R. China.
authors.forename: Yaxing
authors.initials: Y
authors.lastname: Wang
authors.affiliation: School for Radiological and Interdisciplinary Sciences (RAD-X), Soochow University , 215123 Suzhou, P. R. China.|Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions , 215123 Suzhou, P. R. China.
authors.forename: Yumin
authors.initials: Y
authors.lastname: Wang
authors.affiliation: Shanghai Institute of Applied Physics and Key Laboratory of Nuclear Radiation and Nuclear Energy Technology, Chinese Academy of Sciences , 201800 Shanghai, P. R. China.
authors.forename: Linjuan
authors.initials: L
authors.lastname: Zhang
authors.affiliation: School for Radiological and Interdisciplinary Sciences (RAD-X), Soochow University , 215123 Suzhou, P. R. China.|Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions , 215123 Suzhou, P. R. China.
authors.forename: Lanhua
authors.initials: L
authors.lastname: Chen
authors.affiliation: School for Radiological and Interdisciplinary Sciences (RAD-X), Soochow University , 215123 Suzhou, P. R. China.|Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions , 215123 Suzhou, P. R. China.
authors.forename: Zhiyong
authors.initials: Z
authors.lastname: Liu
authors.affiliation: School for Radiological and Interdisciplinary Sciences (RAD-X), Soochow University , 215123 Suzhou, P. R. China.|Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions , 215123 Suzhou, P. R. China.
authors.forename: Xuemiao
authors.initials: X
authors.lastname: Yin
authors.affiliation: School for Radiological and Interdisciplinary Sciences (RAD-X), Soochow University , 215123 Suzhou, P. R. China.|Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions , 215123 Suzhou, P. R. China.
authors.forename: Daopeng
authors.initials: D
authors.lastname: Sheng
authors.affiliation: School for Radiological and Interdisciplinary Sciences (RAD-X), Soochow University , 215123 Suzhou, P. R. China.|Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions , 215123 Suzhou, P. R. China.
authors.forename: Juan
authors.initials: J
authors.lastname: Diwu
authors.affiliation: Shanghai Institute of Applied Physics and Key Laboratory of Nuclear Radiation and Nuclear Energy Technology, Chinese Academy of Sciences , 201800 Shanghai, P. R. China.
authors.forename: Jianqiang
authors.initials: J
authors.lastname: Wang
authors.affiliation: Key Laboratory of Radiation Physics and Technology, Ministry of Education, Institute of Nuclear Science and Technology, Sichuan University , Chengdu 610064, P. R. China.
authors.forename: Ning
authors.initials: N
authors.lastname: Liu
authors.affiliation: School for Radiological and Interdisciplinary Sciences (RAD-X), Soochow University , 215123 Suzhou, P. R. China.|Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions , 215123 Suzhou, P. R. China.
authors.forename: Zhifang
authors.initials: Z
authors.lastname: Chai
authors.affiliation: School for Radiological and Interdisciplinary Sciences (RAD-X), Soochow University , 215123 Suzhou, P. R. China.|Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions , 215123 Suzhou, P. R. China.
authors.forename: Shuao
authors.identifier: http://orcid.org/0000-0002-1526-1102
authors.initials: S
authors.lastname: Wang