CAS OpenIR
Cr(III) Adsorption by Cluster Formation on Boehmite Nanoplates in Highly Alkaline Solution
Cui, Wenwen1,2,3; Zhang, Xin1; Pearce, Carolyn I.4; Chen, Ying1; Zhang, Shuai1,5; Liu, Wen6; Engelhard, Mark H.6; Kovarik, Libor6; Zong, Meirong1,7; Zhang, Hailin1,2,3; Walter, Eric D.6; Zhu, Zihua6; Heald, Steve M.8; Prange, Micah P.1; De Yoreo, James J.1,5; Zheng, Shili2; Zhang, Yi2; Clark, Sue B.1,9; Li, Ping2; Wang, Zheming1; Rosso, Kevin M.1
2019-09-17
Source PublicationENVIRONMENTAL SCIENCE & TECHNOLOGY
ISSN0013-936X
Volume53Issue:18Pages:11043-11055
AbstractThe development of advanced functional nanomaterials for selective adsorption in complex chemical environments requires partner studies of binding mechanisms. Motivated by observations of selective Cr(III) adsorption on boehmite nanoplates (gamma-AIOOH) in highly caustic multi-component solutions of nuclear tank waste, here we unravel the adsorption mechanism in molecular detail. We examined Cr(III) adsorption to synthetic boehmite nanoplates in sodium hydroxide solutions up to 3 M, using a combination of X-ray diffraction (XRD), Raman, X-ray photoelectron spectroscopy (XPS), scanning/transmission electron microscopy (S/TEM), electron energy loss spectroscopy (EELS), high-resolution atomic force microscopy (HR-AFM), time-of-fight secondary ion mass spectrometry (ToF-SIMS), Cr K-edge X-ray absorption near edge structure (XANES)/extended X-ray absorption fine structure (EXAFS), and electron paramagnetic resonance (EPR). Adsorption isotherms and kinetics were successfully fit to Langmuir and pseudo-second-order kinetic models, respectively, consistent with monotonic uptake of Cr(OH)(4)(-) monomers until saturation coverage of approximately half the aluminum surface site density. High resolution AFM revealed monolayer cluster self-assembly on the (010) basal surfaces with increasing Cr(III) loading, possessing a structural motif similar to guyanaite (beta-CrOOH), stabilized by corner-sharing Cr-O-Cr bonds and attached to the surface with edge-sharing Cr-O-Al bonds. The selective uptake appears related to short-range surface templating effects, with bridging metal connections likely enabled by hydroxyl anion ligand exchange reactions at the surface. Such a cluster formation mechanism, which stops short of more laterally extensive heteroepitaxy, could be a metal uptake discrimination mechanism more prevalent than currently recognized.
DOI10.1021/acs.est.9b02693
Language英语
WOS KeywordHEAVY-METAL IONS ; HEXAVALENT CHROMIUM REMOVAL ; GAMMA-ALOOH ; CARBON NANOCOMPOSITES ; MASS-SPECTROMETRY ; AQUEOUS-SOLUTIONS ; THIN-FILMS ; WATER ; NANOPARTICLES ; CELLULOSE
Funding ProjectIDREAM (Interfacial Dynamics in Radioactive Environments and Materials), an Energy Frontier Research Center - U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES) ; U.S. DOE[DE-AC02-06CH11357] ; DOE Office of Biological and Environmental Research ; DOE[DE-AC05-76RL0-1830] ; China Scholarship Council
WOS Research AreaEngineering ; Environmental Sciences & Ecology
WOS SubjectEngineering, Environmental ; Environmental Sciences
Funding OrganizationIDREAM (Interfacial Dynamics in Radioactive Environments and Materials), an Energy Frontier Research Center - U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES) ; U.S. DOE ; DOE Office of Biological and Environmental Research ; DOE ; China Scholarship Council
WOS IDWOS:000487163000054
PublisherAMER CHEMICAL SOC
Citation statistics
Cited Times:7[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.ipe.ac.cn/handle/122111/31076
Collection中国科学院过程工程研究所
Corresponding AuthorZhang, Xin; Li, Ping; Wang, Zheming; Rosso, Kevin M.
Affiliation1.Pacific Northwest Natl Lab, Phys & Computat Sci Directorate, Richland, WA 99354 USA
2.Chinese Acad Sci, Inst Proc Engn, Key Lab Green Proc & Engn, Natl Engn Lab Hydromet Cleaner Prod Technol, Beijing 100190, Peoples R China
3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
4.Pacific Northwest Natl Lab, Energy & Environm Directorate, Richland, WA 99354 USA
5.Univ Washington, Dept Mat Sci & Engn, Seattle, WA 98195 USA
6.Pacific Northwest Natl Lab, Environm Mol Sci Lab, Richland, WA 99354 USA
7.Nanjing Univ, Sch Earth Sci & Engn, Nanjing 210023, Jiangsu, Peoples R China
8.Argonne Natl Lab, Adv Photon Source, Lemont, IL 60439 USA
9.Washington State Univ, Dept Chem, Pullman, WA 99164 USA
Recommended Citation
GB/T 7714
Cui, Wenwen,Zhang, Xin,Pearce, Carolyn I.,et al. Cr(III) Adsorption by Cluster Formation on Boehmite Nanoplates in Highly Alkaline Solution[J]. ENVIRONMENTAL SCIENCE & TECHNOLOGY,2019,53(18):11043-11055.
APA Cui, Wenwen.,Zhang, Xin.,Pearce, Carolyn I..,Chen, Ying.,Zhang, Shuai.,...&Rosso, Kevin M..(2019).Cr(III) Adsorption by Cluster Formation on Boehmite Nanoplates in Highly Alkaline Solution.ENVIRONMENTAL SCIENCE & TECHNOLOGY,53(18),11043-11055.
MLA Cui, Wenwen,et al."Cr(III) Adsorption by Cluster Formation on Boehmite Nanoplates in Highly Alkaline Solution".ENVIRONMENTAL SCIENCE & TECHNOLOGY 53.18(2019):11043-11055.
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