Cr(III) Adsorption by Cluster Formation on Boehmite Nanoplates in Highly Alkaline Solution
文献类型：期刊论文
| 作者 | Cui, Wenwen5,6,7; Zhang, Xin5; Pearce, Carolyn I.8; Chen, Ying5; Zhang, Shuai5,9; Liu, Wen2; Engelhard, Mark H.2; Kovarik, Libor2; Zong, Meirong3,5; Zhang, Hailin5,6,7 |
| 刊名 | ENVIRONMENTAL SCIENCE & TECHNOLOGY
 |
| 出版日期 | 2019-09-17 |
| 卷号 | 53期号:18页码:11043-11055 |
| ISSN号 | 0013-936X |
| DOI | 10.1021/acs.est.9b02693 |
| 英文摘要 | The 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. |
| WOS关键词 | HEAVY-METAL IONS ; HEXAVALENT CHROMIUM REMOVAL ; GAMMA-ALOOH ; CARBON NANOCOMPOSITES ; MASS-SPECTROMETRY ; AQUEOUS-SOLUTIONS ; THIN-FILMS ; WATER ; NANOPARTICLES ; CELLULOSE |
| 资助项目 | IDREAM (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研究方向 | Engineering ; Environmental Sciences & Ecology |
| 语种 | 英语 |
| 出版者 | AMER CHEMICAL SOC |
| WOS记录号 | WOS:000487163000054 |
| 资助机构 | IDREAM (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 |
| 源URL | [http://ir.ipe.ac.cn/handle/122111/31075]  |
| 专题 | 中国科学院过程工程研究所 |
| 通讯作者 | Zhang, Xin; Li, Ping; Wang, Zheming; Rosso, Kevin M. |
| 作者单位 | 1.Washington State Univ, Dept Chem, Pullman, WA 99164 USA 2.Pacific Northwest Natl Lab, Environm Mol Sci Lab, Richland, WA 99354 USA 3.Nanjing Univ, Sch Earth Sci & Engn, Nanjing 210023, Jiangsu, Peoples R China 4.Argonne Natl Lab, Adv Photon Source, Lemont, IL 60439 USA 5.Pacific Northwest Natl Lab, Phys & Computat Sci Directorate, Richland, WA 99354 USA 6.Chinese Acad Sci, Inst Proc Engn, Key Lab Green Proc & Engn, Natl Engn Lab Hydromet Cleaner Prod Technol, Beijing 100190, Peoples R China 7.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 8.Pacific Northwest Natl Lab, Energy & Environm Directorate, Richland, WA 99354 USA 9.Univ Washington, Dept Mat Sci & Engn, Seattle, WA 98195 USA |
| 推荐引用方式 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. |
入库方式： OAI收割
来源：过程工程研究所
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