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Arsenic Adsorption on Lanthanum-Impregnated Activated Alumina: Spectroscopic and DFT Study
Shi, Qiantao; Yan, Li; Chan, Tingshan; Jing, Chuanyong
2015-12-09
Source PublicationACS APPLIED MATERIALS & INTERFACES
Volume7Issue:48Pages:26735-26741
AbstractRare earth-modified adsorbents (REMAs) have been widely used to remove oxyanion pollutants from water, including arsenic (As). However, the molecular-level structural information and reactions at the liquid/solid interface are still murky, which limits the design of applicable REMAs. Herein, a lanthanum-impregnated activated alumina (LAA) was synthesized as a representative REMA, and its As uptake mechanisms were explored using multiple complementary characterization techniques. Our adsorption experiments showed that LAA exhibited 2-(3) times higher As adsorption capacity than AA. In contrast to the bidentate configuration formed on most metal oxide surfaces, our EXAFS and DFT results suggest that As(III) and As(V) form monodentate surface complexes on LAA through As-O-La coordinative bonding. In situ flow cell ATR-FTIR observed a strong dependence of As-O peak positions on pH, which could be interpreted as the change in the fractions of As(V) surface complexes with zero- to double-protonation on LAA, AA, and LaOOH. As(V) on LAA existed as singly and doubly protonated surface species, and the pK(a) of transition from double to single protonation (similar to 5.8) was lower than that for its soluble counterpart (6.97). The surface reaction and structural configuration were incorporated in a CD-MUSIC model to satisfactorily predict macroscopic As adsorption behaviors. The insights gained from the molecular-level reactions shed light on the design and application of REMAs in environmental remediation for As and its structural analogues.
Department环境化学与生态毒理学国家重点实验室
KeywordAdsorption Arsenic Coordination Modes Surface Chemishy Lanthanum
WOS Research AreaNanoscience & Nanotechnology ; Materials Science, Multidisciplinary
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Document Type期刊论文
Identifierhttp://ir.rcees.ac.cn/handle/311016/32518
Collection环境化学与生态毒理学国家重点实验室
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GB/T 7714
Shi, Qiantao,Yan, Li,Chan, Tingshan,et al. Arsenic Adsorption on Lanthanum-Impregnated Activated Alumina: Spectroscopic and DFT Study[J]. ACS APPLIED MATERIALS & INTERFACES,2015,7(48):26735-26741.
APA Shi, Qiantao,Yan, Li,Chan, Tingshan,&Jing, Chuanyong.(2015).Arsenic Adsorption on Lanthanum-Impregnated Activated Alumina: Spectroscopic and DFT Study.ACS APPLIED MATERIALS & INTERFACES,7(48),26735-26741.
MLA Shi, Qiantao,et al."Arsenic Adsorption on Lanthanum-Impregnated Activated Alumina: Spectroscopic and DFT Study".ACS APPLIED MATERIALS & INTERFACES 7.48(2015):26735-26741.
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