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Tracking Internal Electron Shuttle Using X-ray Spectroscopies in La/Zr Hydroxide for Reconciliation of Charge-Transfer Interaction and Coordination toward Phosphate
Xiang, Chao; Wang, Hongjie; Ji, Qinghua; Zhang, Gong; Qu, Jiuhui
2019-07-10
Source PublicationACS APPLIED MATERIALS & INTERFACES
ISSN1944-8244
Volume11Issue:27Pages:24699-24706
AbstractMetallic hydroxides have been applied as the adsorbents of oxyanion contaminants, with the oxygen-bonded metal (M-O) considered as the core site for adsorption. For enhanced adsorption toward oxyanions, multimetallic modification of M-O is a promising approach for high removal performance. Here, bimetallic La/Zr hydroxides were prepared via a solvothermal route with varying La/Zr dosages. Bimetallic La/Zr hydroxides exhibited higher oxyanion adsorption capacity than La or Zr hydroxide. A maximum phosphate adsorption capacity of similar to 160 mg g(-1) was achieved under the La/Zr atomic ratio of 1:1, representing a new record among comparable adsorbents. X-ray photoelectron spectroscopy and X-ray absorption near-edge structure (XANES) spectroscopy showed that the incorporation of [LaO6] and [ZrO6] can induce an internal charge shuttle owing to the electronegativity difference of La and Zr. The charge transfers from La to Zr through the surrounding O 2p ligand, where the electrons in the highest occupied molecular orbitals of the [LaO6] octahedron filled unoccupied it orbitals of [ZrO6]. The as-induced internal electron shuttle in the bimetallic hydroxides primarily strengthened the formation of [MO6]center dot center dot center dot PO4 species (backdonation interaction). Further, the sigma(p-O) donation interaction between [LaO6] and [PO4] was clearly increased via intensification of the covalent coordination with O, as confirmed by the P K-edge XANES spectra for the as-used samples.
Department中国科学院饮用水科学与技术重点实验室
Keywordmetallic hydroxide oxyanion X-ray photoelectron spectroscopy
Document Type期刊论文
Identifierhttp://ir.rcees.ac.cn/handle/311016/43540
Collection中国科学院饮用水科学与技术重点实验室
Affiliation1.Beijing Forestry Univ, Coll Environm Sci & Engn, Beijing 100083, Peoples R China
2.Tsinghua Univ, Sch Environm, State Key Joint Lab Environm Simulat & Pollut Con, Ctr Water & Ecol, Beijing 100084, Peoples R China
3.Chinese Acad Sci, Key Lab Drinking Water Sci & Technol, Res Ctr Ecoenvironm Sci, Beijing 100085, Peoples R China
Recommended Citation
GB/T 7714
Xiang, Chao,Wang, Hongjie,Ji, Qinghua,et al. Tracking Internal Electron Shuttle Using X-ray Spectroscopies in La/Zr Hydroxide for Reconciliation of Charge-Transfer Interaction and Coordination toward Phosphate[J]. ACS APPLIED MATERIALS & INTERFACES,2019,11(27):24699-24706.
APA Xiang, Chao,Wang, Hongjie,Ji, Qinghua,Zhang, Gong,&Qu, Jiuhui.(2019).Tracking Internal Electron Shuttle Using X-ray Spectroscopies in La/Zr Hydroxide for Reconciliation of Charge-Transfer Interaction and Coordination toward Phosphate.ACS APPLIED MATERIALS & INTERFACES,11(27),24699-24706.
MLA Xiang, Chao,et al."Tracking Internal Electron Shuttle Using X-ray Spectroscopies in La/Zr Hydroxide for Reconciliation of Charge-Transfer Interaction and Coordination toward Phosphate".ACS APPLIED MATERIALS & INTERFACES 11.27(2019):24699-24706.
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