材料科学
氢氧化物
跟踪(教育)
电荷(物理)
电子
磷酸盐
电子转移
化学物理
纳米技术
物理化学
无机化学
核物理学
物理
有机化学
化学
心理学
量子力学
教育学
作者
Chao Xiang,Hongjie Wang,Qinghua Ji,Gong Zhang,Jiuhui Qu
标识
DOI:10.1021/acsami.9b05397
摘要
Metallic 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 ∼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 π orbitals of [ZrO6]. The as-induced internal electron shuttle in the bimetallic hydroxides primarily strengthened the formation of [MO6]···PO4 species (backdonation interaction). Further, the σP–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.
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