Selective transformation and removal of As(III) by constructed Fe−N bonds: The generation of singlet oxygen from the photoexcitation of MnPc leads to abundant ZnFe−LDH interface OH radical

插层(化学) 砷酸盐 亚砷酸盐 单线态氧 层状双氢氧化物 化学 无机化学 吸附 磷酸盐 光化学 氧化物 材料科学 氧气 有机化学
作者
Huidi Zhang,Yao Deng,Junhui Yang,Jinglin Yin,Jing Wang,Hongbo Xiao,Lizhi Wang,Cuihong Zhang,Wenlei Wang
出处
期刊:Science of The Total Environment [Elsevier BV]
卷期号:890: 164314-164314 被引量:8
标识
DOI:10.1016/j.scitotenv.2023.164314
摘要

In this study, MnPc intercalated Zn/Fe layered double hydroxides (MnPc/ZF−LDH) were synthesized by pillared intercalation modification with different MnPc intercalation amounts and used for the selective transformation and removal of As(III) from the arsenate-phosphate mixed solution. Fe−N bonds were constructed by the complexation of MnPc and iron ions on the Zn/Fe layered double hydroxides (ZF−LDH) interface. The DFT calculation results show that the binding energy of Fe−N bonded to arsenite (−3.75 eV) was higher than that of phosphate (−3.16 eV), resulting in MnPc/ZnFe−LDH exhibiting high As(III) selective adsorption performance and anchoring it rapidly in the arsenite -phosphate mixed solution. The maximum adsorption capacity of 1MnPc/ZF−LDH for As(III) could reach 180.7 mg·g−1 under dark conditions. MnPc also acts as a photosensitizer to provide more active species for the photocatalytic reaction. A series of experiments demonstrated that MnPc/ZF−LDH exhibits high As(III) selective photocatalytic performance. A total of 10 mg·L−1 of As(III) was completely removed in the reaction system within 50 min in a single As(III) environment. In an environment with As(III) and PO43−, it achieved 80.0 % removal efficiency of As(III) and showed a good reuse effect. The introduction of MnPc could improve the utilization of visible light by the MnPc/ZnFe−LDH. The singlet oxygen generated from photoexciting MnPc leads to abundant ZnFe−LDH interface OH. In addition, MnPc/ZnFe−LDH shows good recyclability, making it a promising multifunctional material for the purification of arsenic-polluted sewage.
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