4.8 Article

Rapid Simultaneous Removal of Toxic Anions [H5eO3]-, [SeO3]2-, and [SeO4]2-, and Metals Hg2+, Cu2+, and Cd2+ by MoS42- Intercalated Layered Double Hydroxide

期刊

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 139, 期 36, 页码 12745-12757

出版社

AMER CHEMICAL SOC
DOI: 10.1021/jacs.7b07123

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资金

  1. National Science Foundations of China [21271028, 21271001, 21471020]
  2. National Science Foundation [MRSEC DMR 1121262, DMR 1708254]

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We demonstrate fast, highly efficient concurrent removal of toxic oxoanions of Se(VI) (SeO42) and Se(IV) (SeO32-/HSeO3- ) and heavy metal ions of Hg2+, Cu2+, and Cd2+ by the MoS42 intercalated Mg/Al layered double hydroxide (MgAl-MoS4-LDH, abbr. MoS4-LDH). Using the MoS4-LDH as a sorbent, we observe that the presence of Hg2+ ions greatly promotes the capture of SeO42, while the three metal ions (Hg2+, Cu2+, Cd2+) enable a remarkable improvement in the removal of SeO32/HSeO3 . For the pair Se(VI)+Hg2+, the MoS4-LDH exhibits outstanding removal rates (> 99.9%) for both Hg2+ and Se(VI), compared to 81% removal for SeO42 alone. For individual SeO32- (without metal ions), 99.1% Se(IV) removal is achieved, while >= 99.9% removals are reached in the presence of Hg2+, Cu2+, and Cd2+. Simultaneously, the removal rates for these metal ions are also > 99.9%, and nearly all concentrations of the elements can be reduced to < 10 ppb, a limit acceptable for drinking water. The maximum sorption capacities for individual Se(VI) and Se(IV) are 85 and 294 mg/g, respectively. The 294 mg/g capacity for Se(IV) reaches a record value, placing the MoS4- LDH among the highest-capacity selenite adsorbing materials described to date. More interestingly, the presence of metal ions extremely accelerates the capture of the selenium oxoanions because of the reactions of the metal ions with the interlayer MoS42- anions. The sorptions of Se(VI)+Hg and Se(IV)+M (M = Hg2+, Cu2+, Cd2+) are exceptionally rapid, showing > 99.5% removals for Hg2+ within 1 min and similar to 99.0% removal for Se(VI) within 30 min, as well as > 99.5% removals for pairs Cu2+ and Se(IV) within 10 min, and Cd2+ and Se(IV) within 30 min. During the sorption of SeO32/HSeO3 , reduction of Se(IV) occurs to Se-0 caused by the S-2 sites in MoS42. Sorption kinetics for the oxoanions follows a pseudo-second-order model consistent with chemisorption. The intercalated material of MoS4-LDH is very promising as a highly effective filter for decontamination of water with toxic Se(IV)/Se(VI) oxoanions along with heavy metals such as Hg2+, Cd2+, and Cu2+.

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