4.7 Article

Development of Cationic Benzimidazole-Containing UiO-66 through Step-by-Step Linker Modification to Enhance the Initial Sorption Rate and Sorption Capacities for Heavy Metal Oxo-Anions

Journal

INORGANIC CHEMISTRY
Volume 61, Issue 30, Pages 11992-12002

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.inorgchem.2c01816

Keywords

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Funding

  1. National Natural Science Foundation of China [22171223, 22077099, 21807087, 21673173, 21572177, 21531007]
  2. Natural Science Foundation of Shaanxi Province of China [2020TG-031, 2022JQ-125, 2022JQ-151]
  3. Key Research and Development Program of Shaanxi [2019KWZ-07]
  4. Xi'an City Science and Technology Project [2019218214 GXRC018CG019-GXYD18.4, 2020KJRC0115]
  5. Shaanxi Key Laboratory of Special Fuel Chemistry and Material [SPCF-SKL-2021-0011]

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In this research, benzimidazole and -CH3 groups were successfully integrated into UiO-66 through a step-by-step linker modification strategy to form Bim-UiO-66 and Bim-UiO-66-Me. Both benzimidazole derivatives showed better performance than UiO-66 in the removal of heavy metal oxo-anions, with Bim-UiO-66-Me exhibiting the highest performance, with sorption rates and capacities 7.5 and 3.0 times higher than UiO-66, respectively. This study not only provides a promising candidate for removal of heavy metal oxo-anions in wastewater treatment but also presents a new strategy for the design of high-performance adsorbents.
Effective and rapid capture of heavy metal oxo-anions from wastewater is a fascinating research topic, but it remains a great challenge. Herein, benzimidazole and -CH3 groups were integrated into UiO-66 in succession via a step-by-step linker modification strategy that was performed by presynthesis modification (to give Bim-UiO-66) and subsequently by postsynthetic ionization (to give Bim-UiO-66-Me). The UiO-66s (UiO-66, Bim-UiO-66, and Bim-UiO-66-Me) were applied in the removal of heavy metal oxo-anions from water. The two benzimidazole derivatives (Bim-UiO-66 and Bim-UiO-66-Me) showed much better performance than UiO-66, as both the initial sorption rate and sorption capacities decreased in the order Bim-UiO-66-Me > Bim-UiO-66 > UiO-66. The maximum performances of Bim-UiO-66 are 5.1 and 1.7 times those of UiO-66. Remarkably, Bim-UiO-66-Me shows 7.5 and 3.0 times better performance than UiO-66. The higher absorptivity of cationic Bim-UiO-66-Me compared with UiO-66 can be attributed to a strong Coulombic interaction as well as an anion-pi interaction and hydrogen bonding between the benzimidazolium functional group and heavy metal oxo-anions. The as-synthesized Bim-UiO-66-Me not only provides a promising candidate for application in removal of heavy metal oxo-anions in wastewater treatment but also opens up a new strategy for the design of high-performance adsorbents.

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