4.8 Article

Trace removal of benzene vapour using double-walled metal-dipyrazolate frameworks

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NATURE MATERIALS
卷 21, 期 6, 页码 689-+

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NATURE PORTFOLIO
DOI: 10.1038/s41563-022-01237-x

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资金

  1. National Natural Science Foundation of China [51621003, 22038001]
  2. Science Foundation Ireland [16/IA/4624]
  3. European Research Council [ADG 885695]
  4. Postdoctoral Science Foundation of Chaoyang District [2020ZZ-8]

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Porous physisorbents are attractive candidates for the removal of volatile organic compounds. In this study, a double-walled metal-organic framework demonstrated high affinity and adsorption capacity towards benzene at low pressures. The findings provide insights into the development of recyclable physisorbents for environmental remediation.
In principle, porous physisorbents are attractive candidates for the removal of volatile organic compounds such as benzene by virtue of their low energy for the capture and release of this pollutant. Unfortunately, many physisorbents exhibit weak sorbate-sorbent interactions, resulting in poor selectivity and low uptake when volatile organic compounds are present at trace concentrations. Herein, we report that a family of double-walled metal-dipyrazolate frameworks, BUT-53 to BUT-58, exhibit benzene uptakes at 298 K of 2.47-3.28 mmol g(-1) at <10 Pa. Breakthrough experiments revealed that BUT-55, a supramolecular isomer of the metal-organic framework Co(BDP) (H2BDP = 1,4-di(1H-pyrazol-4-yl)benzene), captures trace levels of benzene, producing an air stream with benzene content below acceptable limits. Furthermore, BUT-55 can be regenerated with mild heating. Insight into the performance of BUT-55 comes from the crystal structure of the benzene-loaded phase (C6H6@BUT-55) and density functional theory calculations, which reveal that C-H center dot center dot center dot X interactions drive the tight binding of benzene. Our results demonstrate that BUT-55 is a recyclable physisorbent that exhibits high affinity and adsorption capacity towards benzene, making it a candidate for environmental remediation of benzene-contaminated gas mixtures. Volatile organic compounds such as benzene are toxic pollutants that cause health issues even at trace concentrations. Here, a double-walled metal-organic framework is presented that demonstrates high uptake at very low pressures (<10 Pa), allowing the removal of benzene to below acceptable indoor limits.

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