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Enhancing Adsorption Desulfurization Performance Using Enriched Cu(I) Sites over Microenvironment-Modulated HKUST-1.

Ping Lu1,2,3, Zhaoyang Qi2,3, Jie Chen1,2,3

  • 1School of Chemical Engineering, Fuzhou University, Fuzhou, Fujian, 350108, P. R. China.

Small (Weinheim an Der Bergstrasse, Germany)
|August 11, 2023
PubMed
Summary

A new method enhances metal-organic frameworks (MOFs) for efficient removal of sulfur compounds from fuels. This approach creates more active sites, significantly improving sulfur adsorption capacity beyond existing materials.

Keywords:
adsorption desulfurizationcopper-cerium interactionmetal-organic frameworks (MOFs)microenvironment modulationmolecular engineering

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Area of Science:

  • Materials Science
  • Chemical Engineering
  • Environmental Science

Background:

  • Adsorptive desulfurization of liquid hydrocarbon fuels is crucial for environmental protection.
  • Metal-organic frameworks (MOFs) show promise for desulfurization but often suffer from inert metal sites.
  • Modulating the MOF microenvironment is key to enhancing adsorption efficiency.

Purpose of the Study:

  • To develop a novel method for enhancing the desulfurization performance of MOFs.
  • To create abundant high-efficiency Cu(I) and Cu-coordination-unsaturated sites within MOFs.
  • To improve pore structures around adsorptive sites for better sulfur compound capture.

Main Methods:

  • Utilized Cerium(III) as a molecular tool to modulate the coordination microenvironment of HKUST-1 (a type of MOF).
  • Fabricated enhanced MOF structures (CH-250) with improved Cu(I) and Cu-coordination-unsaturated sites.
  • Investigated the adsorption capacities and affinities of the modified MOFs for aromatic sulfur compounds.

Main Results:

  • The optimal CH-250 MOF demonstrated superior adsorptive capacities for thiophene (20.2 mg S g⁻¹), benzo-thiophene (28.0 mg S g⁻¹), and dibenzothiophene (58.3 mg S g⁻¹).
  • The engineered Cu(I) sites exhibited stronger adsorption affinity for dibenzothiophene compared to the original Cu(II) sites.
  • Significantly enhanced in-plane adsorption interactions were observed for dibenzothiophene on the modified MOF.

Conclusions:

  • Ce-enhanced modulation is an effective strategy for fabricating high-performance MOFs for adsorption desulfurization.
  • The engineered MOFs significantly outperform existing materials like zeolites and nanoporous carbons.
  • Molecular engineering of MOF coordination microenvironments holds great potential for deep desulfurization applications.