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

Author:

Lu Ping123ORCID,Qi Zhaoyang23,Chen Jie123,Ye Changshen123ORCID,Qiu Ting1234

Affiliation:

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

2. Qingyuan Innovation Laboratory Quanzhou Fujian 362801 P. R. China

3. Engineering Research Center of Reactive Distillation Fujian Province Higher Education Institutes Fuzhou Fujian 350108 P. R. China

4. Fuzhou University International Joint Laboratory of Thermochemical Conversion of Biomass Fuzhou Fujian 350108 P. R. China

Abstract

AbstractHigh‐efficiency adsorption of aromatic sulfur‐containing compounds from liquid hydrocarbon fuels over metal‐organic frameworks (MOFs) is challenging because of inert metal sites. A new method, the Ce‐enhanced modulation of MOFs’ microenvironment, is proposed to modulate the –COO···Cu(II)– coordination microenvironment of Hong Kong University of Science and Technology (HKUST‐1) using Ce(III) as a molecular scalpel for fabricating abundant high‐efficiency Cu(I) and Cu‐coordination‐unsaturated sites and improving the pore structures around adsorptive sites. The optimal CH‐250 thus exhibits adsorptive capacities for 20.2, 28.0, and 58.3 mg S g–1 of thiophene, benzo‐thiophene, and dibenzothiophene, respectively, which are superior to most reported MOFs, zeolites, and nanoporous carbons. The constructed Cu(I) sites show stronger affinity for dibenzothiophene (−0.86 eV) than the initial Cu(II) (−0.74 eV) for out‐of‐plane adsorption. Further, they are far stronger in‐plane adsorption interactions in DBT/CH‐250 (−0.90 eV) than those in DBT/HKUST‐1 (−0.37 eV). Thus, molecular engineering for modulating the coordination microenvironment of MOFs shows great potential for adsorption desulfurization.

Funder

National Natural Science Foundation of China

Publisher

Wiley

Subject

Biomaterials,Biotechnology,General Materials Science,General Chemistry

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