Density functional theory screening of thiophene adsorbents and study of adsorption mechanism.

• Adopting density functional theory screening method to evaluate MOFs adsorbent. • Three adsorbents were found the best activity with adsorption energy <−1.21 eV. • The adsorption units in action consists of metal centers and coordination atoms. • D-band center of units remain unchanged is the origin of high performance. Sulfides, widely found in fossil fuels, not only corrode equipment but also pollute the atmosphere. Adsorption desulphurization can not only remove sulfide effectively, but also reduce energy consumption, it is very necessary to develop desulphurization adsorbent. Metal-organic framework materials (MOFs) have great potential in adsorption desulfurization due to the unique structural properties. However, selecting high-performance adsorbents in the growing sea of MOFs by experiment still needs theoretical guidance. Therefore, the screening method based on density functional theory was adopted to develop the thiophene adsorbents and explore the overall picture of thiophene adsorption. Through applying a three-step screening strategy which involves, we evaluated adsorption performance of 12,020 computationally-ready experimental MOFs candidates. Three adsorbents were found the best activity with adsorption energy <-1.21 eV. According to the classification and electronic structure analysis, it is found that different combinations of ligand atoms and open metal site can induce different strength of d -band center movement during the adsorption process. The high-performance adsorbents are those d -band center of metal sites remain unchanged in the adsorption of thiophene. These results emphasize the importance of the structure-performance relationship of potential MOFs in adsorption desulfurization. [Display omitted] We evaluated the origin of adsorption capacity of MOFs for thiophene through high-throughput method in this work. By concentrating on the composition, structure and coordination environment, all candidates were subsumed into the 'twenty-two kinds of metal sites, two ligand atoms and four coordination number' matrix of Figure c. Three structures were proved the best thiophene adsorption activity (pentagram represented). [ABSTRACT FROM AUTHOR]