Unraveling the effects of O-doping into h-BN on the adsorptive desulfurization performance by DFT calculations

Li, Hongping; Zhang, Yuan; Lv, Naixia; Yin, Jie; Zhang, Jinrui; Ran, Hongshun; Zhang, Ming; Jiang, Wei; Zhu, Wenshuai

doi:10.1016/j.jece.2021.106463

Cited by 21 publications

(22 citation statements)

References 52 publications

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“…The fully optimized structure and the possible coordination sites of the key species PW 12 O 40 3– are presented in Figure , whereas Figures – show the calculated potential energy profiles for the ODS process. It can be seen from the calculation that when combined with Oc, the required energy is 0, and the structure is relatively stable. , Figure shows the calculated energy profile of the proposed DBT oxidation reaction mechanism without a catalyst. Also, the activation energy barriers for the two steps are 36.2 and 40.6 kcal/mol, respectively.…”

Section: Resultsmentioning

confidence: 99%

“…Therefore, reducing or even totally removing sulfur contents in fuel oils is an inevitable trend, which is also of great significance for improving the global environment and achieving sustainable development. , At present, fuel desulfurization technology can be divided into two categories: hydrodesulfurization (HDS) and non-HDS. Among them, HDS needs to be carried out under high-temperature and high-pressure conditions, making the cost of HDS relatively high. − Compared with other organic sulfur compounds, refractory sulfur (RS) compounds have larger steric hindrances and are more stable and difficult to remove in HDS. , Under this circumstance, researchers have conducted a series of studies on non-HDS approaches such as biological desulfurization, , extractive desulfurization, − adsorptive desulfurization, − oxidative desulfurization (ODS), − etc . Among all these non-HDS methods, ODS has been proved to be an efficient one, in which organic sulfides are oxidized to sulfoxides or sulfones with higher polarities under mild conditions.…”

Section: Introductionmentioning

confidence: 99%

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Experimental and Theoretical Density Functional Theory Approaches for Desulfurization of Dibenzothiophene from Diesel Fuel with Imidazole-Based Heteropolyacid Catalysts

et al. 2023

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Oxidative desulfurization (ODS) has been proved to be an efficient strategy for the removal of aromatic sulfur compounds from diesel oils, which are one of the main sources of air pollution. Heteropolyacid catalysts are highly active species for ODS, but the promotion of their catalytic activity and clarification of their catalytic mechanism remain an important issue. Herein, a series of novel imidazole-based heteropolyacid catalysts are prepared by a one-pot method for multiphase deep ODS of fuel with hydrogen peroxide as an oxidant. The experimental results show that the desulfurization performance of the prepared imidazole-based heteropolyacid catalysts is high up to 99.9% under mild conditions. The catalyst also possesses excellent recovery performance, and the desulfurization activity remains at 97.7% after being recycled seven times. Furthermore, density functional theory calculation is first employed to clarify the origin of the high desulfurization activity, and the results show that with the imidazole-based heteropolyacid (HPW-VIM) as the catalyst, the energy barrier is much lower than that with phosphotungstic acid (HPW) as the catalyst.

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Experimental and Theoretical Density Functional Theory Approaches for Desulfurization of Dibenzothiophene from Diesel Fuel with Imidazole-Based Heteropolyacid Catalysts

et al. 2023

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“…To investigate the ADS performance of Ag-doped h-BN nanosheets, we first evaluate the adsorption capacity of the pristine h-BN monolayer. All the THs and aromatics in Figure S4 are parallel to the h-BN layer via π-π interaction with a vertical distance of ~3.2 Å [22]. The C atoms in the aromatics tend to be located vertically above the B atom.…”

Section: Adsorptionmentioning

confidence: 99%

“…Previous work showed that changing the electronic structure of h-BN is an effective approach [22][23][24]. Furthermore, h-BN can deliver abundant N or B ligands for metal atoms to form stable SAAs.…”

Section: Introductionmentioning

confidence: 99%

Ag Atom Anchored on Defective Hexagonal Boron Nitride Nanosheets As Single Atom Adsorbents for Enhanced Adsorptive Desulfurization via S-Ag Bonds

et al. 2022

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Single atom adsorbents (SAAs) are a novel class of materials that have great potential in various fields, especially in the field of adsorptive desulfurization. However, it is still challenging to gain a fundamental understanding of the complicated behaviors on SAAs for adsorbing thiophenic compounds, such as 1-Benzothiophene (BT), Dibenzothiophene (DBT), and 4,6-Dimethyldibenzothiophene (4,6-DMDBT). Herein, we investigated the mechanisms of adsorptive desulfurization over a single Ag atom supported on defective hexagonal boron nitride nanosheets via density functional theory calculations. The Ag atom can be anchored onto three typical sites on the pristine h-BN, including the monoatomic defect vacancy (B-vacancy and N-vacancy) and the boron-nitrogen diatomic defect vacancy (B-N-divacancy). These three Ag-doped hexagonal boron nitride nanosheets all exhibit enhanced adsorption capacity for thiophenic compounds primarily by the S-Ag bond with π-π interaction maintaining. Furthermore, from the perspective of interaction energy, all three SAAs show a high selectivity to 4,6-DMDBT with the strong interaction energy (−33.9 kcal mol−1, −29.1 kcal mol−1, and −39.2 kcal mol−1, respectively). Notably, a little charge transfer demonstrated that the dominant driving force of such S-Ag bond is electrostatic interaction rather than coordination effect. These findings may shed light on the principles for modeling and designing high-performance and selective SAAs for adsorptive desulfurization.

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“…However, the harsh operating conditions led to high cost. 3,4 Therefore, a considerable number of more economical desulfurization methods have been explored during the last decade, including extractive, 5,6 adsorptive, 7,8 biological 9,10 and oxidative desulfurization (ODS). 11,12 Some of these methods have milder operating conditions and better removal efficiencies for the organic sulfur than HDS.…”

Section: Introductionmentioning

confidence: 99%

Synthesis of modified amphiphilic quaternary ammonium silicotungstate and its application in heterogeneous catalytic oxidative desulfurization

Guo

Liu

2022

React. Chem. Eng.

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Unraveling the effects of O-doping into h-BN on the adsorptive desulfurization performance by DFT calculations

Cited by 21 publications

References 52 publications

Experimental and Theoretical Density Functional Theory Approaches for Desulfurization of Dibenzothiophene from Diesel Fuel with Imidazole-Based Heteropolyacid Catalysts

Experimental and Theoretical Density Functional Theory Approaches for Desulfurization of Dibenzothiophene from Diesel Fuel with Imidazole-Based Heteropolyacid Catalysts

Ag Atom Anchored on Defective Hexagonal Boron Nitride Nanosheets As Single Atom Adsorbents for Enhanced Adsorptive Desulfurization via S-Ag Bonds

Synthesis of modified amphiphilic quaternary ammonium silicotungstate and its application in heterogeneous catalytic oxidative desulfurization

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