Engineering the electronic and geometric structure of VOx/BN@TiO2 heterostructure for efficient aerobic oxidative desulfurization

doi:10.1007/s11705-022-2242-3

Front. Chem. Sci. Eng.

2023, Vol. 17

Issue (3) : 276-287 https://doi.org/10.1007/s11705-022-2242-3

RESEARCH ARTICLE

Engineering the electronic and geometric structure of VO_x/BN@TiO₂ heterostructure for efficient aerobic oxidative desulfurization

Lu Zhang¹, Jixing Liu¹(

), Deqi Huang², Wenfeng Zhang¹, Linjie Lu¹, Mingqing Hua¹, Hui Liu¹, Huifang Cheng¹, Huaming Li¹, Wenshuai Zhu¹(

)

¹. School of Chemistry and Chemical Engineering, Institution for Energy Research, Jiangsu University, Zhenjiang 212013, China
². College of Chemical Engineering, Yangzhou Polytechnic Institute, Yangzhou 225127, China

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Abstract

Particle size governs the electronic and geometric structure of metal nanoparticles (NPs), shaping their catalytic performances in heterogeneous catalysis. However, precisely controlling the size of active metal NPs and thereafter their catalytic activities remain an affordable challenge in ultra-deep oxidative desulfurization (ODS) field. Herein, a series of highly-efficient VO_x/boron nitride nanosheets (BNNS)@TiO₂ heterostructures, therein, cetyltrimethylammonium bromide cationic surfactants serving as intercalation agent, BNNS and MXene as precursors, with various VO_x NP sizes were designed and controllably constructed by a facile intercalation confinement strategy. The properties and structures of the prepared catalysts were systematically characterized by different technical methods, and their catalytic activities were investigated for aerobic ODS of dibenzothiophene (DBT). The results show that the size of VO_x NPs and V⁵⁺/V⁴⁺ play decisive roles in the catalytic aerobic ODS of VO_x/BNNS@TiO₂ catalysts and that VO_x/BNNS@TiO₂-2 exhibits the highest ODS activity with 93.7% DBT conversion within 60 min under the reaction temperature of 130 °C and oxygen flow rate of 200 mL·min^–1, which is due to its optimal VO_x dispersion, excellent reducibility and abundant active species. Therefore, the finding here may contribute to the fundamental understanding of structure-activity in ultra-deep ODS and inspire the advancement of highly-efficient catalyst.

Keywords oxidative desulfurization boron nitride vanadium MXene intercalation confinement

Corresponding Author(s): Jixing Liu,Wenshuai Zhu

Online First Date: 25 December 2022 Issue Date: 17 March 2023

Cite this article:

Lu Zhang,Jixing Liu,Deqi Huang, et al. Engineering the electronic and geometric structure of VO_x/BN@TiO₂ heterostructure for efficient aerobic oxidative desulfurization[J]. Front. Chem. Sci. Eng., 2023, 17(3): 276-287.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-022-2242-3
https://academic.hep.com.cn/fcse/EN/Y2023/V17/I3/276

Scheme1 Illustration of the construction of VO_x/BNNS@TiO₂ heterostructure.

Fig.1 (A) XRD pattern and (B) 12°–25° XRD pattern of the catalysts: (a) VO_x/BNNS, (b) VO_x/BNNS@TiO₂-1, (c) VO_x/BNNS@TiO₂-2 and (d) VO_x/BNNS@TiO₂-3.

Fig.2 TEM images and particle size distribution of the catalysts: (a) VO_x/BNNS, (b) VO_x/BNNS@TiO₂-1, (c) VO_x/BNNS@TiO₂-2, (d) VO_x/BNNS@TiO₂-3 and (e) EDS mapping images of VO_x/BNNS@TiO₂-2.

Tab.1 The relative concentration ratios and surface atomic concentrations of V, B, N, and O on VO_x/BNNS@TiO₂ catalysts

Fig.3 (A) O 1s and (B) V 2p XPS of the catalysts: (a) VO_x/BNNS, (b) VO_x/BNNS@TiO₂-1, (c) VO_x/BNNS@TiO₂-2 and (d) VO_x/BNNS@TiO₂-3.

Fig.4 H₂-TPR profile of (a) VO_x/BNNS, (b) VO_x/BNNS@TiO₂-1, (c) VO_x/BNNS@TiO₂-2, and (d) VO_x/BNNS@TiO₂-3 catalysts.

Fig.5 (A) ODS activity for VO_x/BNNS@TiO₂-2 at different rotation speeds and (B) catalytic performances of (a) BNNS, (b) TiO₂, (c) VO_x/BNNS, (d) VO_x/TiO₂, (e) BNNS/TiO₂, (f) VO_x/BNNS@ TiO₂-1, (g) VO_x/BNNS@TiO₂-2 and (h) VO_x/BNNS@TiO₂-3 catalysts in ODS system (Experimental conditions: v(O₂) = mL?min^–1, T = 130 °C, V(oil) = 20 mL, r = 800 r·min^–1 and m(catalyst) = 0.02 g).

Fig.6 ODS activities for VO_x/BNNS@TiO₂-2 at (A) different reaction temperatures, (B) different DBT concentrations, (C) different substrates and (D) catalytic stability of VO_x/BNNS@TiO₂-2 in ODS system (Experimental conditions: v(O₂) = 200 mL·min^–1, T = 130 °C, V(oil) = 20 mL, r = 800 r·min^–1 and m(catalyst) = 0.02 g).

Fig.7 (A) Pseudo-first-order kinetic plots for the ODS at various reaction temperatures and (B) the Arrhenius activation energy for the ODS of DBT over VO_x/BNNS@TiO₂-2.

Fig.8 (A) GC-MS of the main compounds in the oil phase (m) and catalyst phase (n); (B) investigation of sulfur removal with addition of different scavengers (dimethyl sulfoxide, DMSO; benzoquinone, BQ) by using VO_x/BNNS@TiO₂-2 as catalyst; (C) electron spin resonance (ESR) spectra of VO_x/BNNS@TiO₂-2 with DMPO (dimethyl pyridine N-oxide) as capture agent; (D) proposed reaction mechanism.

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