Highly active and stable MoS2-TiO2 nanocomposite catalyst for slurry-phase phenanthrene hydrogenation

doi:10.1016/S1872-2067(22)64184-6

Abstract

Abstract:

MoS₂-TiO₂ nanocomposite catalysts with Janus structure were synthesized via facile one-step solvothermal method. X-ray diffraction, high resolution transmission electron microscope, NO chemisorption and X-ray photoelectron spectroscopy were applied to characterize the composition and nanostructure of the MoS₂-TiO₂ nanocomposite catalysts. Experimental results revealed that the MoS₂-TiO₂ nanocomposite catalysts with Janus structure were composed of MoS₂ layers (few stacked layers of 1-3 and short slabs of 2-10 nm) and TiO₂ nanoparticles (10-15 nm), which have strong MoS₂-TiO₂ interaction with transferring electrons from TiO₂ to MoS₂. Catalytic performance of MoS₂-TiO₂ nanocomposite catalysts for phenanthrene hydrogenation was investigated and compared with that of MoS₂ catalyst in an autoclave reactor with high temperature and high pressure. The phenanthrene conversion over the MoS₂-TiO₂ nanocomposite catalyst with MoS₂ content of 15.0 wt% (MoS₂-TiO₂-15) can reach 91.6%, which was much higher than 50.4% for MoS₂ catalyst and 76.8% for conventional supported MoS₂/TiO₂-15 catalyst. After 7 cycles of phenanthrene hydrogenation reaction, the phenanthrene conversion over MoS₂-TiO₂-15 nanocatalyst remained at 68.6%, while the phenanthrene conversion over MoS₂ catalyst was reduced to only 25.4%. The MoS₂-TiO₂ nanocomposite catalysts exhibit significantly enhanced catalytic activity and stability for slurry phase hydrogenation. The enhanced catalytic activity originates from the exposure of abundant coordinatively unsaturated Mo atoms. The enhanced stability results from the Janus structure with stable MoS₂-TiO₂ interaction and Mo-O-Ti bonds, which anchor MoS₂ layers on the surface of TiO₂ nanoparticles to avoid the curling, folding and agglomeration of MoS₂ layers. This is an important finding on slurry phase catalytic hydrogenation performances of MoS₂-based nanocomposite catalysts with Janus structure. Shedding light on the research of Janus nanocomposite catalysts in catalytic hydrogenation is significantly crucial for the development of effective and stable hydrogenation catalysts.

Key words: Nanocomposite catalyst, High MoS₂ dispersion, Coordinatively unsaturated Mo atom, MoS₂-TiO₂ interaction, Catalytic hydrogenation

Chenggong Yang, Donge Wang, Rong Huang, Jianqiang Han, Na Ta, Huaijun Ma, Wei Qu, Zhendong Pan, Congxin Wang, Zhijian Tian. Highly active and stable MoS₂-TiO₂ nanocomposite catalyst for slurry-phase phenanthrene hydrogenation[J]. Chinese Journal of Catalysis, 2023, 46: 125-136.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(22)64184-6

https://www.cjcatal.com/EN/Y2023/V46/I3/125

Figures/Tables 10

Table 1 Synthesis of TiO2, MoS2, and MoS2-TiO2 nanocomposite catalysts under different conditions.

Catalyst	ATM (g)	N₂H₄·H₂O (g)	TBT (g)	H₂O (mL)	Ethyl alcohol (mL)
TiO₂	0	0.63	7.7	60	40
MoS₂-TiO₂-5	0.26	0.32	13.0	60	40
MoS₂-TiO₂-15	0.52	0.63	7.7	60	40
MoS₂-TiO₂-25	0.52	0.63	4.1	60	40
MoS₂-TiO₂-35	0.52	0.63	2.5	60	40
MoS₂	0.52	0.63	0	60	40

Fig. 1. XRD patterns of bare TiO2 sample, MoS2 sample, MoS2-TiO2 samples with various MoS2 contents and MoS2/TiO2-15-I sample.

Fig. 2. HRTEM images of bare TiO2 (a), MoS2-TiO2-5 (b), MoS2-TiO2-15(c), MoS2-TiO2-25 (d), MoS2-TiO2-35 (e), MoS2/TiO2-15-I (f) and MoS2 samples (g). (h) HRTEM image and corresponding element mapping of MoS2-TiO2-15 sample.

Fig. 3. Average numbers of stacking layers, average slab lengths and MoS2 dispersion.

Fig. 4. NO adsorption capacity of MoS2 and MoS2-TiO2 nanocomposite samples with different MoS2 percentages.

Fig. 5. XPS spectra of Mo 3d (a), Ti 2p (b) for MoS2 and MoS2-TiO2 nanocomposite samples. (c) XPS spectra of Mo 3d for MoS2, supported MoS2/TiO2-15-I and MoS2-TiO2-15 nanocomposite samples. (d) Negative shifts of binding energy for Mo 3d of MoS2-TiO2 nanocomposite samples compared with that of MoS2 sample.

Fig. 6. The observed structures (a) and the proposed structural models (b) of the MoS2-TiO2 nanocomposite with Janus structure.

Fig. 7. (a) Conversions and HPs of phenanthrene over MoS2 catalyst and MoS2-TiO2 nanocomposite catalysts with different MoS2 contents. (b) Catalytic hydrogenation selectivities to PHx over MoS2 catalyst and MoS2-TiO2 nanocomposite catalysts with different MoS2 contents. (c) Conversions and HPs of phenanthrene over bare TiO2, MoS2, the mixture of bare TiO2 and MoS2, MoS2-TiO2-15-I and MoS2-TiO2-15 catalyst. (d) Catalytic hydrogenation selectivities to PHx over bare TiO2, synthesized MoS2, the mixture of bare TiO2 and MoS2, MoS2-TiO2-15-I and MoS2-TiO2-15 catalyst. Reaction conditions: MoS2 contents of catalyst 0.075 g, phenanthrene 3.0 g, solvent tridecane 30.0 g, initial pressure 8 Mpa, 350 °C, 4 h.

Fig. 8. The stability of MoS2-TiO2-15 nanocomposite catalyst and MoS2 catalyst for phenanthrene hydrogenation.

Fig. 9. (a) The XRD patterns of fresh MoS2, MoS2-C7, fresh MoS2-TiO2-15, and MoS2-TiO2-15-C7. (b) HRTEM images of fresh MoS2, MoS2-C7, fresh MoS2-TiO2-15, and MoS2-TiO2-15-C7. (c) XPS spectra of Mo 3d of fresh MoS2, MoS2-C7, fresh MoS2-TiO2-15, and MoS2-TiO2-15-C7.

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Highly active and stable MoS₂-TiO₂ nanocomposite catalyst for slurry-phase phenanthrene hydrogenation

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