Fabrication of Microwave-responsive CMF@CoS2/MoS2 Catalyst and Highly Efficient Reforming of Lignin Vapor by Microwave Irradiation

doi:10.6023/A24030079

Abstract

To take the place of non-renewable resources derived from traditional petrochemical energy conversing of lignin into high-value platform chemicals has become one of the future research hotspots. Among many conversion technologies, microwave-assisted catalytic depolymerization technology is widely used in the catalytic reforming of lignin due to its advantages of block heating rate, low energy consumption, high product selectivity, etc.. The selection of catalysts plays a crucial role in the reforming of lignin. In this work, microwave-responsive CMF@CoS₂/MoS₂ catalyst was prepared by a one-step hydrothermal method using Anderson-type polymetallic oxides (NH₄)₃[CoMo₆O₂₄H₆]•6H₂O as precursors. The morphological features and microwave absorption properties of CMF@CoS₂/MoS₂ catalysts were characterized through scanning electron microscope (SEM), energy dispersive spectroscopy (EDS), X-ray diffraction (XRD), transmission electron microscope (TEM) and 3656A vector network analyzer. The results showed that CMF@CoS₂/MoS₂ is composed of nanoflowers deposited on the CMF 3D skeleton. And CMF@CoS₂/MoS₂ has excellent microwave absorption properties (dielectric loss angle tangent of 0.23). The catalytic reforming of lignin vapor was carried out using a designed dynamic vapor flow reaction system, and the results showed that the CMF@CoS₂/MoS₂ catalyst possessed highly efficient catalytic reforming ability. The monophenol yield (59.30%) and phenol selectivity (24.69%) of the lignin depolymerization product were increased under the reaction conditions of 400 s, 1000 W, and 600 mL/min N₂. Finite element analysis of the microwave-assisted catalytic depolymerization (MACD) of lignin reveals that the CMF@CoS₂/MoS₂ is capable of generating a “hotspot” effect under microwave irradiation to raise the local temperature of the 3D skeleton to 910 ℃ due to its excellent microwave absorption properties, which is a good example of the MACD of lignin. The heat exchange of lignin vapor with a lower temperature (570 ℃), captured during depolymerization, further promotes the catalytic reforming of lignin vapor. This is key to the efficient catalytic reforming of lignin vapor over the CMF@CoS₂/MoS₂ catalyst. In conclusion, this work provides a promising method for the efficient production of phenols from lignin over bifunctional CMF@CoS₂/MoS₂ catalyst with “wave-absorbing heat transfer” and “catalytic conversion”.

Key words: lignin, microwave, monophenols, phenol, catalyst

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Yishuai Fu, Wenliang Wang, Hui Miao, Yutong Chen, Yangyi Cui, Ziwei Wang, Jiawen Pan, Guowei Xiao. Fabrication of Microwave-responsive CMF@CoS₂/MoS₂ Catalyst and Highly Efficient Reforming of Lignin Vapor by Microwave Irradiation[J]. Acta Chimica Sinica, 2024, 82(6): 596-603.

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Fig. & Tab. 11

Figure 1. (a) Actual picture of MF, CMF and CMF@CoS2/MoS2; (b) actual picture of CMF placed on a dandelion; (c) elasticity test of CMF@CoS2/MoS2 under pressure

Figure 2. (a, d) SEM images of MF at different magnifications; (b, e) SEM images of CMF at different magnifications; (c, f) SEM images of CMF@CoS2/MoS2; (g) SEM image and the corresponding elemental mapping images of Co, Mo, and S for CMF@CoS2/MoS2

Figure 3. (a) TEM image of CMF@CoS2/MoS2 nanoflower; (b) HRTEM image of CMF@CoS2/MoS2; (c) XRD patterns of CMF@CoS2/MoS2 and CMF@MoS2

Figure 4. (a) Catalyst complex dielectric constant real part; (b) catalyst complex dielectric constant imaginary part; (c) catalyst dielectric loss tangent factor; (d) theoretical and practical values of catalyst dielectric loss tangent factors

Figure 5. (a) Product distribution of MAD and MACD reactions; (b) total ion chromatogram of bio-oil; (c) component distribution of bio-oil; (d) phenolic selectivity of bio-oil

Figure 6. The cyclic stability of catalytic reforming with CMF@CoS2/MoS2 in MACD

Figure 7. Distribution of temperature field and electric field with different microwave power. Reaction conditions: reaction time: 400 s; nitrogen flow rate: 600 mL/min

Figure 8. (a) Finite element model for CMF@CoS2/MoS2 set-up conditions; (b) finite element simulation of CMF@CoS2/MoS2 heating rate (a) Finite element model for CMF@CoS2/MoS2 set-up conditions; (b) finite element simulation of CMF@CoS2/MoS2 heating rate

Figure 9. Microwave-assisted dynamic vapor flow reaction system

参数名称	参数值
相对磁导率μ_r	1
相对介电常数(CMF@CoS₂/MoS₂) ε_r	5.00-1.17*j
相对介电常数(CoS₂/MoS₂) ε_r	2.39-0.73*j
相对介电常数(CMF) ε_r	5.01-0.98*j
相对介电常数(木质素(脱碱)) ε_r	3.08-0.13*j
电导率σ/(S•m^-1)	0
比热率	1.24
密度/(kg•m^-3)	12

Table 1. Physical parameters of CMF@CoS2/MoS2

Figure 10. (a) Geometrical model of the microwave reactor; (b) geometrical model of the CMF@CoS2/MoS2 (Cheng, B.)

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微波响应型CMF@CoS₂/MoS₂催化剂的制备及其用于木质素蒸气的催化重整

Fabrication of Microwave-responsive CMF@CoS₂/MoS₂ Catalyst and Highly Efficient Reforming of Lignin Vapor by Microwave Irradiation

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微波响应型CMF@CoS2/MoS2催化剂的制备及其用于木质素蒸气的催化重整