Mo--V--Nb--O-based catalysts for low-temperature selective oxidation of C<sub>α</sub>--OH lignin model compounds

doi:10.1007/s11706-020-0494-8

Front. Mater. Sci.

2020, Vol. 14

Issue (1) : 52-61 https://doi.org/10.1007/s11706-020-0494-8

RESEARCH ARTICLE

Mo--V--Nb--O-based catalysts for low-temperature selective oxidation of C_α--OH lignin model compounds

Lu-Lu ZHANG¹, Kun HAO¹, Rui-Kai WANG¹, Xiu-Qiang MA¹, Tong LIU², Liang SONG¹(

), Qing YU¹, Zhong-Wei WANG¹, Jian-Min ZENG³, Rong-Chang ZENG¹(

)

¹. College of Materials Science and Engineering, Shandong University of Science and Technology, 579 Qianwangang Road, Qingdao 266590, China
². College of Materials Science and Engineering, Qingdao University of Science and Technology, 53 Zhengzhou Road, Qingdao 266000, China
³. Ministry-Province Jointly-Constructed Cultivation Base for State Key Laboratory of Processing for Non-ferrous Metal and Featured Materials, Guangxi University, 100 Daxue East Road, Nanning 530004, China

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Abstract

Mo–V–Nb tri-component oxide catalysts were prepared and firstly used for the selective oxidation of C_α−OH lignin compounds. The catalytic performance of the composite oxides was obviously enhanced due to the synergistic effects of Mo and V elements. Mo₅₋_xV_xO₁₄ phase with a variable Mo/V ratio provided suitable active sites for the oxidative dehydrogenation (ODH) of C_α−OH lignin model compound. The optimized Mo–V–Nb molar composition was confirmed as Mo_0.61V_0.31Nb_0.08O_x/TiO₂, which exhibited the prominent catalytic activity with the turnover frequency of 1.04×10⁻³ mmol· g(cat)⁻¹·s⁻¹. Even at room temperature, the catalysts showed highly-efficient ODH reaction activities. The active phase for selective oxidation reaction and the inhibiting effect of α-MoO₃ phase were also discussed in the study.

Keywords selective oxidation secondary alcohol lignin model compound room temperature

Corresponding Author(s): Liang SONG,Rong-Chang ZENG

Online First Date: 20 January 2020 Issue Date: 05 March 2020

Cite this article:

Lu-Lu ZHANG,Kun HAO,Rui-Kai WANG, et al. Mo--V--Nb--O-based catalysts for low-temperature selective oxidation of C_α--OH lignin model compounds[J]. Front. Mater. Sci., 2020, 14(1): 52-61.

URL:

https://academic.hep.com.cn/foms/EN/10.1007/s11706-020-0494-8
https://academic.hep.com.cn/foms/EN/Y2020/V14/I1/52

Fig.1 XRD patterns of (a) MoVNbO_x/TiO₂ samples with different molar ratios of Mo/V and (b) MoVNbO_x samples in the 2θ region of 20°?23°.

Fig.2 SEM images of MoVNbO_x/TiO₂ samples with different Mo/V molar ratios: (a) Mo_0.23V_0.69Nb_0.08O_x/TiO₂, (b) Mo_0.31V_0.61Nb_0.08O_x/TiO₂, (c) Mo_0.46V_0.46Nb_0.08O_x/TiO₂, (d) Mo_0.61V_0.31Nb_0.08O_x/TiO₂ and (e) Mo_0.69V_0.23Nb_0.08O_x/TiO₂.

Fig.3 (a) TEM image of the MoVNbO_x/TiO₂ sample, (b) distribution of O and Ti elements, and (c) distribution of Mo, V, Nb, O and Ti elements.

Fig.4 The average NP size and the size distribution of MoVNbO_x/TiO₂ samples.

Fig.5 The effect of the Mo/V molar ratio of the MoVNbO_x/TiO₂ catalyst on TOFs of 1-phenyl ethanol.

Fig.6 Effects of calcination temperature and reaction temperature on TOFs of 1-phenyl ethanol.

Fig.7 Reaction stability test of the reused Mo?V?Nb tri-component oxides catalyst.

Fig.8 Relationship between the characteristic diffraction peak shift of Mo₅₋_xV_xO₁₄ phase and TOF of selective oxidation of C_α−OH lignin model compound.

Fig.9 SEM image of α-MoO₃ phase in the Mo_0.69V_0.23Nb_0.08O_x/TiO₂ sample.

Fig.10 Schematic representation of the 2×2 unit cell structure models of (a) the Mo_3.4V_1.6O₁₄ phase and (b) the Mo_2.7V_2.3O₁₄ phase.

Table S1 Precursor amounts for the synthesis of MoVNbO_x/TiO₂ samples

Table S2 Element analysis of Mo?V?Nb tri-component oxides

Fig. S1 The secondary alcohol units on C_α in the b-O-4 structure of the real lignin.

Fig. S2 Linear fitting diagram of GC internal standard curve (alcohol: 1-phenyl ethanol; internal standard: benzyl alcohol).

Fig. S3 Linear fitting diagram of GC internal standard curve (ketone: 1-acetophenone; internal standard: benzyl alcohol).

Fig. S4 XRD patterns of Mo?V?Nb tri-component oxides without supporter.

Fig. S5 EDS images of Mo_0.61V_0.31Nb_0.08O_x/TiO₂ samples.

Fig. S6 The adsorption?desorption isotherm of TiO₂-supported Mo?V?Nb tri-component oxides.

Table S3 1-Phenyl ethanol conversion of Mo_0.61V_0.31NbO_x catalysts with different Nb contents

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