不同助剂对Ni/Al2O3催化顺酐液相加氢选择性的影响

doi:10.19964/j.issn.1006-4990.2023-0417

Abstract

Abstract:

A series of nickel-based maleic anhydride hydrogenation catalysts were prepared by ultrasound-assisted precipitation method using P，Mg，Mo，and Cu additives，respectively.The catalysts were characterized and analyzed by N₂ physical adsorption-desorption，X-ray diffraction（XRD），programmed temperature-raising reduction（H₂-TPR），and ammonia-programmed temperature-raising desorption（NH₃-TPD），to investigate the effects of different additives on the crystalline structure of the catalysts，the reduction performance，acid strength，BET specific surface area and pore structure.The results showed that the additives were highly dispersed in the catalyst system，while the introduction of the additives caused the specific surface area and pore volume of the catalysts to show different degrees of reduction.In addition，the additives increased the reduction temperature of the catalysts and enhanced the interaction force between the active metals and the carriers，which led to the different degrees of reduction of the catalysts，and resulted in different numbers of Ni⁰ and Ni^δ+ with the characteristics of L-acid，which in turn affected the hydrogen activation and the adsorption capacity of the C=C/C=O bonds.The performance of the catalyst was evaluated using a fixed-bed maleic anhydride liquid-phase continuous hydrogenation reaction，and it was found that the Ni-Mo/Al₂O₃ catalyst had the optimal γ-butyrolactone selectivity.Under the process conditions of reaction pressure of 5 MPa，reaction temperature of 150 ℃，molar ratio of 5∶1 for hydrogen anhydride，and space velocity of 1 h^-1，the conversion rate of maleic anhydride was ≥99.5%，the selectivity of γ-butyrolactone was ≥54.34%.

Key words: reagent, Ni/Al₂O₃, maleic anhydride, hydrogenation, γ-butyrolactone

CLC Number:

O643.36

ZHU Jinjian, YANG Xiaxia, MU Zhanpeng, SONG Guoliang, LI Zihan, LIU Wei, XU Yan, ZHANG Jingcheng. Effect of different additives on liquid phase selective hydrogenation performance of maleic anhydride over Ni/Al₂O₃[J]. Inorganic Chemicals Industry, 2024, 56(4): 143-150.

Figures/Tables 11

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催化剂	颗粒尺寸/nm
催化剂	Ni ⁰ （200）	Ni ⁰ （220）	平均颗粒尺寸
Ni/Al₂O₃	6.0	12.8	9.4
Ni-Mg/Al₂O₃	11.4	11.1	11.25
Ni-P/Al₂O₃	5.4	10.2	7.8
Ni-Mo/Al₂O₃	5.7	7.4	6.55
Ni-Cu/Al₂O₃	12.3	8.3	10.3

催化剂	比表面积/（m²·g^-1）	孔容/（cm³·g^-1）	孔径/nm
Ni/Al₂O₃	262	0.42	6.4
Ni-Cu/Al₂O₃	226	0.36	6.4
Ni-Mo/Al₂O₃	262	0.37	5.6
Ni-P/Al₂O₃	182	0.28	6.2
Ni-Mg/Al₂O₃	225	0.37	6.6

催化剂	顺酐转化率/%	丁二酸酐选择性/%	γ-丁内酯选择性/%	其他产物选择性/%
Ni/Al₂O₃	97.30	12.95	45.19	41.86
Ni-Cu/Al₂O₃	99.88	30.49	42.82	26.69
Ni-Mo/Al₂O₃	99.48	18.87	54.34	26.79
Ni-P/Al₂O₃	98.79	73.75	18.59	7.66
Ni-Mg/Al₂O₃	98.34	34.55	41.67	23.78

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Effect of different additives on liquid phase selective hydrogenation performance of maleic anhydride over Ni/Al₂O₃

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Effect of different additives on liquid phase selective hydrogenation performance of maleic anhydride over Ni/Al2O3