Abstract

Ni/MCM-41 catalysts were prepared by an impregnation method for acetylene hydrogenation to ethylene based on the calcium carbide acetylene route. X-ray diffraction and transmission electron microscopy indicated that Ni was uniformly dispersed on the support. Temperature-programmed reduction and X-ray photoelectron spectroscopy demonstrated a strong interaction between Ni and MCM-41, and Ni(0) and Ni(ii) coexisted in the catalyst. We optimized the catalytic activity by optimizing the Ni loading and reaction conditions including temperature, space velocity, and hydrogen/acetylene ratio. The acetylene conversion reached 100%, the ethylene selectivity reached 47%. Additionally, we tested the catalyst stability; the acetylene conversion was maintained at 100% for 25.73 h and was then rapidly reduced. ICP, TEM, FT-IR, thermogravimetric analysis and BET were used to investigate the reasons for catalyst deactivation; it was found that green oil deposition on the catalyst surface was the main reason for the catalyst deactivation.

Highlights

  • Ethylene is an important petrochemical raw material, which can be used to synthesize bers, rubber, plastics, and other materials

  • Ni/MCM-41 catalysts were prepared by an impregnation method for acetylene hydrogenation to ethylene based on the calcium carbide acetylene route

  • ICP, Transmission electron microscopy (TEM), Fourier transform infrared spectroscopy (FT-IR), thermogravimetric analysis and BET were used to investigate the reasons for catalyst deactivation; it was found that green oil deposition on the catalyst surface was the main reason for the catalyst deactivation

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Summary

Introduction

Ethylene is an important petrochemical raw material, which can be used to synthesize bers, rubber, plastics, and other materials. To control Ni dispersion, Dai et al.[12] used the metal organic framework ZIF8 to prepare a single-atom Ni/N–C catalyst for acetylene removal from an ethylene-rich stream, with acetylene conversion and ethylene selectivity both exceeding 90%. Green oil must be considered in the pure acetylene hydrogenation reaction, and as far as we know, almost no one has studied the use of a Ni single metal catalyst in the hydrogenation of pure acetylene to ethylene and discussed the effect of reaction conditions on acetylene conversion. In this work, we used amino functionalized MCM41 to immobilize Ni particles on the support prepared a uniformly dispersed Ni/MCM-41 catalyst and mainly studied the effects of Ni loading, and the reaction conditions (temperature, space velocity, hydrogen/acetylene ratio) for hydrogenation of pure acetylene to ethylene. This work provides a strategy for further study of Nibased catalysts for hydrogenation of pure acetylene to ethylene

Catalyst preparation
Catalyst characterization
Catalyst activity test
Results and discussion
Optimization of Ni content and reaction conditions
Catalyst stability test and regenerative capacity
Investigation of catalyst deactivation
Conclusions

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