Green Chemistry p. 197 - 206 (2018)
Update date:2022-08-11
Topics:
Zhang, Zihao
Yang, Qiwei
Chen, Hao
Chen, Kequan
Lu, Xiuyang
Ouyang, Pingkai
Fu, Jie
Chen, Jingguang G.
In this work, supported Cu-Ni bimetallic catalysts were synthesized and evaluated for the in situ hydrogenation and decarboxylation of oleic acid using methanol as a hydrogen donor. The supported Cu-Ni alloy exhibited a significant improvement in both activity and selectivity towards the production of heptadecane in comparison with monometallic Cu and Ni based catalysts. The formation of the Cu-Ni alloy is demonstrated by high-angle annular dark-field scanning transmission electron microscopy (HADDF-STEM), energy dispersive X-ray spectroscopy (EDS-mapping), X-ray diffraction (XRD) and temperature programmed reduction (TPR). A partially oxidized Cu in the Cu-Ni alloy is revealed by diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) following CO adsorption and X-ray photoelectron spectroscopy (XPS). The temperature programmed desorption of ethylene and propane (ethylene/propane-TPD) suggested that the formation of the Cu-Ni alloy inhibited the cracking of C-C bonds compared to Ni, and remarkably increased the selectivity to heptadecane. The temperature programmed desorption of acetic acid (acetic acid-TPD) indicated that the bimetallic Cu-Ni alloy and Ni catalysts had a stronger adsorption of acetic acid than that of the Cu catalyst. The formation of the Cu-Ni alloy and a partially oxidized Cu facilitates the decarboxylation reaction and inhibits the cracking reaction of C-C bonds, leading to enhanced catalytic activity and selectivity.
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