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Open AccessArticle

Effect of Preparation Method on ZrO2-Based Catalysts Performance for Isobutanol Synthesis from Syngas

1
State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China
2
Institute of Molecular Catalysis and Operando Characterization, College of Chemistry, Fuzhou University, Fuzhou 350108, China
3
Department of Applied Chemistry, University of Toyama, Toyama 930-8555, Japan
*
Author to whom correspondence should be addressed.
Catalysts 2019, 9(9), 752; https://doi.org/10.3390/catal9090752
Received: 15 July 2019 / Revised: 31 August 2019 / Accepted: 3 September 2019 / Published: 6 September 2019
Two types of amorphous ZrO2 (am-ZrO2) catalysts were prepared by different co-precipitation/reflux digestion methods (with ethylenediamine and ammonia as the precipitant respectively). Then, copper and potassium were introduced for modifying ZrO2 via an impregnation method to enhance the catalytic performance. The obtained catalysts were further characterized by means of Brunauer-Emmett-Teller surface areas (BET), X-ray diffraction (XRD), H2-temperature-programmed reduction (H2-TPR), and In situ diffuse reflectance infrared spectroscopy (in situ DRIFTS). CO hydrogenation experiments were performed in a fixed-bed reactor for isobutanol synthesis. Great differences were observed on the distribution of alcohols over the two types of ZrO2 catalysts, which were promoted with the same content of Cu and K. The selectivity of isobutanol on K-CuZrO2 (ammonia as precipitant, A-KCZ) was three times higher than that on K-CuZrO2 (ethylenediamine as precipitant, E-KCZ). The characterization results indicated that the A-KCZ catalyst supplied more active hydroxyls (isolated hydroxyls) for anchoring and dispersing Cu. More importantly, it was found that bicarbonate species were formed, which were ascribed as important C1 species for isobutanol formation on the A-KCZ catalyst surface. These C1 intermediates had relatively stronger adsorption strength than those adsorbed on the E-KCZ catalyst, indicating that the bicarbonate species on the A-KCZ catalyst had a longer residence time for further carbon chain growth. Therefore, the selectivity of isobutanol was greatly enhanced. These findings would extend the horizontal of direct alcohols synthesis from syngas. View Full-Text
Keywords: preparation method; ZrO2-based catalysts; syngas; isobutanol preparation method; ZrO2-based catalysts; syngas; isobutanol
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MDPI and ACS Style

Wu, Y.; Tan, L.; Zhang, T.; Xie, H.; Yang, G.; Tsubaki, N.; Chen, J. Effect of Preparation Method on ZrO2-Based Catalysts Performance for Isobutanol Synthesis from Syngas. Catalysts 2019, 9, 752.

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