Co/Co6Mo6C@C nanoreactors derived from ZIF-67 composite for higher alcohols synthesis

Li, Fuping and Li, Jiaquan and Wang, Kai and Ao, Min and Qiu, Jieshan and Zhang, Xiwang and Wang, Hao and Pham, Gia Hung and Liu, Shaomin (2021) Co/Co6Mo6C@C nanoreactors derived from ZIF-67 composite for higher alcohols synthesis. Composites Part B: Engineering, 209:108608. pp. 1-9. ISSN 1359-8368


Abstract

Direct production of higher alcohols from syngas provides a promising route for the conversion of methane-rich feedstocks into value-added commodity chemicals. However, the rational catalyst design for this process remains a challenge due to severe long-standing sintering problem, low dispersion of active sites and uncontrollable synergism between CO dissociation and CO insertion. Here, we demonstrate the successful development of highly active catalyst for higher alcohols production based on the confined carbonization in metal-organic framework (MOF) matrix. Starting from a compound consisting of cobalt-based MOF host (ZIF-67) and molybdenum-based polyoxometalates guest (H3PMo12O40), Co/Co6Mo6C confined in the carbon matrix is achieved with well-defined morphology and high porosity after carbonation in N2. The Co4.7Mo@C with optimal fraction of Co0 and Co6Mo6C exhibits remarkable performance for higher alcohols synthesis, with a CO conversion of 48% and C2+OH space time yield of 99 mg/gcat.h under 275 °C and 3.0 MPa. Compared to the literature, the developed Co4.7Mo@C catalyst from MOF displayed favourable higher alcohols production rates. The balance of Co0/Co6Mo6C is found to be crucial for the observed reactivity, where Co0 is for CO dissociation and C-C chain growth and Co6Mo6C is highly efficient for CO nondissociative adsorption and CO insertion. Moreover, the synthesized catalyst also displays exceptional stability in a 100 h long-term stability test owing to the uniform dispersion of active centres, demonstrating great potential for large-scale application.


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Item Type: Article (Commonwealth Reporting Category C)
Refereed: Yes
Item Status: Live Archive
Faculty/School / Institute/Centre: Current - Institute for Advanced Engineering and Space Sciences - Centre for Future Materials (1 Jan 2017 -)
Faculty/School / Institute/Centre: Current - Institute for Advanced Engineering and Space Sciences - Centre for Future Materials (1 Jan 2017 -)
Date Deposited: 07 Mar 2022 05:17
Last Modified: 30 Mar 2022 05:13
Uncontrolled Keywords: Bimetallic carbide; Higher alcohols; Metal-organic framework; Synergetic effect; Syngas
Fields of Research (2008): 09 Engineering > 0912 Materials Engineering > 091202 Composite and Hybrid Materials
Fields of Research (2020): 40 ENGINEERING > 4016 Materials engineering > 401602 Composite and hybrid materials
Socio-Economic Objectives (2008): E Expanding Knowledge > 97 Expanding Knowledge > 970109 Expanding Knowledge in Engineering
Socio-Economic Objectives (2020): 28 EXPANDING KNOWLEDGE > 2801 Expanding knowledge > 280110 Expanding knowledge in engineering
Identification Number or DOI: https://doi.org/10.1016/j.compositesb.2021.108608
URI: http://eprints.usq.edu.au/id/eprint/46332

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