Highly Selective Heterogeneous Ethylene Dimerization with a Scalable and Chemically Robust MOF Catalyst
| Autor: | Robert J. Comito, Wei Xu, Jeffrey T. Miller, Mircea Dincă, Guanghui Zhang, Eric D. Metzger, Romain J.-C. Dubey, Zhenwei Wu |
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| Rok vydání: | 2019 |
| Předmět: |
Olefin fiber
X-ray absorption spectroscopy Ethylene Absorption spectroscopy Renewable Energy Sustainability and the Environment Chemistry General Chemical Engineering 1-Butene 02 engineering and technology General Chemistry 010402 general chemistry 021001 nanoscience & nanotechnology Heterogeneous catalysis 01 natural sciences Combinatorial chemistry 0104 chemical sciences Catalysis chemistry.chemical_compound Environmental Chemistry 0210 nano-technology Selectivity |
| Zdroj: | ACS Sustainable Chemistry & Engineering. 7:6654-6661 |
| ISSN: | 2168-0485 |
| DOI: | 10.1021/acssuschemeng.8b05703 |
| Popis: | Metal–organic frameworks (MOFs) hold great promise as structurally tunable catalysts capable of high selectivity in the solid state, yet their comparatively high cost and often limited stability remain significant concerns for their commercialization as heterogeneous catalysts. Here, we report detailed X-ray absorption spectroscopy studies of Co- and Ni-MFU-4l, a class of highly selective MOF catalysts for olefin upgrading, and reveal mechanisms that lead to their deactivation. We further show that Ni-CFA-1, a more scalable and economical alternative to Ni-MFU-4l, reproduces both the local coordination structure and the high selectivity of the latter in ethylene dimerization catalysis. Under optimal conditions, Ni-CFA-1 activated by MMAO-12 achieves a turnover frequency of 37100 per hour and a selectivity of 87.1% for 1-butene, a combination of activity, selectivity, and affordability that is unmatched among heterogeneous ethylene dimerization catalysts. Ni-CFA-1 retains its high activity for at least 12 ... |
| Databáze: | OpenAIRE |
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