Journal
JOURNAL OF CATALYSIS
Volume 379, Issue -, Pages 121-128Publisher
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2019.09.022
Keywords
Carbon dioxide; Lower olefins; Magnesium hydride; Hydrogenation; Carbon confinement
Categories
Funding
- National Natural Science Foundation of China [U1804131, U1610103, 21671114]
- SDUST Research Fund [2014TDJH105]
- Scientific & Technological Project of Henan province [182102210431, 182102310897]
- Key Scientific Research Projects in Colleges and Universities of Henan [20B530003]
- Foundation of State Key Laboratory of High-Efficiency Utilization of Coal and Green Chemical Engineering [2018-K32]
- Shenzhen Supercomputer Center
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The direct production of lower olefins from CO2 hydrogenation has attracted enormous attention for its significant roles in mitigating CO2 emissions and developing green chemistry. For the first time, we report carbon-confined MgH2 nano-lamellae storing solid hydrogen for hydrogenation of CO2 to lower olefins. The carbon-confined MgH2 nano-lamellae achieve high selectivity to C-2(-) - C-4(-) species under low H-2/CO2 ratios, which can significantly increase the efficiency of H-2 utilization comparing with traditional methods. DFT calculations show that the lattice H- of MgH2 can combine to the C site of CO2 molecule to form Mg formate, while the aromatic H+ of carbon can combine to the O site of CO2 molecule to form H2O, which both promote the CO2 hydrogenation. The high selectivity of lower olefins is ascribed to the low concentration of solid hydrogen under low H-2/CO2 ratios, by which the Mg formate can be further hydrogenated to lower olefins before fully hydrogenated to saturated hydrocarbons. This novel conversion method for CO2-to-olefins by carbon-confined MgH2 nano-lamellae can inspire the catalysts design for CO2 to value-added chemicals. (C) 2019 Elsevier Inc. All rights reserved.
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