Journal
JOURNAL OF PHYSICAL CHEMISTRY C
Volume 119, Issue 24, Pages 13758-13766Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.5b03569
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Funding
- National Basic Research Program of China [2011CBA00508]
- Natural Science Foundation of China [21173175, 21303141, 21403178, 21473145]
- Research Fund for the Doctoral Program of Higher Education [20110121130002]
- Fundamental Research Funds for Xiamen University [201412G001]
- Program for Innovative Research Team in Chinese Universities [IRT_14R31]
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Selective hydrogenation of dimethyl oxalate (DMO) derived from syngas to ethylene glycol (EG) over copper (Cu)-based catalysts is an important transformation of modern syngas chemical industry. Methanol, as a product or a solvent, can dissociate on the Cu surfaces by forming adsorbed CO under H-2 atmosphere at 473 K. A small amount of adsorbed CO accelerates Cu redox processes, thus inhibiting catalytic activity with a negative kinetic reaction order. The strong interaction between CO and Cu blocks active sites and disrupts the synergy of Cu+ and Cu-0 species, which are vital in DMO hydrogenation. The Ostwald ripening of Cu crystallites is induced by CO, resulting in aggregation of Cu crystallites. The imbalance of active species and crystallite aggregation lead to deactivation of the Cu catalysts during DMO hydrogenation to EG.
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