Insights into the mechanism of acetic acid hydrogenation to ethanol on Cu(111) surface
作者： Minhua Zhang , Rui Yao , Haoxi Jiang , Guiming Li , Yifei Chen
DOI: 10.1016/J.APSUSC.2017.03.222
关键词: Acetic acid 、 Organic chemistry 、 Catalysis 、 Acetaldehyde 、 Reaction mechanism 、 Bond cleavage 、 Chemistry 、 Adsorption 、 Ethanol 、 Dissociation (chemistry)
摘要: Abstract Density functional theory (DFT) calculations were employed to theoretically explain the reaction mechanism of acetic acid hydrogenation ethanol on Cu catalyst. The activation barriers key elementary steps and adsorption configurations intermediates involved in Cu(111) surface investigated. results indicated that direct dissociation acetyl (CH3COOH → CH3CO + OH) is rate-determined step. barrier scission energy are two descriptors which could determine conversion acid. might have effects selectivity including: acetaldehyde for O H bond formation C2-oxygenates (CH3CO + H → CH3COH, CH3CHO + H → CH3CHOH CH3CH2O + H → CH3CH2OH). These proposed be used as references design new Cu-based catalysts excellent catalytic performance.
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sci-hub.se 参考文章(41)
Jingbo Wang, Yoshiyuki Kawazoe, Qiang Sun, Siewhwa Chan, Haibin Su, The selectivity and activity of catalyst for CO hydrogenation to methanol and hydrocarbon: A comparative study on Cu, Co and Ni surfaces Surface Science. ,vol. 645, pp. 30- 40 ,(2016) , 10.1016/J.SUSC.2015.10.035
Hannes Jónsson, Theoretical Studies of Atomic-Scale Processes Relevant to Crystal Growth Annual Review of Physical Chemistry. ,vol. 51, pp. 623- 653 ,(2000) , 10.1146/ANNUREV.PHYSCHEM.51.1.623
B. Delley, An all‐electron numerical method for solving the local density functional for polyatomic molecules Journal of Chemical Physics. ,vol. 92, pp. 508- 517 ,(1990) , 10.1063/1.458452
B. Delley, From molecules to solids with the DMol3 approach Journal of Chemical Physics. ,vol. 113, pp. 7756- 7764 ,(2000) , 10.1063/1.1316015
Hakan Olcay, Lijun Xu, Ye Xu, George W. Huber, Aqueous‐Phase Hydrogenation of Acetic Acid over Transition Metal Catalysts Chemcatchem. ,vol. 2, pp. 1420- 1424 ,(2010) , 10.1002/CCTC.201000134
Hakan Olcay, Ye Xu, George W. Huber, Effects of hydrogen and water on the activity and selectivity of acetic acid hydrogenation on ruthenium Green Chemistry. ,vol. 16, pp. 911- 924 ,(2014) , 10.1039/C4GC00011K
P. Ferrin, D. Simonetti, S. Kandoi, E. Kunkes, J. A. Dumesic, J. K. Nørskov, M. Mavrikakis, Modeling ethanol decomposition on transition metals: a combined application of scaling and Brønsted-Evans-Polanyi relations. Journal of the American Chemical Society. ,vol. 131, pp. 5809- 5815 ,(2009) , 10.1021/JA8099322
Xuancheng Sun, Riguang Zhang, Baojun Wang, Insights into the preference of CHx(x = 1–3) formation from CO hydrogenation on Cu(111) surface Applied Surface Science. ,vol. 265, pp. 720- 730 ,(2013) , 10.1016/J.APSUSC.2012.11.091
Jingbo Wang, Xiurong Zhang, Qiang Sun, Siewhwa Chan, Haibin Su, Chain growth mechanism on bimetallic surfaces for higher alcohol synthesis from syngas Catalysis Communications. ,vol. 61, pp. 57- 61 ,(2015) , 10.1016/J.CATCOM.2014.12.010
György Onyestyák, Szabolcs Harnos, Cecília Andrea Badari, Eszter Drotár, Szilvia Klébert, Dénes Kalló, Acetic acid hydroconversion over mono-and bimetallic indium doped catalysts supported on alumina and silicas of various textures Central European Journal of Chemistry. ,vol. 13, ,(2014) , 10.1515/CHEM-2015-0060