Surface Structure Dependence of the Dry Dehydrogenation of Alcohols on Cu(111) and Cu(110)

Wang, Zhi-Tao; Xu, Yunfei; El-Soda, Mostafa; Lucci, Felicia R.; Madix, Robert J.; Friend, Cynthia M.; Sykes, E. Charles H.

doi:10.1021/acs.jpcc.7b02957

Surface Structure Dependence of the Dry Dehydrogenation of Alcohols on Cu(111) and Cu(110)

Journal Article · Tue May 23 00:00:00 EDT 2017 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.7b02957· OSTI ID:1388884

Wang, Zhi-Tao ^[1]; Xu, Yunfei ^[2]; El-Soda, Mostafa ^[3]; Lucci, Felicia R. ^[3]; Madix, Robert J. ^[2]; ^[2]; ^[3]

Tufts Univ., Medford, MA (United States); Harvard Univ., Cambridge, MA (United States)
Harvard Univ., Cambridge, MA (United States)
Tufts Univ., Medford, MA (United States)

The non-oxidative dehydrogenation of alcohols is considered as an important method to produce aldehydes for the chemical industry and hydrogen gas. However, current industrial processes are oxidative, meaning that the aldehydes are formed along with water, which, in addition to being less energy efficient, poses separation problems. Herein the production of aldehydes from methanol and ethanol on clean and dry Cu(111) and Cu(110) surfaces was investigated in order to understand the catalytic anhydrous dehydrogenation of alcohols. We report both ethanol and methanol preferentially react under ultrahigh vacuum conditions at surface defects to yield acetaldehyde and formaldehyde, respectively, in the absence of surface oxygen and water. The amount of alkoxide reaction intermediates measured by scanning tunneling microscopy, and aldehyde and hydrogen products detected by temperature programmed reaction, are increased by inducing more defects in the Cu substrates with Ar ion sputtering. This work also reveals that the Cu model surfaces are not poisoned by the reaction and exhibit 100% selectivity for alcohol dehydrogenation to aldehyde and hydrogen.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0012573

OSTI ID:: 1388884

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 23 Vol. 121; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited By (3)

First-Principle Microkinetic Modeling of Ethanol Dehydrogenation on Metal Catalyst Surfaces in Non-oxidative Environment: Design of Bimetallic Alloys Khan, Tuhin S.; Jalid, Fatima; Haider, M. Ali Topics in Catalysis, Vol. 61, Issue 18-19 https://doi.org/10.1007/s11244-018-1028-9	journal	August 2018
Acceptorless dehydrogenative coupling reactions with alcohols over heterogeneous catalysts Hakim Siddiki, S. M. A.; Toyao, Takashi; Shimizu, Ken-ichi Green Chemistry, Vol. 20, Issue 13 https://doi.org/10.1039/c8gc00451j	journal	January 2018
An AIMD study of dissociative chemisorption of methanol on Cu(111) with implications for formaldehyde formation Gerrits, Nick; Kroes, Geert-Jan The Journal of Chemical Physics, Vol. 150, Issue 2 https://doi.org/10.1063/1.5070129	journal	January 2019

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