Modification of Catalytic Properties of Hollandite Manganese Oxide by Ag Intercalation for Oxidative Acetalization of Ethanol to Diethoxyethane

Ding, Jie; Huang, Liang; Ji, Guojing; Zeng, Yuewu; Chen, Zhaoxu; Eddings, Eric G.; Fan, Maohong; Zhong, Qin; Kung, Harold H.

doi:10.1021/acscatal.1c00505

Modification of Catalytic Properties of Hollandite Manganese Oxide by Ag Intercalation for Oxidative Acetalization of Ethanol to Diethoxyethane

Journal Article · Mon Apr 19 00:00:00 EDT 2021 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.1c00505· OSTI ID:2480927

^[1]; ^[2]; Ji, Guojing ^[3]; Zeng, Yuewu ^[4]; ^[5]; Eddings, Eric G. ^[6]; ^[7]; Zhong, Qin ^[8]; ^[9]

Nanjing University of Science and Technology (China); University of Wyoming, Laramie, WY (United States)
Wuhan University of Science and Technology (China)
Nanjing University of Science and Technology, Jiangsu (China)
Zhejiang University (China)
Nanjing University, Jiangsu (China)
University of Utah, Salt Lake City, UT (United States)
University of Wyoming, Laramie, WY (United States); Georgia Institute of Technology, Atlanta, GA (United States)
Nanjing University of Science and Technology (China)
Northwestern University, Evanston, IL (United States)

The effect of addition of Ag to the catalytic properties of hollandite manganese oxide (HMO) was investigated for the oxidative acetalization of ethanol to diethoxyethane. Based on analysis with HRTEM, XRD, and EXAFS, Ag introduced onto HMO by deposition/precipitation was found to be present in different forms in the final catalyst depending on the calcination temperature. It could exist as nanoparticles on the outside surface of HMO nanorods for samples calcined at 60 °C, and as Ag atoms intercalated into the tunnels of the HMO structure for samples calcined at 500 °C. NH₃ desorption results showed that intercalation of Ag resulted in stronger Lewis acidic sites on HMO, which DFT computational results suggested to be due to Ag-induced electron redistribution in the HMO framework. Here, the intercalation of Ag atoms also made the HMO more easily reducible by lowering the H₂ reduction temperature from 500 to 200 °C. Consequently, the sample with intercalated Ag was more active for ethanol oxidation to acetaldehyde, achieving nearly 100% conversion of ethanol and acetaldehyde by 360 °C, and acetalization of acetaldehyde with ethanol to produce diethoxyethane selectively, resulting in 93.5% diethoxyethane yield, which was 10% higher than with samples containing Ag nanoparticles on HMO. This study demonstrated a little-studied phenomenon in which a metal alters the catalytic properties of an oxide electronically but not structurally and without direct participation in the reaction.

View Accepted Manuscript (DOE)

Research Organization:: Northwestern University, Evanston, IL (United States)

Sponsoring Organization:: National Natural Science Foundation of China; National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: FG02-03ER15457

OSTI ID:: 2480927

Alternate ID(s):: OSTI ID: 1849445

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 9 Vol. 11; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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metal intercalation
metal nanoparticles
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Modification of Catalytic Properties of Hollandite Manganese Oxide by Ag Intercalation for Oxidative Acetalization of Ethanol to Diethoxyethane

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