Neutron Insights into Sorption Enhanced Methanol Catalysis

Marin Nikolic; Luke Daemen; Anibal J. Ramirez-Cuesta; Rafael Balderas Xicohtencatl; Yongqiang Cheng; Seth T. Putnam; Nicholas P. Stadie; Xiaochun Liu; Jasmin Terreni; Andreas Borgschulte

doi:10.1007/s11244-021-01461-w

Neutron Insights into Sorption Enhanced Methanol Catalysis

Marin Nikolic, Luke Daemen, Anibal J. Ramirez-Cuesta, Rafael Balderas Xicohtencatl, Yongqiang Cheng, Seth T. Putnam, Nicholas P. Stadie, Xiaochun Liu, Jasmin Terreni, Andreas Borgschulte

Research output: Contribution to journal › Article › peer-review

4 Scopus citations

Abstract

Sorption enhanced methanol production makes use of the equilibrium shift of the CO ₂ hydrogenation reaction towards the desired products. However, the increased complexity of the catalyst system leads to additional reactions and thus side products such as dimethyl ether, and complicates the analysis of the reaction mechanism. On the other hand, the unusually high concentration of intermediates and products in the sorbent facilitates the use of inelastic neutron scattering (INS) spectroscopy. Despite being a post-mortem method, the INS data revealed the change of the reaction path during sorption catalysis. Concretely, the experiments indicate that the varying water partial pressure due to the adsorption saturation of the zeolite sorbent influences the progress of the reaction steps in which water is involved. Experiments with model catalysts support the INS findings.

Original language	English
Pages (from-to)	638-643
Number of pages	6
Journal	Topics in Catalysis
Volume	64
Issue number	9-12
DOIs	https://doi.org/10.1007/s11244-021-01461-w
State	Published - Aug 2021
Externally published	Yes

Funding

This research benefited from the use of the VISION beamline (IPTS-16527) at the Spallation Neutron Source, Oak Ridge National Laboratory (ORNL), which is supported by the Scientific User Facilities Division, Office of Basic Energy Sciences, US Department of Energy (DOE). This work was partly supported by the UZH-UFSP program LightChEC. Financial support from the Swiss National Science Foundation (Grant Number 172662) is greatly acknowledged.

Funders	Funder number
Scientific User Facilities Division
UZH-UFSP
U.S. Department of Energy
Basic Energy Sciences
Oak Ridge National Laboratory
Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung	172662

Keywords

CO hydrogenation
Dimethyl ether
Inelastic neutron scattering
Methanol
Sorption enhanced catalysis

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1007/s11244-021-01461-w

Cite this

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title = "Neutron Insights into Sorption Enhanced Methanol Catalysis",

abstract = "Sorption enhanced methanol production makes use of the equilibrium shift of the CO 2 hydrogenation reaction towards the desired products. However, the increased complexity of the catalyst system leads to additional reactions and thus side products such as dimethyl ether, and complicates the analysis of the reaction mechanism. On the other hand, the unusually high concentration of intermediates and products in the sorbent facilitates the use of inelastic neutron scattering (INS) spectroscopy. Despite being a post-mortem method, the INS data revealed the change of the reaction path during sorption catalysis. Concretely, the experiments indicate that the varying water partial pressure due to the adsorption saturation of the zeolite sorbent influences the progress of the reaction steps in which water is involved. Experiments with model catalysts support the INS findings.",

keywords = "CO hydrogenation, Dimethyl ether, Inelastic neutron scattering, Methanol, Sorption enhanced catalysis",

author = "Marin Nikolic and Luke Daemen and Ramirez-Cuesta, {Anibal J.} and Xicohtencatl, {Rafael Balderas} and Yongqiang Cheng and Putnam, {Seth T.} and Stadie, {Nicholas P.} and Xiaochun Liu and Jasmin Terreni and Andreas Borgschulte",

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doi = "10.1007/s11244-021-01461-w",

language = "English",

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T1 - Neutron Insights into Sorption Enhanced Methanol Catalysis

AU - Nikolic, Marin

AU - Daemen, Luke

AU - Ramirez-Cuesta, Anibal J.

AU - Xicohtencatl, Rafael Balderas

AU - Cheng, Yongqiang

AU - Putnam, Seth T.

AU - Stadie, Nicholas P.

AU - Liu, Xiaochun

AU - Terreni, Jasmin

AU - Borgschulte, Andreas

PY - 2021/8

Y1 - 2021/8

N2 - Sorption enhanced methanol production makes use of the equilibrium shift of the CO 2 hydrogenation reaction towards the desired products. However, the increased complexity of the catalyst system leads to additional reactions and thus side products such as dimethyl ether, and complicates the analysis of the reaction mechanism. On the other hand, the unusually high concentration of intermediates and products in the sorbent facilitates the use of inelastic neutron scattering (INS) spectroscopy. Despite being a post-mortem method, the INS data revealed the change of the reaction path during sorption catalysis. Concretely, the experiments indicate that the varying water partial pressure due to the adsorption saturation of the zeolite sorbent influences the progress of the reaction steps in which water is involved. Experiments with model catalysts support the INS findings.

AB - Sorption enhanced methanol production makes use of the equilibrium shift of the CO 2 hydrogenation reaction towards the desired products. However, the increased complexity of the catalyst system leads to additional reactions and thus side products such as dimethyl ether, and complicates the analysis of the reaction mechanism. On the other hand, the unusually high concentration of intermediates and products in the sorbent facilitates the use of inelastic neutron scattering (INS) spectroscopy. Despite being a post-mortem method, the INS data revealed the change of the reaction path during sorption catalysis. Concretely, the experiments indicate that the varying water partial pressure due to the adsorption saturation of the zeolite sorbent influences the progress of the reaction steps in which water is involved. Experiments with model catalysts support the INS findings.

KW - CO hydrogenation

KW - Dimethyl ether

KW - Inelastic neutron scattering

KW - Methanol

KW - Sorption enhanced catalysis

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DO - 10.1007/s11244-021-01461-w

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SN - 1022-5528

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JO - Topics in Catalysis

JF - Topics in Catalysis

IS - 9-12

ER -

Neutron Insights into Sorption Enhanced Methanol Catalysis

Abstract

Funding

Keywords

UN SDGs

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