A high precision gas flow cell for performing in situ neutron studies of local atomic structure in catalytic materials

Daniel Olds; Katharine Page; Arnold Paecklar; Peter F. Peterson; Jue Liu; Gerald Rucker; Mariano Ruiz-Rodriguez; Michael Olsen; Michelle Pawel; Steven H. Overbury; James R. Neilson

doi:10.1063/1.4978287

A high precision gas flow cell for performing in situ neutron studies of local atomic structure in catalytic materials

Daniel Olds, Katharine Page, Arnold Paecklar, Peter F. Peterson, Jue Liu, Gerald Rucker, Mariano Ruiz-Rodriguez, Michael Olsen, Michelle Pawel, Steven H. Overbury, James R. Neilson

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

9 Scopus citations

Abstract

Gas-solid interfaces enable a multitude of industrial processes, including heterogeneous catalysis; however, there are few methods available for studying the structure of this interface under operating conditions. Here, we present a new sample environment for interrogating materials under gas-flow conditions using time-of-flight neutron scattering under both constant and pulse probe gas flow. Outlined are descriptions of the gas flow cell and a commissioning example using the adsorption of N₂ by Ca-exchanged zeolite-X (Na_78−2xCa_xAl₇₈Si₁₄₄O₃₈₄,x ≈ 38). We demonstrate sensitivities to lattice contraction and N₂ adsorption sites in the structure, with both static gas loading and gas flow. A steady-state isotope transient kinetic analysis of N₂ adsorption measured simultaneously with mass spectrometry is also demonstrated. In the experiment, the gas flow through a plugged-flow gas-solid contactor is switched between N215 and N214 isotopes at a temperature of 300 K and a constant pressure of 1 atm; the gas flow and mass spectrum are correlated with the structure factor determined from event-based neutron total scattering. Available flow conditions, sample considerations, and future applications are discussed.

Original language	English
Article number	034101
Journal	Review of Scientific Instruments
Volume	88
Issue number	3
DOIs	https://doi.org/10.1063/1.4978287
State	Published - Mar 1 2017
Externally published	Yes

Funding

This work was primarily supported under the Department of Energy’s Office of Basic Energy Sciences and the Laboratory Directed Research and Development (LDRD) Program at Oak Ridge National Laboratory (LDRD Seed No. 7735). The presented analysis of neutron powder diffraction data was funded by the BES Early Career Award: Exploiting Small Signatures: Quantifying Nanoscale Structure and Behavior KC04062, under Contract No. DE-AC05-00OR22725. The data presented were measured on the Nanoscale-Ordered Materials Diffractometer (NOMAD) instrument at the Spallation Neutron Source at ORNL. Some samples were prepared and additional characterization was performed at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility. The authors acknowledge and thank Genevieve Martin for contributing the photography used in Figure 2.

Funders	Funder number
Center for Nanophase Materials Sciences
U.S. Department of Energy
Office of Science
Basic Energy Sciences	DE-AC05-00OR22725, KC04062
Oak Ridge National Laboratory	7735
Laboratory Directed Research and Development

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title = "A high precision gas flow cell for performing in situ neutron studies of local atomic structure in catalytic materials",

abstract = "Gas-solid interfaces enable a multitude of industrial processes, including heterogeneous catalysis; however, there are few methods available for studying the structure of this interface under operating conditions. Here, we present a new sample environment for interrogating materials under gas-flow conditions using time-of-flight neutron scattering under both constant and pulse probe gas flow. Outlined are descriptions of the gas flow cell and a commissioning example using the adsorption of N2 by Ca-exchanged zeolite-X (Na78−2xCaxAl78Si144O384,x ≈ 38). We demonstrate sensitivities to lattice contraction and N2 adsorption sites in the structure, with both static gas loading and gas flow. A steady-state isotope transient kinetic analysis of N2 adsorption measured simultaneously with mass spectrometry is also demonstrated. In the experiment, the gas flow through a plugged-flow gas-solid contactor is switched between N215 and N214 isotopes at a temperature of 300 K and a constant pressure of 1 atm; the gas flow and mass spectrum are correlated with the structure factor determined from event-based neutron total scattering. Available flow conditions, sample considerations, and future applications are discussed.",

author = "Daniel Olds and Katharine Page and Arnold Paecklar and Peterson, {Peter F.} and Jue Liu and Gerald Rucker and Mariano Ruiz-Rodriguez and Michael Olsen and Michelle Pawel and Overbury, {Steven H.} and Neilson, {James R.}",

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T1 - A high precision gas flow cell for performing in situ neutron studies of local atomic structure in catalytic materials

AU - Olds, Daniel

AU - Page, Katharine

AU - Paecklar, Arnold

AU - Peterson, Peter F.

AU - Liu, Jue

AU - Rucker, Gerald

AU - Ruiz-Rodriguez, Mariano

AU - Olsen, Michael

AU - Pawel, Michelle

AU - Overbury, Steven H.

AU - Neilson, James R.

PY - 2017/3/1

Y1 - 2017/3/1

N2 - Gas-solid interfaces enable a multitude of industrial processes, including heterogeneous catalysis; however, there are few methods available for studying the structure of this interface under operating conditions. Here, we present a new sample environment for interrogating materials under gas-flow conditions using time-of-flight neutron scattering under both constant and pulse probe gas flow. Outlined are descriptions of the gas flow cell and a commissioning example using the adsorption of N2 by Ca-exchanged zeolite-X (Na78−2xCaxAl78Si144O384,x ≈ 38). We demonstrate sensitivities to lattice contraction and N2 adsorption sites in the structure, with both static gas loading and gas flow. A steady-state isotope transient kinetic analysis of N2 adsorption measured simultaneously with mass spectrometry is also demonstrated. In the experiment, the gas flow through a plugged-flow gas-solid contactor is switched between N215 and N214 isotopes at a temperature of 300 K and a constant pressure of 1 atm; the gas flow and mass spectrum are correlated with the structure factor determined from event-based neutron total scattering. Available flow conditions, sample considerations, and future applications are discussed.

AB - Gas-solid interfaces enable a multitude of industrial processes, including heterogeneous catalysis; however, there are few methods available for studying the structure of this interface under operating conditions. Here, we present a new sample environment for interrogating materials under gas-flow conditions using time-of-flight neutron scattering under both constant and pulse probe gas flow. Outlined are descriptions of the gas flow cell and a commissioning example using the adsorption of N2 by Ca-exchanged zeolite-X (Na78−2xCaxAl78Si144O384,x ≈ 38). We demonstrate sensitivities to lattice contraction and N2 adsorption sites in the structure, with both static gas loading and gas flow. A steady-state isotope transient kinetic analysis of N2 adsorption measured simultaneously with mass spectrometry is also demonstrated. In the experiment, the gas flow through a plugged-flow gas-solid contactor is switched between N215 and N214 isotopes at a temperature of 300 K and a constant pressure of 1 atm; the gas flow and mass spectrum are correlated with the structure factor determined from event-based neutron total scattering. Available flow conditions, sample considerations, and future applications are discussed.

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A high precision gas flow cell for performing in situ neutron studies of local atomic structure in catalytic materials

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