Active Reaction Control of Cu Redox State Based on Real-Time Feedback from in Situ Synchrotron Measurements

Yevgeny Rakita; Daniel O'Nolan; Rebecca D. McAuliffe; Gabriel M. Veith; Peter J. Chupas; Simon J.L. Billinge; Karena W. Chapman

doi:10.1021/jacs.0c09418

Active Reaction Control of Cu Redox State Based on Real-Time Feedback from in Situ Synchrotron Measurements

Yevgeny Rakita, Daniel O'Nolan, Rebecca D. McAuliffe, Gabriel M. Veith, Peter J. Chupas, Simon J.L. Billinge, Karena W. Chapman

Energy Storage & Conversion

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

10 Scopus citations

Abstract

We achieve a target material state by using a recursive algorithm to control the material reaction based on real-time feedback on the system chemistry from in situ X-ray absorption spectroscopy. Without human intervention, the algorithm controlled O2:H2 gas partial pressures to approach a target average Cu oxidation state of 1+ for γ-Al2O3-supported Cu. This approach represents a new paradigm in autonomation for materials discovery and synthesis optimization; instead of iterating the parameters following the conclusion of each of a series of reactions, the iteration cycle has been scaled down to time points during an individual reaction. Application of the proof-of-concept illustrated here, using a feedback loop to couple in situ material characterization and the reaction conditions via a decision-making algorithm, can be readily envisaged in optimizing and understanding a broad range of systems including catalysis.

Original language	English
Pages (from-to)	18758-18762
Number of pages	5
Journal	Journal of the American Chemical Society
Volume	142
Issue number	44
DOIs	https://doi.org/10.1021/jacs.0c09418
State	Published - Nov 4 2020

Funding

This work was supported as part of GENESIS: A Next Generation Synthesis Center, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award Number DE-SC0019212. This research used beamline 9-BM of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. Parts of the research were performed at Oak Ridge National Laboratory (ORNL), managed by UT Battelle, LLC for the U.S. Department of Energy (DOE) under contract DE-AC05-00OR22725. We thank George Sterbinsky for support in using the 9-BM beamline.

Funders	Funder number
U.S. Department of Energy
Office of Science
Basic Energy Sciences	DE-SC0019212
Argonne National Laboratory	DE-AC02-06CH11357
Oak Ridge National Laboratory
UT-Battelle	DE-AC05-00OR22725

Access to Document

10.1021/jacs.0c09418

Cite this

@article{e586fc22543f4859aa33a6b1c5c5a6bc,

title = "Active Reaction Control of Cu Redox State Based on Real-Time Feedback from in Situ Synchrotron Measurements",

abstract = "We achieve a target material state by using a recursive algorithm to control the material reaction based on real-time feedback on the system chemistry from in situ X-ray absorption spectroscopy. Without human intervention, the algorithm controlled O2:H2 gas partial pressures to approach a target average Cu oxidation state of 1+ for γ-Al2O3-supported Cu. This approach represents a new paradigm in autonomation for materials discovery and synthesis optimization; instead of iterating the parameters following the conclusion of each of a series of reactions, the iteration cycle has been scaled down to time points during an individual reaction. Application of the proof-of-concept illustrated here, using a feedback loop to couple in situ material characterization and the reaction conditions via a decision-making algorithm, can be readily envisaged in optimizing and understanding a broad range of systems including catalysis.",

author = "Yevgeny Rakita and Daniel O'Nolan and McAuliffe, {Rebecca D.} and Veith, {Gabriel M.} and Chupas, {Peter J.} and Billinge, {Simon J.L.} and Chapman, {Karena W.}",

note = "Publisher Copyright: {\textcopyright} 2020 American Chemical Society.",

year = "2020",

month = nov,

day = "4",

doi = "10.1021/jacs.0c09418",

language = "English",

volume = "142",

pages = "18758--18762",

journal = "Journal of the American Chemical Society",

issn = "0002-7863",

publisher = "American Chemical Society",

number = "44",

}

TY - JOUR

T1 - Active Reaction Control of Cu Redox State Based on Real-Time Feedback from in Situ Synchrotron Measurements

AU - Rakita, Yevgeny

AU - O'Nolan, Daniel

AU - McAuliffe, Rebecca D.

AU - Veith, Gabriel M.

AU - Chupas, Peter J.

AU - Billinge, Simon J.L.

AU - Chapman, Karena W.

PY - 2020/11/4

Y1 - 2020/11/4

N2 - We achieve a target material state by using a recursive algorithm to control the material reaction based on real-time feedback on the system chemistry from in situ X-ray absorption spectroscopy. Without human intervention, the algorithm controlled O2:H2 gas partial pressures to approach a target average Cu oxidation state of 1+ for γ-Al2O3-supported Cu. This approach represents a new paradigm in autonomation for materials discovery and synthesis optimization; instead of iterating the parameters following the conclusion of each of a series of reactions, the iteration cycle has been scaled down to time points during an individual reaction. Application of the proof-of-concept illustrated here, using a feedback loop to couple in situ material characterization and the reaction conditions via a decision-making algorithm, can be readily envisaged in optimizing and understanding a broad range of systems including catalysis.

AB - We achieve a target material state by using a recursive algorithm to control the material reaction based on real-time feedback on the system chemistry from in situ X-ray absorption spectroscopy. Without human intervention, the algorithm controlled O2:H2 gas partial pressures to approach a target average Cu oxidation state of 1+ for γ-Al2O3-supported Cu. This approach represents a new paradigm in autonomation for materials discovery and synthesis optimization; instead of iterating the parameters following the conclusion of each of a series of reactions, the iteration cycle has been scaled down to time points during an individual reaction. Application of the proof-of-concept illustrated here, using a feedback loop to couple in situ material characterization and the reaction conditions via a decision-making algorithm, can be readily envisaged in optimizing and understanding a broad range of systems including catalysis.

UR - http://www.scopus.com/inward/record.url?scp=85095667554&partnerID=8YFLogxK

U2 - 10.1021/jacs.0c09418

DO - 10.1021/jacs.0c09418

M3 - Article

C2 - 33090780

AN - SCOPUS:85095667554

SN - 0002-7863

VL - 142

SP - 18758

EP - 18762

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

IS - 44

ER -

Active Reaction Control of Cu Redox State Based on Real-Time Feedback from in Situ Synchrotron Measurements

Abstract

Funding

Access to Document

Other files and links

Fingerprint

Cite this