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.
N1 - Funding Information:
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.
Publisher Copyright:
© 2020 American Chemical Society.
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 -