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

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

doi:10.1021/jacs.0c09418

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

Journal Article · Thu Oct 22 00:00:00 EDT 2020 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.0c09418· OSTI ID:1775224

^[1]; O’Nolan, Daniel ^[2];

^[3];

^[3]; Chupas, Peter J. ^[2];

^[4];

^[2]

Columbia Univ., New York, NY (United States)
Stony Brook Univ., NY (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Columbia Univ., New York, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)

We achieve a target material state by using a recursive algorithm to control the material reaction based on real-time 6 feedback on the system chemistry from in situ X-ray absorption spectroscopy. Without human intervention, the algorithm controlled 7 O2:H2 gas partial pressures to approach a target average Cu oxidation state of 1+ for γ-Al2O3-supported Cu. This approach 8 represents a new paradigm in autonomation for materials discovery and synthesis optimization; instead of iterating the parameters 9 following the conclusion of each of a series of reactions, the iteration cycle has been scaled down to time points during an individual 10 reaction. Application of the proof-of-concept illustrated here, using a feedback loop to couple in situ material characterization and 11 the reaction conditions via a decision-making algorithm, can be readily envisaged in optimizing and understanding a broad range of 12 chemical systems including catalysts.

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Stony Brook Univ., NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725; SC0019212

OSTI ID:: 1775224

Alternate ID(s):: OSTI ID: 1774330

Journal Information:: Journal of the American Chemical Society, Vol. 142, Issue 44; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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