title: Complex structural dynamics of nanocatalysts revealed in Operando conditions by correlated imaging and spectroscopy probes.
abstract: Understanding how heterogeneous catalysts change size, shape and structure during chemical reactions is limited by the paucity of methods for studying catalytic ensembles in working state, that is, in operando conditions. Here by a correlated use of synchrotron X-ray absorption spectroscopy and scanning transmission electron microscopy in operando conditions, we quantitatively describe the complex structural dynamics of supported Pt catalysts exhibited during an exemplary catalytic reaction-ethylene hydrogenation. This work exploits a microfabricated catalytic reactor compatible with both probes. The results demonstrate dynamic transformations of the ensemble of Pt clusters that spans a broad size range throughout changing reaction conditions. This method is generalizable to quantitative operando studies of complex systems using a wide variety of X-ray and electron-based experimental probes.
authors.affiliation: Department of Physics, Yeshiva University, New York, New York 10016, USA.
authors.forename: Y
authors.initials: Y
authors.lastname: Li
authors.affiliation: Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York 11973, USA.
authors.forename: D
authors.initials: D
authors.lastname: Zakharov
authors.affiliation: Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York 11973, USA.|Department of Chemistry, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, USA.
authors.forename: S
authors.initials: S
authors.lastname: Zhao
authors.affiliation: Photon Sciences Division, Brookhaven National Laboratory, Upton, New York 11973, USA.
authors.forename: R
authors.initials: R
authors.lastname: Tappero
authors.affiliation: Department of Chemistry, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, USA.
authors.forename: U
authors.initials: U
authors.lastname: Jung
authors.affiliation: Department of Chemistry, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, USA.
authors.forename: A
authors.initials: A
authors.lastname: Elsen
authors.affiliation: Department of Physics, Yeshiva University, New York, New York 10016, USA.
authors.forename: Ph
authors.initials: P
authors.lastname: Baumann
authors.affiliation: Department of Chemistry, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, USA.|School of Chemical Science and Engineering, KTH Royal Institute of Technology, Stockholm 10044, Sweden.
authors.forename: R G
authors.initials: RG
authors.lastname: Nuzzo
authors.affiliation: Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York 11973, USA.
authors.forename: E A
authors.initials: EA
authors.lastname: Stach
authors.affiliation: Department of Physics, Yeshiva University, New York, New York 10016, USA.
authors.forename: A I
authors.initials: AI
authors.lastname: Frenkel