In Situ 3D Imaging of Catalysis Induced Strain in Gold Nanoparticles

Journal Article · Thu Aug 04 00:00:00 EDT 2016 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.6b01038· OSTI ID:1330099

Ulvestad, Andrew; Sasikumar, Kiran; Kim, Jong Woo; Harder, Ross; Maxey, Evan; Clark, Jesse N.; Narayanan, Badri; Deshmukh, Sanket A.; Ferrier, Nicola; Mulvaney, Paul; Sankaranarayanan, Subramanian K. R. S.; Shpyrko, Oleg G.

Multielectron transfer processes are crucially important in energy and biological science but require favorable catalysts to achieve fast kinetics. Nanostructuring catalysts can dramatically improve their properties, which can be difficult to understand due to strain- and size-dependent thermodynamics, the influence of defects, and substrate-dependent activities. Here, we report three-dimensional (3D) imaging of single gold nanoparticles during catalysis of ascorbic acid decomposition using Bragg coherent diffractive imaging (BCDI). Local strains were measured in single nanoparticles and modeled using reactive molecular dynamics (RMD) simulations and finite element analysis (FEA) simulations. RMD reveals the pathway for local strain generation in the gold lattice: chemisorption of hydroxyl ions. FEA reveals that the RMD results are transferable to the nanocrystal sizes studied in the experiment. Our study probes the strain-activity connection and opens a powerful avenue for theoretical and experimental studies of nanocrystal catalysis.

• Research Organization: Argonne National Lab. (ANL), Argonne, IL (United States)
• Sponsoring Organization: USDOE Office of Science (SC), Basic Energy Sciences (BES)
• DOE Contract Number: AC02-06CH11357
• OSTI ID: 1330099
• Journal Information: Journal of Physical Chemistry Letters, Vol. 7, Issue 15; ISSN 1948-7185
• Publisher: American Chemical Society
• Country of Publication: United States
• Language: English