Deciphering nanoconfinement effects on molecular orientation and reaction intermediate by single molecule imaging

Dong, Bin; Pei, Yuchen; Mansour, Nourhan; Lu, Xuemei; Yang, Kai; Huang, Wenyu; Fang, Ning

doi:10.1038/s41467-019-12799-x

Title: Deciphering nanoconfinement effects on molecular orientation and reaction intermediate by single molecule imaging

Journal Article · 23 October 2019 · Nature Communications

DOI: https://doi.org/10.1038/s41467-019-12799-x · OSTI ID:1624206

Dong, Bin ^[1];

^[2]; Mansour, Nourhan ^[3]; Lu, Xuemei ^[4]; Yang, Kai ^[5];

^[2]; Fang, Ning ^[3]

Georgia State Univ., Atlanta, GA (United States). Dept. of Chemistry
Iowa State Univ., Ames, IA (United States) and Ames Lab., Ames, IA (United States). Dept. of Chemistry
Georgia State Univ., Atlanta, GA (United States). Dept. of Chemistry
Soochow University, Suzhou (China). Center for Soft Condensed Matter Physics and Interdisciplinary Research & School of Physical Science and Technology
Soochow University, Suzhou (China). Center for Soft Condensed Matter Physics and Interdisciplinary Research & School of Physical Science and Technology

Nanoconfinement could dramatically change molecular transport and reaction kinetics in heterogeneous catalysis. Here we specifically design a core-shell nanocatalyst with aligned linear nanopores for single-molecule studies of the nanoconfinement effects. The quantitative single-molecule measurements reveal unusual lower adsorption strength and higher catalytic activity on the confined metal reaction centres within the nanoporous structure. More surprisingly, the nanoconfinement effects on enhanced catalytic activity are larger for catalysts with longer and narrower nanopores. Experimental evidences, including molecular orientation, activation energy, and intermediate reactive species, have been gathered to provide a molecular level explanation on how the nanoconfinement effects enhance the catalyst activity, which is essential for the rational design of highly-efficient catalysts.

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Research Organization:: Ames Laboratory (AMES), Ames, IA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-07CH11358

OSTI ID:: 1624206

Journal Information:: Nature Communications, Vol. 10, Issue 1; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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High-Resolution Single-Turnover Mapping Reveals Intraparticle Diffusion Limitation in Ti-MCM-41-Catalyzed Epoxidation De Cremer, Gert; Roeffaers, Maarten B. J.; Bartholomeeusen, Evelyne Angewandte Chemie International Edition, Vol. 49, Issue 5 https://doi.org/10.1002/anie.200905039	journal	December 2009
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High-Resolution Single-Molecule Fluorescence Imaging of Zeolite Aggregates within Real-Life Fluid Catalytic Cracking Particles Ristanović, Zoran; Kerssens, Marleen M.; Kubarev, Alexey V. Angewandte Chemie International Edition, Vol. 54, Issue 6 https://doi.org/10.1002/anie.201410236	journal	December 2014
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Fluorescence Imaging of Single-Molecule Retention Trajectories in Reversed-Phase Chromatographic Particles Cooper, Justin T.; Peterson, Eric M.; Harris, Joel M. Analytical Chemistry, Vol. 85, Issue 19 https://doi.org/10.1021/ac402251r	journal	September 2013
Spectroscopic and Polarization-Dependent Single-Molecule Tracking Reveal the One-Dimensional Diffusion Pathways in Surfactant-Templated Mesoporous Silica Kumarasinghe, Ruwandi; Higgins, Eric D.; Ito, Takashi The Journal of Physical Chemistry C, Vol. 120, Issue 1 https://doi.org/10.1021/acs.jpcc.5b10152	journal	December 2015
Distinguishing Direct and Indirect Photoelectrocatalytic Oxidation Mechanisms Using Quantitative Single-Molecule Reaction Imaging and Photocurrent Measurements Sambur, Justin B.; Chen, Peng The Journal of Physical Chemistry C, Vol. 120, Issue 37 https://doi.org/10.1021/acs.jpcc.6b01848	journal	May 2016
Study of Confinement and Catalysis Effects of the Reaction of Methylation of Benzene by Methanol in H-Beta and H-ZSM-5 Zeolites by Topological Analysis of Electron Density Zalazar, María Fernanda; Paredes, Esteban Nadal; Romero Ojeda, Gonzalo D. The Journal of Physical Chemistry C, Vol. 122, Issue 6 https://doi.org/10.1021/acs.jpcc.7b10297	journal	February 2018
Mechanism and Kinetics of Hydrogen Peroxide Decomposition on Platinum Nanocatalysts Serra-Maia, Rui; Bellier, Marion; Chastka, Stephen ACS Applied Materials & Interfaces, Vol. 10, Issue 25 https://doi.org/10.1021/acsami.8b02345	journal	May 2018
A Link between Reactivity and Local Structure in Acid Catalysis on Zeolites Bhan, Aditya; Iglesia, Enrique Accounts of Chemical Research, Vol. 41, Issue 4 https://doi.org/10.1021/ar700181t	journal	April 2008
Understanding the Optimal Adsorption Energies for Catalyst Screening in Heterogeneous Catalysis Yang, Bo; Burch, Robbie; Hardacre, Christopher ACS Catalysis, Vol. 4, Issue 1 https://doi.org/10.1021/cs400727f	journal	December 2013
Diffusion of Oriented Single Molecules with Switchable Mobility in Networks of Long Unidimensional Nanochannels Jung, Christophe; Kirstein, Johanna; Platschek, Barbara Journal of the American Chemical Society, Vol. 130, Issue 5 https://doi.org/10.1021/ja075927e	journal	February 2008
Evidence for Crystal-Face-Dependent TiO ₂ Photocatalysis from Single-Molecule Imaging and Kinetic Analysis Tachikawa, Takashi; Yamashita, Soichiro; Majima, Tetsuro Journal of the American Chemical Society, Vol. 133, Issue 18 https://doi.org/10.1021/ja201415j	journal	May 2011
Lab-in-a-Shell: Encapsulating Metal Clusters for Size Sieving Catalysis Qiao, Zhen-An; Zhang, Pengfei; Chai, Song-Hai Journal of the American Chemical Society, Vol. 136, Issue 32 https://doi.org/10.1021/ja505903r	journal	August 2014
Mechanistic Aspects of Horseradish Peroxidase Elucidated through Single-Molecule Studies Gorris, Hans H.; Walt, David R. Journal of the American Chemical Society, Vol. 131, Issue 17 https://doi.org/10.1021/ja9008858	journal	May 2009
Quantitative 3D Fluorescence Imaging of Single Catalytic Turnovers Reveals Spatiotemporal Gradients in Reactivity of Zeolite H-ZSM-5 Crystals upon Steaming Ristanović, Zoran; Hofmann, Jan P.; De Cremer, Gert Journal of the American Chemical Society, Vol. 137, Issue 20 https://doi.org/10.1021/jacs.5b01698	journal	April 2015
How Does Confinement Change Ligand–Receptor Binding Equilibrium? Protein Binding in Nanopores and Nanochannels Tagliazucchi, Mario; Szleifer, Igal Journal of the American Chemical Society, Vol. 137, Issue 39 https://doi.org/10.1021/jacs.5b05032	journal	September 2015
Single Molecule Nanospectroscopy Visualizes Proton-Transfer Processes within a Zeolite Crystal Ristanović, Zoran; Kubarev, Alexey V.; Hofkens, Johan Journal of the American Chemical Society, Vol. 138, Issue 41 https://doi.org/10.1021/jacs.6b06083	journal	October 2016
Single-Molecule Fluorescence Microscopy Reveals Local Diffusion Coefficients in the Pore Network of an Individual Catalyst Particle Hendriks, Frank C.; Meirer, Florian; Kubarev, Alexey V. Journal of the American Chemical Society, Vol. 139, Issue 39 https://doi.org/10.1021/jacs.7b07139	journal	September 2017
Molecular Length Dependence of Single Molecule Wobbling within Surfactant- and Solvent-Filled Silica Mesopores Pramanik, Rajib; Ito, Takashi; Higgins, Daniel A. The Journal of Physical Chemistry C, Vol. 117, Issue 29 https://doi.org/10.1021/jp404991m	journal	July 2013
Single-Molecule Tracking Studies of Millimeter-Scale Cylindrical Domain Alignment in Polystyrene–Poly(ethylene oxide) Diblock Copolymer Films Induced by Solvent Vapor Penetration Tran-Ba, Khanh-Hoa; Finley, Jason J.; Higgins, Daniel A. The Journal of Physical Chemistry Letters, Vol. 3, Issue 15 https://doi.org/10.1021/jz300647z	journal	July 2012
How Does a Single Pt Nanocatalyst Behave in Two Different Reactions? A Single-Molecule Study Han, Kyu Sung; Liu, Guokun; Zhou, Xiaochun Nano Letters, Vol. 12, Issue 3 https://doi.org/10.1021/nl203677b	journal	January 2012
Direct Visualization of Dye and Oligonucleotide Diffusion in Silica Filaments with Collinear Mesopores Feil, Florian; Cauda, Valentina; Bein, Thomas Nano Letters, Vol. 12, Issue 3 https://doi.org/10.1021/nl2039474	journal	February 2012
Highly Oriented Mesoporous Silica Channels Synthesized in Microgrooves and Visualized with Single-Molecule Diffusion Rühle, Bastian; Davies, Melari; Lebold, Timo ACS Nano, Vol. 6, Issue 3 https://doi.org/10.1021/nn2042835	journal	February 2012
Kinetics of Proteolytic Reactions in Nanoporous Materials Bi, Hongyan; Qiao, Liang; Busnel, Jean-Marc Journal of Proteome Research, Vol. 8, Issue 10 https://doi.org/10.1021/pr9003954	journal	October 2009
Three-dimensional structural dynamics of myosin V by single-molecule fluorescence polarization Forkey, Joseph N.; Quinlan, Margot E.; Alexander Shaw, M. Nature, Vol. 422, Issue 6930 https://doi.org/10.1038/nature01529	journal	March 2003
Spatially resolved observation of crystal-face-dependent catalysis by single turnover counting Roeffaers, Maarten B. J.; Sels, Bert F.; Uji-i, Hiroshi Nature, Vol. 439, Issue 7076 https://doi.org/10.1038/nature04502	journal	February 2006
Visualizing single-molecule diffusion in mesoporous materials Zürner, Andreas; Kirstein, Johanna; Döblinger, Markus Nature, Vol. 450, Issue 7170, p. 705-708 https://doi.org/10.1038/nature06398	journal	November 2007
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