Are the Brønsted acid sites in amorphous silica-alumina bridging?

Salvia, William S.; Zhao, Tommy Yunpu; Chatterjee, Puranjan; Huang, Wenyu; Perras, Frédéric A.

doi:10.1039/d3cc04237e

Title: Are the Brønsted acid sites in amorphous silica-alumina bridging?

Journal Article · Wed Nov 01 00:00:00 EDT 2023 · ChemComm

DOI:https://doi.org/10.1039/d3cc04237e· OSTI ID:2204498

^[1];

^[2];

^[3];

^[3]

Miami Univ., Oxford, OH (United States); Ames Laboratory (AMES), Ames, IA (United States)
Ames Laboratory (AMES), Ames, IA (United States)
Iowa State Univ., Ames, IA (United States); Ames Laboratory (AMES), Ames, IA (United States)

Competing models exist to explain the differences in the activity of zeolites and amorphous silica–aluminas. Some postulate that silica–alumina contains dilute zeolitic bridging acid sites, while others favor a pseudo-bridging silanol model. Here, we employed a selective isotope labeling strategy to assess the existence of Si–O(H)–Al bonds using NMR-based distance measurements.

This content will become publicly available on Fri Nov 01 00:00:00 EDT 2024

Cite

Export

Save

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); USDOE

Grant/Contract Number:: AC02-07CH11358

OSTI ID:: 2204498

Alternate ID(s):: OSTI ID: 2204746

Report Number(s):: IS-J-11,177

Journal Information:: ChemComm, Vol. 59, Issue 94; ISSN 1359-7345

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

References (45)

Detection of Brønsted acid sites in zeolite HY with high-field 17O-MAS-NMR techniques Peng, Luming; Liu, Yun; Kim, Namjun Nature Materials, Vol. 4, Issue 3 https://doi.org/10.1038/nmat1332	journal	February 2005
Strong Brønsted Acidity in Amorphous Silica−Aluminas Xu, Bin; Sievers, Carsten; Lercher, Johannes A. The Journal of Physical Chemistry C, Vol. 111, Issue 32 https://doi.org/10.1021/jp073677i	journal	July 2007
Brønsted acid sites of zeolitic strength in amorphous silica-alumina Poduval, Dilip G.; van Veen, J. A. Rob; Rigutto, Marcello S. Chemical Communications, Vol. 46, Issue 20 https://doi.org/10.1039/c000019a	journal	January 2010
Heteronuclear NMR Spectroscopy as a Surface-Selective Technique: A Unique Look at the Hydroxyl Groups of γ-Alumina. Taoufik, Mostafa; Szeto, Kai C.; Merle, Nicolas Chemistry - A European Journal, Vol. 20, Issue 14 https://doi.org/10.1002/chem.201304883	journal	March 2014
NMR investigation of proton mobility in zeolites Kanellopoulos, Johanna; Gottert, Clemens; Schneider, Denis Journal of Catalysis, Vol. 255, Issue 1 https://doi.org/10.1016/j.jcat.2008.01.028	journal	April 2008
Hydrogen Bonds Dominate Brønsted Acid Sites in Zeolite SSZ‐42: A Classification of Their Diversity Schroeder, Christian; Zones, Stacey I.; Hansen, Michael Ryan Angewandte Chemie International Edition, Vol. 61, Issue 3 https://doi.org/10.1002/anie.202109313	journal	November 2021
Characterizing the First and Second ²⁷Al Neighbors of Brønsted and Lewis Acid Protons in Zeolites and the Distribution of ²⁷Al Quadrupolar Couplings by ¹H{²⁷Al} Offset REAPDOR Koller, Hubert; Uesbeck, Tobias; Hansen, Michael Ryan The Journal of Physical Chemistry C, Vol. 121, Issue 46 https://doi.org/10.1021/acs.jpcc.7b09544	journal	November 2017
A novel application of nuclear spin-echo double-resonance to aluminophosphates and aluminosilicates van Eck, E. R. H.; Janssen, R.; Maas, W. E. J. R. Chemical Physics Letters, Vol. 174, Issue 5 https://doi.org/10.1016/S0009-2614(90)87174-P	journal	November 1990
Measurement of hetero-nuclear distances using a symmetry-based pulse sequence in solid-state NMR Chen, Lei; Wang, Qiang; Hu, Bingwen Physical Chemistry Chemical Physics, Vol. 12, Issue 32 https://doi.org/10.1039/b926546e	journal	January 2010
Pentacoordinated Aluminum Species: New Frontier for Tailoring Acidity-Enhanced Silica–Alumina Catalysts Wang, Zichun; Jiang, Yijiao; Baiker, Alfons Accounts of Chemical Research, Vol. 53, Issue 11 https://doi.org/10.1021/acs.accounts.0c00459	journal	October 2020
Brønsted acidity of amorphous silica–alumina: The molecular rules of proton transfer Leydier, Fabien; Chizallet, Céline; Chaumonnot, Alexandra Journal of Catalysis, Vol. 284, Issue 2 https://doi.org/10.1016/j.jcat.2011.08.015	journal	December 2011
Toward the Atomic Scale Simulation of Intricate Acidic Aluminosilicate Catalysts Chizallet, Céline ACS Catalysis, Vol. 10, Issue 10 https://doi.org/10.1021/acscatal.0c01136	journal	April 2020
Isopropanol Dehydration on Amorphous Silica-Alumina: Synergy of Brønsted and Lewis Acidities at Pseudo-Bridging Silanols Larmier, Kim; Chizallet, Céline; Maury, Sylvie Angewandte Chemie International Edition, Vol. 56, Issue 1 https://doi.org/10.1002/anie.201609494	journal	December 2016
Pseudo-Bridging Silanols as Versatile Brønsted Acid Sites of Amorphous Aluminosilicate Surfaces Chizallet, Céline; Raybaud, Pascal Angewandte Chemie International Edition, Vol. 48, Issue 16 https://doi.org/10.1002/anie.200804580	journal	January 2009
IR studies of OH groups in mesoporous aluminosilicates Góra-Marek, K.; Datka, J. Applied Catalysis A: General, Vol. 302, Issue 1 https://doi.org/10.1016/j.apcata.2005.12.027	journal	March 2006
Nature, Structure and Strength of the Acidic Sites of Amorphous Silica Alumina: An IR and NMR Study Crépeau, G.; Montouillout, V.; Vimont, A. The Journal of Physical Chemistry B, Vol. 110, Issue 31 https://doi.org/10.1021/jp062252d	journal	August 2006
Brønsted acid sites based on penta-coordinated aluminum species Wang, Zichun; Jiang, Yijiao; Lafon, Olivier Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms13820	journal	December 2016
Enhanced surface acidity in mixed alumina–silicas: a low-temperature FTIR study Daniell, W.; Schubert, U.; Glöckler, R. Applied Catalysis A: General, Vol. 196, Issue 2 https://doi.org/10.1016/S0926-860X(99)00474-3	journal	April 2000
Characterization of hydrogen bonding in zeolites by proton solid-state NMR spectroscopy White, Jeffery L.; Beck, Larry W.; Haw, James F. Journal of the American Chemical Society, Vol. 114, Issue 15 https://doi.org/10.1021/ja00041a041	journal	July 1992
Assessment, Control, and Impact of Brønsted Acid Site Heterogeneity in Zeolite HZSM-5 Abdolrahmani, Maryam; Chen, Kuizhi; White, Jeffery L. The Journal of Physical Chemistry C, Vol. 122, Issue 27 https://doi.org/10.1021/acs.jpcc.8b04283	journal	June 2018
Acidity Characterization of Amorphous Silica–Alumina Hensen, Emiel J. M.; Poduval, Dilip G.; Degirmenci, Volkan The Journal of Physical Chemistry C, Vol. 116, Issue 40 https://doi.org/10.1021/jp309182f	journal	October 2012
Identification of distinct Brønsted acidic sites in zeolite mordenite by proton localization and [²⁷Al]-¹H REAPDOR NMR Ganapathy, Subramanian; Kumar, Rajiv; Delevoye, Laurent Chem. Commun., Issue 16 https://doi.org/10.1039/B304548J	journal	January 2003
Location and orientation of adsorbed molecules in zeolites from solid-state REAPDOR NMR Holland, Gregory P.; Alam, Todd M. Physical Chemistry Chemical Physics, Vol. 7, Issue 8 https://doi.org/10.1039/b418943d	journal	January 2005
INTERFACES. A program for determining the 3D structures of surfaces sites using NMR data Cunningham, James; Perras, Frédéric A. Journal of Magnetic Resonance Open, Vol. 12-13 https://doi.org/10.1016/j.jmro.2022.100066	journal	December 2022
Direct Detection of Multiple Acidic Proton Sites in Zeolite HZSM-5 Chen, Kuizhi; Abdolrhamani, Maryam; Sheets, Eric Journal of the American Chemical Society, Vol. 139, Issue 51 https://doi.org/10.1021/jacs.7b10940	journal	December 2017
Proton-Selective ¹⁷ O− ¹ H Distance Measurements in Fast Magic-Angle-Spinning Solid-State NMR Spectroscopy for the Determination of Hydrogen Bond Lengths Brinkmann, Andreas; Kentgens, Arno P. M. Journal of the American Chemical Society, Vol. 128, Issue 46 https://doi.org/10.1021/ja065415k	journal	November 2006
Brønsted–Brønsted Synergies between Framework and Noncrystalline Protons in Zeolite H-ZSM-5 Chen, Kuizhi; Abdolrahmani, Maryam; Horstmeier, Sarah ACS Catalysis, Vol. 9, Issue 7 https://doi.org/10.1021/acscatal.9b01583	journal	May 2019
Measuring multiple carbon–nitrogen distances in natural abundant solids using R-RESPDOR NMR Gan, Zhehong Chem. Commun., Issue 45 https://doi.org/10.1039/B611447D	journal	January 2006
Promoting Aromatic C–H Activation through Reactive Brønsted Acid–Base Pairs on Penta-Coordinated Al-Enriched Amorphous Silica–Alumina Wang, Zichun; Jiang, Yijiao; Baiker, Alfons The Journal of Physical Chemistry Letters, Vol. 13, Issue 2 https://doi.org/10.1021/acs.jpclett.1c03489	journal	January 2022
FT-IR Studies on Light Olefin Skeletal Isomerization Catalysis Trombetta, Marcella; Busca, Guido; Rossini, Stefano Journal of Catalysis, Vol. 179, Issue 2 https://doi.org/10.1006/jcat.1998.2251	journal	October 1998
Revealing Brønsted Acidic Bridging SiOHAl Groups on Amorphous Silica–Alumina by Ultrahigh Field Solid-State NMR Wang, Zichun; Chen, Kuizhi; Jiang, Yijiao The Journal of Physical Chemistry Letters, Vol. 12, Issue 47 https://doi.org/10.1021/acs.jpclett.1c02975	journal	November 2021
Alkane C−H Bond Activation in Zeolites: Evidence for Direct Protium Exchange Truitt, Matthew J.; Toporek, Stan S.; Rovira-Truitt, Rosimar Journal of the American Chemical Society, Vol. 128, Issue 6 https://doi.org/10.1021/ja0558802	journal	January 2006
Acidity of Amorphous Silicaâ€“Alumina: From Coordination Promotion of Lewis Sites to Proton Transfer Chizallet, CÃ©line; Raybaud, Pascal ChemPhysChem, Vol. 11, Issue 1 https://doi.org/10.1002/cphc.200900797	journal	January 2010
The Initial Stages of Solid Acid-Catalyzed Reactions of Adsorbed Propane. A Mechanistic Study by in Situ MAS NMR Haouas, Mohamed; Walspurger, Stéphane; Taulelle, Francis Journal of the American Chemical Society, Vol. 126, Issue 2 https://doi.org/10.1021/ja0377549	journal	January 2004
In situ H and C MAS NMR study of the mechanism of H/D exchange for deuterated propane adsorbed on H-ZSM-5 Stepanov, A.; Arzumanov, S.; Luzgin, M. Journal of Catalysis, Vol. 235, Issue 1 https://doi.org/10.1016/j.jcat.2005.08.002	journal	October 2005
Silica-alumina catalytic materials: A critical review Busca, Guido Catalysis Today, Vol. 357 https://doi.org/10.1016/j.cattod.2019.05.011	journal	November 2020
Trace water amounts can increase benzene H/D exchange rates in an acidic zeolite Chen, Kuizhi; Gumidyala, Abhishek; Abdolrhamani, Maryam Journal of Catalysis, Vol. 351 https://doi.org/10.1016/j.jcat.2017.04.026	journal	July 2017
CO adsorption on amorphous silica–alumina: electrostatic or Brønsted acidity probe? Leydier, Fabien; Chizallet, Céline; Costa, Dominique Chemical Communications, Vol. 48, Issue 34 https://doi.org/10.1039/c2cc30655g	journal	January 2012
The active site of acidic aluminosilicate catalysts Haag, W. O.; Lago, R. M.; Weisz, P. B. Nature, Vol. 309, Issue 5969 https://doi.org/10.1038/309589a0	journal	June 1984
Acidity enhancement through synergy of penta- and tetra-coordinated aluminum species in amorphous silica networks Wang, Zichun; Li, Tong; Jiang, Yijiao Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-019-13907-7	journal	January 2020
Al–O–Al and Si–O–Si sites in framework aluminosilicate glasses with Si/Al=1: quantification of framework disorder Lee, Sung Keun; Stebbins, Jonathan F. Journal of Non-Crystalline Solids, Vol. 270, Issue 1-3 https://doi.org/10.1016/S0022-3093(00)00089-2	journal	May 2000
Observation of Low-γ Quadrupolar Nuclei by Surface-Enhanced NMR Spectroscopy Nagashima, Hiroki; Trébosc, Julien; Kon, Yoshihiro Journal of the American Chemical Society, Vol. 142, Issue 24 https://doi.org/10.1021/jacs.9b13838	journal	May 2020
Revisiting carbenium chemistry on amorphous silica-alumina: Unraveling their milder acidity as compared to zeolites Leydier, Fabien; Chizallet, Céline; Costa, Dominique Journal of Catalysis, Vol. 325 https://doi.org/10.1016/j.jcat.2015.02.012	journal	May 2015
Kinetic NMR and Density Functional Study of Benzene H/D Exchange in Zeolites, the Most Simple Aromatic Substitution Beck, Larry W.; Xu, Teng; Nicholas, John B. Journal of the American Chemical Society, Vol. 117, Issue 46 https://doi.org/10.1021/ja00151a031	journal	November 1995
Qualitative and Quantitative Analysis of Acid Properties for Solid Acids by Solid-State Nuclear Magnetic Resonance Spectroscopy Yang, Wenjie; Wang, Zichun; Huang, Jun The Journal of Physical Chemistry C, Vol. 125, Issue 19 https://doi.org/10.1021/acs.jpcc.1c01887	journal	May 2021

Similar Records

On the nature of strong acidic Bronsted sites of amorphous silica-aluminas

Journal Article · Fri Apr 01 00:00:00 EST 1983 · J. Catal.; (United States) · OSTI ID:2204498

Borovkov, V Y; Alexeev, A A; Kazansky, V B

Shedding light on the atomic-scale structure of amorphous silica–alumina and its Brønsted acid sites

Journal Article · Wed Sep 11 00:00:00 EDT 2019 · Physical Chemistry Chemical Physics. PCCP · OSTI ID:2204498

Perras, Frédéric A.; Wang, Zichun; Kobayashi, Takeshi; +3 more

Rates of levoglucosanol hydrogenolysis over Brønsted and Lewis acid sites on platinum silica-alumina catalysts synthesized by atomic layer deposition

Journal Article · Tue May 26 00:00:00 EDT 2020 · Journal of Catalysis · OSTI ID:2204498

Krishna, Siddarth H.; Zhang, Lifeng; Hermans, Ive; +3 more

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Title: Are the Brønsted acid sites in amorphous silica-alumina bridging?

Citation Formats

References (45)

Similar Records

Related Subjects