Revealing long- and short-range structural modifications within phosphorus-treated HZSM-5 zeolites by atom probe tomography, nuclear magnetic resonance and powder X-ray diffraction
Abstract
In this study, the average and the local structure of phosphorus-treated HZSM-5 zeolites were investigated by means of atom probe tomography, powder X-ray diffraction (at ambient and cryogenic temperatures) and 1H, 29Si, 27Al, and 31P magic angle spinning (MAS) solid state nuclear magnetic resonance (NMR) spectroscopy. Phosphatation to yield a product with P/Al ≤ 1 followed by thermal treatment leads to breaking of the Si–OH–Al bridging groups, and subsequent partial dealumination of the zeolite framework, as shown by the contraction of the orthorhombic unit-cell volume and by the loss of tetrahedral framework Al, as observed in the 27Al Multiple Quantum (MQ) MAS NMR spectrum. Most of the framework Al is present in an electronic environment distorted by the presence of phosphorus and appears not to be involved in classic Si–OH–Al Brønsted acid sites. The 31P MAS NMR signals indicate that phosphorus interacts with the zeolitic framework to locally form silico-aluminophosphate (SAPO) domains and the presence of a new kind of acidic site was confirmed by the resonance at ~8.6 ppm in the 1H MAS NMR spectra, attributed to P–OH groups. Increasing the phosphorus loading (P/Al >> 1) promotes further dealumination of the framework and cross-dehydroxylation between P–OH and Si–OH species,more »
- Authors:
-
[1];
[1];
[2];
[2];
[3];
[2];
[1];
[4]
- Utrecht University (The Netherlands). Inorganic Chemistry and Catalysis
- Utrecht University (The Netherlands). NMR Spectroscopy, Bijvoet Center for Biomolecular Research
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
- Utrecht University (The Netherlands). Inorganic Chemistry and Catalysis; Albemarle Catalyst Company BV, Amsterdam (The Netherlands)
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1482432
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Chemistry Chemical Physics. PCCP
- Additional Journal Information:
- Journal Volume: 20; Journal Issue: 44; Journal ID: ISSN 1463-9076
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE
Citation Formats
Danisi, Rosa Micaela, Schmidt, Joel E., Lucini Paioni, Alessandra, Houben, Klaartje, Poplawsky, Jonathan D., Baldus, Marc, Weckhuysen, Bert M., and Vogt, Eelco T. C. Revealing long- and short-range structural modifications within phosphorus-treated HZSM-5 zeolites by atom probe tomography, nuclear magnetic resonance and powder X-ray diffraction. United States: N. p., 2018.
Web. doi:10.1039/c8cp03828g.
Danisi, Rosa Micaela, Schmidt, Joel E., Lucini Paioni, Alessandra, Houben, Klaartje, Poplawsky, Jonathan D., Baldus, Marc, Weckhuysen, Bert M., & Vogt, Eelco T. C. Revealing long- and short-range structural modifications within phosphorus-treated HZSM-5 zeolites by atom probe tomography, nuclear magnetic resonance and powder X-ray diffraction. United States. https://doi.org/10.1039/c8cp03828g
Danisi, Rosa Micaela, Schmidt, Joel E., Lucini Paioni, Alessandra, Houben, Klaartje, Poplawsky, Jonathan D., Baldus, Marc, Weckhuysen, Bert M., and Vogt, Eelco T. C. Thu .
"Revealing long- and short-range structural modifications within phosphorus-treated HZSM-5 zeolites by atom probe tomography, nuclear magnetic resonance and powder X-ray diffraction". United States. https://doi.org/10.1039/c8cp03828g. https://www.osti.gov/servlets/purl/1482432.
@article{osti_1482432,
title = {Revealing long- and short-range structural modifications within phosphorus-treated HZSM-5 zeolites by atom probe tomography, nuclear magnetic resonance and powder X-ray diffraction},
author = {Danisi, Rosa Micaela and Schmidt, Joel E. and Lucini Paioni, Alessandra and Houben, Klaartje and Poplawsky, Jonathan D. and Baldus, Marc and Weckhuysen, Bert M. and Vogt, Eelco T. C.},
abstractNote = {In this study, the average and the local structure of phosphorus-treated HZSM-5 zeolites were investigated by means of atom probe tomography, powder X-ray diffraction (at ambient and cryogenic temperatures) and 1H, 29Si, 27Al, and 31P magic angle spinning (MAS) solid state nuclear magnetic resonance (NMR) spectroscopy. Phosphatation to yield a product with P/Al ≤ 1 followed by thermal treatment leads to breaking of the Si–OH–Al bridging groups, and subsequent partial dealumination of the zeolite framework, as shown by the contraction of the orthorhombic unit-cell volume and by the loss of tetrahedral framework Al, as observed in the 27Al Multiple Quantum (MQ) MAS NMR spectrum. Most of the framework Al is present in an electronic environment distorted by the presence of phosphorus and appears not to be involved in classic Si–OH–Al Brønsted acid sites. The 31P MAS NMR signals indicate that phosphorus interacts with the zeolitic framework to locally form silico-aluminophosphate (SAPO) domains and the presence of a new kind of acidic site was confirmed by the resonance at ~8.6 ppm in the 1H MAS NMR spectra, attributed to P–OH groups. Increasing the phosphorus loading (P/Al >> 1) promotes further dealumination of the framework and cross-dehydroxylation between P–OH and Si–OH species, leading to the formation of a crystalline silicon orthophosphate phase. With decreasing Al content, the monoclinic HZSM-5 structure becomes preferred, especially at 85 K where the strain relaxation is higher. Nevertheless, the presence of a higher amount of silicophosphate impurities hinders the low-temperature strain release of the framework, indicating that some of these species are localized in the zeolite pores and contribute to the strain build up.},
doi = {10.1039/c8cp03828g},
journal = {Physical Chemistry Chemical Physics. PCCP},
number = 44,
volume = 20,
place = {United States},
year = {Thu Aug 23 00:00:00 EDT 2018},
month = {Thu Aug 23 00:00:00 EDT 2018}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 14 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
An Improved Broadband Decoupling Sequence for Liquid Crystals and Solids
journal, January 2000
- Fung, B. M.; Khitrin, A. K.; Ermolaev, Konstantin
- Journal of Magnetic Resonance, Vol. 142, Issue 1
Phosphorus-modified ZSM-5 for conversion of ethanol to propylene
journal, August 2010
- Song, Zhaoxia; Takahashi, Atsushi; Nakamura, Isao
- Applied Catalysis A: General, Vol. 384, Issue 1-2
Nanoscale Chemical Imaging of Zeolites Using Atom Probe Tomography
journal, July 2018
- Schmidt, Joel E.; Peng, Linqing; Poplawsky, Jonathan D.
- Angewandte Chemie International Edition, Vol. 57, Issue 33
Shape-selective catalysis by phosphate modified ZSM-5: Generation of new acid sites with pore narrowing
journal, February 2014
- Janardhan, H. L.; Shanbhag, G. V.; Halgeri, A. B.
- Applied Catalysis A: General, Vol. 471
Hydrothermal stabilization of ZSM-5 catalytic-cracking additives by phosphorus addition
journal, January 2006
- Blasco, T.; Corma, A.; Martineztriguero, J.
- Journal of Catalysis, Vol. 237, Issue 2
Catalytic properties of postsynthesis phosphorus-modified H-ZSM5 zeolites
journal, February 1989
- Vinek, H.
- Journal of Catalysis, Vol. 115, Issue 2
Monoclinic–Orthorhombic Phase Transition in ZSM-5 Zeolite: Spontaneous Strain Variation and Thermodynamic Properties
journal, March 2015
- Ardit, Matteo; Martucci, Annalisa; Cruciani, Giuseppe
- The Journal of Physical Chemistry C, Vol. 119, Issue 13
Effect of Phosphate Modification on the Brønsted Acidity and Methanol-to-Olefin Conversion Activity of Zeolite ZSM-5
journal, August 2013
- Dyballa, Michael; Klemm, Elias; Weitkamp, Jens
- Chemie Ingenieur Technik, Vol. 85, Issue 11
Solid-state MAS NMR studies on the hydrothermal stability of the zeolite catalysts for residual oil selective catalytic cracking
journal, November 2004
- Zhuang, J.; Ma, D.; Yang, G.
- Journal of Catalysis, Vol. 228, Issue 1
Solid state 1H NMR study, humidity sensitivity and protonic conduction of gel derived phosphosilicate glasses
journal, October 2002
- Clayden, N. J.; Esposito, S.; Pernice, P.
- Journal of Materials Chemistry, Vol. 12, Issue 12
Transformation of Active Sites in Fe/SSZ-13 SCR Catalysts during Hydrothermal Aging: A Spectroscopic, Microscopic, and Kinetics Study
journal, March 2017
- Kovarik, Libor; Washton, Nancy M.; Kukkadapu, Ravi
- ACS Catalysis, Vol. 7, Issue 4
Dehydration of silica-aluminas monitored by high-resolution solid-state proton NMR
journal, March 1987
- Bronnimann, Charles E.; Chuang, I. Suer; Hawkins, Bruce L.
- Journal of the American Chemical Society, Vol. 109, Issue 5
Methanol to propylene: Effect of phosphorus on a high silica HZSM-5 catalyst
journal, June 2009
- Liu, Jian; Zhang, Chenxi; Shen, Zhenhao
- Catalysis Communications, Vol. 10, Issue 11
Discerning the Location and Nature of Coke Deposition from Surface to Bulk of Spent Zeolite Catalysts
journal, November 2016
- Devaraj, Arun; Vijayakumar, Murugesan; Bao, Jie
- Scientific Reports, Vol. 6, Issue 1
Catalytic and physical properties of phosphorus-modified ZSM-5 zeolite
journal, January 1982
- Vedrine, J.
- Journal of Catalysis, Vol. 73, Issue 1
Solid state 29Si and 31P NMR study of gel derived phosphosilicate glasses
journal, January 2001
- Clayden, Nigel J.; Esposito, Serena; Pernice, Pasquale
- Journal of Materials Chemistry, Vol. 11, Issue 3
ZFiltering in MQMAS NMR
journal, November 1996
- Amoureux, Jean-Paul; Fernandez, Christian; Steuernagel, Stefan
- Journal of Magnetic Resonance, Series A, Vol. 123, Issue 1
Characterization of extra-framework species of steamed and acid washed faujasite by MQMAS NMR and IR measurements
journal, February 2001
- Menezes, S. M. C.; Camorim, V. L.; Lam, Y. L.
- Applied Catalysis A: General, Vol. 207, Issue 1-2
Modification of H-ZSM-5 zeolites with phosphorus. 1. Identification of aluminum species by 27Al solid-state NMR and characterization of their catalytic properties
journal, October 2006
- Cabral de Menezes, S. M.; Lam, Y. L.; Damodaran, K.
- Microporous and Mesoporous Materials, Vol. 95, Issue 1-3
1H N M R magic angle spinning (MAS) studies of heterogeneous catalysis
journal, January 1991
- Mastikhin, V. M.; Mudrakovsky, I. L.; Nosov, A. V.
- Progress in Nuclear Magnetic Resonance Spectroscopy, Vol. 23, Issue 3
NMR and IR studies of zeolite H-ZSM-5 modified with orthophosphoric acid
journal, August 1990
- Caro, J.
- Journal of Catalysis, Vol. 124, Issue 2
Modification of H-ZSM-5 zeolites with phosphorus. 2. Interaction between phosphorus and aluminum studied by solid-state NMR spectroscopy
journal, October 2006
- Damodaran, K.; Wiench, J. W.; Cabral de Menezes, S. M.
- Microporous and Mesoporous Materials, Vol. 95, Issue 1-3
Hexane Cracking over Steamed Phosphated Zeolite H-ZSM-5: Promotional Effect on Catalyst Performance and Stability
journal, November 2014
- van der Bij, Hendrik E.; Meirer, Florian; Kalirai, Sam
- Chemistry - A European Journal, Vol. 20, Issue 51
Crystal structure and structure-related properties of ZSM-5
journal, July 1981
- Olson, D. H.; Kokotailo, G. T.; Lawton, S. L.
- The Journal of Physical Chemistry, Vol. 85, Issue 15
Proton‐enhanced NMR of dilute spins in solids
journal, July 1973
- Pines, A.; Gibby, M. G.; Waugh, J. S.
- The Journal of Chemical Physics, Vol. 59, Issue 2
Verification and quantitative determination of a new type of Brønsted acid sites in H-ZSM-5 by 1H magic-angle spinning nuclear magnetic resonance spectroscopy
journal, January 1995
- Brunner, E.; Beck, K.; Koch, M.
- Microporous Materials, Vol. 3, Issue 4-5
Stabilization effect of phosphorus on steamed H-MFI zeolites
journal, November 2006
- Caeiro, G.; Magnoux, P.; Lopes, J. M.
- Applied Catalysis A: General, Vol. 314, Issue 2
Nanoscale tomography in materials science
journal, December 2007
- Möbus, Günter; Inkson, Beverley J.
- Materials Today, Vol. 10, Issue 12
Determining the location and nearest neighbours of aluminium in zeolites with atom probe tomography
journal, July 2015
- Perea, Daniel E.; Arslan, Ilke; Liu, Jia
- Nature Communications, Vol. 6, Issue 1
ZSM-5-type materials. Factors affecting crystal symmetry
journal, October 1979
- Wu, E. L.; Lawton, S. L.; Olson, D. H.
- The Journal of Physical Chemistry, Vol. 83, Issue 21
Nanoscale Chemical Imaging of Coking Mechanisms in a Zeolite ZSM-5 Crystal by Atom Probe Tomography
journal, July 2017
- Poplawsky, Jonathan D.; Schmidt, Joel E.; Mazumder, Baishakhi
- Microscopy and Microanalysis, Vol. 23, Issue S1
Understanding the enhancement of catalytic performance for olefin cracking: Hydrothermally stable acids in P/HZSM-5
journal, May 2007
- Xue, N.; Chen, X.; Nie, L.
- Journal of Catalysis, Vol. 248, Issue 1
Study of H-ZSM-5 acidity by 1H NMR: broad-line at 4 K and high resolution MAS at 300 K; Brønsted acidity scale and comparison with other zeolites
journal, August 1996
- Heeribout, L.; Batamack, P.; Dorémieux-Morin, C.
- Colloids and Surfaces A: Physicochemical and Engineering Aspects, Vol. 115
P-ZSM-5 Pretreated by High-Temperature Calcination as Durable Catalysts for Steam Cracking of n-Hexane
journal, October 2013
- Yamaguchi, Aritomo; Jin, Dingfeng; Ikeda, Takuji
- Catalysis Letters, Vol. 144, Issue 1
Coke Formation in a Zeolite Crystal During the Methanol-to-Hydrocarbons Reaction as Studied with Atom Probe Tomography
journal, August 2016
- Schmidt, Joel E.; Poplawsky, Jonathan D.; Mazumder, Baishakhi
- Angewandte Chemie International Edition, Vol. 55, Issue 37
Flexibility of the framework structure in highly crystalline silicalite during the reversible monoclinic/orthorhombic solid state polymorphic phase transition
journal, October 1993
- Mentzen, B. F.; Sacerdote-Peronnet, M.
- Materials Research Bulletin, Vol. 28, Issue 10
Controlled decrease of acid strength by orthophosphoric acid on ZSM5
journal, August 1986
- Lercher, J. A.; Rumplmayr, G.
- Applied Catalysis, Vol. 25, Issue 1-2
Spectroscopic and physicochemical characterization of P-Modified H-ZSM-5
journal, November 1991
- Lischke, G.
- Journal of Catalysis, Vol. 132, Issue 1
Fluid catalytic cracking: recent developments on the grand old lady of zeolite catalysis
journal, January 2015
- Vogt, E. T. C.; Weckhuysen, B. M.
- Chemical Society Reviews, Vol. 44, Issue 20
Neutron powder diffraction study of orthorhombic and monoclinic defective silicalite
journal, February 2000
- Artioli, G.; Lamberti, C.; Marra, G. L.
- Acta Crystallographica Section B Structural Science, Vol. 56, Issue 1
Silicalite, a new hydrophobic crystalline silica molecular sieve
journal, February 1978
- Flanigen, E. M.; Bennett, J. M.; Grose, R. W.
- Nature, Vol. 271, Issue 5645
Non-aqueous template-assisted synthesis of mesoporous nanocrystalline silicon orthophosphate
journal, January 2015
- Styskalik, Ales; Skoda, David; Moravec, Zdenek
- RSC Advances, Vol. 5, Issue 90
EXPGUI , a graphical user interface for GSAS
journal, April 2001
- Toby, Brian H.
- Journal of Applied Crystallography, Vol. 34, Issue 2
Water Interactions in Zeolite Catalysts and Their Hydrophobically Modified Analogues
journal, November 2015
- Chen, Kuizhi; Kelsey, Jarred; White, Jeffery L.
- ACS Catalysis, Vol. 5, Issue 12
Effect of phosphorus on HZSM-5 catalyst for C4-olefin cracking reactions to produce propylene
journal, May 2007
- Zhao, G.; Teng, J.; Xie, Z.
- Journal of Catalysis, Vol. 248, Issue 1
High performance phosphorus-modified ZSM-5 zeolite for butene catalytic cracking
journal, March 2010
- Gao, Xionghou; Tang, Zhicheng; Zhang, Haitao
- Korean Journal of Chemical Engineering, Vol. 27, Issue 3
Production of chemicals from methanol I. Low molecular weight olefins
journal, January 1980
- Kaeding, W.
- Journal of Catalysis, Vol. 61, Issue 1
High-temperature (350 K) orthorhombic framework structure of zeolite H-ZSM-5
journal, December 1990
- van Koningsveld, H.
- Acta Crystallographica Section B Structural Science, Vol. 46, Issue 6
Structural and Mechanistic Investigation of a Phosphate-Modified HZSM-5 Catalyst for Methanol Conversion
journal, May 2006
- Abubakar, Saifudin M.; Marcus, David M.; Lee, Jeffrey C.
- Langmuir, Vol. 22, Issue 10
On the preparation of a monoclinic (nearly) single crystal of zeolite HZSM-5
journal, May 1989
- van Koningsveld, H.; Tuinstra, F.; Jansen, J. C.
- Zeolites, Vol. 9, Issue 3
High-resolution solid-state 29Si and 31P NMR of silicon-phosphorous compounds containing six-coordinated silicon
journal, October 1985
- Mudrakovskii, I. L.; Mastikhin, V. M.; Shmachkova, V. P.
- Chemical Physics Letters, Vol. 120, Issue 4-5
The orthorhombic/monoclinic transition in single crystals of zeolite ZSM-5
journal, November 1987
- van Koningsveld, H.; Jansen, J. C.; van Bekkum, H.
- Zeolites, Vol. 7, Issue 6
Magic-angle spinning nuclear magnetic resonance studies of water molecules adsorbed on Brønsted- and Lewis-acid sites in zeolites and amorphous silica–aluminas
journal, January 1991
- Hunger, Michael; Freude, Dieter; Pfeifer, Harry
- J. Chem. Soc., Faraday Trans., Vol. 87, Issue 4
Spectroscopic study of phosphorus modified H-ZSM-5
journal, June 2011
- Göhlich, M.; Reschetilowski, W.; Paasch, S.
- Microporous and Mesoporous Materials, Vol. 142, Issue 1
Modification of siliceous zeolites using phosphorus pentachloride
journal, July 1992
- Kojima, M.; Lefebvre, F.; Ben Taârit, Y.
- Zeolites, Vol. 12, Issue 6
Phosphorous Modified ZSM-5 Zeolites: Impact on Methanol Conversion into Olefins
journal, August 2015
- Losch, Pit; Laugel, Guillaume; Martinez-Espin, Juan S.
- Topics in Catalysis, Vol. 58, Issue 14-17
Aluminum-Phosphate Binder Formation in Zeolites as Probed with X-ray Absorption Microscopy
journal, December 2014
- van der Bij, Hendrik E.; Cicmil, Dimitrije; Wang, Jian
- Journal of the American Chemical Society, Vol. 136, Issue 51
Ab-initio structure determination of LiSbWO6 by X-ray powder diffraction
journal, March 1988
- Le Bail, A.; Duroy, H.; Fourquet, J. L.
- Materials Research Bulletin, Vol. 23, Issue 3
Local silico-aluminophosphate interfaces within phosphated H-ZSM-5 zeolites
journal, January 2014
- van der Bij, Hendrik E.; Weckhuysen, Bert M.
- Physical Chemistry Chemical Physics, Vol. 16, Issue 21
Solid Phosphoric Acid Catalyst: A Multinuclear NMR and Theoretical Study
journal, August 1998
- Krawietz, Thomas R.; Lin, Ping; Lotterhos, Karen E.
- Journal of the American Chemical Society, Vol. 120, Issue 33
Isotropic Spectra of Half-Integer Quadrupolar Spins from Bidimensional Magic-Angle Spinning NMR
journal, May 1995
- Frydman, Lucio; Harwood, John S.
- Journal of the American Chemical Society, Vol. 117, Issue 19
Multinuclear solid-state NMR studies of acidic and non-acidic hydroxyl protons in zeolites
journal, February 1996
- Hunger, Michael
- Solid State Nuclear Magnetic Resonance, Vol. 6, Issue 1
Orthorhombic to monoclinic phase transition in high-Ti-loaded TS-1: an attempt to locate Ti in the MFI framework by low temperature XRD
journal, November 2000
- Marra, G. L.; Artioli, G.; Fitch, A. N.
- Microporous and Mesoporous Materials, Vol. 40, Issue 1-3
Phosphorus promotion and poisoning in zeolite-based materials: synthesis, characterisation and catalysis
journal, January 2015
- van der Bij, Hendrik E.; Weckhuysen, Bert M.
- Chemical Society Reviews, Vol. 44, Issue 20
Phosphatation of Zeolite H-ZSM-5: A Combined Microscopy and Spectroscopy Study
journal, January 2014
- van der Bij, Hendrik E.; Aramburo, Luis R.; Arstad, Bjørnar
- ChemPhysChem, Vol. 15, Issue 2
Unit Cell Volume as a Measure of Dealumination of ZSM-5 in Fluid Catalytic Cracking Catalyst
journal, October 2014
- Knöll, Jürgen; Singh, Udayshankar; Nicolich, Jeffrey
- Industrial & Engineering Chemistry Research, Vol. 53, Issue 42
Aluminum Polyphosphate Thermoreversible Gels: A Study by31P and27Al NMR Spectroscopy
journal, December 1995
- de Oliveira Lima, Emilia Celma; Moita Neto, José Machado; Fujiwara, Fred Yukio
- Journal of Colloid and Interface Science, Vol. 176, Issue 2
Nanoscale tomography reveals the deactivation of automotive copper-exchanged zeolite catalysts
journal, November 2017
- Schmidt, Joel E.; Oord, Ramon; Guo, Wei
- Nature Communications, Vol. 8, Issue 1
Coke Formation in a Zeolite Crystal During the Methanol-to-Hydrocarbons Reaction as Studied with Atom Probe Tomography
journal, August 2016
- Schmidt, Joel E.; Poplawsky, Jonathan D.; Mazumder, Baishakhi
- Angewandte Chemie, Vol. 128, Issue 37
Works referencing / citing this record:
Coated sulfated zirconia/SAPO-34 for the direct conversion of CO 2 to light olefins
journal, January 2020
- Ramirez, Adrian; Dutta Chowdhury, Abhishek; Caglayan, Mustafa
- Catalysis Science & Technology, Vol. 10, Issue 5
Atom Probe Tomography for Catalysis Applications: A Review
journal, July 2019
- Barroo, Cédric; Akey, Austin J.; Bell, David C.
- Applied Sciences, Vol. 9, Issue 13