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Title: Elementary Steps of Faujasite Formation Followed by in Situ Spectroscopy

Abstract

Ex situ and in situ spectroscopy was used to identify the kinetics of processes during the formation of the faujasite (FAU) zeolite lattice from a hydrous gel. Using solid-state 27Al MAS NMR, the autocatalytic transformation from the amorphous gel into the crystalline material was monitored. Al-XANES shows that most Al already adopts a tetrahedral coordination in the X-ray-amorphous aluminosilicate at the beginning of the induction period, which hardly changes throughout the rest of the synthesis. Using 23Na NMR spectroscopy, environments in the growing zeolite crystal were identified and used to define the processes in the stepwise formation of the zeolite lattice. The end of the induction period was accompanied by a narrowing of the 27Al and 23Na MAS NMR peak widths, indicating the increased long-range order. The experiments show conclusively that the formation of faujasite occurs via the continuous formation and subsequent condensation of intermediary sodalite-like units that constitute the key building block of the zeolite. Acknowledgement The authors thank T. Huthwelker for assistance with XAFS experiment setup at the Swiss Light Source (PSI, Switzerland). Further, we would like to acknowledge V. Shutthanandan and B.W. Arey for performing Helium ion microscopy as well as Z. Zhao, N.R. Jaeger, M. Weng,more » C. Wan and M. Hu for aiding in the NMR experimental procedure. T. Varga is acknowledged for his help with the capillary XRD. A.V., D.M.C., J.H., J.L.F and J.A.L. were supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences. S.P. and M.A.D. acknowledge support by the Materials Synthesis and Simulation Across Scales (MS3 Initiative) conducted under Laboratory Directed Research & Development Program at PNNL. The in situ NMR experiments were supported by the U. S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Biosciences and Geosciences. Part of the research described in this paper was performed in the Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility sponsored by the DOE’s Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory (PNNL). PNNL is operated for the US DOE by Battelle.« less

Authors:
ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2]
  1. Institute for Integrated Catalysis, Pacific Northwest National Laboratory, P.O. Box 999, Richland, Washington 99352, United States
  2. Institute for Integrated Catalysis, Pacific Northwest National Laboratory, P.O. Box 999, Richland, Washington 99352, United States; Department of Chemistry and Catalysis Research Institute, TU München, Lichtenbergstrasse 4, 85748 Garching, Germany
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1430418
Report Number(s):
PNNL-SA-130041
Journal ID: ISSN 0897-4756
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Chemistry of Materials; Journal Volume: 30; Journal Issue: 3
Country of Publication:
United States
Language:
English
Subject:
zeolite synthesis; in situ characterization; solid-state NMR; x-ray absorption spectroscopy; faujasite

Citation Formats

Prodinger, Sebastian, Vjunov, Aleksei, Hu, Jian Zhi, Fulton, John L., Camaioni, Donald M., Derewinski, Miroslaw A., and Lercher, Johannes A. Elementary Steps of Faujasite Formation Followed by in Situ Spectroscopy. United States: N. p., 2018. Web. doi:10.1021/acs.chemmater.7b04554.
Prodinger, Sebastian, Vjunov, Aleksei, Hu, Jian Zhi, Fulton, John L., Camaioni, Donald M., Derewinski, Miroslaw A., & Lercher, Johannes A. Elementary Steps of Faujasite Formation Followed by in Situ Spectroscopy. United States. doi:10.1021/acs.chemmater.7b04554.
Prodinger, Sebastian, Vjunov, Aleksei, Hu, Jian Zhi, Fulton, John L., Camaioni, Donald M., Derewinski, Miroslaw A., and Lercher, Johannes A. Wed . "Elementary Steps of Faujasite Formation Followed by in Situ Spectroscopy". United States. doi:10.1021/acs.chemmater.7b04554.
@article{osti_1430418,
title = {Elementary Steps of Faujasite Formation Followed by in Situ Spectroscopy},
author = {Prodinger, Sebastian and Vjunov, Aleksei and Hu, Jian Zhi and Fulton, John L. and Camaioni, Donald M. and Derewinski, Miroslaw A. and Lercher, Johannes A.},
abstractNote = {Ex situ and in situ spectroscopy was used to identify the kinetics of processes during the formation of the faujasite (FAU) zeolite lattice from a hydrous gel. Using solid-state 27Al MAS NMR, the autocatalytic transformation from the amorphous gel into the crystalline material was monitored. Al-XANES shows that most Al already adopts a tetrahedral coordination in the X-ray-amorphous aluminosilicate at the beginning of the induction period, which hardly changes throughout the rest of the synthesis. Using 23Na NMR spectroscopy, environments in the growing zeolite crystal were identified and used to define the processes in the stepwise formation of the zeolite lattice. The end of the induction period was accompanied by a narrowing of the 27Al and 23Na MAS NMR peak widths, indicating the increased long-range order. The experiments show conclusively that the formation of faujasite occurs via the continuous formation and subsequent condensation of intermediary sodalite-like units that constitute the key building block of the zeolite. Acknowledgement The authors thank T. Huthwelker for assistance with XAFS experiment setup at the Swiss Light Source (PSI, Switzerland). Further, we would like to acknowledge V. Shutthanandan and B.W. Arey for performing Helium ion microscopy as well as Z. Zhao, N.R. Jaeger, M. Weng, C. Wan and M. Hu for aiding in the NMR experimental procedure. T. Varga is acknowledged for his help with the capillary XRD. A.V., D.M.C., J.H., J.L.F and J.A.L. were supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences. S.P. and M.A.D. acknowledge support by the Materials Synthesis and Simulation Across Scales (MS3 Initiative) conducted under Laboratory Directed Research & Development Program at PNNL. The in situ NMR experiments were supported by the U. S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Biosciences and Geosciences. Part of the research described in this paper was performed in the Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility sponsored by the DOE’s Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory (PNNL). PNNL is operated for the US DOE by Battelle.},
doi = {10.1021/acs.chemmater.7b04554},
journal = {Chemistry of Materials},
number = 3,
volume = 30,
place = {United States},
year = {Wed Jan 24 00:00:00 EST 2018},
month = {Wed Jan 24 00:00:00 EST 2018}
}