skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: X-ray and Neutron Scattering Study of the Formation of Core–Shell-Type Polyoxometalates

Abstract

A typical type of core-shell polyoxometalates can be obtained through the Keggin-type polyoxometalate-templated growth of a layer of spherical shell structure of {Mo 72Fe 30}. Small angle X-ray scattering is used to study the structural features and stability of the core-shell structures in aqueous solutions. Time-resolved small angle X-ray scattering is applied to monitor the synthetic reactions and a three-stage formation mechanism is proposed to describe the synthesis of the core-shell polyoxometalates based on the monitoring results. Quasi-elastic and inelastic neutron scattering are used to probe the dynamics of water molecules in the core-shell structures and two different types of water molecules, the confined and structured water, are observed. These water molecules play an important role in bridging core and shell structures and stabilizing the cluster structures. A typical type of core shell polyoxometalates can be obtained through the Keggin-type polyoxometalate-templated growth of a layer of spherical shell structure of {Mo 72Fe 30}. Small-angle X-ray scattering is used to study the structural features and stability of the core shell structures in aqueous solutions. Time-resolved small-angle X-ray scattering is applied to monitor the synthetic reactions, and a three-stage formation mechanism is proposed to describe the synthesis of the core shell polyoxometalatesmore » based on the monitoring results. New protocols have been developed by fitting the X-ray data with custom physical models, which provide more convincing, objective, and completed data interpretation. Quasi-elastic and inelastic neutron scattering are used to probe the dynamics of water molecules in the core shell structures, and two different types of water molecules, the confined and structured water, are observed. These water molecules play an important role in bridging core and shell structures and stabilizing the cluster structures.« less

Authors:
 [1];  [2];  [1];  [1];  [1];  [3];  [3];  [4];  [4];  [4];  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical and Engineering Materials Division
  2. Univ. of Tennessee, Knoxville, TN (United States). Department of Physics and Astronomy, Joint Institute of Neutron Science
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1240563
Alternate Identifier(s):
OSTI ID: 1340274
Grant/Contract Number:  
AC05-00OR22725; DE-AC02- 06CH11357; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 138; Journal Issue: 8; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE

Citation Formats

Yin, Panchao, Wu, Bin, Mamontov, Eugene, Daemen, Luke L., Cheng, Yongqiang, Li, Tao, Seifert, Soenke, Hong, Kunlun, Bonnesen, Peter V., Keum, Jong Kahk, and Ramirez-Cuesta, Anibal J. X-ray and Neutron Scattering Study of the Formation of Core–Shell-Type Polyoxometalates. United States: N. p., 2016. Web. doi:10.1021/jacs.5b11465.
Yin, Panchao, Wu, Bin, Mamontov, Eugene, Daemen, Luke L., Cheng, Yongqiang, Li, Tao, Seifert, Soenke, Hong, Kunlun, Bonnesen, Peter V., Keum, Jong Kahk, & Ramirez-Cuesta, Anibal J. X-ray and Neutron Scattering Study of the Formation of Core–Shell-Type Polyoxometalates. United States. doi:10.1021/jacs.5b11465.
Yin, Panchao, Wu, Bin, Mamontov, Eugene, Daemen, Luke L., Cheng, Yongqiang, Li, Tao, Seifert, Soenke, Hong, Kunlun, Bonnesen, Peter V., Keum, Jong Kahk, and Ramirez-Cuesta, Anibal J. Fri . "X-ray and Neutron Scattering Study of the Formation of Core–Shell-Type Polyoxometalates". United States. doi:10.1021/jacs.5b11465. https://www.osti.gov/servlets/purl/1240563.
@article{osti_1240563,
title = {X-ray and Neutron Scattering Study of the Formation of Core–Shell-Type Polyoxometalates},
author = {Yin, Panchao and Wu, Bin and Mamontov, Eugene and Daemen, Luke L. and Cheng, Yongqiang and Li, Tao and Seifert, Soenke and Hong, Kunlun and Bonnesen, Peter V. and Keum, Jong Kahk and Ramirez-Cuesta, Anibal J.},
abstractNote = {A typical type of core-shell polyoxometalates can be obtained through the Keggin-type polyoxometalate-templated growth of a layer of spherical shell structure of {Mo72Fe30}. Small angle X-ray scattering is used to study the structural features and stability of the core-shell structures in aqueous solutions. Time-resolved small angle X-ray scattering is applied to monitor the synthetic reactions and a three-stage formation mechanism is proposed to describe the synthesis of the core-shell polyoxometalates based on the monitoring results. Quasi-elastic and inelastic neutron scattering are used to probe the dynamics of water molecules in the core-shell structures and two different types of water molecules, the confined and structured water, are observed. These water molecules play an important role in bridging core and shell structures and stabilizing the cluster structures. A typical type of core shell polyoxometalates can be obtained through the Keggin-type polyoxometalate-templated growth of a layer of spherical shell structure of {Mo72Fe30}. Small-angle X-ray scattering is used to study the structural features and stability of the core shell structures in aqueous solutions. Time-resolved small-angle X-ray scattering is applied to monitor the synthetic reactions, and a three-stage formation mechanism is proposed to describe the synthesis of the core shell polyoxometalates based on the monitoring results. New protocols have been developed by fitting the X-ray data with custom physical models, which provide more convincing, objective, and completed data interpretation. Quasi-elastic and inelastic neutron scattering are used to probe the dynamics of water molecules in the core shell structures, and two different types of water molecules, the confined and structured water, are observed. These water molecules play an important role in bridging core and shell structures and stabilizing the cluster structures.},
doi = {10.1021/jacs.5b11465},
journal = {Journal of the American Chemical Society},
number = 8,
volume = 138,
place = {United States},
year = {2016},
month = {2}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 8 works
Citation information provided by
Web of Science

Save / Share:

Works referencing / citing this record:

Unprecedented Halide‐Ion Binding and Catalytic Activity of Nanoscale Anionic Metal Oxide Clusters
journal, July 2019


Two new Keggin-type polyoxometalate-based organic-inorganic hybrid compounds with metal ions and chelate ligands
journal, February 2017


Two copper(II)-bbtz modified Keggin and β -octamolybdate compounds captured in one-pot under hydrothermal conditions
journal, February 2017