In situ X-ray diffraction monitoring of a mechanochemical reaction reveals a unique topology metal-organic framework

Chemical and physical transformations by milling are attracting enormous interest for their ability to access new materials and clean reactivity, and are central to a number of core industries, from mineral processing to pharmaceutical manufacturing. While continuous mechanical stress during milling...

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Published in:Nature communications Vol. 6; no. 1; p. 6662
Main Authors: Katsenis, Athanassios D., Puškarić, Andreas, Štrukil, Vjekoslav, Mottillo, Cristina, Julien, Patrick A., Užarević, Krunoslav, Pham, Minh-Hao, Do, Trong-On, Kimber, Simon A. J., Lazić, Predrag, Magdysyuk, Oxana, Dinnebier, Robert E., Halasz, Ivan, Friščić, Tomislav
Format: Journal Article
Language:English
Published: London Nature Publishing Group UK 23.03.2015
Nature Publishing Group
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ISSN:2041-1723, 2041-1723
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Abstract Chemical and physical transformations by milling are attracting enormous interest for their ability to access new materials and clean reactivity, and are central to a number of core industries, from mineral processing to pharmaceutical manufacturing. While continuous mechanical stress during milling is thought to create an environment supporting nonconventional reactivity and exotic intermediates, such speculations have remained without proof. Here we use in situ , real-time powder X-ray diffraction monitoring to discover and capture a metastable, novel-topology intermediate of a mechanochemical transformation. Monitoring the mechanochemical synthesis of an archetypal metal-organic framework ZIF-8 by in situ powder X-ray diffraction reveals unexpected amorphization, and on further milling recrystallization into a non-porous material via a metastable intermediate based on a previously unreported topology, herein named katsenite ( kat ). The discovery of this phase and topology provides direct evidence that milling transformations can involve short-lived, structurally unusual phases not yet accessed by conventional chemistry. Ball milling chemical reactions are of interest due to their environmental credentials and potential to achieve new reactions and materials. Here, the authors isolate a metastable material with a previously unknown net topology by in situ monitoring of the mechanosynthesis of a metal organic framework.
AbstractList Chemical and physical transformations by milling are attracting enormous interest for their ability to access new materials and clean reactivity, and are central to a number of core industries, from mineral processing to pharmaceutical manufacturing. While continuous mechanical stress during milling is thought to create an environment supporting nonconventional reactivity and exotic intermediates, such speculations have remained without proof. Here we use in situ , real-time powder X-ray diffraction monitoring to discover and capture a metastable, novel-topology intermediate of a mechanochemical transformation. Monitoring the mechanochemical synthesis of an archetypal metal-organic framework ZIF-8 by in situ powder X-ray diffraction reveals unexpected amorphization, and on further milling recrystallization into a non-porous material via a metastable intermediate based on a previously unreported topology, herein named katsenite ( kat ). The discovery of this phase and topology provides direct evidence that milling transformations can involve short-lived, structurally unusual phases not yet accessed by conventional chemistry. Ball milling chemical reactions are of interest due to their environmental credentials and potential to achieve new reactions and materials. Here, the authors isolate a metastable material with a previously unknown net topology by in situ monitoring of the mechanosynthesis of a metal organic framework.
Chemical and physical transformations by milling are attracting enormous interest for their ability to access new materials and clean reactivity, and are central to a number of core industries, from mineral processing to pharmaceutical manufacturing. While continuous mechanical stress during milling is thought to create an environment supporting nonconventional reactivity and exotic intermediates, such speculations have remained without proof. Here we use in situ, real-time powder X-ray diffraction monitoring to discover and capture a metastable, novel-topology intermediate of a mechanochemical transformation. Monitoring the mechanochemical synthesis of an archetypal metal-organic framework ZIF-8 by in situ powder X-ray diffraction reveals unexpected amorphization, and on further milling recrystallization into a non-porous material via a metastable intermediate based on a previously unreported topology, herein named katsenite (kat). The discovery of this phase and topology provides direct evidence that milling transformations can involve short-lived, structurally unusual phases not yet accessed by conventional chemistry.
Chemical and physical transformations by milling are attracting enormous interest for their ability to access new materials and clean reactivity, and are central to a number of core industries, from mineral processing to pharmaceutical manufacturing. While continuous mechanical stress during milling is thought to create an environment supporting nonconventional reactivity and exotic intermediates, such speculations have remained without proof. Here we use in situ, real-time powder X-ray diffraction monitoring to discover and capture a metastable, novel-topology intermediate of a mechanochemical transformation. Monitoring the mechanochemical synthesis of an archetypal metal-organic framework ZIF-8 by in situ powder X-ray diffraction reveals unexpected amorphization, and on further milling recrystallization into a non-porous material via a metastable intermediate based on a previously unreported topology, herein named katsenite (kat). The discovery of this phase and topology provides direct evidence that milling transformations can involve short-lived, structurally unusual phases not yet accessed by conventional chemistry.Chemical and physical transformations by milling are attracting enormous interest for their ability to access new materials and clean reactivity, and are central to a number of core industries, from mineral processing to pharmaceutical manufacturing. While continuous mechanical stress during milling is thought to create an environment supporting nonconventional reactivity and exotic intermediates, such speculations have remained without proof. Here we use in situ, real-time powder X-ray diffraction monitoring to discover and capture a metastable, novel-topology intermediate of a mechanochemical transformation. Monitoring the mechanochemical synthesis of an archetypal metal-organic framework ZIF-8 by in situ powder X-ray diffraction reveals unexpected amorphization, and on further milling recrystallization into a non-porous material via a metastable intermediate based on a previously unreported topology, herein named katsenite (kat). The discovery of this phase and topology provides direct evidence that milling transformations can involve short-lived, structurally unusual phases not yet accessed by conventional chemistry.
ArticleNumber 6662
Author Puškarić, Andreas
Dinnebier, Robert E.
Halasz, Ivan
Pham, Minh-Hao
Lazić, Predrag
Magdysyuk, Oxana
Katsenis, Athanassios D.
Užarević, Krunoslav
Kimber, Simon A. J.
Julien, Patrick A.
Do, Trong-On
Friščić, Tomislav
Štrukil, Vjekoslav
Mottillo, Cristina
Author_xml – sequence: 1
  givenname: Athanassios D.
  surname: Katsenis
  fullname: Katsenis, Athanassios D.
  organization: Department of Chemistry, McGill University
– sequence: 2
  givenname: Andreas
  surname: Puškarić
  fullname: Puškarić, Andreas
  organization: Ruđer Bošković Institute
– sequence: 3
  givenname: Vjekoslav
  surname: Štrukil
  fullname: Štrukil, Vjekoslav
  organization: Department of Chemistry, McGill University, Ruđer Bošković Institute
– sequence: 4
  givenname: Cristina
  surname: Mottillo
  fullname: Mottillo, Cristina
  organization: Department of Chemistry, McGill University
– sequence: 5
  givenname: Patrick A.
  surname: Julien
  fullname: Julien, Patrick A.
  organization: Department of Chemistry, McGill University
– sequence: 6
  givenname: Krunoslav
  surname: Užarević
  fullname: Užarević, Krunoslav
  organization: Ruđer Bošković Institute
– sequence: 7
  givenname: Minh-Hao
  surname: Pham
  fullname: Pham, Minh-Hao
  organization: Department of Chemical Engineering, Université Laval
– sequence: 8
  givenname: Trong-On
  surname: Do
  fullname: Do, Trong-On
  organization: Department of Chemical Engineering, Université Laval
– sequence: 9
  givenname: Simon A. J.
  surname: Kimber
  fullname: Kimber, Simon A. J.
  organization: ESRF—The European Synchrotron
– sequence: 10
  givenname: Predrag
  surname: Lazić
  fullname: Lazić, Predrag
  organization: Ruđer Bošković Institute
– sequence: 11
  givenname: Oxana
  surname: Magdysyuk
  fullname: Magdysyuk, Oxana
  organization: Scientific Service Group X-ray Diffraction, Max Planck Institute for Solid State Research
– sequence: 12
  givenname: Robert E.
  surname: Dinnebier
  fullname: Dinnebier, Robert E.
  organization: Scientific Service Group X-ray Diffraction, Max Planck Institute for Solid State Research
– sequence: 13
  givenname: Ivan
  surname: Halasz
  fullname: Halasz, Ivan
  email: ihalasz@irb.hr
  organization: Ruđer Bošković Institute
– sequence: 14
  givenname: Tomislav
  surname: Friščić
  fullname: Friščić, Tomislav
  email: tomislav.friscic@mcgill.ca
  organization: Department of Chemistry, McGill University
BackLink https://www.ncbi.nlm.nih.gov/pubmed/25798542$$D View this record in MEDLINE/PubMed
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ContentType Journal Article
Copyright Springer Nature Limited 2015
Copyright Nature Publishing Group Mar 2015
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SubjectTerms 119/118
639/301/930/1032
639/638/11/879
639/638/263/406
Acids
Humanities and Social Sciences
Mineral processing
multidisciplinary
Porous materials
Radiation
Science
Science (multidisciplinary)
Topology
X-ray diffraction
X-rays
Title In situ X-ray diffraction monitoring of a mechanochemical reaction reveals a unique topology metal-organic framework
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