Panoramic Synthesis as an Effective Materials Discovery Tool: The System Cs/Sn/P/Se as a Test Case.

The common approach to the synthesis of a new material involves reactions held at high temperatures under certain conditions such as heating in a robust vessel in the dark for a period until it is judged to have concluded. Analysis of the vessel contents afterward provides knowledge of the final pro...

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Publicado en:Journal of the American Chemical Society Vol. 139; no. 31; pp. 10814 - 10822
Autores principales: Haynes, Alyssa S., Stoumpos, Constantinos C., Haijie Chen, Chica, Daniel, Kanatzidis, Mercouri G.
Formato: Artículo
Publicado: American Chemical Society 8/9/2017
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Acceso en línea:Ver este registro en EBSCOhost
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      dt: 8/9/2017
      vid: 139
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      pub: American Chemical Society
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        10.1021/jacs.7b05423
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        atl: Panoramic Synthesis as an Effective Materials Discovery Tool: The System Cs/Sn/P/Se as a Test Case.
      aug:
        au:
          Haynes, Alyssa S.
          Stoumpos, Constantinos C.
          Haijie Chen
          Chica, Daniel
          Kanatzidis, Mercouri G.
        affil:
          Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States
          Materials Science Division, Argonne National Laboratory, Lemont, Illinois 60439, United States
      su:
        Heating
        X-ray diffraction
        Ships
        Synchrotrons
        Crystallization
      sug:
        subj:
          Heating
          X-ray diffraction
          Ships
          Synchrotrons
          Crystallization
      ab: The common approach to the synthesis of a new material involves reactions held at high temperatures under certain conditions such as heating in a robust vessel in the dark for a period until it is judged to have concluded. Analysis of the vessel contents afterward provides knowledge of the final products only. Intermediates that may form during the reaction process remain unknown. This lack of awareness of transient intermediates represents lost opportunities for discovering materials or understanding how the final products form. Here we present new results using an emerging in situ monitoring approach that shows high potential in discovering new compounds. In situ synchrotron X-ray diffraction studies were conducted in the Cs/Sn/P/Se system. Powder mixtures of CsSe, Sn, and PSe were heated to 650 °C and then cooled to room temperature while acquiring consecutive in situ synchrotron diffraction patterns from the beginning to the end of the reaction process. The diffraction data was translated into the relationship of phases present versus temperature. Seven known crystalline phases were observed to form on warming in the experiment: Sn, CsSe, CsSe, CsSe, CsSnSe, CsPSe, and CsPSe. Six unknown phases were also detected; using the in situ synchrotron data as a guide three of them were isolated and characterized ex situ. These are CsSn(PSe), α-CsSnPSe, and Cs(SnSe)[Sn(PSe )]. Cs(SnSe)[Sn(PSe )] is a two-dimensional compound that behaves as an n-type doped semiconductor below 50 K and acts more like a semimetal at higher temperatures. Because all crystalline phases are revealed during the reaction, we call this approach "panoramic synthesis".
      pubtype: Academic Journal
      doctype: Article
      src: R
    language: English
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