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Müscher‐Polzin, Philipp; Poschmann, Michael; Näther, Christian; Bensch, Wolfgang

Room Temperature Synthesis of [Pd(cyclam)]5{H3Nb6O19}2 ⋅ 26H2O: a Suitable Precursor for the in‐situ Generation of a Highly Active Catalyst for Light‐Driven Hydrogen Evolution

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  • Medientyp: E-Artikel
  • Titel: Room Temperature Synthesis of [Pd(cyclam)]5{H3Nb6O19}2 ⋅ 26H2O: a Suitable Precursor for the in‐situ Generation of a Highly Active Catalyst for Light‐Driven Hydrogen Evolution
  • Beteiligte: Müscher‐Polzin, Philipp; Poschmann, Michael; Näther, Christian; Bensch, Wolfgang
  • Erschienen: Wiley, 2021
  • Erschienen in: European Journal of Inorganic Chemistry, 2021 (2021) 43, Seite 4482-4488
  • Sprache: Englisch
  • DOI: 10.1002/ejic.202100616
  • ISSN: 1434-1948; 1099-0682
  • Schlagwörter: Inorganic Chemistry
  • Entstehung:
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  • Beschreibung: <jats:title>Abstract</jats:title><jats:p>The first Pd<jats:sup>2+</jats:sup> containing polyoxoniobate [Pd(cyclam)]<jats:sub>5</jats:sub>{H<jats:sub>3</jats:sub>Nb<jats:sub>6</jats:sub>O<jats:sub>19</jats:sub>}<jats:sub>2</jats:sub> ⋅ 26H<jats:sub>2</jats:sub>O (<jats:bold>I</jats:bold>) was prepared at room temperature. In the structure, two hexaniobate clusters are surrounded by a bi‐capped cube formed by Pd<jats:sup>2+</jats:sup> centered complexes. This motif is arranged in a layer‐like fashion with crystal water molecules located between cations and anions. Temperature resolved <jats:italic>in‐situ</jats:italic> X‐ray diffraction experiments demonstrate that successive removal of the crystal water molecules leads to formation of several crystalline intermediate phases. Water sorption investigations show that thermally removed H<jats:sub>2</jats:sub>O can be successfully reintegrated proceeding via two distinct steps. The catalytic performance for the light‐driven hydrogen evolution reaction (HER) was investigated in a sacrificial system and fluorescein Na<jats:sup>+</jats:sup> salt as sensitizer yielding a high value of 90 μmol/h H<jats:sub>2</jats:sub>. Surprisingly, a composite Pd@Na<jats:sub>7</jats:sub>[HNb<jats:sub>6</jats:sub>O<jats:sub>19</jats:sub>] ⋅ 15H<jats:sub>2</jats:sub>O is <jats:italic>in‐situ</jats:italic> formed during the catalytic reaction by cation exchange with simultaneous reduction of Pd<jats:sup>2+</jats:sup> nanoparticles decorating the hexaniobate support. The recovered catalyst was even more active producing 157 μmol/h H<jats:sub>2</jats:sub> with an apparent quantum efficiency of 1.85 %. Photocatalytic experiments performed with <jats:italic>ex‐situ</jats:italic> generated Pd nanoparticles deposited on Na<jats:sub>7</jats:sub>[HNb<jats:sub>6</jats:sub>O<jats:sub>19</jats:sub>] ⋅ 15H<jats:sub>2</jats:sub>O show much lower activities indicating a synergistic effect of the <jats:italic>in‐situ</jats:italic> generated Pd@Na<jats:sub>7</jats:sub>[HNb<jats:sub>6</jats:sub>O<jats:sub>19</jats:sub>] ⋅ 15H<jats:sub>2</jats:sub>O catalyst.</jats:p>