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The combined atomic and molecular layer deposition (ALD/MLD) technique offers a unique way to build-both known and previously unknown-crystalline coordination polymer materials directly from gaseous precursors in a high-quality thin-film form. Here, we demonstrate the ALD/MLD of crystalline Li-, Na-, and K-based 3,5-pyridinedicarboxylate (3,5-PDC) thin films; the Li -3,5-PDC films are of the known Li-ULMOF-4 crystal structure whereas the other as-deposited crystalline films possess structures not previously reported. Another exciting possibility offered by ALD/MLD is the deposition of well-defined but amorphous metal-organic thin films, such as our Mg-, Ca-, Sr-, and Ba-based 3,5-PDC films, which can then be crystallized into water-containing structures through a post-deposition humidity treatment. All together, the new metal-organic structures realized in this study through ALD/MLD comprise a majority of the (anhydrous and water-containing) members of the s-block metal 3,5-pyridinedicarboxylate family.
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http://dx.doi.org/10.1002/chem.201901034 | DOI Listing |
J Am Chem Soc
August 2024
TUM School of Natural Sciences, Department of Chemistry, Institute of Silicon Chemistry and Catalysis Research Center, Technische Universität München, Lichtenbergstraße 4, Garching bei München 85748, Germany.
The activation of C-F bonds has long been regarded as the subject of research in organometallic chemistry, given their synthetic relevance and the fact that fluorine is the most abundant halogen in the Earth's crust. However, C-F bond activation remains a largely unsolved challenge due to the high bond dissociation energies, which was historically dominated by transition metal complexes. Main group elements that can cleave unactivated monofluorobenzene are still quite rare and restricted to s-block complexes with a biphilic nature.
View Article and Find Full Text PDFJ Am Chem Soc
August 2024
Institut für Chemie und Biochemie-Anorganische Chemie, Freie Universität Berlin, Fabeckstrasse 34/36, Berlin 14195, Germany.
Terminal oxygen radicals involving p- and d-block atoms are quite common, but s-block compounds with an oxygen radical character remain rare. Here, we report that alkaline-earth metal beryllium atoms react with OF to form the oxygen beryllium fluorides OBeF and OBeF. These species are characterized by matrix-isolation infrared spectroscopy with isotopic substitution and quantum-chemical calculations.
View Article and Find Full Text PDFAdv Sci (Weinh)
September 2024
College of Materials Science and Engineering, Pinghu Institute of Advanced Materials, Zhejiang University of Technology, Hangzhou, 310014, P. R. China.
Organometallics
June 2024
WestCHEM, Department of Pure and Applied Chemistry, University of Strathclyde, Glasgow G1 1XL, U.K.
Rubidium and cesium are the least studied naturally occurring s-block metals in organometallic chemistry but are in plentiful supply from a sustainability viewpoint as highlighted in the periodic table of natural elements published by the European Chemical Society. This underdevelopment reflects the phenomenal success of organometallic compounds of lithium, sodium, and potassium, but interest in heavier congeners has started to grow. Here, the synthesis and structures of rubidium and cesium bis(amido)alkyl magnesiates [(AM)MgN'alkyl], where N' is the simple heteroamide N(SiMe)(Dipp), and alkyl is Bu or CHSiMe, are reported.
View Article and Find Full Text PDFJ Mol Model
June 2024
Sorbonne Université CNRS, LCT, UMR7616, F-75005, Paris, France.
Context: The s-block metals dissolved in ammonia form metal-ammonia complexes with diffuse electrons which could be used for redox catalysis. In this theoretical paper, we investigated the possibility of the d-bloc transition metals (Mn, Fe, Co, Ni, and Cu) solvated by ammonia. It has been demonstrated that both Mn and Fe atoms undergo into an oxidative reaction with NH forming an inserted species, HMNH.
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