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Link to Densify: Topological Transitions and Origin of Hysteresis During the Compression and Decompression of Amorphous Ices.
Phys Rev Lett
December 2024
BM Research Europe, Hartree Centre, Daresbury WA4 4AD, United Kingdom.
In this Letter, we study the phase transition between amorphous ices and the nature of the hysteresis cycle separating them. We discover that a topological transition takes place as the system transforms from low-density amorphous ice (LDA) at low pressures to high-density amorphous ice (HDA) at high pressures. Specifically, we uncover that the hydrogen bond network (HBN) displays qualitatively different topologies in the LDA and HDA phases: the former characterized by disentangled loop motifs, with the latter displaying topologically complex long-lived Hopf-linked and knotted configurations.
View Article and Find Full Text PDFTransient Triplet Metallopnictinidenes M-Pn (M = Pd, Pt; Pn = P, As, Sb): Characterization and Dimerization.
J Am Chem Soc
January 2025
Institut für Anorganische Chemie and International Center for Advanced Studies of Energy Conversion, Georg-August-Universität Göttingen, Tammannstr 4, 37077 Göttingen, Germany.
Nitrenes (R-N) have been subject to a large body of experimental and theoretical studies. The fundamental reactivity of this important class of transient intermediates has been attributed to their electronic structures, particularly the accessibility of triplet vs singlet states. In contrast, electronic structure trends along the heavier pnictinidene analogues (R-Pn; Pn = P-Bi) are much less systematically explored.
View Article and Find Full Text PDFCo-organic 'soft' metallo-supramolecular polymer nanofibers for efficient photoreduction of CO.
Chem Sci
January 2025
Chemistry and Physics of Materials Unit, School of Advanced Materials (SAMat), Jawaharlal Nehru Centre for Advanced Scientific Research Jakkur Bangalore 560064 India https://www.jncasr.ac.in/faculty/tmaji.
Coordination-driven metallo-supramolecular polymers hold significant potential as highly efficient catalysts for photocatalytic CO reduction, owing to the covalent integration of the light harvesting unit, catalytic center and intrinsic hierarchical nanostructures. In this study, we present the synthesis, characterization, and gelation behaviour of a novel low molecular weight gelator (LMWG) integrating a benzo[1,2-:4,5-']dithiophene core with terpyridine (TPY) units alkyl amide chains (TPY-BDT). The two TPY ends of the TPY-BDT unit efficiently chelate with metal ions, enabling the formation of a metallo-supramolecular polymer that brings together the catalytic center and a photosensitizer in close proximity, maximizing catalytic efficiency for CO reduction.
View Article and Find Full Text PDFSequential and Time-Controlled Sol-Gel Transitions by Mechanical Switching of Molecular Tweezers.
J Am Chem Soc
January 2025
Sorbonne Université, CNRS, Institut Parisien de Chimie Moléculaire, IPCM, 4 place Jussieu, Paris 75005, France.
Controlling the motion of molecular machines to influence higher-order structures is well-established in biological systems but remains a significant challenge for synthetic analogs. Herein, we aim to harness the mechanical switching of switchable molecular tweezers to modulate their self-assembly and produce stimuli-responsive organogels. We report a series of terpy(Pt-salphen) molecular tweezers functionalized with alkyl chains that act as low-molecular-weight gelators (LMWGs) in their open conformation.
View Article and Find Full Text PDFPreparation of ,-[Pt(py)(N)(OH)] via Photoinduced Reactivity of [Pt(NO)] Anion.
Inorg Chem
January 2025
Nikolaev Institute of Inorganic Chemistry, Siberian Branch of the Russian Academy of Science, 630090 Novosibirsk, Russia.
The photoinduced reaction of [Pt(NO)] with pyridine or its derivatives (L) was found to result in the formation of [PtL](NO) salts in high yield. This transformation was successfully probed for methyl- and carboxyethyl-substituted pyridines, and the corresponding [PtL](NO) salts were isolated and fully characterized using single-crystal X-ray diffraction (SCXRD). Anation of the [Pt(py)] cationic complex with N was studied by H NMR spectroscopy in aqueous and water/dimethyl sulfoxide solutions of [Pt(py)](NO).
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