Modulating Inorganic Dimensionality of Ultrastable Lead Halide Coordination Polymers for Photocatalytic CO2 Reduction to Ethanol

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(16)

Published: Feb. 22, 2024

Lead halide hybrids have shown great potentials in CO

Language: Английский

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Enhancing the Water‐Stability of 1D Hybrid Manganese Halides by a Cationic Engineering Strategy

Advanced Optical Materials, Journal Year: 2024, Volume and Issue: 12(13)

Published: Feb. 13, 2024

Abstract Although the luminescent performance of organic–inorganic metal halides (OIMHs) have obtained significant advances, achieving intrinsic water‐stable OIMHs remain a substantial challenge due to fragile ionic nature hybrid halide structure. To overcome these challenges, structural design strategy is proposed that involves use highly hydrophobic cations as protective layer improve water stability OIMH. Herein, an aprotic trimethylsulfoxonium [TMSO] + selected cation and successfully assemble two new manganese based (TMSO)MnCl 3 (TMSO)MnBr through facile solid liquid phase reaction methods. Remarkably, exhibit strong red light emissions with high quantum yields recorded at 86.1% 53.4%, respectively, originating from octahedral [MnX 6 ] 4− one‐dimensional (1D) − chain. Most significantly, present extraordinary stabilities toward continuous corrosion by humid air, water, acid‐aqueous solution for more than one month, suggesting promising application prospects in extreme chemical environments. In‐depth Hirshfeld surface calculations demonstrate ultrahigh water‐stability benefits abundant hydrogen bonds electrostatic interactions between ions, which provides underlying insight into mechanism. This enhancement represents breakthrough engineering rationally

Language: Английский

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Water‐Stable 0D Hybrid Manganese Halides with Adjustable Crystal Structure and Emission Color

Advanced Optical Materials, Journal Year: 2023, Volume and Issue: 11(23)

Published: July 27, 2023

Abstract Despite the ultra‐high photoluminescence quantum yield (PLQY) of 0D hybrid manganese halides as state‐of‐the‐art luminescent materials, intrinsic water stability remains an unsurpassable barrier due to serious hygroscopicity hydrogen‐bonding structure. Herein, a synthetic strategy that realizes adjustable emission color and high resistance in chloride family based on same cation [H 2 TMDAP] 2+ (TMDAP = N , ′, ′‐tetramethyl‐1,3‐diaminopropane) is reported. Specifically, direct solution or solid‐state reaction precursor materials generates 3 [MnCl 4 ] [Mn Cl 6 ], while additional Zn ‐doping structural directing agent results TMDAP]Mn 0.63 0.37 . Functionally, [Mn/ZnCl 2− tetrahedron displays green light at 521 nm with PLQY 63.9%. composed 4− octahedron chain discrete tetrahedron, but it only exhibits single red 628 48.1%. Compared water‐instable represents extraordinary chemical humid air over 1 month, manifested by unchanged lattice sufficient intensity. Significantly, proof performance nearly unmatchable among all previously reported far known. The combined merits tunable wavelength, PLQY, highlight potential applications title lighting display diodes.

Language: Английский

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Solar‐Driven Conversion of CO₂ to C₂ Products by the 3d Transition Metal Intercalates of Layered Lead Iodides

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(30)

Published: May 2, 2024

Abstract Photocatalytic CO 2 reduction to high‐value‐added C 2+ products presents significant challenges, which is attributed the slow kinetics of multi‐e − photoreduction and high thermodynamic barrier for C–C coupling. Incorporating redox‐active Co /Ni cations into lead halide photocatalysts has potentials improve carrier transport introduce charge polarized bimetallic sites, addressing kinetic issues, respectively. In this study, a coordination‐driven synthetic strategy developed 3d transition metals interlamellar region layered organolead iodides with atomic precision. The resultant hybrids exhibit selective H 5 OH using O vapor at evolution rates 24.9–31.4 µmol g −1 h selectivity 89.5–93.6%, while pristine iodide yields only 1 products. Band structure calculations photoluminescence studies indicate that interlayer species greatly contribute frontier orbitals enhance exciton dissociation free carriers, facilitating between adjacent layers. addition, Bader distribution in situ experimental spectroscopic reveal asymmetric Ni–O–Pb catalytic sites intrinsic polarization, promoting coupling leading formation key *OC–CHO intermediate.

Language: Английский

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Highly Stable MOF‐Type Lead Halide Luminescent Ferroelectrics

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(29)

Published: May 15, 2024

Abstract Lead halide molecular ferroelectrics represent an important class of luminescent ferroelectrics, distinguished by their high chemical and structural tunability, excellent processability distinctive characteristics. However, inherent instability, prone to decomposition upon exposure moisture light, hinders broader ferroelectric applications. Herein, for the first time, we present a series isoreticular metal–organic framework (MOF)‐type lead demonstrating exceptional robustness under ambient conditions at least 15 months even when subjected aqueous boiling conditions. Unlike conventional metal‐oxo secondary building units (SBUs) in MOFs adopting highly centrosymmetric structure with limited distortion, our halide‐based occupy structurally deformable [Pb 2 X] + (X=Cl − /Br /I ) SBUs that facilitate c ‐axis‐biased displacement Pb 2+ centers substantially contribute thermoinducible transformation. Importantly, this MOF‐type undergo ferroelectric‐to‐paraelectric phase transitions remarkably Curie temperature up 505 K, superior most ferroelectrics. Moreover, covalent bonding between phosphorescent organic component light‐harvesting inorganic achieves efficient spin‐orbit coupling intersystem crossing, resulting long‐lived afterglow emission. The compelling combination stability, ferroelectricity emission exhibited opens many potential opportunities energy‐conversion

Language: Английский

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Implanting MOF Co-doped carbon nanotubes into PVP as flame-retardant to fabricate high performance PVA/SA aerogel nanocomposites

Journal of environmental chemical engineering, Journal Year: 2024, Volume and Issue: 12(2), P. 111977 - 111977

Published: Feb. 1, 2024

Language: Английский

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Promoting the formation of metal–carboxylate coordination to modulate the dimensionality of ultrastable lead halide hybrids

Chemical Science, Journal Year: 2024, Volume and Issue: 15(8), P. 2848 - 2856

Published: Jan. 1, 2024

Crystal engineering of metal halide hybrids is critical to investigate their structure-property relationship and advance photophysical applications, but there have been limited efforts employ coordination chemistry precisely control the dimensionality sublattices. Herein, we present a coordination-assembly synthetic strategy developed for rational modulation lead dimensionality, realizing transition from 2D 3D architectures. This manipulation achieved by utilizing three organocarboxylates featuring identical cyclohexane backbone unit. Specifically, 1,4-cyclohexanedicarboxylate 1,2,4,5-cyclohexanetetracarboxylate ligands facilitate formation quasi-2D layered structures, characterized weakly corrugated strongly layers, respectively. Importantly, introduction 1,2,3,4,5,6-cyclohexanehexacarboxylate ligand results in architectures chloride/bromide The templated affords extended wavelength coverage superior carrier transport properties compared analogues. both halide-based polymers exhibit high aqueous stability over wide pH range, outperforming conventional ionic-bound halides. Notably, chemically stable bromide exhibits efficient photocatalytic ethylbenzene oxidation with conversion rate 498 μmol g

Language: Английский

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Syntheses and photochemically antibiotic degradation of two Co(II)-based coordination polymers

Polyhedron, Journal Year: 2024, Volume and Issue: 255, P. 116958 - 116958

Published: March 30, 2024

Language: Английский

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Synthesis and characterization of mixed ligands based Co(II)-based coordination polymers and study their photochemically antibiotic degradation

Inorganica Chimica Acta, Journal Year: 2024, Volume and Issue: 569, P. 122133 - 122133

Published: May 10, 2024

Language: Английский

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A novel iodo bridged 1D CuI coordination polymer containing N,N-bidentate Schiff base ligand: Synthesis, structure, theoretical studies, electrochemical properties, and catalytic activity in the synthesis of tetrahydropyrimidines

Polyhedron, Journal Year: 2023, Volume and Issue: 249, P. 116754 - 116754

Published: Nov. 29, 2023

Language: Английский

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