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Metal-organic frameworks (MOFs) are useful synthetic materials that are built by the programmed assembly of metal nodes and organic linkers. The success of MOFs results from the isoreticular principle, which allows families of structurally analogous frameworks to be built in a predictable way. This relies on directional coordinate covalent bonding to define the framework geometry. However, isoreticular strategies do not translate to other common crystalline solids, such as organic salts, in which the intermolecular ionic bonding is less directional. Here we show that chemical knowledge can be combined with computational crystal-structure prediction (CSP) to design porous organic ammonium halide salts that contain no metals. The nodes in these salt frameworks are tightly packed ionic clusters that direct the materials to crystallize in specific ways, as demonstrated by the presence of well-defined spikes of low-energy, low-density isoreticular structures on the predicted lattice energy landscapes. These energy landscapes allow us to select combinations of cations and anions that will form thermodynamically stable, porous salt frameworks with channel sizes, functionalities and geometries that can be predicted a priori. Some of these porous salts adsorb molecular guests such as iodine in quantities that exceed those of most MOFs, and this could be useful for applications such as radio-iodine capture. More generally, the synthesis of these salts is scalable, involving simple acid-base neutralization, and the strategy makes it possible to create a family of non-metal organic frameworks that combine high ionic charge density with permanent porosity.
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http://dx.doi.org/10.1038/s41586-024-07353-9 | DOI Listing |
Adv Sci (Weinh)
December 2024
Key Lab of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education, College of Chemistry and Materials, Jiangxi Normal University, Nanchang, 330022, China.
Oxygen evolution reaction (OER) is an indispensable anode reaction for sustainable hydrogen production from water electrolysis, yet overreliance on metal-based catalysts featured with vibrant d-electrons. It still has notable gap between metal-free and metal-based electrocatalysts, due to lacking accurate and efficient p-band regulation methods on non-metal atoms. Herein, a molecular modularization strategy is proposed for fine-tuning the p-orbital states of series metal-free covalent organic frameworks (COFs) for realizing OER performance beyond benchmark precious metal catalysts.
View Article and Find Full Text PDFTrends Ecol Evol
December 2024
Conservation Science Group, Department of Zoology, Cambridge University, The David Attenborough Building, Pembroke Street, Cambridge, CB2 3QZ, UK.
We discuss the outcomes of our 16th horizon scan of issues that are novel or represent a considerable step-change and have the potential to substantially affect conservation of biological diversity in the coming decade. From an initial 96 topics, our international panel of 32 scientists and practitioners prioritised 15 issues. Technological advances are prominent, including metal and non-metal organic frameworks, deriving rare earth elements from macroalgae, synthetic gene drives in plants, and low-emission cement.
View Article and Find Full Text PDFInt J Biol Macromol
December 2024
The Petroleum and Petrochemical College, Chulalongkorn University, Bangkok 10330, Thailand; Center of Excellence on Petrochemical and Materials Technology, Bangkok 10330, Thailand. Electronic address:
Photocatalytic oxidation emerges as an eco-friendly approach for chemically degrading water-borne organic pollutants. Establishing a more sustainable process for synthesizing photocatalyst membranes with higher efficiency and reusability is crucial for advancing safe water remediation solutions. In this study, we present a novel photocatalytic membrane incorporating bacterial cellulose (BC), a naturally occurring biopolymer with an intricate fibrous network, and graphitic carbon nitride (g-CN), a visible light-responsive non-metal photocatalyst.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
October 2024
Key Laboratory of Advanced Ceramics and Machining Technology, Ministry of Education, School of Materials Science and Engineering, Tianjin University, Tianjin, 300072, China.
Selective CO photoreduction into high-energy-density and high-value-added C products is an ideal strategy to achieve carbon neutrality and energy shortage, but it is still highly challenging due to the large energy barrier of the C-C coupling step and severe exciton annihilation in photocatalysts. Herein, strong and localized charge polarization is successfully induced on the surface of melon-based organic semiconductors by creating dual active sites with a large charge asymmetry. Confirmed by multiscale characterization and theoretical simulations, such asymmetric charge distribution, originated from the oxygen dopants and nitrogen vacancies over melon-based organic semiconductors, reduces exciton binding energy and boosts exciton dissociation.
View Article and Find Full Text PDFCurr Pharm Des
September 2024
Department of Pharmaceutical Chemistry, Institute of Pharmaceutical Research, GLA University, Mathura 281406, India.
A double bond between the nitrogen and carbon atoms characterizes a wide class of compounds known as Schiff bases. The flexibility of Schiff bases is formed from several methods and may be combined with alkyl or aryl substituents. The group is a part of organic compounds, either synthetic or natural, and it serves as a precursor and an intermediate in drugs that have therapeutic action.
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