Angewandte Chemie International Edition
Atomically precise coinage metal nanoclusters possess well-defined structures and distinctive optoelectronic properties. However, their assembly through weak van der Waals interactions often results in inefficient charge migration and rapid electron-hole recombination. Hydrogen-bonded organic frameworks (HOFs) offer an alternative strategy to integrate functional clusters into ordered crystalline…
Efficient xenon/krypton separation remains challenging due to their similar physicochemical properties. Herein, we demonstrate that ligand isomerism can be leveraged as an effective structural handle for constructing new metal-organic frameworks from readily available, low-cost amino acids. Using leucine and isoleucine-two constitutional regioisomers among proteinogenic amino acids that possess t…
Polycarbonate (PC) is among the most challenging plastics to recycle because its robust aromatic C─O linkages resist conventional depolymerization strategies. Here, we report the first visible-light-driven photocatalytic system for the reductive depolymerization and hydrodeoxygenation of PC under ambient conditions, selectively producing propane-2,2-diyldicyclohexane (DCHP), a saturated hydrocarb…
Chemoselective cysteine modification is pivotal for chemical biology and drug discovery. While photochemical strategies offer spatiotemporal control, most current methods rely on exogenous catalysts, complicating purification processes. Furthermore, the structural diversity of accessible conjugates remains limited. Here, we report an additive/catalyst-free, visible-light-driven platform for diver…
Chirality is an important determinant of drug action, as enantiomers can exhibit markedly different pharmacological and toxicological profiles. Although the importance of stereochemistry in drug efficacy is well established, its role in drug metabolism and disposition remains comparatively underexplored, despite the inherently stereoselective nature of drug metabolizing enzymes. Given the high pr…
As a fundamental phenomenon in nature, chirality has been extensively studied in molecular structures; however, it remains underexplored at the electronic level. Understanding how structural chirality transfers into electronic states is crucial for uncovering the essence of many chiral effects. In this study, we report the engineering and direct visualization of chiral electronic states within an…
Solvent-free solid polymer electrolytes (SPEs) suffer from sluggish and discontinuous Li<sup>+</sup> transport. Although high-polarity fillers enhance dissociation, liberated Li<sup>+</sup> tends to be trapped on filler surfaces due to the spatial and dynamic mismatches, hindering Li<sup>+</sup> long-range migration. To bridge this gap, we establish a consecutive Li<sup>+</sup> transport pathway …
High-potential organic redox-active molecules are crucial for high-energy-density aqueous organic flow batteries (AOFBs). Azopyridine (AZO) derivatives with high redox potential (0.86 V vs. SHE) suffer from structural rearrangement instability and slow redox kinetics during the oxidation process. Herein, we achieve dual-target modulation of the electronic structure and dynamic steric hindrance, w…
Lithium-sulfur batteries (LSBs) hold great promise as next-generation energy storage devices, owing to their ultrahigh theoretical energy density (2600 Wh kg<sup>-1</sup>). However, their real-world implementation is limited by the polysulfide shuttle effect and the poor electrical conductivity of sulfur species. To address these problems and achieve high-performance LSBs, it is crucial to develo…
Quantum chemical calculation using density functional theory at the BP86-D3(BJ)/def2-TZVPP level and ab initio theory at the CCSD(T)/def2-TZVPP level have been carried out for the homoleptic and heteroleptic borylones L1-B(Ph)-L2 with the ligands L1, L2 = PPh<sub>3</sub>, SPh<sub>2</sub>, N<sub>2</sub>, CO, CS, NHC<sup>Me</sup>, CAAC<sup>Me</sup>. The computation of the bond dissociation energy s…
Proteolysis-targeting chimeras (PROTACs) are an emerging therapeutic modality via targeted protein degradation, but plagued by concerns about systemic toxicity and a poor pharmacokinetic profile. To tackle the issues, we have devised a photo-click proteolysis targeting chimera (PCPTAC) that enables spatiotemporally controllable intracellular synthesis of PROTACs by photo-triggered bioorthogonal l…
Safe and efficient hydrogen storage is pivotal for enabling a clean hydrogen economy. Liquid organic hydrogen carriers (LOHCs) offer a practical solution, but their deployment is hindered by the lack of highly active and economical dehydrogenation catalysts. Here, we report a metal-free catalyst design that overcomes the long-standing trade-off between crystallinity and surface area in two-dimens…
Low-symmetry mechanically interlocked molecules (MIMs) remain challenging targets because of their anisotropic structures and synthetic complexity. We devised a self-sorting strategy employing two unsymmetric flexible bidentate ligands, L<sup>ab</sup> and L<sup>cd</sup>, which co-assemble with two size-differentiated rigid chelating building blocks and half-sandwich organometallic units. This app…
Designing advanced halide-based solid electrolytes (SEs) combining high ionic conductivity and exceptional (electro)chemical stability is crucial for all-solid-state Na-ion batteries (ASSNIBs). However, most sodium-based halide systems remain restricted in high-voltage ASSNIB applications, due to their low conductivity from blocked ion-diffusion channels, and insufficient oxidation stability caus…
O<sub>2</sub> binding to metal ions is an essential step in the oxygen reduction reaction (ORR). Tailoring O<sub>2</sub> binding is anticipated to realize highly active and selective four-electron ORR. Herein, we report on fine-tuning the molecular pocket of Co porphyrins to get a trade-off between thermodynamics and kinetics of O<sub>2</sub> binding for ORR with high activity and selectivity. Th…
l-(+)-Muscarine is a widespread fatal toxin produced by various mushrooms that pose a severe threat to human health when they are mistaken for edible species. Apart from a single 1970s study that assumed l-glutamate and pyruvate were the building blocks of this unusual quaternary amine, surprisingly little is known about the toxin's biogenesis. We used Collybia rivulosa (syn. Clitocybe rivulosa),…
Because cancer cells have heightened protein homeostasis (proteostasis) requirements, there is interest in targeting proteostasis machinery, including the 70 kDa heat shock proteins (HSP70s), as potential cancer therapeutics. However, studies have shown that the HSP70 family is differentially regulated across cancers, and global targeting may produce unwanted toxicities. For this reason, our lab …
Electronegativity Adaption Approach for Solar‐Blind UV Birefringent Crystals With Ultrawide Bandgaps
Birefringent crystals are essential for modern optics for their ability to modulate light polarization. The steretochemically active lone-pair (SCALP) effect can typically confer high birefringence for materials by driving anisotropic distribution of an electronic clouds. However, a major limitation of SCALP-based birefringent crystals is the obvious red-shift of UV transparency window. Herein, w…
G protein-coupled receptors (GPCRs) are involved in most human physiological processes and one of the largest families of approved drug-targeted proteins. Heterotrimeric Gαβɣ proteins bind to the intracellular cavity of the activated receptor mainly through the C-terminal α5 helix of the Gα subunit (GαCT). Modulation of GPCR activity through intracellular GPCR binding sites is emerging. Here we d…
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