The selective functionalization of sp3 C–H bonds is a versatile tool for the diversification of organic compounds. Combining attractive features of homogeneous and enzymatic catalysts, artificial metalloenzymes offer an ideal means to selectively modify these inert motifs. Herein, we report on a copper(I) heteroscorpionate complex embedded within streptavidin that catalyzes the intramolecular insertion

The development of photopolymers that can be depolymerized and subsequently re-cured using the same light stimulus presents a significant technical challenge. A bio-sourced terpenoid structure, l-carvone, inspired the creation of a re-curable photopolymer in which the orthogonal reactivity of an irreversible thioether and a dynamic thiol-Michael bond enables both photopolymerization and thermally driven

Photosynthetic water oxidation is catalyzed by a manganese–calcium oxide cluster, which experiences five “S-states” during a light-driven reaction cycle. The unique “distorted chair”-like geometry of the Mn4CaO5(6) cluster shows structural flexibility that has been frequently proposed to involve “open” and “closed”-cubane forms from the S1 to S3 states. The isomers are interconvertible in the S1 and

α-Synuclein (α-Syn) is an intrinsically disordered protein which self-assembles into highly organized β-sheet structures that accumulate in plaques in brains of Parkinson’s disease patients. Oxidative stress influences α-Syn structure and self-assembly; however, the basis for this remains unclear. Here we characterize the chemical and physical effects of mild oxidation on monomeric α-Syn and its aggregation

A dual catalytic manifold that enables site-selective functionalization of unactivated sp3 C–O bonds in cyclic acetals with aryl and alkyl halides is reported. The reaction is triggered by an appropriate σ*–p orbital overlap prior to sp3 C–O cleavage, thus highlighting the importance of conformational flexibility in both reactivity and site selectivity. The protocol is characterized by its excellent

The well-known limitation of alkaline fuel cells is the slack kinetics of the cathodic half-cell reaction, the oxygen reduction reaction (ORR). Platinum, being the most active ORR catalyst, is still facing challenges due to its corrosive nature and sluggish kinetics. Many novel approaches for substituting Pt have been reported, which suffer from stability issues even after mighty modifications. Designing

Hydrogen peroxide (H2O2) plays an important role in various signal transduction pathways and regulates important cellular processes. However, monitoring and quantitatively assessing the distribution of H2O2 molecules inside living cells requires a nanoscale sensor with molecular-level sensitivity. Herein, we show the first demonstration of sub-10 nm-sized fluorescent nanodiamonds (NDs) as catalysts

Reaction of [TiCp*Cl3] (Cp* = η5-C5Me5) with one equivalent of magnesium in tetrahydrofuran at room temperature affords the paramagnetic trinuclear complex [{TiCp*(μ-Cl)}3(μ3-Cl)], which reacts with dinitrogen under ambient conditions to give the diamagnetic derivative [{TiCp*(μ-Cl)}3(μ3-η1:η2:η2-N2)] and the titanium(III) dimer [{TiCp*Cl(μ-Cl)}2]. The structure of the trinuclear mixed-valence complexes

Vinylbenziodoxolones have recently been identified as efficient hypervalent iodine(III) reagents for electrophilic vinylations under transition metal-free conditions. Their unique reactivity allows synthesis of either internal or terminal alkenes, depending on the nucleophile class. This paper constitutes the first mechanistic investigation of VBX vinylations, and makes use of NMR studies, deuterium

Ammonia oxidation catalyzed by molecular compounds is of current interest as a carbon free source of dihydrogen. Activation of N-H bonds through coordination to transition metal centers is a key reaction in this process. We report the substantial activation of ammonia via reaction with low valent molybdenum complexes of a diborate pentadentate ligand system. Spontaneous loss of hydrogen atoms from

Hybrid CO 2 electroreduction in which carbon dioxide reduction reaction (CO 2 RR) is coupled with a thermodynamically more favorable anodic oxidation reaction is recognized as a very important strategy to improve the total value of redox products and energy conversion efficiency. In this work, a coordination catalyst model system for hybrid electrocatalytic full reaction, including Ni 8 -TET with active

We report here fast A-site cation cross-exchange between APbX 3 perovskite nanocrystals (NCs) made of different A-cations (Cs (Cesium), FA (formamidinium), and MA (methylammonium)) at room temperature. Surprisingly, the A-cation cross-exchange proceeds as fast as the halide (X=Cl, Br, or I) exchange with the help of free A-oleate complexes present in the freshly prepared colloidal perovskite NC solutions

A series of platinum(II) calix[4]arene-based molecular tweezers was synthesized. The studies of the host-guest association with a charge-neutral cyclometalated platinum(II) complex showed a drastic color change and the turning on of near-infrared emission resulting from Pt⋯Pt and π−π interactions. Control of the host-guest assembly process by varying the solvent composition can lead to a change from

Recently the fruitful merger of organoboron chemistry and photocatalysis has come to the forefront of organic synthesis resulting in the development of new technologies to access complex (non)borylated frameworks. Central to the success of this combination is control of boron hybridisation. Contingent on the photoactivation mode, boron as its neutral planar form or tetrahedral boronate can be used

Supramolecular polymers (SPs) of d 8 transition metal complexes have received considerable attention by virtue of their rich photophysical properties arising from metal-metal interactions. However, thus far, the molecular design is restricted to complexes with chelating ligands due to their advantageous preorganization and strong ligand fields. Herein, we demonstrate unique pathway-controllable me

Reported here is a multi-response anisotropic poly(N-isopropylacrylamide) hydrogel developed by using a rotating magnetic field to align magnetic double stacks (MDSs) that are fixed by polymerization. The magneto-orientation of MDSs originates from the unique structure with g-Fe2O3 nanoparticles sandwiched by two silicate nanosheets. The resultant gels not only exhibit anisotropic optical and mechanical

Recent discoveries of light-driven inward proton-pumping rhodopsins have opened new avenues to exploring the mechanism of unidirectional transport because these proteins transport protons in the opposite direction to conventional proton-pumping rhodopsins, despite their similar protein structure and membrane topology. Schizorhodopsin (SzR) is a newly discovered rhodopsin family of light-driven inward

Circulating extracellular vesicles (EVs) have emerged as a valuable source of cancer biomarkers. However, the high degree of EV heterogeneity and the complexity of clinical samples pose a challenge in the sensitive identification of tumor-derived EVs. Here we introduce a one-step thermophoretic AND gate operation (Tango) assay that integrates polyethylene glycol (PEG)-enhanced thermophoretic accumulation

Despite the remarkable multiple resonances (MR) optoelectronic properties of organic nanographenes with boron and nitrogen atoms disposed para to each other, the synthetic procedures are sophisticated with low yields and the molecular skeletons are limited. Here, a new paradigm of easy-to-access MR emitter is constructed by simplifying the multiborylation through the amine-directed formation of B-N

Active component management and microengineering of metal nanoparticles are significant challenges for efficient M/N/C electrocatalysts, as a crucial electrode material for reversible zinc–air batteries, because of the lack of a multifunctional structural strategy in the electrocatalytic preparation process. Here, a convenient, one-step pyrolysis method was introduced into the preparation process of

The ever-increasing attention on environmental problems and sustainability has highlighted several problems related to the use of conventional pesticides in the agricultural industry, e.g., toxic residues in the soil and hazards to the environment and human health. In the search for natural antimicrobial and insecticide alternatives, essential oils (EOs) and their active components have emerged as

Sustainable agriculture can be achieved by upcycling and repurposing organic wastes for high-value applications. Keratin and cellulose are two natural biopolymers which are plentiful in biowastes such as hair, poultry feathers, wood shavings, and vegetable trimmings. In this study, these waste-derived biopolymers are converted into bioactive nutrient substrates that can support crop development in

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In the microfluidic systems, the structure of micromixer is one of the important influence factors for the mixing performance. The traditional trial-and-error method for the optimization design of micromixer structure is difficult to consider both the mixing performance and power dissipation. Here we show the topology optimization method of designing the passive micromixer with the minimum power dissipation

A separator coupling cyclone with a built-in granular bed filter is proposed for gas purification. Due to the complicated mutual influences between the outer cyclone shell and the inner granular bed, the dust deposition is different from that in the traditional granular bed filter. By using the intrusive sampling method, the dusts deposited in the bed are sampled under varying inlet dust concentrations