Photosynthesis is regarded as the foundation for sustaining planet living, and light-harvesting is the initial step of photosystems and activates the subsequent photochemical reactions. However, the incomplete match between the solar radiation spectrum and absorption profile of chloroplasts limited the full absorption and utilization of sunlight by the photosynthetic pigments. Here, we designed two new aggregation-induced emission (AIE)-active molecules with activated alkyl groups (TPE-PPO and TPA-TPO), and realized the substantial manipulation of live chloroplasts via facile metal-free “Click” reaction. Owing to the matched photophysical properties, the AIE luminogens (AIEgens) could harvest harmful ultraviolet radiation (HUVR) and photosynthetically inefficient radiation (PIR), and further convert them into photosynthetically active radiation (PAR) for chloroplasts absorption. As a result, the AIEgen-chloroplasts bioconjugation exhibited better capability of water splitting and election separation for adenosine triphosphate (ATP) generation, which are important processes in photosynthesis. This is the first AIEgen-based conjugation strategy reported for improving solar-energy utilization and augmenting photosynthetic efficiency.

The quantum mechanical/molecular mechanical (QM/MM) method is a hybrid molecular simulation technique that increases the accessibility of local electronic structures of large systems. The technique combines the benefit of accuracy found in the QM method and that of cost efficiency found in the MM method. However, it is difficult to directly apply the QM/MM method to the dynamics of solution systems, particularly for proton transfer. As explained in the Grotthuss mechanism, proton transfer is a structural interconversion between hydronium ions and solvent water molecules. Hence, when the QM/MM method is applied, an adaptive treatment, namely on-the-fly revisions on molecular definitions, is required for both the solute and solvent. Although several solvent-adaptive methods have been proposed, a full adaptive framework, which is an approach that also considers adaptation for solutes, remains untapped. In this paper, we propose a new numerical expression for the coordinates of the excess proton and its control algorithm. Furthermore, we confirm that this method can stably and accurately simulate proton transfer dynamics in bulk water.

Iminophosphoranes are reported as convenient precursors to amides, ureas, carbamates and other carbonyl-containing molecules through CO2-fixation. Key to this transformation with stable isotopes and carbon-11 is interception of the reactive isocyanate intermediate. Automated synthesis and isolation of PET radiopharmaceuticals is achieved.

The C19–C30 bis-THF fragment of the proposed structure of iriomoteolide-13a has been synthesized. The w-mesyloxy-substituted stereotetrad possessing three continuous hydroxy groups was generated by anti-aldol reaction and asymmetric dihydroxylation (AD). Upon heating in pyridine the stereotetrad underwent an SN2 cyclization to form the C19–C22 THF ring. It was followed by an intramolecular syn-oxypalladation of the C28 chiral allylic alcohol to give the C23–C26 THF ring.

A detailed analysis of a complete set of the local potentials that appear in the Euler equation for electron density is carried out for noncovalent interactions in the uracil derivative using experimental X-ray charge density. The interplay between the quantum theory of atoms in molecules and crystals and the local potentials and corresponding inner-crystal electronic forces of electrostatic and kinetic origin is explored. Novel physically grounded bonding descriptors derived within the orbital-free quantum crystallography provided the detailed examination of pi-stacking and intricate C=O...pi interactions and nonclassical hydrogen bonds. The donor-acceptor character of these interactions is revealed by analysis of Pauli and von Weizsäcker potentials together with more well-known functions. Partitioning of crystal space into atomic-like potential basins led us to the definite description of the charge transfer. In this way, our analysis throws light on aspects of these closed-shell interactions hitherto hidden from the description.

We report a novel vapour phase procedure to perform the Soai reaction in an absolute asymmetric synthesis fashion: the substrate is confined in the pores of the UiO-type MOFs, and vapour phase reactions with Zn(i-Pr)2 are performed in a sealed environment, Different MOFs lead to different outcomes in terms of enantiomeric excess, handedness of the product and reaction rate. This is one of the first examples of absolute asymmetric synthesis performed inside a MOF.

Hydrogenation of electron deficient ,-unsaturated carbonyl derivativesusing O-mesityl(sulfonyl)hydroxylamine in the presence of catalytic amount of ytterbiumtriflate to obtain good to excellent is described.

The objective of this study was to evaluate the effects of CEPT for leachate and sewage co-treatment in a POTW. The results showed that ferric and aluminum coagulants remove about 54 - 74% organic matter where ferric performed better than aluminum coagulant. However, ferric coagulant was found to exacerbate the UV absorbance after coagulation at high dose due to the interaction with dissolved organic matter by forming soluble transition metal complexes. These organo-metal complexes have been found to increase the UV absorbance and this study provides the scientific background for such phenomenon.

The severe acute respiratory syndrome coronavirus-2 (SARS-CoV-2) an enveloped, positive-sense single-stranded RNA virus that is responsible for the COVID-19 pandemic. The viral spike is a class I viral fusion glycoprotein that extends from the viral surface and is responsible for viral entry into the host cell, and is the primary target of neutralizing antibodies. However, antibody recognition often involves variable surface epitopes on the spike, and the receptor binding domain (RBD) of the spike hides from immune recognition underneath a glycan shield aside from brief dynamic excursions to search for the host-cell surface receptor ACE2. Using an atomistic model of the glycosylated wild-type spike in the closed and 1-up RBD conformations, we identified specific interactions that stabilize the closed RBD, and mapped the free energy landscape for RBD opening. We characterized a transient pocket associated with a hinge motion during opening of the RBD, suggesting the possibility of allosteric control of the RBD via this region. Substitution of a conserved alanine to bulkier leucine in the pocket shifted the RBD equilibrium to favor the open, exposed state, as did removal of a conserved lysine that forms a critical salt-bridge in the closed, hidden state. Results from our virtual screening, MD simulations and free energy landscape calculations for wild-type spike suggest that small molecules can spontaneously bind to the highly conserved hinge pocket, and that such binding can shift the RBD equilibrium to favor the open state. Stabilizing the open state may facilitate antibody recognition by forcing the spike to expose critical RBD epitopes, and also could increase the likelihood of premature triggering of the spike fusion machinery via S1 shedding, neutralizing the infectious ability of the virus.

Enantioselective addition of trimethylsilyl cyanide (TMSCN) to aldehydes is one of the most extensively studied organic reactions in asymmetric catalysis. Herein, we report our intensive kinetic investigation on the asymmetric addition of TMSCN to benzaldehyde, catalyzed by a covalently bridged dinuclear (salen)titanium complex 2, which has been one of the most efficient artificial chiral catalysts reported so far for this reaction. It was found that the method of initial rates for kinetic investigation is not appropriate in this case because of the presence of a significant incubation period in the catalysis, while the method of progress rates proved to be more reliable and efficient for judging the kinetic orders of this catalytic system. The kinetic results revealed that the reaction follows first order with respect to the catalyst and is nearly independent of concentrations of both benzaldehyde and TMSCN. A detailed catalytic mechanism for cyanosilylation of benzaldehyde in the presence of 2 was proposed, wherein the key active dinuclear species works in a cooperative manner for dual activation of both reactants.