e., immediate and sustained release was achieved by varying the acidity of the aqueous media; (IV) the photoirradiation time did not significantly affect the release kinetics under different pH conditions; and (V) the pH-responsive release properties were regulated by changing the polymer composition in P(DEAEMA-CEMA). Furthermore, by exploiting the pH-responsiveness, capsule particles are successfully obtained via an all-aqueous process from spherical polymer particles. The advantages of the all-aqueous encapsulation process allowed the water-soluble biomacromolecules such as DNA and saccharides to be successfully encapsulated in the P(DEAEMA-CEMA) hollow particles. With this simple interfacial photo-cross-linking strategy, we envision the ready synthesis of sophisticated particulate materials for broad application in advanced research fields.We demonstrate liquid-liquid phase separation involving both coacervation and coil-to-globule phase transition of a thermoresponsive polymer. By focusing a near-infrared laser beam into an aqueous solution of poly(N-isopropylacrylamide) (PNIPAM), a single phase-separated polymer microdroplet can be formed and stably trapped at the focal point. Such droplet formation is induced by a local elevation in temperature (induced by a photothermal effect) and an optical force. The technique allows us to selectively analyze a single polymer droplet trapped at the focal point. In this study, we applied this technique to poly(N,N-diethylacrylamide) (PDEA) in water and generated a double-layered PDEA droplet. Such an inhomogeneous and complex microstructure has not been previously observed both in steady-state heating of a PDEA solution and in the PNIPAM system. Moreover, we used micro-Raman spectroscopy to clarify that PDEA underwent dehydration due to a coil-to-globule phase transition. Despite this, the polymer concentration (Cpoly) of the trapped PDEA droplet was very low and was around 30 wt %. Cpoly depended on the molecular weight of PDEA and the laser power that regulates the temperature elevation. These results strongly indicate that PDEA undergoes coacervation in addition to a coil-to-globule phase transition. This study will help provide us with a fundamental understanding of the phase separation mechanisms of thermoresponsive polymers.Electrochemical disinfection-a method in which chemical oxidants are generated in situ via redox reactions on the surface of an electrode-has attracted increased attention in recent years as an alternative to traditional chemical dosing disinfection methods. Because electrochemical disinfection does not entail the transport and storage of hazardous materials and can be scaled across centralized and distributed treatment contexts, it shows promise for use both in resource limited settings and as a supplement for aging centralized systems. In this Critical Review, we explore the significance of treatment context, oxidant selection, and operating practice on electrochemical disinfection system performance. We analyze the impacts of water composition on oxidant demand and required disinfectant dose across drinking water, centralized wastewater, and distributed wastewater treatment contexts for both free chlorine- and hydroxyl-radical-based systems. Drivers of energy consumption during oxidant generation are identified, and the energetic performance of experimentally reported electrochemical disinfection systems are evaluated against optimal modeled performance. We also highlight promising applications and operational strategies for electrochemical disinfection and propose reporting standards for future work.Serine hydrolases cleave peptide and ester bonds and are ubiquitous in nature, with applications in biotechnology, in materials, and as drug targets. The serine hydrolase two-step mechanism employs a serine-histidine-aspartate/glutamate catalytic triad, where the histidine residue acts as a base to activate poor nucleophiles (a serine residue or a water molecule) and as an acid to allow the dissociation of poor leaving groups. This mechanism has been the subject of debate regarding how histidine shuttles the proton from the nucleophile to the leaving group. To elucidate the reaction mechanism of serine hydrolases, we employ quantum mechanics/molecular mechanics-based transition path sampling to obtain the reaction coordinate using the Aspergillus niger feruloyl esterase A (AnFaeA) as a model enzyme. The optimal reaction coordinates include terms involving nucleophilic attack on the carbonyl carbon and proton transfer to, and dissociation of, the leaving group. During the reaction, the histidine residue undergoes a reorientation on the time scale of hundreds of femtoseconds that supports the "moving histidine" mechanism, thus calling into question the "ring flip" mechanism. We find a concerted mechanism, where the transition state coincides with the tetrahedral intermediate with the histidine residue pointed between the nucleophile and the leaving group.  https://www.selleckchem.com/products/fht-1015.html  Moreover, motions of the catalytic aspartate toward the histidine occur concertedly with proton abstraction by the catalytic histidine and help stabilize the transition state, thus partially explaining how serine hydrolases enable poor nucleophiles to attack the substrate carbonyl carbon. Rate calculations indicate that the second step (deacylation) is rate-determining, with a calculated rate constant of 66 s-1. Overall, these results reveal the pivotal role of active-site dynamics in the catalytic mechanism of AnFaeA, which is likely similar in other serine hydrolases.Chemists visualize chemical reactions as motion along one-dimensional "reaction coordinates" over free energy barriers. Various rate theories, such as transition state theory and the Kramers theory of diffusive barrier crossing, differ in their assumptions regarding the mathematical specifics of this motion. Direct experimental observation of the motion along reaction coordinates requires single-molecule experiments performed with unprecedented time resolution. Toward this goal, recent single-molecule studies achieved time resolution sufficient to catch biomolecules in the act of crossing free energy barriers as they fold, bind to their targets, or undergo other large structural changes, offering a window into the elusive reaction "mechanisms". This Perspective describes what we can learn (and what we have already learned) about barrier crossing dynamics through synergy of single-molecule experiments, theory, and molecular simulations. In particular, I will discuss how emerging experimental data can be used to answer several questions of principle.