Molten Hydroxide Direct Carbon Fuel Cells (MH-DCFCs) represent significant potential for efficient and sustainable energy conversion. Its actual performance is highly dependent on the distribution of concentration and temperature gradients at the electrode/electrolyte interface. Existing models commonly employ the isothermal-homogeneous assumptions, resulting in significant deviations in concentration and thermal distribution predictions. This study develops a dual-gradient multi-physics coupling model that incorporates concentration, temperature, electrochemistry reactions, and heat transfer processes. Three comparative models are created: the Isothermal Homogeneous Model (IHMM), the Isothermal Heterogeneous Model (IHTM), and the Non-Isothermal Heterogeneous Model (NIHM). COMSOL Multiphysics investigates the effect of electrolyte concentration, temperature gradients, and voltage losses on cell performance, filling gaps in modelling the non-uniformity of electrode-electrolyte interactions in MH-DCFCs. Simulation results show that NIHM better captures the cell's internal features, as electrolyte heterogeneity increases anode/cathode current densities by 10.23 % and 78.25 %, respectively, compared to IHMM. Reaction heat raises electrode temperatures by 8.61 %-12.5 %, increasing peak power density by 34.08 %-61.5 mW/cm(2). NIHM predictions are more accurate than IHMM (OCV error <1.2 %, peak power deviation 2.76 %). A Multi-Layer Perceptron (MLP) neural network learns from NIHM-enabled simulations across a wider range of operating conditions, increasing model versatility. This research provides an optimization model for MH-DCFCs and offers novel research perspectives for energy conversion technologies.

We investigated the ionization and dissociation processes of ammonia clusters ranging from dimer to pentamer in-duced by 800-nm femtosecond laser fields.Time-of-flight(TOF)mass spectra of the ammonia clusters were recorded over a range of laser intensities from 2.1 × 1012 W/cm2 to 5.6× 1012 W/cm2.The protonated ion signals dominate the spectra,which is consistent with the stability of the geometric structures.The ionization and dissociation channels of ammonia clusters are discussed.The competition and switching among observed dissociation channels are revealed by analyzing the variations in the relative ionic yields of specific protonated and unprotonated clusters under different laser intensities.These results indicate that the ionization of the neutral multiple-ammonia units,produced through the dissociation of cluster ions,may start to contribute,as well as the additional processes to consume protonated ions and/or produce unprotonated ions induced by the femtosecond laser fields when the laser intensity is above～4× 1012 W/cm2.These findings provide deeper insights into the ionization and dissociation dynamics in multi-photon ionization experiments involving ammonia clusters.

A solvent-controlled unprecedented tandem reaction of readily accessible SeO2, a wide variety of sulfonyl hydrazides, and alkynes has been established for the chemodivergent construction of structurally complex 1,2-bis((E)-1-aryl-2-arylsulfonylvinyl)diselanes and bis((E)-1-aryl-2-(arylsulfonyl)vinyl)selanes via a catalyst-free one-pot three-component approach, respectively. The adjustable and controlled synthetic strategy shows good yields and chemoselectivities for most substrates under mild and simple conditions.

This catalyst- and additive-free strategy could efficiently introduce the isoxazolidine skeleton into nucleoside analogues, oxazole molecules and indole derivatives.

Facile and ultrasensitive detection of Pb2+ in water for remote or resource-limited environments remains challenging. DNAzyme-based colorimetric nanobiosensors have been extensively studied to regulate the assembly of functionalized gold nanoparticles (AuNPs). However, these nanobiosensors have been criticized for their low sensitivity owing to the difficulty of dissociating DNAzyme embedded in AuNP aggregates. To address this issue, we rationally designed a DNAzyme by introducing an adenine-cytosine (A-C) mismatch to strengthen the disassembly of DNAzyme-linked nanostructures. As proof of concept, a "turn on" colorimetric nanobiosensor integrated with mismatched DNAzyme and functionalized AuNPs was first developed for Pb2+ detection. Under the optimal detection conditions, the obtained typical calibration curve shows a detection limit of 8.6 nmol/L, with an approximately 11-fold sensitivity improvement in Pb2+ detection compared with unmismatched DNAzyme, and a linear response range from 10 to 300 nmol/L. This nanobiosensor demonstrated robust selectivity and satisfactory recovery rates between 86.5% and 106.4% for Pb2+ in spiked environmental water samples. Additionally, the detection process is user-friendly and can be completed within 30 min, requiring only a simple water sample addition step. Considering the extensive applications of DNAzyme in conjunction with nanoparticles, this study provides a valuable reference for designing other DNAzyme-powered nanoparticle assemblies in biosensing systems.

A general and practical method for the construction of various 3,4,5-trisubstituted 1,2,4-triazoles via I2-catalyzed cycloaddition of N-functionalized amidines with hydrazones is reported. This strategy features cheap and readily available catalyst and starting materials, broader substrate scope, and moderate-to-good yields. The mechanism study shows that the existence of hydrogen on the nitrogen of hydrazones is crucial for this transformation.

Catalyst-controlled regioselective [3 + 2] cascade annulation of allenes with N-monosubstituted hydroxylamines for precise construction of two types of isoxazolidine regiomers has been developed. The Ce(OTf)3 and MgCl2 can guide the nitrogen and oxygen atoms of N-hydroxyarylamides to both ends of the consecutive double bond of allenes, respectively, to afford two kinds of isomeric products. Notably and remarkably, the consecutive double bond of allenes served as a C3 synthon.

A new type of polycarboxylic acid crosslinking agent 2-(2,4,5-tricarboxybenzyloxy)-1,2,3-propanetricarboxylic acid (TBPTA) with the morphology similar to the regular arrangement of the foliar morphology of Araucaria was synthesized by dissolving carboxylic acid system of 1, 2, 3, 4-butane tetracarboxylic acid (PMDA) and citric acid (CA) in the molar ratio of 1: 1 in tetrahydrofuran (THF) at 68 °C. On this basis, a novel adsorbent TEMPO-derived nanocellulose (CNF)/TBPTA with excellent adsorption properties for methylene blue (MB) was prepared by mixing CNF, TBPTA as raw materials and sodium hypophosphite (SHP) as catalyst in various proportions. The X-ray diffraction (XRD) spectra showed that the cross-linking effect of TBPTA transformed the crystal structure of CNF from type I to type II. The MB adsorption results suggested that the maximum adsorption capacity of CNF/TBPTA was 1152 mg g-1, which was 321.58 % higher than that of CNF without TBPTA esterification crosslinking modification. The adsorption process can be described by Langmuir isothermal adsorption model and pseudo-second-order kinetic model, involving electrostatic force, hydrogen bond and π-π conjugation effect. CNF/TBPTA demonstrates a strong potential for reuse, maintaining 92 % of its initial MB adsorption efficiency after undergoing 7 successive adsorption-desorption cycles.

Highly functionalized 1,5,2-dioxazinanes could be smoothly produced via a Sc(OTf)(3)-catalyzed chemoselective [3 + 3] cycloaddition of various N-arylnitrones with a series of donor-acceptor oxiranes. This reaction involves in situ generation of 1,3-dipoles through Sc(OTf)(3)-catalyzed C-C bond cleavage of oxiranes and moderate to high yields were obtained for most substrates. This transformation features C-C bond cleavage of donor-acceptor oxiranes, accessible starting materials and mild reaction conditions.

A tandem strategy for the construction of an array of 3-CF 3 -4-acyl functionalized quinolines via a sequential formation of C−N, C−O and C−C bonds has been described from nitrosoarenes and β-CF 3 -1,3-enynes as starting materials.

The Cu(OAc)(2)-catalyzed one-pot three-component cycloaddition of malonates, nitrosoarenes and alkenes is described. A wide range of isoxazolidines could be obtained in moderate to excellent yields via this method. Mechanistic investigations indicated that the key step in this catalytic system is the straightforward formation of nitrone intermediates through the Cu(OAc)(2)-catalyzed reaction of malonates with nitrosoarenes.

1,2-Dihydro-1,3,5-triazine compounds were synthesized through three sets of reactions of amidines with, respectively, paraformaldehyde, aldehydes and N-arylnitrones under different conditions. The catalysts used in these three reactions were Cu(OAc)2, ZnI2 and CuCl2·2H2O, respectively. Most of the substrates tested for these reactions provided the target products in moderate to good yields. In the reactions involving paraformaldehyde, Cu(OAc)2 also accelerated the release of formaldehyde from paraformaldehyde during the catalytic reaction process. In the case of the reactions involving nitrones, CuCl2·2H2O not only catalyzed the normal progress of the main reaction, but also promoted the reaction of nitrones to produce nitroso compounds and aldehydes.

Symmetrical diaryl sulfides and diaryl disulfides have been efficiently and selectively constructed via the homocoupling of sodium arenesulfinates. The selectivity of products relied on the different reaction systems: symmetrical diaryl sulfides were predominately obtained under the Pd(OAc)2 catalysis, whereas symmetrical diaryl sulfides were exclusively yielded in the presence of the reductive Fe/HCl system.

3,4-Bisthiolated pyrroles constitute key cores in pyrrole-based semiconductors, and their electronic properties could be improved by the bisthio groups via the S-effect. Herein, a convenient method for the synthesis of 3,4-bisthiolated pyrroles has been developed through the AlCl3-catalyzed thiolation/cyclization of homopropargylic azides, and cyclic voltammetry and DFT calculations indicated that the desired 3,4-bisthiolated pyrroles had higher HOMO orbital energies and lower band gaps than the parent unsubstituted 2,5-diphenylpyrrole.

Aryl alkyl ethers and diaryl ethers represent ubiquitous structural motifs in natural products, medicinally relevant compounds, biologically active compounds, agrochemicals and organic materials, and they are also useful building blocks in organic synthesis. Therefore, many transformations have been reported for the synthesis of these two kinds of compounds. Among these versatile methods, transition-metal-free approaches using different reagents as starting materials have been developed as promising and alternative protocols. Although one example for transition-metal-catalyzed transformation of arenesulfonates into aryl alkyl ethers and diaryl ethers has been reported, there are no reports about the formation of aryl ethers utilizing arenesulfonates as starting materials via a transition-metal-free protocol, and existing methods for providing sterically hindered ortho-substituted diaryl ethers using electrophiles substituted by electron-deficient groups, particularly by a bulky one at the ortho-position as starting materials are very rare. We will report a K2CO3-mediated method for the synthesis of aryl alkyl ethers using arenesulfonates as starting materials via two alternative paths. One path is the cross-coupling of aryl arenesulfonates with alcohols through their S-O bond cleavage, and the other uses the reactions of alkyl arenesulfonates with phenols via their C-O bond cleavage. Additionally, we also report the K3PO4-promoted preparation of bulky ortho-substituted diaryl ethers via the C-S bond cleavage of aryl arenesulfonates or arenesulfonyl chlorides bearing electron-withdrawing groups at 2-, 2,4- or 2,6-position of the phenyl ring in the presence of phenols, respectively. General procedure for the reactions of aryl arenesulfonates with various alcohols: to an oven-dried glass tube, aryl arenesulfonate 1 (0.2 mmol), K2CO3 (2 equiv.) and 0.5 mL alcohol 2 were added in turn. The reaction system was then stirred at 65 degrees C until the aryl arenesulfonate 1 was completely consumed as determined by thin layer chromatography. Finally, the reaction mixture was purified by silica gel column chromatography to afford the desired product 3. General procedure for the reactions of aryl o-substituted arenesulphonates with the corresponding phenols: to an oven-dried glass tube, aryl o-substituted arenesulfonate 7 (0.2 mmol), K3PO4 (3 equiv.), the corresponding phenol 5 (1.2 equiv.) and 1.0 mL toluene were added in turn. The reaction system was then stirred at 100 degrees C until the reaction was over as determined by TLC. Finally, the reaction mixture was purified by silica gel column chromatography to afford the desired product 8.

An efficient approach to obtain highly functionalized imidazolones bearing α-amino acid esters through KOH-mediated one-pot three-component annulation of amidines, nitrosoarenes and malonic esters is reported. This reaction features broad substrate scope, a cheap and readily available promoter, good to high yields for most substrates and mild reaction conditions. The mechanism study shows that the KOH-mediated formation of the imine intermediate via the reaction of nitrosoarenes with malonic esters is a key step.

A general and practical strategy for the construction of various keto-substituted isoxazolidines via one-pot three-component reaction of easily accessible, safer and more stable sulfoxonium ylides, nitrosoarenes and olefins is described. This three-component approach features remarkably much broader substrate scope, good functional group tolerance, good to high yields, operational safety and mild reaction conditions, and this method is also catalyst-free, additive-free and operationally simple.

Hydrazones have been employed as the starting materials in a KOH-mediated one-pot three-component cycloaddition with readily accessible nitroso compounds and olefins to construct various isoxazolidines. Compared with diazo compounds as starting materials, this methodology could afford a wider range of products in good to excellent yields and diastereoselectivities for most substrates, and hydrazones are cheaper, more accessible, and safer substrates. The experimental study shows that the choice of suitable hydrazones is crucial.

N-Alkyl nitrones are used as starting materials to construct N-aryl isoxazolidines, instead of N-alkyl isoxazolidines or N–H 1,3-oxazinanes via a catalyst-free one-pot three-component reaction with nitrosoarenes and olefins.

Thiolation/cyclization of homopropargylic tosylamides allowed the selective synthesis of 3-thiolated pyrroles and pyrrolines controlled by solvents. Moreover, the desired 3-thiolated pyrroles were readily transformed to organic fluorophores benzothienopyrrole and bisthiolated boron dipyrromethene (S-BODIPY).