Visible-Light-Induced Annulation of Benzothioamides with Sulfoxonium Ylides To Construct Thiazole Derivatives.

Herein, visible-light-induced annulation of benzothioamides with sulfoxonium ylides to furnish thiazole derivatives is developed under transition-metal-, photocatalyst-, and oxidant-free conditions. This protocol exhibits good substrate scope, affording the desired products with satisfied yields in a mild and green manner. Detailed mechanistic studies suggest that the benzothioamide substrate plays a dual role in this reaction.

Temperature-Responsive Formation Cycling Enabling LiF-Rich Cathode-Electrolyte Interphase.

Formation of LiF-rich cathode-electrolyte interphase is highly desirable for wide-temperature battery, but its application is hindered by the unwanted side reactions associated with conventional method of introducing fluorinated additives. Here, we developed an additive-free strategy to produce LiF-rich cathode electrolyte interphase (CEI) by low-temperature formation cycling. Using LiNiMnCoO as a model cathode, the atomic ratio of LiF in the CEI formed at -5 °C is about 17.

Surface Defect and Wettability Engineering of Porous SnO for Reliable Bioassays with High Selectivity and Wide Linear Dynamic Range.

Bioassay systems that can selectively detect biomarkers at both high and low levels are of great importance for clinical diagnosis. In this work, we report an enzyme electrode with an oxygen reduction reaction (ORR)-tolerant HO reduction property and an air-liquid-solid triphase interface microenvironment by regulating the surface defects and wettability of nanoporous tin oxide (SnO). The enzyme electrode allows the oxygen that is required for the oxidase catalytic reaction to be transported from the air phase to the reaction zone, which greatly enhances the enzymatic kinetics and increases the linear detection upper limit.

Organo-Photocatalytic Anti-Markovnikov Hydroamidation of Alkenes with Sulfonyl Azides: A Combined Experimental and Computational Study.

The construction of C(sp)-N bonds via direct N-centered radical addition with olefins under benign conditions is a desirable but challenging strategy. Herein, we describe an organo-photocatalytic approach to achieve anti-Markovnikov alkene hydroamidation with sulfonyl azides in a highly efficient manner under transition-metal-free and mild conditions. A broad range of substrates, including both activated and unactivated alkenes, are suitable for this protocol, providing a convenient and practical method to construct sulfonylamide derivatives.

Computational insights into the zeolite-supported gold nanocluster-catalyzed ethanol dehydrogenation to acetaldehyde.

Zeolite-supported gold nanoclusters play increasingly important roles in heterogeneous catalysis and exhibit unique catalytic properties for ethanol dehydrogenation to acetaldehyde. Nevertheless, the reaction mechanism and potential roles of the zeolite-encapsulated gold nanoclusters during the catalytic process remain unclear. Herein, computational studies were carried out to gain mechanistic insights into ethanol dehydrogenation to acetaldehyde under both aerobic and anaerobic conditions catalyzed by a silicalite-1 zeolite-encapsulated Au cluster cation (Au-S1).

A novel parallel ant colony optimization algorithm for mobile robot path planning.

With the continuous development of mobile robot technology, its application fields are becoming increasingly widespread, and path planning is one of the most important topics in the field of mobile robot research. This paper focused on the study of the path planning problem for mobile robots in a complex environment based on the ant colony optimization (ACO) algorithm. In order to solve the problems of local optimum, susceptibility to deadlocks, and low search efficiency in the traditional ACO algorithm, a novel parallel ACO (PACO) algorithm was proposed.

Computational Insights into the Photoinduced Dimeric Gold-Catalyzed Divergent Dechloroalkylation of -Dichloroalkanes with Alkenes.

The employment of dinuclear Au(I) catalysts in photomediated modern organic transformations has attracted significant attention over the past decade, which commonly demonstrates unique catalytic performance compared with the corresponding mononuclear gold complexes. Nevertheless, detailed mechanisms of dinuclear gold catalysis remain ambiguous, and further mechanistic understanding is highly desirable. Herein, computational studies were carried out to gain mechanistic insights into the photoinduced dinuclear gold-catalyzed divergent dechloroalkylation of -dichloroalkanes.

A Bioorthogonal Decaging Chemistry of -Oxide and Silylborane for Prodrug Activation both and .

Bioorthogonal decaging chemistry with both fast kinetics and high efficiency is highly demanded for in vivo applications but remains very sporadic. Herein, we describe a new bioorthogonal decaging chemistry between -oxide and silylborane. A simple replacement of "C" in boronic acid with "Si" was able to substantially accelerate the -oxide decaging kinetics by 10 fold (: up to 10 M s).

Reacting Molecular Oxygen with Butanone under Visible Light Irradiation: A General Aerobic Oxidation of Alkenes, Sulfides, Phosphines, and Silanes.

Here, we present a novel oxidation technique by reacting molecular oxygen with butanone under visible light irradiation. This method enables the mild oxidation of various functionalized compounds, including olefins, sulfides, phosphines, and silanes. Preliminary mechanistic experiments and theoretical calculations suggest that visible light triggers molecular oxygen to produce singlet oxygen in butanone.

Construction of α-Acyloxy Ketones via Photoredox-Catalyzed O-H Insertion of Sulfoxonium Ylides with Carboxylic Acids.

Herein, a photoredox-catalyzed insertion of sulfoxonium ylides with carboxylic acids was advanced under mild and simple conditions, offering a practical approach for preparing α-acyloxy ketones with a broad scope of carboxylic acids. A combined experimental and computational study suggests that this reaction proceeds via a stepwise proton-assisted electron transfer mechanism.

A Novel Algorithm for Solving the Prize Collecting Traveling Salesman Problem Based on DNA Computing.

DNA computing is a new pattern of computing that combines biotechnology and information technology. As a new technology born in less than three decades, it has developed at an extremely rapid rate, which can be attributed to its advantages, including high parallelism, powerful data storage capacity, and low power consumption. Nowadays, DNA computing has become one of the most popular research fields worldwide and has been effective in solving certain combinatorial optimization problems.

Solving the Min-Max Clustered Traveling Salesmen Problem Based on Genetic Algorithm.

The min-max clustered traveling salesmen problem (MMCTSP) is a generalized variant of the classical traveling salesman problem (TSP). In this problem, the vertices of the graph are partitioned into a given number of clusters and we are asked to find a collection of tours to visit all the vertices with the constraint that the vertices of each cluster are visited consecutively. The objective of the problem is to minimize the weight of the maximum weight tour.

Mechanistic Insights into Enantioselective C(sp )-H Acylation to Construct α-Amino Ketones via Photoredox and Ni(II) Dual Catalysis: A DFT Study.

The development of the merger of a Ni(II) catalyst with an appropriate photocatalyst under visible-light irradiation provides a new strategy for realizing direct functionalization of C(sp )-H bonds. Mechanistically, whether the reduction of Ni catalyst to form a Ni(0) species is necessary in the dual catalysis still remains under debate. Herein, DFT calculations were carried out to gain a mechanistic insight into the enantioselective acylation of α-amino C(sp )-H bonds to furnish α-amino ketones via photoredox and Ni dual catalysis.

Cobalt-Promoted Noble-Metal Catalysts for Efficient Hydrogen Generation from Ammonia Borane Hydrolysis.

Ammonia borane (AB) has been regarded as a promising material for chemical hydrogen storage. However, the development of efficient, cost-effective, and stable catalysts for H generation from AB hydrolysis remains a bottleneck for realizing its practical application. Herein, a step-by-step reduction strategy has been developed to synthesize a series of bimetallic species with small sizes and high dispersions onto various metal oxide supports.

Computational Understanding of Dual Gold and Photoredox-Catalyzed Regioselective Thiosulfonylation of Alkenes.

Herein, a computational work was carried out to gain mechanistic insights into dual gold and photoredox-catalyzed regioselective thiosulfonylation of alkenes with PhSOSCF. Computational results suggest that it is more favorable for the complex of Au(I) with PhSOSCF (), instead of an Au(I) catalyst or individual substrates, to quench the excited *[Ru] photocatalyst in a single-electron oxidative manner to afford [Ru]. The complexation of the Au(I) catalyst with PhSOSCF could lead to a substantially lowered energy level of the lowest unoccupied molecular orbital, which may be mainly responsible for the feasibility of in quenching the excited photocatalyst.

Iron-catalyzed dual decarboxylative coupling of α-amino acids and dioxazolones under visible-light to access amide derivatives.

An iron-catalyzed decarboxylative C-N coupling of α-amino acids with dioxazolones is described herein to synthesize amide derivatives under visible-light. The desired products can be given in good to excellent yields under simple, mild, and oxidant-free conditions. This protocol provides a practical route for the transformation of α-amino acids to the corresponding amides.

Aerosol Spray Drying Guided Synthesis of Ultrasmall Alloyed Bimetallic Nanoparticles Supported on Silica for Catalytic Semihydrogenation.

Supported bimetallic nanoparticles (NPs) with ultrasmall sizes and homogeneous alloying are attractive for catalysis. However, facile synthesis of this type of material remains very challenging. Here, the aerosol drying impregnation method for rapid, scalable, and general synthesis of silica-supported bimetallic NPs is proposed.

Facile preparation of dihydro-1,4-benzothiazine derivatives oxidative ring-expansion of 2-aminobenzothiazoles with olefins.

A concise and efficient approach to prepare dihydro-1,4-benzothiazine derivatives is described oxidative ring-expansion of 2-aminobenzothiazoles with olefins under metal-free conditions. This protocol is applicable for a wide range of readily accessible 2-aminobenzothiazoles and olefins with moderate-to-good yields. The [4+2] heteroannulation between the intermediacy of oxidative ring-opening of 2-aminobenzothiazoles and olefins is suggested to rationalize the formation of the product.

Solving the Family Traveling Salesperson Problem in the Adleman-Lipton Model Based on DNA Computing.

The Family Traveling Salesperson Problem (FTSP) is a variant of the Traveling Salesperson Problem (TSP), in which all vertices are divided into several different families, and the goal of the problem is to find a loop that concatenates a specified number of vertices with minimal loop overhead. As a Non-deterministic Polynomial Complete (NP-complete) problem, it is difficult to deal with it by the traditional computing. On the contrary, as a computer with strong parallel ability, the DNA computer has incomparable advantages over digital computers when dealing with NP problems.

[2 + 2 + 1] Cycloaddition of -tosylhydrazones, -butyl nitrite and alkenes: a general and practical access to isoxazolines.

-Tosylhydrazones have proven to be versatile synthons over the past several decades. However, to our knowledge, the construction of isoxazolines based on -tosylhydrazones has not been examined. Herein, we report the first demonstrations of [2 + 2 + 1] cycloaddition reactions that allow the facile synthesis of isoxazolines, employing -tosylhydrazones, -butyl nitrite (TBN) and alkenes as reactants.

Acyclic nitronate olefin cycloaddition (ANOC): regio- and stereospecific synthesis of isoxazolines.

We report the first demonstrations of intra- and intermolecular acyclic nitronate olefin cycloaddition (ANOC) reactions that enable the highly efficient syntheses of isoxazolines bearing various functional groups. This general approach to accessing γ-lactone fused isoxazolines was hitherto unprecedented. The room temperature transformations reported herein exhibit wide substrate scopes, as evidenced by more than 70 examples, including the generation of five tricyclic isoxazolines.

Synthesis of Spiro 3,3'-Cyclopropyl Oxindoles Via N-Bromosuccinimide-Mediated Ring-Closing and Contraction Cascade.

An N-bromosuccinimide-mediated cascade reaction involving the cyclization/oxygen-migration/ring-contraction process of 3-(β, β-diaryl) indolylethanol was disclosed. A variety of spiro 3,3'-cyclopropyl oxindole derivatives were efficiently synthesized in good yields under mild reaction conditions. A possible mechanism was suggested based on intermediate isolation and computational studies.

Synthesis and anticancer activities of substituted -(4'-nitrophenyl)-l-prolinamides.

Prolinamides are present in secondary metabolites and have wide-ranging biological properties as well as antimicrobial and cytotoxic activities. -(4'-substituted phenyl)--prolinamides - were synthesized in two steps, starting from the condensation of -fluoronitrobenzene - with -proline -, under aqueous-alcoholic basic conditions to afford -aryl--prolines -, which underwent amidation via a two-stage, one-pot reaction involving SOCl and amines, to furnish -prolinamides in 20-80% yield. The cytotoxicities of - against four human carcinoma cell lines (SGC7901, HCT-116, HepG2 and A549) were evaluated by 3-(4,5-dimethylthiazol-2-yl)-2,5-diphenyltetrazolium bromide (MTT) assay; with good tumour inhibitory activities (79.

Radical-Mediated Distal Ipso-Migration of O/S-Containing Heteroaryls and DFT Studies for Migratory Aptitude.

Herein we describe an efficient distal ipso-migration of - and -containing heteroaryls and the radical heteroarylation of unactivated alkenes. The migration is triggered by various fluoroalkyl radicals, leading to valuable multifunctionalized ketones. The comparisons of migratory aptitude for -/-containing heteroaryls are comprehensively investigated.