General One-pot Strategy Research Articles

A General One-Pot Protocol for Hindered N-Alkyl Azaheterocycles from Tertiary Carboxylic Acids.

In this letter, we report a general one-pot strategy that utilizes three elementary steps (decarboxylative hydrazination, Boc deprotection, and heterocycle condensation) to regioselectively prepare hindered C(sp3) substituted pyrazoles and triazoles. The operational simplicity of this sequence and ubiquity of tertiary carboxylic acids allow rapid access to hindered N-alkyl azaheterocycles that will be useful to practitioners of medicinal chemistry and agro-chemistry.

Octahedral gold-silver nanoframes with rich crystalline defects for efficient methanol oxidation manifesting a CO-promoting effect

Three-dimensional bimetallic nanoframes with high spatial diffusivity and surface heterogeneity possess remarkable catalytic activities owing to their highly exposed active surfaces and tunable electronic structure. Here we report a general one-pot strategy to prepare ultrathin octahedral Au3Ag nanoframes, with the formation mechanism explicitly elucidated through well-monitored temporal nanostructure evolution. Rich crystalline defects lead to lowered atomic coordination and varied electronic states of the metal atoms as evidenced by extensive structural characterizations. When used for electrocatalytic methanol oxidation, the Au3Ag nanoframes demonstrate superior performance with a high specific activity of 3.38 mA cm−2, 3.9 times that of the commercial Pt/C. More intriguingly, the kinetics of methanol oxidation on the Au3Ag nanoframes is counter-intuitively promoted by carbon monoxide. The enhancement is ascribed to the altered reaction pathway and enhanced OH− co-adsorption on the defect-rich surfaces, which can be well understood from the d-band model and comprehensive density functional theory simulations.

General One-Pot Synthesis of Transition-Metal Phosphide/Nitrogen-Doped Carbon Hybrid Nanosheets as Ultrastable Anodes for Sodium-Ion Batteries.

Sodium-ion batteries (SIBs) have been considered as promising energy storage devices in grid-level applications, owing to their largely reduced cost compared with that of lithium-ion batteries. However, the practical application of SIBs has been seriously hindered because of the lack of appropriate anode materials, limited by the thermodynamics perspective, which is one of the central task at current stage. Herein, we have developed a general one-pot strategy for the synthesis of transition-metal phosphide (TMP) based hybrid nanosheets composed of carbon-coated TMP nanoparticles anchored to the surface of nitrogen-doped carbon nanosheets. This facile and cost-effective method is quite universal and holds potential to be further extended to other metal phosphide materials. Significantly, the hybrid nanosheet electrode possesses excellent sodium storage properties as anodes for SIBs, including high specific capacity, an ultra-long cycle life and a remarkable rate performance. This work makes a significant contribution to not only the synthetic methodology of TMP-carbon two-dimensional hybrid nanostructures, but also the application of TMP-based anodes for high-energy SIBs.

A general one-pot strategy for the synthesis of Au@multi-oxide yolk@shell nanospheres with enhanced catalytic performance.

By integrating redox self-assembly and redox etching processes, we report a general one-pot strategy for the synthesis of Au@multi-M x O y (M = Co, Ce, Fe, and Sn) yolk@shell nanospheres. Without any additional protecting molecule or reductant, the whole reaction is a clean redox process that happens among the inorganic metal salts in an alkaline aqueous solution. By using this method, Au@Co3O4/CeO2 (Au@Co-Ce), Au@Co3O4/Fe2O3 (Au@Co-Fe), and Au@CeO2/SnO2 (Au@Ce-Sn) yolk@shell nanospheres with binary oxides as shells, Au@Co3O4/CeO2/Fe2O3 (Au@Co-Ce-Fe) yolk@shell nanospheres with ternary oxides as shells and Au@Co3O4/CeO2/Fe2O3/SnO2 (Au@Co-Ce-Fe-Sn) yolk@shell nanospheres with quaternary oxides as shells can be obtained. Subsequently, the catalytic CO oxidation was selected as the catalytic model, and the Au@Co-Ce system was chosen as the catalyst. It was found that the catalytic activity of Au@Co-Ce yolk@shell nanospheres can be optimized by altering the relative proportion of Co and Ce oxides.

General one-pot strategy to prepare Ag–TiO2 decorated reduced graphene oxide nanocomposites for chemical and biological disinfectant

A multifunctional Ag–TiO2/reduced graphene oxide (rGO) nanocomposite was prepared by a simple one-step hydrothermal reaction using TiO2 NP (Degussa P25), AgNO3, and graphene oxide (GO) without reducing agents. Growth of the Ag–TiO2 NPs over GO and reduction of GO were simultaneously carried out under hydrothermal condition. This method provides the notable advantages of a single-step reaction without employing toxic solvents or reducing agents, thereby providing a novel green synthetic route to produce the nanocomposite of Ag–TiO2/rGO. Further, it enhances the optical response of the nanocomposites and contributed for the absorption of light in the visible spectrum through localized surface plasmon resonance effects. The superior photocatalytic activities, antibacterial properties, and the easy recovery make the Ag– TiO2/rGO nanocomposite a good promising candidate for wastewater treatment.

A General Approach to Fabricate Diverse Noble‐Metal (Au, Pt, Ag, Pt/Au)/Fe2O3 Hybrid Nanomaterials

A novel, facile, and general one-pot strategy is explored for the synthesis of diverse noble-metal (Au, Pt, Ag, or Pt/Au)/Fe(2)O(3) hybrid nanoparticles with the assistance of lysine (which is a nontoxic, user friendly amino acid that is compatible with organisms) and without using any other functionalization reagents. Control experiments show that lysine, which contains both amino and carboxylic groups, plays dual and crucial roles as both linker and capping agents in attaching noble metals with a small size and uniform distribution onto an Fe(2)O(3) support. Considering the perfect compatibility of lysine with organism, this approach may find potentials in biochemistry and biological applications. Furthermore, this novel route is also an attractive alternative and supplement to the current methods using a silane coupling agent or polyelectrolyte for preparing hybrid nanomaterials. To demonstrate the usage of such hybrid nanomaterials, a chemical gas sensor has been fabricated from the as-synthesized Au/Fe(2)O(3) nanoparticles and investigated for ethanol detection. Results show that the hybrid sensor exhibits significantly improved sensor performances in terms of high sensitivity, low detection limit, better selectivity, and good reproducibility in comparison with pristine Fe(2)O(3). Most importantly, this general approach can be further employed to fabricate other hybrid nanomaterials based on different support materials.