Efficient removal of oil pollutant via simultaneous adsorption and photocatalysis using La–N–TiO2–cellulose/SiO2 difunctional aerogel composite

Research on Chemical Intermediates - Nano-TiO2 photocatalysts doped with La–N(La–N–TiO2) were prepared by solgel method. The La–N–TiO2 was loaded on the cellulose/SiO2...     

Bimetallic Covalent Organic Frameworks for Constructing Multifunctional Electrocatalyst

Covalent organic frameworks (COFs) are a new class of crystalline porous polymers comprised mainly of carbon atoms, and are versatile for the integration of heteroatoms such as B, O, and N into the skeletons. The designable structure and abundant composition render COFs useful as precursors for heteroatom-doped porous carbons for energy storage and conversion. Herein, we describe a multifunctional electrochemical catalyst obtained through pyrolysis of a bimetallic COF. The catalyst possesses hierarchical pores and abundant iron and cobalt nanoparticles embedded with standing carbon layers. By integrating these features, the catalyst exhibits excellent electrochemical catalytic activity in the oxygen reduction reaction (ORR), with a 50 mV positive half-wave potential, a higher limited diffusion current density, and a much smaller Tafel slope than a Pt-C catalyst. Moreover, the catalyst displays superior electrochemical performance toward the hydrogen evolution reaction (HER), with overpotentials of −0.26 V and −0.33 V in acidic and alkaline aqueous solution, respectively, at a current density of 10 mA cm⁻². The overpotential in the catalysis of the oxygen evolution reaction (OER) was 1.59 V at the same current density.     

Controlled Synthesis of N‐Doped Carbon Nanospheres with Tailored Mesopores through Self‐Assembly of Colloidal Silica

Limited strategies have been established to prepare monodisperse mesoporous carbon nanospheres (MCNs) with tailored pore sizes. In this work, a method is reported to synthesize MCNs by combining polymerization of aniline with co‐assembly of colloidal silica nanoparticles. The controlled self‐assembly behavior of colloidal silica enables the formation of uniform composite nanospheres and convenient modulation over mesopores. After carbonization and removal of sacrificial templates, the resultant MCNs possess tunable mesopores (7–42 nm) and spherical diameters (90–300 nm), as well as high surface area (785–1117 m² g^?1), large pore volume (1.46–2.01 cm³ g^?1) and abundant nitrogen moieties (5.54–8.73 at %). When serving as metal‐free electrocatalysts for the oxygen reduction reaction (ORR), MCNs with an optimum pore size of 22 nm, compared to those with 7 and 42 nm, exhibit the best ORR performance in alkaline medium.     

Highly Selective Photoelectroreduction of Carbon Dioxide to Ethanol over Graphene/Silicon Carbide Composites

Using sunlight to produce valuable chemicals and fuels from carbon dioxide (CO₂), i.e., artificial photosynthesis (AP) is a promising strategy to achieve solar energy storage and a negative carbon cycle. However, selective synthesis of C₂ compounds with a high CO₂ conversion rate remains challenging for current AP technologies. We performed CO₂ photoelectroreduction over a graphene/silicon carbide (SiC) catalyst under simulated solar irradiation with ethanol (C₂H₅OH) selectivity of>99 % and a CO₂ conversion rate of up to 17.1 mmol g_cat⁻¹ h⁻¹ with sustained performance. Experimental and theoretical investigations indicated an optimal interfacial layer to facilitate the transfer of photogenerated electrons from the SiC substrate to the few-layer graphene overlayer, which also favored an efficient CO₂ to C₂H₅OH conversion pathway.     

Synchronous Dual Electrolyte Additive Sustains Zn Metal Anode with 5600 h Lifespan

Despite conspicuous merits of Zn metal anodes, the commercialization is still handicapped by rampant dendrite formation and notorious side reaction. Manipulating the nucleation mode and deposition orientation of Zn is a key to rendering stabilized Zn anodes. Here, a dual electrolyte additive strategy is put forward via the direct cooperation of xylitol (XY) and graphene oxide (GO) species into typical zinc sulfate electrolyte. As verified by molecular dynamics simulations, the incorporated XY molecules could regulate the solvation structure of Zn²⁺, thus inhibiting hydrogen evolution and side reactions. The self-assembled GO layer is in favor of facilitating the desolvation process to accelerate reaction kinetics. Progressive nucleation and orientational deposition can be realized under the synergistic modulation, enabling a dense and uniform Zn deposition. Consequently, symmetric cell based on dual additives harvests a highly reversible cycling of 5600 h at 1.0 mA cm⁻²/1.0 mAh cm⁻².     

KI-Mediated Chlorine Gas-Free Synthesis of 3,3-Dichloro-2-oxindole Derivatives

An efficient and environmentally friendly methodology for 3,3-dichlorination and 2-oxidation of indole derivatives is described. Using KI as promotor, MCl (M=K, Na) as chlorine source, and oxone as oxidant, the reaction proceeds smoothly affording various functionalized 3,3-dichloro-2-oxindoles in moderate to excellent yields. This strategy can also be extended to 3-substituted indoles. With a broad substrate scope, it is a practical approach to 3,3-disubstituted-2-oxindoles.     

Palladium-Catalyzed Asymmetric Trifluoromethylated Allylic Alkylation of N-Substituted Glycine Ethyl Esters with α-(Trifluoromethyl)alkenyl Acetates

An efficient strategy for asymmetric trifluoromethylated allylic alkylation of easily available N-substituted glycine ethyl esters with α-(trifluoromethyl)alkenyl acetates has been developed. Catalyzed by a [Pd(C₃H₅)Cl]₂/(R)-BINAP, various trifluoromethyl-containing N-substituted glycine ethyl ester derivatives are afforded with good yields and excellent enantioselectivities. The product can be readily converted into diverse fluoro-substituted species, which shows the practicability of this method.     

Photovoltammetric behavior and photoelectrochemical determination of p-phenylenediamine on CdS quantum dots and graphene hybrid film

A photoelectroactive film composed of CdS quantum dots and graphene sheets (GS) was coated on F-doped SnO₂ (FTO) conducting glass for studying the electrochemical response of p-phenylenediamine (PPD) under photoirradiation. The result indicated that the cyclic voltammogram of PPD on CdS–GS hybrid film became sigmoidal in shape after exposed under visible light, due to the photoelectrocatalytic reaction. Such a photovoltammetric response was used to rapidly optimize the photoelectrocatalytic activity of hybrid films composed of different ratios of CdS to GS toward PPD. The influences of scan rate and pH on the photovoltammetric behavior of PPD on CdS–GS film revealed that although the controlled step for electrochemical process was not changed under photoirradiation, more electrons than protons might participate the photoelectrocatalytic process. Furthermore, the photoelectroactive CdS–GS hybrid film was explored for PPD determination based on the photocurrent response of film toward PPD. Under optimal conditions, the photocurrent signal on CdS–GS film was linearly proportional to the concentration of PPD ranging from 1.0 × 10⁻⁷ to 3.0 × 10⁻⁶ mol L⁻¹, with a detection limit (3S/N) of 4.3 × 10⁻⁸ mol L⁻¹. Our work based on CdS–GS hybrid film not only demonstrated a new facile photovoltammetric way to study the photoinduced electron transfer process of PPD, but also developed a sensitive photoelectrochemical strategy for PPD determination.     

开口谐振环阵列在太赫兹波段的谐振特性实验研究

实验制备了单元尺寸在微米量级的开口谐振环周期阵列样品,测试了其在0.1~2 THz频段的散射系数,验证了不同极化方向的垂直入射可产生单独的电谐振或同时产生磁谐振的传输特性,验证了材料电导率对样品的谐振频率的影响。结合仿真计算结果,得到了等效的负介电常数和负磁导率随频率的变化关系,及其电、磁谐振频率与谐振环单元尺寸增大倍数k的关系曲线。实验和仿真均表明,样品的电谐振频率与1/k线性相关,而磁谐振频率与1/k成正比关系。