Latest ArticlesThree-dimensional (3D) printing, also known as additive manufacturing, has the advantages of low cost, easy structure operation, rapid prototyping, and easy customization. In the past few years, materials with different structures, compositions, and properties have been widely studied as prospects in the field of 3D printing. This paper reviews the synthesis methods and morphologies of one-, two- and three-dimensional micro/nano materials and their composites, as well as their applications in electrochemistry, such as supercapacitors, batteries and electrocatalysis. The latest progress and breakthroughs in the synthesis and application of different structural materials in 3D-printing materials, as well as the challenges and prospects of electrochemical applications, are discussed.
Radical-mediated reactions have many advantages in the construction of complex molecular scaffolds by forging chemical bonds of high challenge. Diazenes, including 1, 1-diazenes and 1, 2-diazenes, can generate biradical species via nitrogen extrusion under thermal or photochemical conditions. The superior reactivity of the generated biradical enables various types of synthetic transformations with excellent chemoselectivity and has been applied to the complex natural products synthesis. In this mini-review, the modes of reaction are summarized and discussed, namely ring contraction via nitrogen deletion, homo or heterodimerization, trimethylenemethane (TMM)-diyl cycloaddition. Applications of these classes of reactions in complex natural product synthesis are illustrated. Last but not least, the current state, future directions, and opportunities for dinitrogen extrusion reaction from diazenes are highlighted and discussed.
Electrochemical degradation performances of three non-steroidal anti-inflammatory drugs (NSAIDs), acetaminophen (ACT), aspirin (ASP) and ibuprofen (IBP), were investigated and compared in their alone and mixture conditions using Ti/SnO2-Sb/La-PbO2. The pseudo-first-order degradation kinetics (k) order was kIBP-A (0.110 min−1) > kASP-A (0.092 min−1) > kACT-A (0.066 min−1) in their alone condition, while that was kACT-M (0.088 min−1) > kASP-M (0.063 min−1) > kIBP-M (0.057 min−1) in their mixture condition. The •OH apparent production rate constant of 5.23 mmol L−1 min−1 m−2 and an electrical energy per order (EEO) value of 6.55 Wh/L could ensure the synchronous degradation of the NSAIDs mixture. The mineralization efficiency of NSAIDs mixture was 86.9% at 240 min with a mineralization current efficiency of 1.67%. Acetic acid and oxalic acid were the main products in the mineralization process for the both conditions. In the mixture condition, there were higher k values at lower initial concentrations and higher current density, while the presence of carbonate and humic acid inhibited their degradation. The results indicated electrochemical advanced oxidation process can effectively and synchronously mineralize NSAIDs mixture in wastewater.
A kind of CdS/Cd-BiOCl immobilized films photocatalyst was prepared. The optical and physicochemical properties of the CdS/Cd-BiOCl photocatalysts were analysed, and the detailed characterization revealed CdS/Cd-BiOCl films photocatalyst with good charge carrier separation effect. The reusabilities and photocatalytic properties of the samples were studied. The 15%CdS/Cd-BiOCl photocatalyst exhibited superior performance in photocatalytic degradation of tetracycline (TC) and favorable stability under visible light irradiation. As for the photodegradation rate of TC, 15%CdS/Cd-BiOCl exhibited an excellent photodegradation activity, which is 4.06 and 9.53 times higher than that of CdS/Cd and BiOCl, respectively. The results showed that dominant active species are •O2− and •OH radicals during photodegradation. The charge transfer in Z-scheme CdS/Cd-BiOCl films photocatalyst could synchronously generate conduct band (CB) electrons in BiOCl and valence band (VB) holes in CdS, and metal Cd served as electron mediator. This work can be a reference for the design of film photocatalysts and new insight for photodegradating towards contaminants.
Semiconductor-employed photocatalytic CO2 reduction has been regarded as a promising approach for environmental-friendly conversion of CO2 into solar fuels. Herein, TiO2/Cu2O composite nanorods have been successfully fabricated by a facile chemical reduction method and applied for photocatalytic CO2 reduction. The composition and structure characterization indicates that the Cu2O nanoparticles are coupled with TiO2 nanorods with an intimate contact. Under light illumination, all the TiO2/Cu2O composite nanorods enhance the photocatalytic CO2 reduction. In particular, the TiO2/Cu2O-15% sample exhibits the highest CH4 yield (1.35 µmol g-1 h-1) within 4 h irradiation, and it is 3.07 and 15 times higher than that of pristine TiO2 nanorods and Cu2O nanoparticles, respectively. The enhanced photoreduction capability of the TiO2/Cu2O-15% is attributed to the intimate construction of Cu2O nanoparticles on TiO2 nanorods with formed p-n junction to accelerate the separation of photogenerated electron-hole pairs. This work provides a reference for rational design of a p-n heterojunction photocatalyst for CO2 photoreduction.
Eggshell-loaded CoFe2O4 catalyst was synthesized via a convenient hydrothermal method during our work, then the surface morphology and elemental composition of the composites were systematically investigated. Performance of CoFe2O4/eggshell-activated peroxymonosulfate (PMS) system was evaluated by selecting florfenicol (FF) as the model pollutant, and effects of operating parameters and water matrices on the FF removal efficiency in this system were investigated. In addition, main radicals involved in FF degradation were identified by EPR tests and radical quenching experiments, and possible mechanism was proposed. The reduction of toxicity during FF degradation was confirmed, and in combination with HP-LC tests, it was found that dehalogenation and defluorination were effectively carried out during FF degradation. In addition, the prepared CoFe2O4 polyvinylidene fluoride (PVDF) membrane effectively improved the stability of the material and reduced the precipitation of metals.
Self-supported transition-metal single-atom catalysts (SACs) facilitate the industrialization of electrochemical CO2 reduction, but suffer from high structural heterogeneity with limited catalytic selectivity. Here we present a facile and scalable approach for the synthesis of self-supported nickel@nitrogen-doped carbon nanotubes grown on carbon nanofiber membrane (Ni@NCNTs/CFM), where the Ni single atoms and nanoparticles (NPs) are anchored on the wall and inside of nitrogen-doped carbon nanotubes, respectively. The side effect of Ni NPs was further effectively inhibited by alloying Ni with Cu atoms to alter their d-band center, which is theoretically predicted and experimentally proved. The optimal catalyst Ni9Cu1@NCNTs/CFM exhibits an ultrahigh CO Faradic efficiency over 97% at −0.7 V versus reversible hydrogen electrode. Additionally, this catalyst shows excellent mechanical strength which can be directly used as a self-supporting catalyst for Zn-CO2 battery with a peak power density of ~0.65 mW/cm2 at 2.25 mA/cm2 and a long-term stability for 150 cycles. This work opens up a general avenue to facilely prepare self-supported SACs with unitary single-atom site for CO2 utilization.
As a common volatile organic compound, benzene (C6H6) exists in home decoration pollution gas widely, which causes great harm to the environment and human health. Therefore, it is necessary to rationally design advanced materials with high selectivity to detect and capture C6H6. Herein, combined with the d-band center theory and cohesive energy, a new two-dimensional metal-organic framework material, Ni-doped hexaaminobenzene-based coordination polymer (Ni-HAB-CP) is designed, and its application potential as a C6H6 sensor are systematically investigated by using first principles calculation. The result shows that Ni-HAB-CP has a strong adsorption for C6H6 without any additional method. In addition, Ni-HAB-CP can maintain good conductivity before and after adsorption, and C6H6 can be easily desorbed from the surface of Ni-HAB-CP by charge control. Moreover, the I-V curve calculated by Atomistix Toolkit (ATK) reveals that Ni-HAB-CP has high sensitivity and selectivity to C6H6. Hence, Ni-HAB-CP is expected to be used as a potential material for a highly efficient and recyclable C6H6 sensor in the future. The calculation and analysis methods used in this paper could provide a certain theoretical basis and reference for the future research of gas sensors.
Designing visible light photocatalysts with a metal oxide semiconductor as the starting material could expand a new horizon for the conversion and storage of solar energy. Here, the benchmark photocatalyst TiO2 was used to pursue this goal by anchoring aromatic acids. Extending the aromatic acid was strategically deployed to design TiO2 complexes with violet light-induced selective aerobic oxidation of sulfide as the probe reaction. With benzoic acid (BA) as the initial molecule, horizontally extending one or two benzene rings furnishes 2-naphthoic acid (2-NA) and 2-anthracene acid (2-AA). Moreover, triethylamine (TEA), an electron transfer mediator, was introduced to maintain the integrity of the anchored aromatic acids. Notably, there was a direct correlation between the π-conjugation of aromatic acid ligand and the selective aerobic oxidation of sulfides. Among the three aromatic acids, 2-AA delivered the best result over TiO2 due to the most extensive π-conjugated system. Ultimately, violet light-induced selective aerobic oxidation of sulfides into corresponding sulfoxides was conveniently realized by cooperative photocatalysis of 2-AA-TiO2 with 10 mol% of TEA. This work affords an extending strategy for designing the next-generation ligands for semiconductors to expand visible light-induced selective reactions.
Elemental doping confined in atomically-thin 2D semiconductors offers a compelling strategy for constructing high performance photocatalysts. Although impressive progress has been achieved based on co-thermolysis method, the choices of dopants as well as semiconductor hosts are still quite limited to yield the elaborate photocatalyst with atomic-layer-confined doping defects, owing to the difficulty in balancing the reaction kinetics of different precursors. This study shows that the cation exchange reaction, which is dictated by the Pearson's hard and soft acids and bases (HSAB) theory and allowed to proceed at mild temperatures, can be developed into a conceptually new protocol for engineering elemental doping confined in semiconductor atomic layers. To this aim, the two atomic layers of a new type of 2D photocatalyst PdSeO3 (PdSeO3 2ALs, 1.1 nm) are created by liquid exfoliation and exploited as a proof-of-concept prototype. It is demonstrated that the Mn(II) dopants with controlled concentrations can be incorporated into PdSeO3 2ALs via topological Mn2+-for-Pd2+ cation exchange performed in water/isopropanol solution at 30 ℃. The resulting Mn-doped PdSeO3 2ALs present enhanced capacity for driving photocatalytic oxidation reactions in comparison with their undoped counterparts. The findings here suggest that the new route mediated by post synthetic cation exchange promises to give access to manifold 2D confined-doping photocatalysts, with little perturbations on the thickness, morphology, and crystal structure of the atomically-thin semiconductor hosts.
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