Solvothermal Method Research Articles

Two 2D Metal-Organic Frameworks Based on Purine Carboxylic Acid Ligands for Photocatalytic Oxidation of Sulfides and CO2 Chemical Fixation.

Two two-dimensional (2D) layered metal-organic frameworks (MOFs), namely, {[Yb(L)(H2O)2NO3]·2H2O}n (Yb-MOF) and [Er(L)(H2O)3Cl]n (Er-MOF) (H2L = 5-((6H-purin-6-yl)amino)isophthalic acid), were constructed by a solvothermal method and characterized. The catalytic performance study showed that the Yb-MOF could efficiently catalyze the oxidation of sulfides to sulfoxides under 15 W light-emitting diode (LED) blue light irradiation. Electron paramagnetic resonance spectroscopy and free-radical trapping experiments demonstrated that the photocatalytic reaction process involved •O2-, and the corresponding mechanism was proposed. Moreover, Er-MOF exhibited good catalytic efficiency and excellent substrate tolerance in the cycloaddition reaction of CO2, and the reaction conditions were mild. After 5 cycles, the catalytic activities of two MOFs did not significantly decrease, and the framework structures remained unchanged. Therefore, the Yb-MOF and Er-MOF were considered efficient and stable heterogeneous catalysts.

Highly Selective Electroreduction of Nitrobenzene to Aniline by Co-Doped 1T-MoS2.

The selective electrocatalytic reduction of nitrobenzene (NB) to aniline demands a desirable cathodic catalyst to overcome the challenges of the competing hydrogen evolution reaction (HER), a higher overpotential, and a lower selectivity. Here, we deposit Co-doped 1T MoS2 on Ti mesh by the solvothermal method with different doping percentages of Co as x % Co-MoS2 (where x = 3, 5, 8, 10, and 12%). Because of the lowest overpotential, lower charge-transfer resistance, strong suppression of the competing HER, and higher electrochemical surface area, 8% Co-MoS2 achieves 94% selectivity of aniline with 54% faradaic efficiency. The reduction process follows first-order dynamics with a reaction coefficient of 0.5 h-1. Besides, 8% Co-MoS2 is highly stable and retains 81% selectivity even after 8 cycles. Mechanistic studies showed that the selective and exothermic adsorption of the nitro group at x % Co-MoS2 leads to a higher rate of NB reduction and higher selectivity of aniline. The aniline product is successfully removed from the solution by polymerization at FTO. This study signifies the impact of doping metal atoms in tuning the electronic arrangement of 1T-MoS2 for the facilitation of organic transformations.

Photocatalytic Degradation of Tartrazine and Naphthol Blue Black Binary Mixture with the TiO2 Nanosphere under Visible Light: Box-Behnken Experimental Design Optimization and Salt Effect

In this study, TiO2 nanospheres (TiO2-NS) were synthesized by the solvothermal method. Firstly, the synthesized nanomaterial was characterized by X-ray diffraction (XRD), Fourier Transformed Infrared (FTIR), scanning electron microscopy (SEM) and UV-Vis Diffuse Reflectance Spectroscopy (DRS). To study the photocatalytic degradation of Tartrazine (TTZ) and Naphthol Blue Black (NBB) in a binary mixture, the influence of some key parameters such as pH, pollutant concentration and catalyst dose was taken into account under visible and UV light. The results show a 100% degradation efficiency for TTZ after 150 min of UV irradiation and 57% under visible irradiation at 180 min. The kinetic study showed a good pseudo-first-order fit to the Langmuir–Hinshelwood model. Furthermore, in order to get closer to the real conditions of textile wastewater, the influence of the presence of salt on TiO2-NS’s photocatalytic performance was explored by employing NaCl as an inorganic ion. The optimum conditions provided by the Response Surface Methodology (RSM) were low concentrations of TTZ (2 ppm) and NBB (2.33 ppm) and negligible salt (NaCl) interference. The percentage of photodegradation was high at low pollutant and NaCl concentrations. However, this yield became very low as NaCl concentrations increased. The photocatalytic treatment leads to 31% and 53% of mineralization yield after 1 and 3 h of visible light irradiation. The synthesis of TiO2-NS provides new insights that will help to develop an efficient photocatalysts for the remediation of contaminated water.

Comparative evaluation of antimicrobial activity of spinel structured transition metal ferrites supported on reduced graphene oxide against pathogenic strains of bacteria and fungi.

One of the global challenges for living things is to provide pollution and harmful microbes-free environment. In this study, magnetically retrievable spinel-structured manganese zinc ferrite (Mn0.5Zn0.5Fe2O4) (MZF) was synthesized by a facile solvothermal method. Further, the MZF with different weight percentages (10wt%, 50wt%, and 80wt%) were supported on reduced graphene oxide (rGO). The phase purity and morphology of MZF and MZF/rGO nanocomposite were confirmed by X-ray diffraction technique and scanning electron microscopy, respectively. The Fourier transform infrared spectroscopy, Raman, UV-visible spectroscopy, and thermogravimetric analyses of the as-synthesized nanocomposites were examined for the detection of various chemical groups, band gap, and thermal properties, respectively. The MZF/rGO nanocomposite exhibited significant antibacterial and antifungal activity against Eggerthella lenta, Enterococcus faecalis, Klebsiella pneumonia, Pseudomonas aeruginosa, and Candida albicans compared to bare MZF and rGO. The high surface area of rGO plays a crucible role in antimicrobial analysis. Additionally, the anti-bacterial and fungal activity is compared by synthesizing various metal ferrites such as MnFe2O4, ZnFe2O4, and Fe3O4. The 50wt% MZF/rGO nanocomposite exhibits significantly high antibacterial activity. However, 10wt% MZF/rGO nanocomposite shows good antifungal activity than Fe3O4, MnFe2O4, ZnFe2O4, MnZnFe2O4, 50wt%, and 80wt% MZF/rGO nanocomposites. These findings suggest that the prepared ferrite nanocomposites hold promise for microbial inhibition.

Introduction of Organic Dyes into Cadmium(II) MOF for Tunable Light Emission and Highly Sensitive Probing Antibiotics

A honeycomb porous cadmium(II) metal–organic framework {[Cd(L)(H2O)]·NMP·5H2O}n (1, H2L = 1‐(4‐carboxyphenyl)‐1H‐pyrazole‐3‐carboxylic acid and NMP = 1‐methyl‐2‐pyrrolidinone) was obtained using the solvothermal method. The luminescent molecules rhodamine B (RhB) and fluorescein (FL) were encapsulated in 1 using the immersion method to prepare RhB@1 and FL@1 dual emission composites. Additionally, a series of RhBx/FL1‐x@1 composites with varying luminescence properties were generated by altering the molar ratio of RhB to FL. Furthermore, the photoluminescence of RhB@1 and FL@1 was demonstrated to be caused by photoelectron transfer and fluorescence resonance energy transfer from 1 to the encapsulated guest module. Notably, RhB@1 showed the considerable improvement in fluorescence selectivity and detection limit (10‐6 M) for metronidazole and dimetronidazole with remarkable recyclability.

Preparation and optical properties of rare earth fluoride and its related composite materials

Rare earth fluoride and its composite materials have shown broad application prospects in fields such as optoelectronics and photocatalysis. In this study, we prepared rare earth fluoride (β-NaYF4 nanocrystals) and its related composite materials (β-NaYF4/ZnO composite and GQDs@NaYF4 nanomaterials) using a solvothermal method and investigated their optical performance. The characterization and performance of the prepared materials were analyzed using a transmission electron microscope, X-ray diffraction, upconversion emission spectra, and fluorescence lifetime imaging microscopy. The results show that the crystal thickness of β-NaYF4 nanocrystals is approximately 45.0 nm when the F−: Ln3+ value is 6. Furthermore, X-ray diffraction analysis reveals that diffraction peak positions in β-NaYF4 nanocrystals correspond to the peak positions of standard card at different doping concentrations of Zn2+ Moreover, it was observed that the highest fluorescence lifetime of Tm3+ ion in 1G4 is 778 μs when the doping concentration of Zn2+ is 1 mol%. When the concentration of exonuclease III increases to 22.5U, the upconversion fluorescence emission intensity of GQDs@NaYF4 nanomaterial is about 34 ∗ 106 a.u. When the activation reaction time is 90 minutes, the upconversion emission intensity of GQDs@NaYF4 nanomaterial is about 37 ∗ 106 a.u. In conclusion, we successfully prepared rare earth fluoride and its composite materials with excellent optical properties through the solvothermal method.

Environmental-related applications of ZnO nanopowders: Photocatalytic activity and photoluminescence response to ethanol

Zinc oxide (ZnO) and copper-doped zinc oxide (ZnO:Cu) nanopowders were synthesized via solvothermal methods using methanol and hexamethylenetetramine (HMTA). Undoped ZnO nanopowders underwent calcination in O2-rich and H2-rich atmospheres at 600 °C. Samples were studied by scanning electron microscopy, Brunauer–Emmett–Teller (BET) surface area analysis, X-ray diffraction (XRD), and Raman, photoluminescence (PL) and UV–vis absorbance spectroscopies. The doping and calcinations led to a reduction of the optical bandgap of the nanopowders, while their structure remained hexagonal wurtzite with some changes in lattice parameters and average nanoparticle sizes. The Cu2+ doping led to a BET surface area and violet PL component increase. Samples were also examined for environmental related applications, namely as photocatalyzers for dye degradation and as ethanol optical sensors. For photocatalytic activity in methylene blue degradation under UV, H2-rich calcined powders excelled, with a rate constant of −0.076 min−1, surpassing −0.057 min−1 (ZnO:Cu), −0.056 min−1 (O2-rich calcination), and −0.041 min−1 (as-grown ZnO). We propose that this improvement can be attributed to the formation of ZnO/Zn interfaces stemming from the reduction of surface interstitial zinc by H2 during calcination, in addition to the observed reduction of the ZnO bandgap. The doped nanopowders PL also showed excellent response when exposed to ethanol vapor.

Transition-Metal-Based Nanozymes: Synthesis, Mechanisms of Therapeutic Action, and Applications in Cancer Treatment.

Cancer, as one of the leading causes of death worldwide, drives the advancement of cutting-edge technologies for cancer treatment. Transition-metal-based nanozymes emerge as promising therapeutic nanodrugs that provide a reference for cancer therapy. In this review, we present recent breakthrough nanozymes for cancer treatment. First, we comprehensively outline the preparation strategies involved in creating transition-metal-based nanozymes, including hydrothermal method, solvothermal method, chemical reduction method, biomimetic mineralization method, and sol-gel method. Subsequently, we elucidate the catalytic mechanisms (catalase (CAT)-like activities), peroxidase (POD)-like activities), oxidase (OXD)-like activities) and superoxide dismutase (SOD)-like activities) of transition-metal-based nanozymes along with their activity regulation strategies such as morphology control, size manipulation, modulation, composition adjustment and surface modification under environmental stimulation. Furthermore, we elaborate on the diverse applications of transition-metal-based nanozymes in anticancer therapies encompassing radiotherapy (RT), chemodynamic therapy (CDT), photodynamic therapy (PDT), photothermal therapy (PTT), sonodynamic therapy (SDT), immunotherapy, and synergistic therapy. Finally, the challenges faced by transition-metal-based nanozymes are discussed alongside future research directions. The purpose of this review is to offer scientific guidance that will enhance the clinical applications of nanozymes based on transition metals.

Synergistic Effect of bimetallic active sites on Ce doped NH2–MIL-125 for promoting photocatalytic conversion of nitrogen to NH3

Ammonia (NH3), one of the most abundant inorganic compounds in the world, is highly demanded in the international market. NH3 is mainly synthesized using Haber-Bosch technology, which severely pollutes the environment and consumes high quantities of energy. In this study, a series of Ce doped NH2–MIL-125 (Ce–NH2–MIL-125) was prepared using a one-step solvothermal method to assess the activity of photocatalytic nitrogen fixation. The applied light energy interval of Ce–NH2–MIL-125 was widened, and the establishment of a Ce–O–Ti chemical bond optimized the transport path of the photogenerated carriers. This excellent photoelectric performance represents a significant improvement in the separation capacity of the photogenerated electrons and holes in Ce–NH2–MIL-125. Doping with Ce resulted in the generation of dual active sites, Ti4+/Ti3+ and Ce4+/Ce3+, in NH2–MIL-125; additionally, the increase in the amount of Ti3+ was significantly higher than that of the initial NH2–MIL-125. The synergistic effect of the bimetallic active sites in Ce–NH2–MIL-125 accelerated the photocatalytic nitrogen fixation reaction. Under full spectrum radiation, the ammonia generation rate of NH2–MIL-125 was 10.6 µmol g−1 h−1. Ce–NH2–MIL-125-1.0 exhibited the highest capacity for nitrogen fixation; the highest ammonia formation rate was 39.4 µmol g−1 h−1. The photocatalytic activity of Ce–NH2–MIL-125-1.0 was 3.7 times higher than that of NH2–MIL-125. This study provides a reference for catalytic research on modified NH2–MIL-125.

In-situ construct CuInS2/Bi/Bi2MoO6 S-scheme/schottky dual heterojunctions catalyst for enhanced photocatalytic degradation of diclofenac sodium.

In this paper, the S-scheme/Schottky heterojunction photocatalyst (CuInS2/Bi/Bi2MoO6, CIS/Bi/BMO) was successfully constructed via a facile in-situ solvothermal method, aimed at enhancing its photocatalytic performance. The results of the study on the photocatalytic degradation of diclofenac sodium (DCF) under simulated solar light irradiation revealed that the as-prepared composite exhibited remarkable catalytic efficiency in comparison to the pristine Bi2MoO6 and CuInS2. The plasmonic bismuth (Bi) was formed during the solvothermal process. Subsequently, CuInS2 and Bi were grown on the surface of Bi2MoO6 leading to forming CIS/BMO S-scheme heterojunction, along with a Schottky junction between Bi and Bi2MoO6. The use of ethylene glycol as a support was the main reason for the significant improvement in photocatalytic efficiency in the degradation of DCF. Moreover, the probable photocatalytic mechanisms for the degradation of DCF had been proposed based on the active species quenching experiments. The eleven degradation products were detected by HPLC-MS, and the degradation reaction pathway of DCF was deduced. Additionally, the CIS/Bi/BMO photocatalyst exhibited a consistently high removal rate after four cycles. This study proposes a new strategy for designing efficient S-scheme/Schottky heterojunction photocatalysts for solar energy conversion.

Size Control of Carbon Xerogel Spheres as Key Factor Governing the H2O2 Selectivity in Metal-Free Bifunctional Electro-Fenton Catalysts for Tetracycline Degradation

Carbon xerogel spheres co-doped with nitrogen and eco-graphene were synthesized using a typical solvothermal method. The results indicate that the incorporation of eco-graphene enhances the electrochemical properties, such as the current density (JK) and the selectivity for the four transferred electrons (n). Additionally, nitrogen doping has a significant effect on the degradation efficiency, varying with the size of the carbon xerogel spheres, which could be attributed to the type of nitrogenous group doped in the carbon material. The degradation efficiency improved in the nanometric spheres (48.3% to 61.6%) but decreased in the micrometric-scale spheres (58.6% to 53.4%). This effect was attributed to the N-functional groups present in each sample, with N-CNS-5 exhibiting a higher percentage of graphitic nitrogen (35.7%) compared to N-CMS-5 (15.3%). These findings highlight the critical role of sphere size in determining the type of N-functional groups present in the sample. leading to enhanced degradation of pollutants as a result of the electro-Fenton process.

Improved properties of CoFe2O4@rGO/PVDF composites prepared through a solution-mixing approach

In this work, a hybrid material based on CoFe2O4 nanoparticles immobilized on reduced graphene oxide (CoFe2O4@rGO) was successfully synthesized through a one-step green solvothermal method. Subsequently, the resultant CoFe2O4@rGO was further modified by aminopropyltriethoxysilane to form the A-CoFe2O4@rGO hybrid, serving as the filler of poly(vinylidene fluoride) (PVDF). The facile preparation of A-CoFe2O4@rGO was confirmed through various microstructural characterization techniques. PVDF-based composites with varying contents of A-CoFe2O4@rGO (1 wt%, 3 wt%, 5 wt%, 7 wt%, and 10 wt%) were prepared using a solution-mixing approach. SEM results revealed uniform distribution of the A-CoFe2O4@rGO filler within the PVDF matrix. The XPS results indicated an obvious interfacial interaction between the A-CoFe2O4@rGO filler and PVDF matrix. Consequently, the crystallization degree and β crystalline content of PVDF matrix in the A-CoFe2O4@rGO(7 wt%)/PVDF composite were enhanced to 52.3 % and 32.1 %, respectively, compared to 42.2 % and 26.0 %, respectively, in pure PVDF. The A-CoFe2O4@rGO(10 wt%)/PVDF composite enhanced electrical conductivity and dielectric constant at 100 Hz, with values of 1.33 × 10−7 S/m and 22.1, respectively, compared to 1.86 × 10−9 S/m and 8.6, respectively, in pure PVDF. In addition, despite the non-magnetic nature of pure PVDF, the A-CoFe2O4@rGO(10 wt%)/PVDF composite possessed a magnetization value of 1.64 emu/g at 60,000 Oe. The comprehensive enhancement in crystallization behavior, electrical, dielectric, and magnetic properties demonstrates the potential of the A-CoFe2O4@rGO/PVDF composite for various applications.

Au- ZnFe2O4 hollow microspheres based gas sensor for detecting the mustard gas simulant 2-chloroethyl ethyl sulfide.

Mustard gas, a representative of blister agents, poses a severe threat to human health. Although the structure of 2-chloroethyl ethyl sulfide (2-CEES) is similar to mustard gas, 2-CEES is non-toxic, rendering it a commonly employed simulant in related research. ZnFe2O4-based semiconductor gas sensors exhibit numerous advantages, including structural stability, high sensitivities, and easy miniaturization. However, they exhibit insufficient sensitivity at low concentrations and require high operating temperatures. Owing to the effect of electronic and chemical sensitization, the gas-sensing performance of a sensor may be remarkably enhanced via the sensitization method of noble metal loading. In this study, based on the morphologies of ZnFe2O4 hollow microspheres, a solvothermal method was adopted to realize different levels of Au loading. Toward 1 ppm of 2-CEES, the gas sensor based on 2 wt.% Au-loaded ZnFe2O4 hollow microspheres exhibited a response sensitivity twice that of the gas sensor based on pure ZnFe2O4; furthermore, the response/recovery times decreased. Additionally, the sensor displayed excellent linear response to low concentrations of 2-CEES, outstanding selectivity in the presence of several common volatile organic compounds, and good repeatability, as well as long-term stability. The Au-loaded ZnFe2O4-based sensor has considerable potential for use in detecting toxic chemical agents and their simulants.

Synthesis and characterization nitrogen-doped carbon dots from candlenut shells using hydrothermal and solvothermal methods

Synthesis and characterization nitrogen-doped carbon dots from candlenut shells using hydrothermal and solvothermal methods

Garnet-based solid state batteries benefitting from an ionic/electronic mixed conductive interface constructed by lithiation of porous FeS2

Garnet-based solid-state lithium metal batteries are considered as the potential candidates for the next-generation energy storage systems due to their high energy density, wide operating temperature, and high safety. However, the poor wettability of the lithium metal anode/garnet interface, the large interface resistance, and the risk of lithium dendrites growing and even penetrating electrolytes during cycling limit the practical application of garnet-based solid-state lithium metal batteries. In this work, a porous network FeS2 with an amorphized structure is prepared by using the solvothermal method and used as the Li/garnet interface modification layer. The porous FeS2 can be in situ converted into a Li2S/Fe mixed conductive layer by the thermal lithiation of molten metallic lithium. This mixed conductive layer can significantly reduce the interface resistance, ensure the close contact between Li and garnet, and inhibit the growth of lithium dendrites. The interface resistance of the modified Li/FeS2-LLZTO (LLZTO is Li6.5La3Zr1.5Ta0.5O12) interface at 60 °C is as small as 15.20 Ω cm2. The ionic conductivity of fully lithiated FeS2 is estimated to be 1.58 × 10−6 S cm−1 at room temperature. The Li/FeS2-LLZTO/Li symmetrical cell can cycle stably for more than 400 h at a high current density of 400 μA cm−2, with the voltage polarization of only about 25 mV, and can withstand a larger current density of 600 μA cm−2 without the polarization exceeding 50 mV. These results demonstrate the feasibility of in situ lithiation of porous iron sulfide into a mixed ion/electron conductive layer as a solid-state garnet interface modification strategy and provide the new interface method for the development of high-performance solid-state lithium metal batteries.

Comparing The Catalytic Activity of Mg-BTC Metal Organic Framework and Post Synthetically Modified (TiO2 @ Mg-BTC) Metal Organic Framework for Cyanosilylation of Aldehydes

Metal organic frameworks (MOFs) are an emerging class of porous crystalline hybrid materials synthesised by the coordination of inorganic connectors and organic linkers, which has numerous potential applications in various fields. Here we report a comparative study on Mg-BTC MOF and TiO @Mg-BTC MOF as a heterogeneous catalyst. Mg-BTC MOF was synthesised by solvothermal method and subjected to comparative study with its post synthetically modified (PSM) counterpart to understand their catalytic behaviour for cyanosilylation of aldehydes. The synthesised Mg-BTC MOF and TiO @Mg-BTC MOF were characterised by powder XRD, BET surface area, SEM, FT-IR, TGA techniques. A detailed characterization study was performed to understand the correlation between catalytic activity and morphology of the assynthesized MOF and PSM-MOF. The catalytic activity of the hybrid materials were evaluated by GC-MS analysis. The results of the catalytic reactions revealed that post synthetically modified (TiO @Mg-BTC) MOF exhibited significantly higher catalytic activity compared to Mg-BTC MOF. The enhanced catalytic efficiency is due to the incorporation of TiO nanoparticles, which provides active sites for catalytic reactions under heterogeneous conditions. Even after repeated recycling and reuse, the catalytic ability of the catalyst retains. The impact of TiO on the framework shows variation in texture, surface area, thermal stability and catalytic behaviour on the MOF materials. Thus, our study emphasizes

Co3O4/RGO Nanoparticles Fabricated by Facile Solvothermal Method as an Anode Material for High‐Performance Lithium‐Ion Batteries

AbstractA potential anode material for lithium‐ion batteries (LIBs), Co3O4 has been widely considered by many scholars because of its excellent properties in terms of electrochemical characteristics and theoretical specific capacity. However, according to the existing research results, we found that the improvement of the electrochemical performance of Co3O4 has encountered a bottleneck because its intrinsic conductivity is not high enough, and more importantly, the volume expansion is too significant during the charge and discharge process, which leads to the material structure breaking. Therefore, this paper proposes a simple and scalable solvothermal and subsequent calcination method to prepare Co3O4 and reduced graphene oxide (RGO) composite nanoparticles with superior microstructures, and their morphological and electrochemical properties were investigated at different calcination temperatures. As a high‐performance anode material for lithium‐ion batteries, the Co3O4/RGO nanoparticles obtained at 550 °C exhibited terrific initial discharge capacity of 1714.2 mAh g−1, the reversible specific capacity of 1191.9 mAh g−1 with quality coulombic efficiency 98.17 % at 0.5 A g−1 after 100 cycles and extraordinary rate performance (907.6 mAh g−1 with a coulombic efficiency of 99.2 % at 2 A g−1). The facile synthesis method and excellent findings have led to better application prospects for Co3O4/RGO nanoparticles.

Microwave‐assisted Fast Synthesis of a Donor‐Acceptor Covalent Organic Framework towards Photooxidative Amidation Catalysis

The synthesis of covalent organic frameworks (COFs) at bulk scale require robust, straightforward, and cost‐effective techniques. However, the traditional solvothermal synthetic methods of COFs suffer low scalability as well as requirement of sensitive reaction environment and multiday reaction time (2‐10 days) which greatly restricts their practical application. Here, we report  microwave assisted  rapid  and optimized synthesis of a donor‐acceptor (D−A) based highly crystalline COF, TzPm‐COF in second (10 sec) to minute (10 min) time scale. With the increasing of the time from seconds to minutes crystallinity, porosity and morphological changes are also observed for TzPm‐COF. Owing to visible range light absorption, suitable band alignment, and low exciton binding energy (Eb=64.6 meV), TzPm‐COF can efficaciously produce superoxide radical anion (O2•−) after activating molecular oxygen (O2) which eventually drives aerobic photooxidative amidation reaction with high recyclability. This photocatalytic approach works well with a variety of substituted aromatic aldehydes having electron‐withdrawing or donating groups and cyclic, acyclic, primary or secondary amines with moderate to high yield. Furthermore, catalytic mechanism was established by monitoring the real‐time reaction progress through in‐situ diffuse reflectance infrared Fourier transform spectroscopic (DRIFTS) study.

Microwave-assisted Fast Synthesis of a Donor-Acceptor Covalent Organic Framework towards Photooxidative Amidation Catalysis.

The synthesis of covalent organic frameworks (COFs) at bulkscalerequire robust, straightforward, andcost-effective techniques. However, the traditional solvothermal synthetic methods of COFs suffer low scalability as well as requirement of sensitive reaction environment and multiday reaction time (2-10 days) which greatly restricts their practical application. Here, we report microwave assisted rapid and optimized synthesis of a donor-acceptor (D-A) based highly crystalline COF, TzPm-COF in second (10 sec) to minute (10 min) time scale. With the increasing of the time from seconds to minutes crystallinity, porosity and morphological changes are also observed for TzPm-COF. Owing to visible range light absorption, suitable band alignment, and low exciton binding energy (Eb=64.6meV),TzPm-COF canefficaciously produce superoxide radical anion (O2•-) after activating molecular oxygen (O2) which eventually drives aerobic photooxidative amidation reaction with high recyclability. This photocatalytic approach works well with a variety of substituted aromatic aldehydes having electron-withdrawing or donating groups and cyclic, acyclic, primary or secondary amines with moderate to high yield. Furthermore, catalytic mechanism was established by monitoring the real-time reaction progress through in-situ diffuse reflectance infrared Fourier transform spectroscopic (DRIFTS) study.

Facile and efficient synthesis of sweater-ball shaped metal-organic framework/nickel sulfide nanoheterojunction for boosting electrochemical glucose sensing

The synthesis of heterojunction materials is regarded as an efficient way to enhance catalytic activities in various catalytic reactions. However, the existing fabrication approaches often rely on complex multi-step synthesis process. In this work, we fabricate sweater-ball shaped nanostructured MOF/TMS (Ni-MOF/NiS1.03) heterojunction by one-pot, one-step solvothermal method. According to the results of discrete Fourier transform (DFT) calculations and experiments, the formation of Ni-MOF/NiS1.03 heterojunction interfaces improves electron transfer and charge redistribution, and increases the adsorption energy of glucose molecules as well, which is conducive to enhance electrochemical activity of electrode materials. The as-prepared Ni-MOF/NiS1.03 heterojunction exhibit enhanced glucose sensitivity, wide detection range and low detection limit. This study paves the way towards the development of MOF-based heterojunctions for electrochemical applications.