Latest ArticlesAs an antibiotic, sulfadiazine has posed a serious threat to humans and ecosystems due to its chronic toxicity. The advanced oxidation processes (AOPs) via heterogeneous catalytic activation of peroxymonosulfate (PMS) have significant potential for the degradation of antibiotics. However, there are multiple restrictions including non-specifically binding to target contaminants, which would deplete oxidation capacity, and lacking energy effectiveness due to inefficient utilization of reactive oxygen species (ROS). To overcome these obstacles, we adopted the "bait-hook & destroy" strategy in this study. Herein, we synthesized a novel micrometer-sized NiOOH hierarchical spheres assembled from nanosheets, which have relatively large specific surface areas and yield specified cavities to "bait-hook" sulfadiazine and PMS onto the surface cavities. This process was further conductive to effective generation of ROS and subsequently "destruction" of sulfadiazine with elevated mass transformation rate. 20.4% of sulfadiazine can adsorb to NiOOH surface in less than 30 min (0.0051 min−1), and then sulfadiazine was completely degraded in 90 min intervals in the NiOOH/PMS system. The degradation rate constant (k = 0.0537 min−1) was about 5.3, 2.5 and 2.2 times higher than that in Ni2O3/PMS, NiO/PMS and Ni(OH)2/PMS system, respectively. This was ascribed to the synergistic catalytic oxidation and adsorption process occurred on the surface of NiOOH. Appreciably, there were both non-radicals (1O2) and radicals (O2•− and SO4•−) involved in the NiOOH/PMS system, and 1O2 was distinguished as the dominated ROS for degradation of sulfadiazine. This study provides a novel strategy via synergistic adsorption and catalytic oxidation, and indicates that the micrometer-sized NiOOH hierarchical sphere as heterogeneous catalyst is an attractive candidate for potential application of the SR-AOPs technology in water treatment.
The construction of core-shell structure is an effective strategy for promoting the emission efficiency of upconversion nanocrystals (UCNCs). In this work, the UCNCs based on Nd-doping with a multilayer core-shell nanostructure are fabricated toward achieving efficient upconversion for 808 nm excitation, which have great potential for optical applications, especially photobiological applications.
In this study, natural mackinawite (FeS), a chalcophilic mineral, was utilized to prepare iron/copper bimetallic oxides (CuO@FexOy) by displacement plating and calcination process. Various characterization methods prove that Cu0 is successfully coated on the surface of FeS, which were further oxidized to CuO, Fe3O4 and/or Fe2O3 during calcination process, respectively. CuO@FexOy performed highly efficient capacity to activate PMS for the degradation of various emerging pollutants including sulfamethoxazole (SMX), carbamazepine (CBZ), bisphenol A (BPA), 2, 4-dichlorophenol (2, 4-DCP) and diclofenac (DCF) in aqueous solution. Complete removal of the above pollutants was observed after 8 min of CuO@FexOy/PMS treatment. Taking SMX as an example, the key parameters including CuO@FexOy dosage, PMS dosage and initial pH were optimized. The results show that the catalytic system can be worked in a wide pH range (3.0-9.0). The quenching experiments and electron spin resonance (ESR) test demonstrated that the main reactive oxygen species in CuO@FexOy/PMS system were hydroxyl radicals (•OH) and sulfate radicals (SO4•–), and SO4•– was the primary reactive species. Besides, the influence of coexisting anions (i.e., Cl–, NO3–, HCO3– and H2PO4–) for the degradation of SMX was explored. CuO@FexOy/PMS system can maintain good catalytic activity and reusability in different water bodies and long-term running. This work provided a green strategy to fabricate the efficient catalyst in PMS-based advanced oxidation processes.
To obtain a high-performance heterogeneous photo-catalyst, herein, the hetero-structured ZnIn2S4-NiO@MOF (ZNM) nano-sheets are designed and prepared by partial pyrolysis of nickel-based MOFs (Ni-MOF) combined with the low-temperature solvo-thermal method. The results indicate that the NiO nanoparticles, produced by partial pyrolysis of the Ni-MOF, have a high density of the surface active sites with limited aggregation, which act as a co-catalyst to capture photo-induced charge carriers. In addition, the morphology and structure of Ni-MOF nano-sheets were preserved in ZNM, which is beneficial to the reduction of the conduction barrier for the photo generated electron-hole pairs. With the synergetic advantages of co-catalyst and unique two-dimensional hetero-structure, ZNM nano-sheets exhibited significantly improved activity for photo-catalytic hydrogen production.
Exploring platinum group metal-free electrocatalysts with superior catalytic performance and favorable durability for oxygen reduction reaction is a remaining bottleneck in process of developing sustainable techniques in energy storage and conversion. Herein, a hierarchical porous single atomic Fe electrocatalyst (Fe/Z8-E-C) is rationally designed and synthesized via acid etching, calcination, adsorption of Fe precursor and recalcination processes. This unique electrocatalyst Fe/Z8-E-C shows excellent oxygen reduction performance with a half-wave potential of 0.89 V in 0.1 mol/L KOH, 30 mV superior to that of commercial Pt/C (0.86 V), which is also significantly higher than that of typical Fe-doped ZIF-8 derived carbon nanoparticles (Fe/Z8-C) with a half-wave potential of 0.84 V. Furthermore, Fe/Z8-E-C-based Zn-air battery exhibits greatly enhanced peak power density and specific capacity than those of original Fe/Z8-C, verifying the remarkable performance and practicability of this specially designed hierarchical structure due to its efficient utilization of the active sites and rapid mass transfer. This present work proposes a new method to rationally synthesize single atom electrocatalysts loaded on hierarchical porous frame materials for catalysis and energy conversion.
Development of low-cost electrode materials with long cycle life and high volumetric capacity is important for large-scale applications of lithium-ion batteries (LIBs). Here, an electrode made from Fe2O3 encapsulated with N-doped carbon (Fe2O3@N-C) via ZIF-8 coating and carbonization process is reported. A cavity was generated between the Fe2O3 and N-C material during the carbonization process that is conducive to alleviating the volume expansion of Fe2O3. As a result, the Fe2O3@N-C composite exhibits a high specific capacity (1064 mAh/g at 0.1 A/g) and cycle stability (803.6 mAh/g at 1.0 A/g after 1100 cycles) when used as the LIB anode. In addition, the influence of carbonization under air on the LIB performance was investigated by controllably changing the crystal phase of Fe2O3 and the thickness of the carbon layer. This work provides a new method for the design and fabrication of yolk-shell composite electrodes for LIBs and other applications.
Anthrones are key structural motifs in many natural products, bioactive compounds and pharmaceutical chemicals. Earth-abundant-metal-catalyzed asymmetric functionalization of anthrones has not proved to be viable. Herein, we disclosed a highly enantioselective propargylic substitution of anthrones with propargylic esters using copper salts with chiral N, N, P-ligand. This strategy is amenable to a broad range of substrates, uses readily available starting materials, provides excellent yields with remarkable enantioselectivity under mild conditions, and enables attractive products diversification routes.
Geometries of molecule-molecule interfaces strongly influence the current passing from one molecule to another. The contact conductance of molecule-molecule junctions which consist of fullerene and tin phthalocyanine molecules is investigated with a low-temperature scanning tunneling microscope. Two types of molecules are deposited onto Cu(111). Fullerene molecules are transferred to tips through controlled contact of STM tips on molecules. The molecule-molecule junctions are formed by approaching fullerene-terminated tips to tin phthalocyanine molecules on Cu(111). Our experimental method can be extended to study the intermolecular charge transport of a range of molecular junctions.
Traditional soft lithography based PDMS device fabrication requires complex procedures carried out in a clean room. Herein, we report a photolithography-free method that rapidly produces PDMS devices in 30 min. By using a laser cutter to ablate a tape, a male photoresist mold can be obtained within 5 min by a simple heating-step, which offers significant superiority over currently used photolithographybased method. Since it requires minimal energy to cut the tape, our fabrication strategy shows good resolution (~ 100 μm) and high throughput. Furthermore, the micro-mold height can be easily controlled by changing the tape types and layers. As a proof-of-concept, we demonstrated that the fabricated PDMS devices are compatible with biochemical reactions such as quenching reaction of KI to fluorescein and cell culture/staining. Collectively, our strategy shows advantages of low input, simple operation procedure and short fabrication time, therefore we believe this photolithography-free method could serve as a promising way for rapid prototyping of PDMS devices and be widely used in general biochemical laboratories.
The biological activities of a series of 3, 3′-spirocyclic indole derivatives containing CF2, phosphine oxide, indole, and cyano functional groups were evaluated, and these derivatives were found to exhibit anti-TMV, fungicidal, and insecticidal activities.
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