Latest ArticlesCrystalline engineering and heterostructure have attracted much attention as effective strategies to improve the electrocatalytic activity for hydrogen evolution reaction (HER). In this study, a new heterostructure catalyst (Ru/RuS2@N-rGO) with low crystallinity was fabricated by a simple and low-temperature method for HER in alkaline solution, applying the Na2SO4 as S source and polypyrrole as N source. Optimizing through the controllable crystalline engineering and composition ratio of Ru and RuS2, the Ru/RuS2@N-rGO heterocatalyst at the calcining 500 ℃ revealed highly efficient HER activity with overpotential 18 mV at a current density 10 mA/cm2 and remarkable stability for 24 h in 1.0 mol/L KOH. This work provides a facile and effective method in designing advanced electrocatalysts for HER in the alkaline electrolytes by synergistically structural and component modulations.
In this paper, a hydrothermal approach is utilized for the first time in integrating graphene oxide (GO), acetic acid (HAc) and nickel foam to prepare hydrogenated graphene (HG). There are two primary aims of this study: one is to ascertain the structure of the as-prepared HG, and the other one is to investigate the ferromagnetism of the HG. Under hydrothermal conditions, GO was reduced and hydrogenated by HAc, while the nickel foam served as a catalyst. This work provides a novel and facile route for the synthesis of hydrogenated graphene, which may lead to the application of hydrogenated graphene in spin electronic devices.
Surface oxidized iron-nickel nanorods coupling with reduced graphene architectures (FeNi-O-rGA) are successfully constructed via hydrothermal, freeze-drying, and thermal activation approaches. The hierarchical structure can provide lots of pathways for fast ion diffusion and charge transfer, and expose abundant catalytic sites. Meanwhile, the activity of FeNi-O-rGA is boosted by the optimized metal-oxygen bond strength in FeNi3 alloys. Partial oxidized FeNi nanorods are strongly coupled with rGA by the formation of metal-O-C bonds, which can impede the aggregation of FeNi3 alloys and increase the utilization of active sites. The special structure and partially oxidized FeNi nanorods for FeNi-O-rGA can result in excellent OER activity and catalytic stability. Only 215 mV of overpotential is required to drive the current density of 10 mA/cm2 as well as the Tafel slope of 50.9 mV/dec in 1 mol/L KOH. The change of surface chemistry of FeNi-O-rGA is confirmed by XPS after the OER test, which indicates the highly catalytic stability of FeNi-O-rGA due to the formation of intermediate metal oxyhydroxide.
Potassium-ion batteries (KIBs) have become the most promising alternative to lithium-ion batteries for large-scale energy storage system due to their abundance and low cost. However, previous reports focused on the intercalation-type cathode materials usually showed an inferior capacity, together with a poor cyclic life caused by the repetitive intercalation of large-size K-ions, which hinders their practical application. Here, we combine the strategies of carbon coating, template etching and hydrothermal selenization to prepare yolk-shelled FeSe2@N-doped carbon nanoboxes (FeSe2@C NBs), where the inner highly-crystalline FeSe2 clusters are completely surrounded by the self-supported carbon shell. The integrated and highly conductive carbon shell not only provides a fast electron/ion diffusion channel, but also prevents the agglomeration of FeSe2 clusters. When evaluated as a conversion-type cathode material for KIBs, the FeSe2@C NBs electrode delivers a relatively high specific capacity of 257 mAh/g at 100 mA/g and potential platform of about 1.6 V, which endow a high energy density of about 411 Wh/kg. Most importantly, by designing a robust host with large internal void space to accommodate the volumetric variation of the inner FeSe2 clusters, the battery based on FeSe2@C NBs exhibits ultra-long cycle stability. Specifically, even after 700 cycles at 100 mA/g, a capacity of 221 mAh/g along with an average fading rate of only 0.02% can be retained, which achieves the optimal balance of high specific capacity and long-cycle stability.
The angle dependence of photonic crystals (PCs) dramatically limits their practical applications in the colorimetrical sensing of humidity and volatile organic compound (VOC) vapors. In addition, it is challenging for inverse opal PCs to colorimetrically distinguish between vapors with similar refractive indices. Different from the mechanism of PC-based sensors, here, we report an angle-independent polyacrylamide (PAAm) organogel structural color film based on the mechanisms of retroreflection, total internal reflection (TIR) and interference with a shape similar to a single-sided "egg waffle". During the process of responding to humidity and VOC vapors, the color of the film remains angle-independent in the normal angle range of 0° to 45° under coaxial illumination and observation conditions. At the same time, the film can colorimetrically distinguish between vapors with similar refractive indices, such as methanol and ethanol, which is mainly due to the differences in their polarity and solubility parameters. The film shows good stability, reversibility and selectivity when exposed to vapors. A colorimetric sensor with a new response mechanism is proposed and has the potential to effectively distinguish between vapors with similar refractive indices. Furthermore, this responsive retroreflective structural color film (RRSCF) provides a universal strategy to develop targeted angle-independent structural color sensors by selecting optimized materials.
The development of the preparation strategy for high-quality and large-size graphene via eco-friendly routes is still a challenging issue. Herein, we have successfully developed a novel route to chemically exfoliate natural graphite into high-quality and large-size graphene in a binary-peroxidant system. This system is composed of urea peroxide (CO(NH2)2·H2O2) and hydrogen peroxide (H2O2), where CO(NH2)2·H2O2 is used in preparing graphene for the first time. Benefiting from the complete decomposition of CO(NH2)2·H2O2 and H2O2 into gaseous species under microwave (MW) irradiation, no water-washing and effluent-treatment are needed in this chemical exfoliation procedure, thus the preparation of graphene in an eco-friendly way is realized. The resultant graphene behaves a large-size, high-quality and few-layer feature with a yield of ~100%. Then 4 µm-thick ultrathin graphene paper fabricated from the as-exfoliated graphene is used as an electromagnetic interference (EMI) shielding material. And its absolute effectiveness of EMI shielding (SSE/t) is up to 34, 176.9 dB cm2/g, which is, to the best of our knowledge, among the highest values so far reported for typical EMI shielding materials. The EMI shielding performance demonstrates a great application potential of graphene paper in meeting the ever-increasingly EMI shielding demands in miniaturized electronic devices.
A hydrophobic carbon dots (Glc-OCDs) derived from octadecylamine and glucose were successfully synthesized for the first time and then grafted onto the porous silica surface by the "Nano-on-Micro" strategy, which was served as a new stationary phase (Sil-Glc-OCDs) for reversed-phase liquid chromatography. The structure of this stationary phase was carefully verified by laser scanning confocal microscope, Fourier transform infrared spectrometry, elemental analysis, contact angle measurement, etc. Several analytes including seven polycyclic aromatic hydrocarbons, eight alkylbenzenes, eight phenols and seven sulfonamides can be well separated on this stationary phase. Better separation performance for certain analytes over commercial C18 column was obtained. Interestingly, this stationary phase exhibited excellent chromatographic selectivity in the separation of the isomers of tert‑butylbenzene, sec‑butylbenzene, isobutylbenzene and n-butylbenzene. In addition, this new Sil-Glc-OCDs column was also applied for detection of calycosin-7-glucoside, ononin, calycosin, formononetin, genistein and isorhamnetin in the extract of Radix Astragali, which were found that the concentration was 0.15 g/L, 0.088 g/L, 0.14 g/L, 0.086 g/L, 0.18 g/L and 0.29 g/L, respectively. We believe that this CDs-grafted silica materials are promising for chromatographic separation.
This work presents a novel strategy for engineering a GC stationary phase with high selectivity, inertness and thermal stability by introducing the 3D π-rich TP moieties to the terminals of a polar chain polymer. Herein, we provide the first example, i.e., a new TP-terminated polycaprolactone polymer (TPP) as the stationary phase for GC analyses. As demonstrated, the TPP column achieved distinctly improved inertness to fatty acids and aldehydes, and dramatically enhanced thermal stability (about 100 ℃ higher) over the PCL column. Also, the TPP column exhibited high resolving capability towards the positional isomers of phenols, anilines and alkylated/halobenzenes and showed good potential in detecting minor impurities in chemical products. Importantly, the proposed strategy is facile, feasible and generally applicable to analogous polymers.
In this work, a very simple dual-readout lateral flow test strip (LFTS) platform was developed for sensitive detection of alkaline phosphatase (ALP) based on a portable device. In this assay, quantum dots (QDs) conjugated with bovine serum albumin (QDs-BSA) were chosen as fluorescence signal labels. In the absence of ALP, MnO2 nanosheets aggregate on the test line and exhibit an obvious brown color, which can be observed by naked eyes to realize semi-qualitative analysis. Meanwhile, fluorescence intensity of QDs-BSA can also be effectively quenched by MnO2 nanosheets due to inner-filter effect. Correspondingly, in the presence of ALP, ALP can catalyze the hydrolysis of ascorbic acid 2-phosphate (AAP) to generate L-ascorbic acid (AA), which can reduce MnO2 into Mn2+, accompanying with the obvious fluorescence recovery of the QDs. By simply monitoring the change of colorimetric and fluorescent signal on the test line, trace amount of ALP can be quantitatively detected. Under the optimal conditions, measurable evaluation of ALP was reached in a linear range from 1 U/L to 20 U/L with a detection limit of 0.7 U/L based on fluorescence signal. Furthermore, this colorimetric/fluorescent dual-readout assay was successfully applied to monitor ALP in human serum samples, showing its great potential as a point of care biosensor for clinical diagnosis.
The existence of many anions in wastewater reduces the removal efficiency of phosphate by adsorbents under realistic conditions. Facing this challenge, the study reports on an insistent and stable composite adsorbent of molybdate complexes Fe-(MoOx) embedded in a macroporous anion exchange resin (D-201). [Fe(MoOx)]-D-201 shows 93.7% adsorption capacity (28.3 mg/g) for phosphate even when the molar concentration of coexisting ions is 5 times higher than phosphate. The capacity of adsorbent is maintained more than 84.2% after five regeneration cycles to remove phosphate in the wastewater containing coexisting ions. The ability of highly selective removal of phosphate is maintained during the regeneration cycles explained by the change of the binding of molybdate clusters with phosphate, which is due to the different structures of molybdate clusters depending on various pH. In general, this work puts forward a new idea for the development of phosphorus removal adsorbents for the treatment of wastewater containing coexisting ions.