Latest ArticlesMetal–organic frameworks (MOFs) have a regular porous structure and high porosity, which make them ideal electrode materials for supercapacitors. However, their capacitance performance is greatly limited by their poor conductivity. In this study, a multi-component hierarchical structure was obtained by growing NiCoFeLDH on the surface of ZIF-67, which increased the electron transfer between the MOF particles and greatly improved the capacitance of ZIF-67. The formation mechanism of the multi-component layered hollow structure indicated that the hydrolysis acidity of metal ions and the coordination ability with ligands were the key factors for forming nanosheets and hollow structures. By controlling the type and valence state of the doped metals and the reaction time, the morphology transformation of MOF composites can be effectively controlled. Electrochemical studies showed that the specific capacitance of hollow NiCoFeLDH@ZIF-67 composite is 1202.08F/g (0.5 A/g). In addition, aqueous devices were assembled and carefully tested. This scheme is crucial for the design of MOF-based materials used in supercapacitor devices and serves as a guide for the design of MOF-based composites.
Low-efficiency charge transfer is a critical factor to limit the photocatalytic H2 evolution activity of semiconductor photocatalysts. The interface design is a promising approach to achieve high charge-transfer efficiency for photocatalysts. Herein, a new 2D/2D atomic double-layer WS2/Nb2O5 shell/core photocatalyst (DLWS/Nb2O5) is designed. The atom-resolved HAADF-STEM results unravel the presence of an unusual 2D/2D shell/core interface in DLWS/Nb2O5. Taking advantage of the advanced femtosecond-resolved ultrafast TAS spectra, the average lifetime of charge carriers for DLWS/Nb2O5 (180.97 ps) is considerably shortened as compared to that of Nb2O5 (230.50 ps), strongly indicating that the 2D/2D shell/core interface enables DLWS/Nb2O5 to achieve ultrafast charge transfer from Nb2O5 to atomic double-layer WS2, thus yielding a high photocatalytic H2 evolution rate of 237.6 μmol/h, up to 10.8 times higher than that of pure Nb2O5 nanosheet. This study will open a new window for the development of high-efficient photocatalytic systems through the interface design.
We have developed a facile strategy to fabricate model multicolor hydrogels via a straightforward mixing process of poly acrylonitrile-grafted methacrylamide (PANMAM), polymethacrylic acid (PMAA) and doped lanthanide (Eu/Tb) and zinc ions to form the interpenetrating dual-polymer gel networks. The hydrogels exhibit excellent tunability of multi-spectrum emission colors (including white light) by simply varying the stoichiometry of metal ions. Furthermore, taking the advantage of different metal ion response mechanisms, we have demonstrated the reversible acidity/alkalinity stimuli-responsive behaviors of white-light-emitting hydrogel (WLE gel). Meanwhile, the unique cross-linked network formed through hydrogen-bonding, metal-ligand coordination and ionic interaction is introduced to achieve favorable mechanical strength of hydrogels. These properties enable the possibility in obtaining fluorescent patterns on hydrogels, which are promising candidate for encrypted information with improved security.
Ammonia (NH3) is considered an attractive candidate as a clean, highly efficient energy carrier. The electrocatalytic nitrogen reduction reaction (NRR) can reduce energy input and carbon footprint; therefore, rational design of effective electrocatalysts is essential for achieving high-efficiency electrocatalytic NH3 synthesis. Herein, we report that the enzymatic mechanism is the more favourable pathway for NRR, due to lower limiting potential (−0.44 V), lower free energy (only 0.02 eV) of the first hydrogenation step (*N–N to *NH–N), and more electron transfer from Fe2B2 to the reaction species. In addition, both vacancies and dopants can be helpful in reducing the reaction energy barrier of the potential-determining step. Therefore, we have demonstrated that Fe2B2 is a potential new candidate for effective NRR and highlighted its potential for applications in electrocatalytic NH3 synthesis.
The disinfection of waterborne pathogens from drinking water is extremely important for human health. Although countless efforts have been devoted for drinking water inactivation, challenges still exist in terms of relative high energy consumption and complicated to implement and maintain. Here, silver nanoparticles anchoring wood carbon (Ag NPs/WC) membrane is developed as cost-effective, high flux, scalable filter for highly efficient electric field disinfection of water. Under electric field of 4 V voltage, the designed membrane achieved more than 5 log (99.999%) disinfection performance for different model bacteria, including Escherichia coli (E. coli), Enterococcus faecalis (E. faecalis), Salmonella enterica serovar Typhimirium (S. Typhimurium) and Bacillus subtilis (B. subtilis) with a high flux of 3.8 × 103 L m−2 h−1, extremely low energy consumption of 2 J L−1 m−2 and fantastic durability (7 days). The high disinfection performance of Ag NPs/WC membrane is attributed to the synergistic disinfection of carbon nanofibrils, Ag nanoparticles as well as the low tortuous structure of the channels in wood carbon. The Ag NPs/WC membrane presents a promising strategy for point-of-use drinking water electric field disinfection treatment.
In this paper, a novel BC3N2 monolayer has been found with a graphene-like structure using the developed particle swarm optimization algorithm in combination with ab initio calculations. The predicted structure meets the thermodynamical, dynamical, and mechanical stability requirements. Interestingly, the BC3N2 plane shows a metallic character. Importantly, BC3N2 has an in-plane stiffness comparable to that of graphene. We have also investigated the adsorption characteristics of CO2 on pristine monolayer and Mo functionalized monolayer using density functional theory. Subsequently, electronic structures of the interacting systems (CO2 molecule and substrates) have been preliminarily explored. The results show that Mo/BC3N2 has a stronger adsorption capacity towards CO2 comparing with the pristine one, which can provide a reference for the further study of the CO2 reduction mechanism on the transition metal-functionalized surface as well as the new catalyst's design.
Accurate detection of hydrogen sulfide (H2S) is of great significance for environmental monitoring and protection. We propose a colorimetric method for the detection of H2S by the use of mixed-node Cu-Fe metal organic frameworks (Cu-Fe MOFs) as highly efficient mimic enzymes for target-induced deactivation. The Cu-Fe MOFs were synthesized by a simple solvothermal method and could catalyze the H2O2 mediated oxidation of 3, 3′, 5, 5′-tetramethylbenzidine (TMB) to oxTMB with a blue color. The presence of dissolved H2S would deactivate the mimic enzymes, and then the blue color disappeared. The mechanism of the sensor was discussed by steady-state kinetic analysis. The designed assay was highly sensitive for H2S detection with a linear range of 0−80 μmol/L and a detection limit of 1.6 μmol/L. Moreover, some potential substances in the water samples had no interference. This method with the advantages of low cost, high sensitivity, selectivity, and visual readout with the naked eye was successfully applied to the determination of H2S in industrial wastewater samples.
Durability is one of the critical issues to restrict the commercialization of proton exchange membrane fuel cells (PEMFCs) for the vehicle application. The practical dynamic operation significantly affects the PEMFCs durability by corroding its key components. In this work, the degradation behavior of a single PEMFC has been investigated under a simulated automotive load-cycling operation, with the aim of revealing the effect of load amplitude (0.8 and 0.2 A/cm2 amplitude for the current density range of 0.1−0.9 and 0.1−0.3 A/cm2, respectively) on its performance degradation. A more severe degradation on the fuel cell performance is observed under a higher load amplitude of 0.8 A/cm2 cycling operation, with ~10.5% decrease of cell voltage at a current density of 1.0 A/cm2. The larger loss of fuel cell performance under the higher load amplitude test is mainly due to the frequent fluctuation of a wider potential cycling. Physicochemical characterizations analyses indicate that the Pt nanoparticles in cathodic catalyst layer grow faster with a higher increase extent of particle size under this circumstance because of their repeated oxidation/reduction and subsequent dissolution/agglomeration process, resulting in the degradation of platinum catalyst and thus the cell performance. Additionally, the detected microstructure change of the cathodic catalyst layer also contributes to the performance failure that causes a distinct increase in mass transfer resistance.
Trimethoprim (TMP) is a typical antibiotic to treat infectious disease, which is among the most commonly detected antibacterial agents in natural waters and municipal wastewaters. In the present study, the impacts of dissolved oxygen (DO) on the oxidation efficiency and pathways of TMP by reaction with sulfate radicals (SO4·−) were investigated. Our results revealed that the presence of DO was favourable for TMP degradation. Specifically, TMP would react initially with SO4·− via electron-transfer process to form a carbon-centered radical. In the absence of oxygen, the carbon-centered radical could undergo hydrolysis to produce α-hydroxytrimethoprim (TMP−OH), followed by the further oxidation which generated α-ketotrimethoprim (TMP = O). However, in the presence of oxygen, the carbon-centered radical would alternatively combine with oxygen, leading to a sequential reaction in which peroxyl radical and a tetroxide were formed, and finally generated TMP−OH and TMP=O simultaneously. The proposed pathways were further confirmed by density functional theory (DFT) calculations. The results obtained in this study would emphasize the significance of DO on the oxidation of organic micro-pollutants by SO4·−.
In this study, Si-doped ferrihydrite (Si-Fh) was successfully synthesized by a simple coprecipitation method for removal of heavy metals in water. Subsequently, the physicochemical properties of Si-Fh before and after adsorption were further studied using several techniques. The Si-Fh exhibited good adsorption capacity for heavy metal ions such as Pb(Ⅱ) and Cd(Ⅱ). The maximum adsorption capacities of lead and cadmium are respectively 105.807, 37.986mg/g. The distribution coefficients of the materials for Pb(Ⅱ) and Cd(Ⅱ) also showed a great affinity (under optimal conditions). Moreover, it was found that the adsorption fit well with the Freundlich isotherm and pseudo-second-order kinetic model which means this was a chemical adsorption process. It can be conducted from both characterization and model results that adsorption of Pb(Ⅱ) and Cd(Ⅱ) was mainly through the complexation interaction of abundance oxygen functional groups on the surface of Si-Fh. Overall, the Si-Fh adsorbents with many superiorities have potential for future applications in the removal of Pb(Ⅱ) and Cd(Ⅱ) from wastewater.
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