Latest ArticlesFe-Nx sites have been identified as core descriptors for Fe-N/C based oxygen reduction reaction catalysts. However, the low density and less utilization of Fe-Nx sites render these catalysts with inefficient catalytic performance. Herein, we develop an organic carboxylate-assisted engineering to construct Fe, N co-doped porous carbon interlinked carbon nanotubes (Fe/N-CCNTs) with high-density and sufficiently exposed Fe-Nx sites based on self-catalyzed effect. The existing forms of Fe include Fe-imidazole configuration and coordination with unsaturated Zn sites via organic carboxylate as linkers, leading to high-density Fe-Nx sites after pyrolysis. Besides, hexatomic carbon rings of organic carboxylate lower cyclization energy barrier for CNT formation, resulting in CNTs interlinked with separated active sites through "active point-conductive line-active point" connections. The optimal sample (Fe-BOAc-PNC) exhibits the onset potential of 0.93 V (vs. RHE) and half-wave potential of 0.84 V in alkaline solution. The liquid-state Zn-air battery (ZAB) employing Fe-BOAc-PNC generates large power density (160 mW/cm2) and stability over 160 h. Moreover, the assembled flexible ZAB displays superb power density of 93 mW/cm2 with robust flexibility. This work provides an insightful perspective for designing Fe-N/C catalysts with high-density and sufficiently exposed active sites for energy storage application.
A huge amount of waste printed circuit boards (WPCBs) was produced while the electronic manufacturing industry developed rapidly. WPCBs mainly consist of organic compounds, which makes it possible to prepare them into porous carbon as valuable adsorbent. However, WPCBs are also rich in valuable metals. Cu makes up the most of these metals. It is worth studying whether the residual metal will affect the application of carbon materials. In this study, the porous active carbon (AC) was prepared from WPCBs as an adsorbent. Sulfadiazine (SD), a widely detected antibiotic contaminant, was used as a target pollutant. Nitric acid (HNO3) was used to modify AC (AC-HNO3) to remove the residual Cu. The experiment results showed that the adsorption kinetics of SD by AC (k = 0.0025) and AC-HNO3 (k = 0.0029) can be described better using a pseudo-second-order kinetic equation. The adsorption isotherms of AC and AC-HNO3 on SD could be fitted by the Langmuir model. AC had a larger adsorption capacity than AC-HNO3. Density functional theory (DFT) calculation results suggested that the −OH group and Cu on the surface of AC could be the adsorption sites and promote the SD adsorption. This work provides practical methods to recycle WPCBs into wealth and realized waste control by waste.
The rational construction of electrocatalysts with desired features is significant but challenging for superior water splitting at high current density. Herein, amorphous CoNiS nanosheets are synthesized on nickel foam (NF) through a facile structure evolution strategy and present advanced performance at high current densities in water splitting. The high catalytic activity can be attributed to the sufficient active sites exposed by the flexible amorphous configuration. Moreover, the hydrophilicity and aerophobicity of a-CoNiS/NF promote surface wettability of the self-supporting electrode and avoid the aggregation of bubbles, which expedites the diffusion of electrolyte and facilitates the mass transfer. As a result, the optimized electrode demonstrates low overpotentials of 289 and 434 mV at 500 mA/cm2 under alkaline conditions for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), respectively. Impressively, an electrolytic water splitting cell assembled by bifunctional a-CoNiS/NF operates with a low cell voltage of 1.46 V@10 mA/cm2 and reaches 1.79 V at 500 mA/cm2. The strategy sheds light on a competitive platform for the reasonable design of non-precious-metal electrocatalysts under high current density.
Organic radical as a powerful tool has been extensively applied in synthetic chemistry. However, harnessing radical-mediated noncovalent interactions to fabricate soft materials remains elusive. Here we report a new category of supramolecular hydrogel system held by multiple radical-radical (polyradical) interactions, and its photosensitive cross-linking structure. A simple polyacrylamide with triarylamine (TAA) pendants is designed as the precursor. The TAA units in polymer can be converted into active TAA•+ radical cations with light and further associate each other via TAA•+‒TAA•+ stacking interactions to form stable supramolecular network. Temporal control of the light irradiation dictates the degree of radical stacks, thus regulating the mechanical performance of the resulting hydrogel materials on-demand. Moreover, the reversible collapse of this hydrogels can be promoted by adding radical scavenger or exerting reduction voltage.
Metal-organic frameworks (MOFs), a class of hybrid materials, consist of organic linkers and bridging metal ions or clusters. Their tunable pore sizes, large surface area, good biocompatibility, structural variability in combination with materials and chemicals, and osteogenic effects provide potential approaches for bone tissue engineering and bone diseases. And there are more and more research on MOFs in the field of osteogenesis in recent years. This review presents an overall summary of the application in the bone tissue engineering and bone diseases of MOFs and their composites, starting with the synthesis of MOFs, which discusses the advantages and disadvantages of different syntheses. Then, the biological functions of MOFs are discussed, which are the basics of MOFs applied in the organism. Importantly, mechanisms and abundant applications of MOFs are detailed in the bone tissue engineering and bone diseases. Finally, some prospects of MOFs are discussed, for instance, exploring whether MOFs can be used to treat other bone diseases.
Diabetic patients often have problems such as residual tumor and wound infection after tumor resection, causing severe clinical problems. It is urgent to develop effective therapies to reach oncotherapy/anti-infection/promotion of wound healing combined treatment. Herein, we propose CS/MnO2-GOx (CMGOx) nanocatalysts for the specific catalytic generation of •OH to inhibit tumors and bacteria in a hyperglycemic environment. The good biocompatible chitosan (CS), as a carrier for the catalyst, exhibits excellent antibacterial effect as well as promotes wound healing. Glucose oxidase (GOx) is loaded on the surface of CS nanoparticles to generate H2O2 and gluconic acid by consuming glucose (starvation therapy, ST) and O2. The MnO2 depletes glutathione (GSH) to produce Mn2+, amplifying oxidative stress and further promoting the activity of Mn2+-mediated Fenton-like reaction to produce •OH (chemodynamic therapy, CDT) in weak acidic environment. Moreover, the produced gluconic acid lowers the pH of the environment, enhancing chemodynamic therapy (ECDT). The tumor cells and bacteria are efficiently eliminated by the synergistic effect of ST and ECDT. The MnO2 nanoparticles at neutral environment decomposes H2O2 into O2, which cooperate with CS to promote healing. The self-enhanced cascade reaction of CMGOx in situ exhibits excellent effects of antitumor/antibacterial therapy and promotion of wound healing, offering a promising integrated treatment for diabetic patients after tumor surgical resection.
Ammonia (NH3), as an important chemical substance and clean energy carrier, plays an indispensable role in industrial and agricultural production. The electrocatalytic synthesis of NH3 under mild conditions has attracted worldwide attention in the energy field due to its environmental friendliness and cost efficiency, but unsatisfactory NH3 yields and Faradaic efficiencies are restricting its development. The introduction of defect has been demonstrated as a feasible way to overcome the disadvantages of electrochemistry, as it can regulate the electronic structure and modulate coordination environment of electrocatalysts, which further create active sites and enhance nitrogen adsorption. In this regard, it is necessary to understand the effects of various types of defects on electrocatalysts based on the latest progress in the defect engineering for nitrogen reduction reaction (NRR). In this review, the concept, classifications, and characterization of defects as well as the approaches to create them in electrocatalysts are firstly discussed. Then, certain types of defects (vacancy, dopant, amorphism, edge/corner, and porousness) affecting the performances of various electrocatalysts are further described. Finally, the summary and challenges of electrocatalytic ammonia synthesis are proposed to design advanced electrocatalysts with high efficiency.
Ultra-long room temperature phosphorescence (URTP) has been increasingly recognized in pure organic luminophor in recent years. Through a simpler molecular design and charge separation-recombination pathway, organic luminophor can achieve even better URTP properties. In this work, we achieved URTP in a system of host-guest doped benzophenone derivatives whose phosphorescence is visible to the naked eye. The differences in the wavelength lifetimes of luminescent emission correspond to different photophysical mechanisms. Through a combination of theoretical calculations and experiments, the host acts as a powerful substrate that restricts the motion of the guest and inhibits the non-radiative transitions of the guest, accompanied by a charge transfer separation-recombination process between the host and the guest, resulting in an URTP phenomenon. Transient absorption results demonstrate the existence of a charge-separated state. The design strategy via charge separation is generic and easy to implement, providing a direction for the future design of doped URTP.
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