Latest ArticlesThe oxygen reduction reaction (ORR), an important process in Zn-air batteries (ZABs), shows sluggish reaction kinetics, which significantly impairs the further improvement of battery performance. Thus, rationally designing cathodic catalysts for ZABs has drawn sufficient attention. We herein synthesize and characterize Fe/N/F-tridoped CNTs (FeNFCs) by annealing the postsynthesized trifluoroacetic anhydride-modified Fe-MIL-88B-NH2 nanocrystals with melamine at high temperature in a N2 atmosphere. Benefiting from the Fe/N/F element doping, high specific surface area, and CNT structure, the FeNFC800 catalyst prepared at 800 ℃ exhibits a preferable half-wave potential of 0.829 V vs. RHE. The Zn-air battery equipped with FeNFC800 shows a high open-circuit voltage of 1.47 V, a gratifying peak power density of 196 mW/cm2, and extraordinary long-term stability, outperforming the benchmark 20% Pt/C.
Wastewater management and energy/resource recycling have been extensively investigated via photo(electro)catalysis. Although both operation processes are driven effectively by the same interfacial charge, each system is practiced separately since they require very different reaction conditions. In this review, we showcase the recent advancements in photo(electro)catalytic process that enables the wastewater treatment and simultaneous energy/resource recovery (WT-ERR). Various literatures based on photo(electro)catalysis for wastewater treatment coupled with CO2 conversion, H2 production and heavy metal recovery are summarized. Besides, the fundamentals of photo(electro)catalysis and the influencing factors in such synergistic process are also presented. The essential feature of the catalysis lies in effectively utilizing hole oxidation for pollutant degradation and electron reduction for energy/resource recovery. Although in its infancy, the reviewed technology provides new avenue for developing next-generation wastewater treatment process. Moreover, we expect that this review can stimulate intensive researches to rationally design photo(electro)catalytic systems for environmental remediation accompanied with energy and resource recovery.
Electrocatalytic nitrate reduction to ammonia (NRA) under ambient conditions is significant for carbon-neutral synthetic fuels. Nevertheless, the lack of efficient electrocatalysts with tunable nanostructure for NRA remains a grand challenge. Herein, NbWO6 nanosheets with oxygen vacancy (NbWO6-x) was demonstrated via thermal treatment and exfoliation with NH3 selectivity of 86.8% and Faradaic efficiency of 85.7% toward NRA. 1H nuclear magnetic resonance spectra coupled with 15N isotope labeling experiments proved that NH3 originated from NO3−. The function of oxygen vacancy was revealed by computational studies in NRA. Moreover, the reaction mechanism and pathway of NRA could be deduced based on the results of online differential electrochemical mass spectrometry (DEMS). This work provides a selective NH3 generation strategy to decarbonize the energy-chemical sector, bridging the gap between batteries and biofuels.
With increasing attention to personalized healthcare, miniaturized and easily implementable devices are desired for point-of-care testing (POCT). Herein, hydrophilic patterns were designed on freestanding TiO2 nanotube arrays (TiNTs) as nanoreactors for a naked-eye colorimetric assay. With a high aspect ratio, TiNTs can provide a long observation length combined with a limited volume. Moreover, by combining the photocatalytic property of TiO2 and spatiotemporal controllability of light, hydrophilic nanoreactors were fabricated with minimal volume, and thus the indicator and analyte are limited in a confined void by the hydrophobic surroundings, thus allowing a higher sensitivity for sensing. We believe the proposed sensing platform could provide a promising strategy in developing POCT devices for routine health monitoring.
Information-carrying capacity has become an important factor in the development of encryption and anti-counterfeiting. Herein, a hydrogen-bonded organic framework (HOF-PyTTA) was developed as novel anti-counterfeiting ink without rare metals and a smartphone-based APP was written for encryption and anti-counterfeiting. We found that the fluorescence of HOF-PyTTA can be quenched by Fe3+ ions and recovered by the addition of ascorbic acid. And the fluorescence of HOF-PyTTA can be enhanced by the increasing concentrations of ethanol. Based on these stimulus-response properties, four anti-counterfeiting models with gradually increased security were studied. Mode one was printed by HOFs ink and decrypted by UV light. Mode two was based on HOF-PyTTA and CsPbBr3 inks (or HOF-PyTTA-Fe3+) which are used to separately print the genuine and pirated information. A decryption reagent was applied to get the genuine information. Furthermore, we successfully construct a dynamic information encryption anti-counterfeiting model using a fluorescence array in combination with an information encryption anti-counterfeiting APP. The circular array is printed by several concentrations of HOF-PyTTA ink and different RGB thresholds are set with the help of the information encryption anti-counterfeiting APP, to obtain distinct encrypted anti-counterfeiting information, thus accomplishing a high information-carrying capacity.
As for the emerging and cut edge spatially resolved metabolomics, mass spectrometry imaging (MSI) is a powerful tool that can map thousands of metabolites from bio-tissue sections without chemical labels. However, the stability, sensitivity and spatial resolution of MSI are always limited by the performance of its ionization probe. Herein, two types of probes (fine probe (P-100) and large probe (P-200)) were designed and characterized to perform air-flow assisted desorption electrospray ionization (AFA-DESI) MSI analysis for spatially resolved metabolomics. It was determined that the spray introduced by P-100 was homogenous and stable under the spray solvent at a flow rate of 5-10µL/min, while P-200 can endure a high flow rate of up to 10-30µL/min. Moreover, the MSI images were acquired by AFA-DESI-MSI with P-100 from rat brain tissue section and with P-200 from whole-body tissue section of mouse, and these results presented unambiguous tissue structure with the distribution information of numerous metabolites. Furthermore, the spatially resolved metabolomic analysis of tumor tissue was successfully realized to discover the tumor associated biomarkers. As the key parts of AFA-DESI-MSI system, it has been demonstrated that the designed probs have excellent performance for spatially resolved metabolomics, and it will further promote its application in life science, and drug research and development.
We designed a disulfide-crosslinked mini-protein with a two-helical topology consisting of L- and D-amino acids, which was exceptionally stable in serum. Therefore, we further used it as a scaffold to design mini-proteins targeting p53 positive tumor cells. Based on bifunctional grafting, key residues from the transactivation domain of p53 and a designed unnatural amino acid were grafted into the helix constituted by L-amino acids to confer the mini-protein with MDM2 inhibitory activity. Meanwhile, ten Arg residues were introduced to improve its membrane penetrating capacity. Among the mini-proteins, UPROL-10e showed nano-molar binding affinity on MDM2 and cellular toxicity on p53 expressing HCT116 cells.
A novel palladium-catalyzed carbonylative cyclization of alkene-tethered indoles with phenols or arylboronic acids is described, which provides a facile approach to access indolo[2,1-a]isoquinoline scaffolds. This method employs benzene-1,3,5-triyl triformate (TFBen) as the CO surrogate for the incorporation of a carbonyl group into indolo[2,1-a]isoquinoline scaffolds, and a variety of carbonyl-containing indolo[2,1-a]isoquinoline derivatives are prepared in good yields.
Molybdenum disulfide (MoS2) has attracted great attention in hydrogen peroxide (H2O2) activation as a Fenton-like catalyst and cocatalyst, but the distinct mechanism of generating •OH remains unclear. In this paper, the metallic 1T phase and semiconducting 2H phase of MoS2 nanosheets were prepared and applied in MoS2/H2O2 and MoS2/Fe2+/H2O2 systems with and without light irradiation. Compared with 2H-MoS2, 1T-MoS2 exhibited superior removal rates in degrading organic pollutants in the two systems under light irradiation. However, the phase had little effect on activating H2O2 in the MoS2/H2O2 system under dark conditions. This is because it was difficult for the surface •OHads generated in the MoS2/H2O2 system to diffuse into solution, while the •OHfree radicals were mainly responsible for degrading organic pollutants. When introducing light irradiation, external energy may accelerate the desorption of •OHads into •OHfree. Interestingly, the conversion between Mo4+ and Mo5+ triggered the decomposition of H2O2 in the Fenton-like reaction, while the cycle of Mo4+/Mo6+ promoted the regeneration of Fe3+ when employing 1T-MoS2 as a cocatalyst. Meanwhile, the 1T-MoS2 catalysts exhibited excellent stability and ability to degrade various organics in the two systems. This work offers deeper insight into the MoS2-based Fenton-like and cocatalytic mechanisms.
As one of the most promising and practical advanced oxidation processes (AOPs), the catalytic ozonation is triggered by the active components of catalyst, which are usually derived from metals or metal oxides. To avoid the metal pollution from catalyst, here the amorphous boron (A-boron) is used as a metal-free catalyst for catalytic ozonation to produce free radicals for effective degradation of atrazine (ATZ), the world-widely used herbicide and also a widespread pollutant in environment. A-boron exhibits an outstanding performance for catalytic ozonation to remove ATZ from water. As A-boron is introduced into ozonation, the degradation efficiency in 10 min is promoted to 97.1%, much higher than that of 15.1% under ozonation. The mechanism is that the B–B bonds and internal suboxide B in A-boron serve as the main active sites to donate electrons to accelerate ozone decomposition to produce reactive oxygen species (ROS), including •O2− and 1O2, and further enhance ATZ degradation via ROS reactions. Moreover, the A-boron is still highly active with a degradation efficiency of ATZ over 95% in 10 min even after four successive cycles. This work shows A-boron could be an alternative for the active components of metal or metal oxide in catalytic ozonation.
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