Latest ArticlesElectrocatalytic nitrate reduction reaction (NO3−RR) is a green and competitive method for removing nitrate from water, requiring highly active and long-term stable electrocatalysts. In this work, we report a Cu0 nanorod catalyst with disordered structure (re-Cu NRs), prepared by electrochemical in situ reconfiguration of copper-based nitrides (Cu3N NRs). The amorphous structure allows the exposure of abundant active sites to enhance the electrocatalytic activity because of the disordered atomic arrangement. At a potential of −1.2 V vs. Ag/AgCl, the re-Cu NRs catalyst achieved nearly 100% nitrate conversion within 120 min at a low nitrate concentration (50 mg/L), without the accumulation of nitrite. In-situ DEMS detection reveals that the NO3−RR on re-Cu NRs followed the pathway of *NO3−→ *NO2−→ *NO → *N → *NH → *NH2 → *NH3. Furthermore, combining this proposed pathway with electrochlorination could efficiently transform ammonia into harmless N2 (~99.41%). Theoretical calculations confirm that the amorphous structure on the surface of re-Cu NRs catalysts can facilitate strongly adsorbed nitrate, weaken the rate-determining step of *NH3 → NH3, and suppress hydrogen evolution reaction (HER). This study provides a new approach for designing efficient and stable amorphous catalysts for electrocatalytic nitrate reduction.
A porous lanthanum (La) carbonate-carbon composite (LaCC) was prepared by vacuum-freeze-drying and pyrolysis techniques to remove phosphorus (P) from wastewater. Using polyethylene glycol as a carbon skeleton template, and the organic ligands are removed during pyrolysis, resulting in the creation of many pore structures. The LaCC showed excellent P removal performance and selectivity over a wide pH range (3–10). It exhibited a rapid adsorption rate and could hold up to 119.5 mg P/g. Fixed-bed column experiments showed that under dynamic conditions, just 1 g of LaCC effectively treated 60 L of P-contaminated wastewater with an initial concentration of 2 mg/L, meeting the primary discharge standard of <0.5 mg/L according to the comprehensive sewage guidelines of China. Bacterial experiments showed that the LaCC could inhibit the growth of Escherichia coli, indicating that it has both P removal and bacterial inhibition effects, which can greatly improve the application range of adsorbents.
A convenient photocatalytic multi-component reaction of alkenes, quinoxalin-2(1H)-ones, and diazo compounds has been developed in the presence of water. A number of ester-containing quinoxalin-2(1H)-ones could be efficiently obtained in moderate to good yields at room temperature. This metal-free visible-light-driven tandem reaction was conducted through proton-coupled electron transfer (PCET) process using water as the hydrogen donor and 1,2,3,5-tetrakis(carbazol-9-yl)-4,6-dicyanobenzene (4CzIPN) as the photocatalyst.
Programmed cell death protein 1/programmed cell death 1 ligand 1(PD-1/PD-L1) protein-protein interaction represents an appealing target for cancer therapy. Several antibody drugs have been developed to target this interaction, but they are less effective in the treatment of melanoma. To overcome the limitations, the first proteolysis-targeting chimeric (PROTAC) small molecules simultaneously targeting PD-L1 and Src homology phosphotyrosyl phosphatase 2 (SHP2) were designed. By employment of PD-1/PD-L1 inhibitors BMS01 or BMS-37, SHP2 inhibitor SHP099 and E3 ligase ligands, a series of potent PD-L1 and SHP2 dual PROTACs were synthesized. The most promising compounds BS-7C-V2 and BS327V2 efficiently induced PD-L1 and SHP2 degradation and demonstrated significantly improved immune potency in B16-F10 and A375 cell lines. More importantly, the efficacy of BS-7C-V2 and BS327V2 in a B16-F10 transplanted mouse model was further evaluated based on their degradation ability in vivo. Taken together, our work qualifies the new dual PROTACs as a potent degrader of PD-L1 and SHP2. The biological and mechanism investigations with BS-7C-V2 and BS327V2 prove that dual PROTACs can play an anti-tumor role in vivo and in vitro, and can provide a new therapeutic strategy for melanoma.
Breath analysis can be used to diagnose diseases non-invasively. Accurate measurement of volatolomics is critical for breath analysis to be a gold standard. Tedlar bags (TB) are often used to collect breath samples, but they emit contaminants that affect accuracy. This issue was overlooked in previous studies. We found contamination issues with TB (e.g., siloxanes and aromatic impurities) that affect the identification of volatile organic compounds (VOCs) due to impurities. Then, home-designed equipment (HD) made with poly-tetrafluoride (PTFE) and quartz glass for breath collection was developed and employed in clinical trials. 15 healthy individuals and 32 non-small cell lung cancer (NSCLC) patients at IA stage participated in this study. 610 VOCs can be collected through TB, which is less than HD (1109 VOCs), demonstrating that the inner wall of the TB easily adsorbs VOCs, leading to decreased detection concentrations. Otherwise, utilizing orthogonal partial least squares discriminant analysis (OPLS-DA), we identified chemical markers with significant discriminatory power (VIP > 1.5, P < 0.05). The HD method identified 12 target VOCs, surpassing the 3 target VOCs discerned by the TB method. A model combined with a machine learning algorithm for distinguishing early-stage lung cancer patients was established based on biomarkers, which were selected based on OPLS-DA. The results showed strong predictive capabilities for the HD-based model. It indicated that 12 biomarkers derived from the HD model were more effective in distinguishing NSCLC patients, with an AUC value of 0.92, compared to the AUC value of 0.5 from 3 markers obtained from the TB model. The sensitivity and specificity in the confusion matrix reached 100% and 80% for the HD test, but TB test reached only 40% and 60%. This work demonstrated that optimizing and standardizing VOCs collection methodology from breath of lung cancer patients is essential to identify actual volatiles, which could promote disease volatolomics worldwide.
Pollutants contained in wastewater pose serious harm to the environment. Graphene-based water treatment materials show significant advantages in wastewater treatment. However, with the development of graphene-based materials, its progress in water treatment has reached a bottleneck. The challenge lies in effectively enhancing its performance in water treatment and ensuring its practicality. By employing biomimetic approaches, some exceptional properties and structures found in nature can be mimicked in graphene materials, effectively enhancing graphene’s adsorption and mechanical properties. Current biomimetic methods include biomimetic mineralization, self-assembly, and templating. unfortunately, all of the above methods suffer from the disadvantages of complexity and poor bionic effect. Nevertheless, 3D printing, a form of additive manufacturing (AM) technology, offers integrated molding and excellent biomimetic performance in creating biomimetic materials. This paper will cover the following aspects: (1) An overview of objects suitable for bionics in terms of functional and structural aspects, along with their properties, and a discussion of various bionic objects combined with graphene materials in water treatment and related research; (2) a comparison of different methods for preparing graphene-based bionic materials; (3) an examination of the current drawbacks and limitations of graphene-based biomimetic materials; and (4) a conclusion and future prospects, exploring the potential of using 3D printing technology to produce graphene biomimetic materials. This review aims to serve as a guide for effectively leveraging natural inspirations to create graphene-based biomimetic materials and enhance graphene properties.
Although the powder Fenton-like catalysts have exhibited high catalytic performances towards pollutant degradation, they cannot be directly used for Fenton-like industrialization considering the problems of loss and recovery. Therefore, the membrane fixation of catalyst is an important step to realize the actual application of Fenton-like catalysts. In this work, an efficient catalyst was developed with Co-Nx configuration facilely reconstructed on the surface of Co3O4 (Co-Nx/Co3O4), which exhibited superior catalytic activity. We further fixed the highly efficient Co-Nx/Co3O4 onto three kinds of organic membranes and one kind of inorganic ceramic membrane installing with the residual PMS treatment device to investigate its catalytic stability and sustainability. Results indicated that the inorganic ceramic membrane (CM) can achieve high water flux of 710 L m-2 h-1, and the similar water flux can be achieved by Co-Nx/Co3O4/CM even without the pressure extraction. We also employed the Co-Nx/Co3O4/CM system to the wastewater secondary effluent, and the pollutant in complicated secondary effluent could be highly removed by the Co-Nx/Co3O4/CM system. This paper provides a new point of view for the application of metal-based catalysts with M-Nx coordination in catalytic reaction device.
Electrochemical nitrate reduction (NO3RR) offers a promising avenue for treating nitrate-contaminated water and recovering ammonia (NH3), yet the complexities of direct electron transfer (DET) and hydrogen atom transfer (HAT) mechanisms crucial for efficiency remain elusive. This study bridges the gap with a combined experimental and theoretical approach, elucidating the impact of catalyst structure on NO3RR pathways. We discover that catalysts favoring strong NO3− adsorption and efficient water dissociation were more inclined towards DET, enhancing denitrification. The Fe@Fe3O4/FF cathode, leveraging the synergistic interplay between metallic Fe and Fe3O4, excelled in NO3RR via DET, achieving an NH3 yield of 0.28 mmol h−1 cm−2 and a Faradaic efficiency of 95.7% for NH3 at -1.6 V (vs. SCE), with minimal nitrite accumulation at 100 mmol/L nitrate. Conversely, the Fe/FF and Fe3O4/CC cathodes showed reduced NH3 production and increased nitrite levels, attributed to the lack of Fe3O4 and metallic Fe, respectively, resulting in a dominant HAT mechanism. Moreover, Fe@Fe3O4/FF facilitated complete denitrification in real wastewater treatment by harnessing Cl− for electrochemically mediated breakpoint chlorination. This research not only deepens our understanding of NO3RR mechanisms but also paves the way for designing superior nitrate reduction catalysts.
Photoredox-mediated reversible-deactivation radical polymerization (RDRP) is an effective approach to synthesize polymers with defined composition and architecture. Current photoinduced RDRP primarily depends on outer-sphere electron transfer or homolysis mechanisms. Herein, we describe an example of iodine-mediated RDRP facilitated by photoinduced charge transfer complex (CTC) catalysis. The approach uses cheap and easily accessible N-heterocyclic nitrenium salt (NHN+···I-) as the photoactive CTC. Upon the irradiation of visible light, NHN+···I- undergoes single electron transfer to generate NHN• and I• radicals. The NHN• radical activates dormant Pn-I polymers via inner-sphere single electron transfer, leading to the propagating Pn• radical for chain growth and the I- anion for recovering the CTC, and the I• radical deactivates the polymerization via coupling with Pn•.
Metal halide perovskite nanocrystals (MHP NCs) are of great candidates in photocatalytic applications due to their extreme light utilization efficiency. However, the instability towards humid environment severely restrict their practical application. Herein, the CsPbBr3/CsPb2Br5 heteronanocrystals (HNCs) were successfully encapsulated into ZIF-8 through a thermal injection method via controlling the molar ratio of Cs+/Pb2+. The surface of ZIF-8 was then modified with hydrophobic copolymer of poly(methyl methacrylate) (PMMA) to improve the water stability. Benefiting from the intimate interfacial interaction and staggered energy band structure, the type-Ⅱ heterojunction of CsPbBr3/CsPb2Br5 guarantees efficient separation and migration of photogenerated electron/hole pairs. Meanwhile, the formation of Z-scheme heterojunction between ZIF-8 and CsPbBr3/CsPb2Br5 HNCs contributes to the adsorption and enrichment of pollutants, further accelerates the photocatalytic antibiotic degradation efficiency towards tetracycline hydrochloride (TCH) in aqueous solution. Nearly 87% of TCH (40 mg/L, 50 mL) was degraded by 40 mg catalyst within 100 min. This work offers a feasible approach in assembling high-performance MHP NCs-based efficient photocatalyst with expanding application in aqueous solution.
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