Latest ArticlesThe efficient removal and conversion of nitrate (NO3-) from wastewater is an urgent environmental issue. The catalytic nitrate reduction reaction (NO3RR) process, which involves transferring eight electrons and nine protons, poses significant challenges in improving hydrogen atom transfer (HAT). In this study, we synthesized Bi4O5X2 (BOX, X = Cl, Br, I) nanosheets to enhance HAT efficiency by managing halogen vacancies and optimizing oxidation half-reactions. This approach significantly increased ammonia selectivity. We found that larger halogen radii and higher vacancy concentrations improve water dissociation, boosting HAT efficiency. Additionally, replacing the challenging water oxidation half-reaction with ethylene glycol (EG) oxidation aligned with NO3- reduction further improved HAT efficiency, achieving an NH4+ selectivity of 97.2%. Rapid-scan in situ Fourier transform infrared (FT-IR) spectroscopy showed that iodine-rich vacancy surfaces accelerated the conversion of EG hydroxyl groups into carbonyls, releasing active hydrogen atoms and suppressing NO2- formation. This process efficiently converted nitrate to ammonia, presenting a promising method for photocatalytic NO3RR pollutant resourcing. These findings offer valuable strategies for enhancing the production of reactive hydrogen atoms and effectively managing nitrate-nitrogen pollution.
Despite the compelling potential of metal-organic framework (MOF) membranes for water remediation, their poor membrane-forming crystallinity, limited solution-processability, and propensity to aggregate have impeded industrial deployment. Through interfacial cooperative assembly, we construct a well-dispersed 2D/3D nanofluidic composite membrane by coupling novel three-dimensional CoBDC-NH2 nanocrystals (one-dimensional channels, 7 Å × 8.6 Å) with two-dimensional graphene oxide (GO). The synergistic interfacial interactions between flexible GO and rigid MOF components create a highly uniform architecture while furnishing rapid electron-transfer pathways and strong electrostatic repulsion; the rigid CoBD-CNH2 imparts angstrom-scale molecular sieving, ultrafast water-transport channels, and catalytically active Co sites. This interfacial synergy delivers an exceptional pure-water flux of 737.5 L m−2 h−1 bar−1 together with 99.8% rejection of bulky anionic dyes, decisively breaking the canonical flux-selectivity trade-off. XDLVO theory analysis confirms pronounced antifouling propensity, and density-functional-theory (DFT) calculations show that interfacial cooperative effects between GO and MOF lower the activation barrier for peroxymonosulfate (PMS) activation, enabling a self-cleaning cycle that restores 90.3% of the initial flux after fouling. By integrating molecular-precision sieving, charge-regulated transport, and in-situ catalytic regeneration within a scalable platform via interfacial cooperative assembly, this work offers a versatile blueprint for next-generation high-performance MOF membranes and signals broad opportunities in sustainable wastewater treatment and beyond.
Ultraviolet (UV) disinfection has some disadvantages such as unstable disinfection effect and bacterial revival. The UV/ozone (O3) co-disinfection process can be capable of solving the above-mentioned problems, but the current technology has the disadvantages of high costs and high operational risk. In this study, a new type of simultaneous O3-producing microwave electrodeless UV lamp (O3−MWUVL) was developed. The device can emit 254 nm and 185 nm UV, which can produce O3 while disinfecting. The O3−MWUVL exhibited significant disinfecting effects against Escherichia coli (E. coli) and Bacillus subtilis (B. subtilis). The disinfection effect of MWUV/O3 was better than that of MWUV or O3. The inactivation rate of E. coli disinfected by MWUV/O3 can reach 3.44 log when the UV dose was 16 mJ/cm2, and the inactivation rate of B. subtilis disinfected by MWUV/O3 can reach 4.64 log when the UV dose was 30 mJ/cm2. At the same time, the MWUV/O3 treatment can effectively inhibit the photoreactivation of E. coli. The maximum photoreactivation rate of E. coli treated by MWUV/O3 was only 0.11%. Additionally, the disinfection efficacy of the O3−MWUVL on actual wastewater was investigated, revealing that O3 pretreatment enhanced the UV inactivation capacity significantly. Furthermore, it was found that sequential disinfection using O3−MWUV or MWUV/O3 synergistic approach yielded superior results compared to MWUV-O3 sequential disinfection. Finally, investigation into the disinfection mechanism in the MWUV/O3 disinfection process substantiated the generation of hydroxyl radicals (•OH) within the system, while observations from scanning electron microscopy and laser confocal scanning microscopy also demonstrated that O3 plays an important role in dismantling cellular structures.
Herein, we propose a synergistic regulation strategy that combines steric hindrance with the multiple resonance (MR) effect to design and synthesize a thermally activated delayed fluorescent (TADF) emitter, SF-PhDABNA. This is achieved by incorporating spirofluorene units and introducing meta-position phenyl linkages into the DABNA-1 core. As a result, SF-PhDABNA exhibits narrowband pure blue emission centered at 472 nm with a full width at half maximum (FWHM) of 23 nm. The unique steric hindrance structure of the material effectively suppresses π-π interaction, while maintaining a tightly ordered molecular arrangement through C–H···π and C–H···B weak intermolecular interactions. This special packing pattern ensures a high photoluminescence quantum yield (PLQY) of 86% in the doped film. Moreover, the significant directionality of the transition dipole moment (TDM) further enhances the light output coupling efficiency, thereby significantly improving the electroluminescence (EL) performance. The corresponding TADF-sensitized (TSF) OLED based on SF-PhDABNA achieves a maximum external quantum efficiency (EQEmax) of 23.9% with CIE coordinates of (0.121, 0.284).
Azulene derivatives are promising for optoelectronics but suffer from weak fluorescence due to anti-Kasha behavior. This study designed and synthesized four asymmetric 1-azaazulene-based BF2 complexes (Ph-NN, Ph-ON, Ca-NN, Py-NN) to explore their optoelectronic potential. Unlike azulene derivatives, which predominantly exhibit S2→S0 emission, 1-azaazulene constructs demonstrate effective S1-S0 transitions, resulting in enhanced fluorescence. Py-NN, incorporating a pyrrole group, achieved a remarkable photoluminescence quantum yield (PLQY) of 19.3% at 560 nm, attributed to enhanced HOMO-LUMO orbital overlap with an oscillator strength (f) of 0.4973, resulting in a high radiative rate (kr = 9.51 × 107 s−1) and suppressed non-radiative decay (knr = 0.40 × 109 s−1). OLEDs employing Py-NN as an emitter exhibited orange electroluminescence at 565 nm with a maximum external quantum efficiency (EQE) of 3.0%. The results demonstrate that 1-azaazulene can serve as a versatile platform for developing efficient fluorescent materials with applications in optoelectronics.
Utilizing sunlight to directly convert CO2 into value-added chemicals presents a pivotal strategy for sustainable CO2 conversion and mitigating environmental challenges. Herein, a surface-mounted 5,10,15,20-tetra(4-carboxyphenyl)porphyrin copper(Ⅱ) (CuTCPP) anchoring on Bi12O17Br2 nanotubes (CuTCPP/Bi12O17Br2) heterojunction was employed as an operable platform for photocatalytic CO2 reduction. The built-in electric field at the interface facilitates the efficient electron transfer from Bi12O17Br2 to CuTCPP, significantly enhancing photoexcited charge separation and transfer kinetics. Besides, the Cu(Ⅱ) sites in CuTCPP act as supplementary catalytic centers that reduce the adsorption and activation energy barrier of CO2, thus accelerating the formation of *CO intermediates. The CuTCPP/Bi12O17Br2 heterojunction exhibits enhanced photoreduction activity of CO2, achieving a CO evolution rate of 92.2 μmol g-1 h-1, which represents a 4.0-fold enhancement over Bi12O17Br2. This work offers new insights into the development of heterojunctions with synergistically optimized charge transfer and active sites.
Water-based lubrication systems incorporating nanoparticles as highly promising additives are of great importance for enabling sustainable and environmentally benign tribological solutions. However, persistent limitations encompass pronounced substrate dependence, inadequate dynamic responsiveness under operating conditions, and intrinsically constrained lubrication performance, collectively impeding their transition from laboratory potential to robust industrial deployment. To tackle these challenges, we have developed a substrate-adaptable and dual-responsive lysine-based surfactant (LBS) as a cutting-edge water-based lubrication additive. LBS achieves substrate-independent adsorption through multiple interactions between its head group and substrates of varying properties. LBS maintains consistent lubrication performance with minimal COF variation across substrates with divergent surface charges, confirming its adaptability to diverse tribological substrates. Notably, the engineered surfactant demonstrates outstanding lubricating properties, achieving a coefficient of friction (COF) of ~0.06 under extreme pressure condition (~500 MPa), a 95% reduction in COF compared to pure water and maintaining stable lubrication over 25,000 cycles without significant wear or interfacial degradation. Additionally, by leveraging the pH sensitivity of the molecular structure and the temperature responsiveness of the micellar assembly, the COF can be rapidly modulated over a 10-fold range in response by changes pH and temperature. By synergistically integrating universal substrate adaptability with stimuli-responsive behavior, this work not only ensures stable lubrication in complex substrates, but also opens new avenues for the intelligent design of surfactants, offering significant potential for large-scale applications in intelligent lubrication.
The surface activity and continuous photosynthesis with easy product separation are two main concerns for practical H2O2 photogeneration which calls for integration of efficient photocatalyst with specifically designed reactor. Taking advantage of the intrinsic superior charge separation and electron transfer of the one-dimensional CN, herein, N-vacancy abundant carbon nitride nanorod arrays (CNNRs) were demonstrated as an efficient photocatalyst either in convention photocatalysis or in emerging flow photocatalytic H2O2 production. The N-vacancies multifunctionally enhance light harvesting, elevate conduction band, adsorb and activate O2 molecules. As a result, the N-defective CNNRs delivered 5.2 and 2.1 times higher H2O2 yield in its powder form than common CN nanosheets and defect-free CNNRs, reaching 18.8 mmol g-1 h-1 with AQY of 13.4% at 400 nm in ethanol-containing solution. Moreover, the CNNRs on glass, as a photocatalyst panel, exhibits remarkable fixed-bed and continuous flow photocatalytic H2O2 production performances, with yield up to 23.6 and 14.2 mmol m-2 h-1, respectively. Mechanism investigation discloses the sequential two-step 1e oxygen reduction pathway that accounts for H2O2 photogeneration, with further thermal-dynamical confirmation by DFT calculation. This work introduces a new paradigm by combining photocatalyst design with advanced flow reactors to achieve continuous photosynthesis of H2O2, which may inspire many other photo-to-chemical conversions as well.
The utilization of solid electrolytes as substitutes for flammable liquid electrolytes represents a crucial strategy for enhancing both the safety and energy density of lithium metal batteries. However, the poor solid-solid contact between electrodes/electrolytes and the inherent difficulties of Li dendrite growth have seriously hindered their practical applications. Among the various types of solid electrolytes, polymer electrolytes are highly regarded for their potential high ionic conductivity, good deformability, and wide electrochemical window. In-situ curing technology has been demonstrated to be an effective solution to these problems and shows great application prospects in polymer electrolyte all-solid-state lithium-metal batteries. This paper will provide a comprehensive review of the three primary types of polymerization methods: free radical polymerization, ring-opening metathesis polymerization, and ionic polymerization. The technical principles, research progress, and performance optimization of in-situ polymerized solid state electrolytes will be reviewed, and the review will look forward to the future development of in-situ curing. The emerging challenges faced by the field and the potential opportunities in practical applications will be pointed out. As research progresses and technology advances, in-situ curing technology is poised to reinvigorate the development of all-solid-state batteries, propelling them towards enhanced safety, efficiency, and reliability.
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