The escalating contamination of seawater with radioactive cesium ions (Cs+) poses severe environmental and health challenges, requiring remediation strategies that are both efficient and sustainable. However, current approaches often suffer from limited selectivity, low adsorption capacity, and poor adaptability in complex ionic environments. Herein, a multifunctional Li+ - intercalated vermiculite-based photothermal aerogel evaporator is designed to synergistically couple interfacial solar evaporation (ISE) with highly selective Cs+ capture. Solardriven interfacial evaporation increases the local chemical potential of hydrated ions, while the negatively charged vermiculite nanochannels electrostatically facilitate Cs+ desolvation and intercalation, enabling active ion pumping instead of passive adsorption. Consequently, the Li-V@CNTs aerogel exhibits an excellent evaporation rate of 3.33 kg.m(-2).h(-1) under 1 sun illumination, exceeding typical cellulose or graphene oxide systems (approximate to 2.2-2.8 kg.m(-2).h(-1)). As a Cs+ sorbent, it achieves capacities up to 450 mg.g(-1) in Cs+-spiked seawater, outperforming zeolite A (approximate to 51 mg.g(-1)) and representative Zn-based metal-organic frameworks (approximate to 221 mg.g(-1)). Integrated into a sunflower-inspired solar-tracking device, the aerogel evaporator delivers clean-water yield and Cs+ removal from real seawater. Fabricated from vermiculite and bacterial cellulose via a simple, lowtemperature process (estimated material cost approximate to US$1.5 m(-2)) and operated solely by solar energy without secondary pollution, this ion-pumping platform offers a scalable platform with strong potential for sustainable radioactive seawater remediation.

Covalent organic frameworks (COFs) have proven to be appealing photocatalysts for hydrogen evolution reaction (HER) due to their tunable optical and electronic structures, as well as promising chemical stability for water splitting, yet their catalytic performance remains limited by the absence of active metal sites, insufficient charge transfer and slow exciton transport. Metal-containing COFs endow conventional metal-free polymers with metal catalytic sites and tailored coordination environments, thereby favoring enhanced photocatalytic HER performance. Herein, we report that the charge carrier transport of COFs is accelerated by incorporating copper (Cu)-based species into organic building blocks and subsequently assembling few-layer two-dimensional (2D) MXene with Cu-containing polymers. The resulting covalent metal-organic frameworks (CMOFs)/MXene heterojunctions show highly improved hydrogen production performance and long-term stability. Photoelectrochemical measurements and in situ characterizations, such as X-ray photoelectron spectroscopy (XPS), Kelvin probe force microscopy (KPFM), verify that the heterojunction photocatalysts have lower exciton binding energies and more efficient charge carrier transport than their corresponding bulk counterparts.

The electrocatalytic performance of oxygen evolution/reduction reactions (OER/ORR) is related to the spin-state of the transition metal, which can be modulated by magnetic element doping. This work proposes an innovative strategy involving non-magnetic element doping to engineer spin polarization channels through the formation of Co-O-Ru covalent bonds, which can induce a spin-state transition in Co sites from intermediate-spin state () in S CoOOH to high-spin state () in S CoOOH-Ru. The optimized S CoOOH-Ru achieves a remarkably low potential difference of 0.67 V between the E 1/2 for ORR and the eta 10 for OER, demonstrating an approximately 140 mV reduction compared with its low-spin state S CoOOH. Density functional theory (DFT) calculation reveals that the RuOx layer on CoO-termination transforms CoOOH from a paramagnetic to a ferromagnetic material, indicating the generation of high-spin Co3+ sites. This optimized Co electronic structure combined with the intrinsically active Ru sites reduces free energy barriers of key ORR/OER intermediates (*OH -> *O -> *OOH) and accelerates the reaction kinetics, enhancing catalytic performance. This work not only unveils the remote control capability of non-magnetic elements on spin states but also establishes a novel paradigm for spin engineering in the design of advanced oxygen electrocatalysts.

The dissolution of lithium polysulfides (Li2Sx, 4 ≤ x ≤ 8, LiPSs) intermediates and slow redox kinetics are the main factors leading to the rapid capacity degradation of lithium-sulfur batteries (LSBs), significantly limits the practical development of LSBs. To overcome challenges, NbN embedded in nitrogen-doped carbon nanotubes (NbN@NCNT) composites were synthesized here as sulfur hosts by taking advantage of the superior electrical conductivity and excellent catalytic activity of the metal nitride NbN. The incorporation of NbN enhanced the polysulfides conversion efficiency and suppressed the shuttling effect, thereby enhancing cycling stability in LSBs. XPS results revealed the formation of Li2S, indicating that Li2S8 was sufficiently effectively reduced and catalytically converted to the Li2S. Consequently, after 100 cycles, the capacity retention rate of LSBs using the S/NbN@NCNT electrode reached 71.5% at a current density of 2 mA/cm2 with a high sulfur loading of 3 mg/cm2. More importantly, even at high current density of 8 mA/cm2, the battery assembled with NbN@NCNT was still able to reach the high capacity of 878.14 mAh/g, demonstrating outstanding rate capability. This study offered novel insights into the potential for enhancing the sulfur reaction kinetics in LSBs.

Developing highly efficient and robust Pt-based electrocatalysts for oxygen reduction reaction (ORR) remains a substantial challenge due to the sluggish kinetics of proton-coupled electron transfer (PCET) process. Herein, an effective innovation strategy involves the rational construction of supported high-entropy intermetallics (HEIs) Pt4FeCoNiSn, and its coupling with the ionic liquid [MTBD](+) is developed to simultaneously facilitate PCET steps of ORR. The anchoring effect of the substrate Co-NC and the induction effect of Sn atom conspicuously promote the formation of ordered Pt4FeCoNiSn intermetallics at lower temperature. The multiple electron effects of HEIs and strong metal-support interactions enable Pt4FeCoNiSn/CoNC with the half-wave potential (E-1/2) of 0.906 V in 0.1 mol L-1 HClO4 solution and 0.958 V in 0.1 mol L-1 KOH solution, and long-term stability over 70 K cycles. Further [MTBD](+) modification of electrocatalyst leads to the enhancement in ORR performance, where the [MTBD](+) promotes the accumulation of reaction intermediates and increases the proportion of weakly hydrogen-bonded water at the electrode-electrolyte interface, thereby accelerating proton transfer rate during the ORR process. The Zn-air battery assembled by Pt4FeCoNiSn/CoNC as oxygen electrode exhibits a high maximal power density of 190.2 mW cm(-2) at current density of 279.4 mA cm(-2), superior to those of Pt/C. (c) 2026, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.

The selectivity of two-electron oxygen reduction reaction (2e- ORR) is predominantly determined by the adsorption strength of the key intermediate *OOH on the catalyst active sites, which has often been tuned by 3d transition-metal doping. Herein, we fabricate rare earth Ce doped bismuth oxyhalide (BiOX, X = Cl, Br, I) catalysts. The built in Ce–O–Bi local configuration triggers efficient charge rearrangement and tunes the surface electron density of Ce active centers. Meanwhile, the differences in ionic radius and electronegativity among halogen species can modulate the symmetry of the Bi–O lattice, thereby forming a typical volcano-type correlation between the bond length and 2e- ORR catalytic performance. The synergistic effect of Ce doping and halogen modulation endows the 2.5%Ce-BOB catalyst with optimal 2e- ORR performance. It delivers a H2O2 selectivity of over 90% within the potential range of 0.2-0.6 V and achieves a H2O2 production rate of 2631.4 mmol g-1 h-1 at 0.1 V. Furthermore, this optimized catalyst demonstrates potential application in organic wastewater treatment, where the degradation efficiency of methylene blue (MB) reaches approximately 95% in 40 min and that of rhodamine B (RhB) approaches 99% in 15 min. This work provides new insights into the rational design of electrocatalysts and environmental applications of electrosynthesized H2O2 via the synergistic regulation of rare-earth metal doping and halogen modulation.

Poly(heptazine imide) (PHI) nanosheets hold great potential for photocatalytic hydrogen evolution due to their high crystallinity and extended It-conjugation, which enhance light absorption and charge transfer. However, conventional molten-salt synthesis only yields bulk PHI that fails to exploit these advantages. Here, we developed a cyanuric acid (CA)-LiCl ionic-cocrystal-mediated topotactic-templated conversion strategy to directly fabricate atomic-layered PHI (Li-PHIS). Structural characterizations reveal that the CA-LiCl cocrystal exhibits topological matching with Li-PHIS, where CA molecules form {00l}-oriented layer frameworks. The resulting Li-PHIS maintains crystallographically equivalent arrangement with heptazine ring constructing the {00l}-orientation. This topotactic-templated conversion strategy efficiently eliminates long-range diffusion, preserving the cocrystal's layered framework. The Li-PHIS features a thickness of 3-4 atomic layers with large specific surface area of 155.0 m2 g-1, which significantly facilitates active site exposure. Concurrently, reduced stacking density expands interlayer spacing, endowing a thermodynamically favorable band structure. Further in combination with the rapid charge migration dynamics provided by high crystallinity and Li' content in framework, Li-PHIS achieves a H2 production rate of 4001 lmol h-1 g-1 with Pt-cocatalyst, surpassing bulk Li-PHI and C3N4 by 3-fold and 40-fold, respectively. This cocrystal-mediated pathway provides a new paradigm for dimensionally controlled carbon nitrides and avoids irreversible structural damage from traditional exfoliation. (c) 2026 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights are reserved, including those for text and data mining, AI training, and similar technologies.

Dynamic modulation of upconversion with spatiotemporal spectral features is essential for advanced optical multiplexing in anti-counterfeiting applications. However, achieving reversible dynamic control of upconversion emissions in a simple nanostructure of fixed composition under external stimulation remains challenging. Here we show that orthogonal upconversion luminescence in erbium-doped bismuth oxyhalides can be temporally modulated by exploiting the interplay of oxygen vacancies and erbium activators. Alternating ultraviolet irradiation and water bleaching enables reversible regulation of the upconversion emissions with high switching contrast and excellent fatigue resistance. Experimental and theoretical evidences reveal that the introduction of oxygen vacancies and lanthanide activators as well as their interactions contributes to the photochromism-induced dynamic modulation of orthogonal upconversion luminescence. Inspired by their special luminescent performance, the developed materials facilitate evolutionary upconversion color and intensity displays in both spatial and temporal dimensions, offering a promising route for high-level anti-counterfeiting and high-capacity optical storage.

Coral reefs, vital marine ecosystems, are increasingly threatened by global warming and chemical pollutants such as benzophenone-3 (BP-3), a widely used UV filter. To address this challenge, we present a carbon-doped graphitic carbon nitride (g-C3N4) photocatalyst with efficient singlet oxygen (1O2) generation for BP-3 degradation and coral vitality restoration under simulated seawater conditions. The photocatalyst exhibits improved stability and photocatalytic performance in complex seawater environments, with enhanced charge separation and an approximately eightfold increase in the apparent degradation rate of BP-3 compared with pristine g-C3N4. Toxicity assessments indicate reduced ecological risks of degradation intermediates and significant recovery of zooxanthellae density and coral–algal symbiosis. Immobilized catalyst architectures further minimize material loss and provide a suitable substrate for coral attachment. In this work, we demonstrate a seawater-stable, 1O2-driven photocatalytic strategy that enables efficient BP-3 removal and promotes coral vitality recovery, thereby offering a scalable approach for marine environmental remediation and coral ecosystem restoration. A carbon-rich photocatalyst enables efficient degradation of sunscreen pollutants in seawater while supporting coral vitality recovery through singlet oxygen generation.

The integration of CO2 mineralization with solid waste utilization offers a promising pathway toward sustainable carbon management; however, achieving efficient Ca extraction and controllable carbonate crystallization under mild conditions remains challenging. Herein, we develop an amino acid salt-mediated system to couple Ca leaching from fly ash with CO2 mineralization, enabling simultaneous carbon capture and polymorph-controlled CaCO3 synthesis. Three representative amino acid salts (glycine, lysine, and aspartic acid potassium salts) with different side-chain functional groups were employed to regulate Ca2+ coordination, CO2 absorption, and crystallization pathways. The results demonstrate that amino acid salts significantly enhance Ca leaching efficiency through complexation, while simultaneously promoting CO2 capture via amine functionalities. Temperature plays a decisive role in polymorphic evolution and Ca conversion. Under mild conditions at 60 °C, the calcium conversion rates of the three amino acid systems reached 99.13% (GlyK), 99.32% (LysK), and 99.03% (AspK), respectively, within 30 min, accompanied by CaCO3 yields of 174.92, 123.95, and 284.71 g/kg. These results indicate highly efficient Ca utilization and rapid mineralization kinetics under mild conditions. Notably, AspK exhibits superior capability in stabilizing vaterite and regulating crystal growth, which can be attributed to its dual-carboxyl structure that enhances Ca2+ coordination and leads to adsorption-induced inhibition of crystal growth. A preliminary carbon footprint assessment further indicated that the process can achieve potential net-negative carbon emissions through CO2 sequestration and substitution of conventional CaCO3. Overall, this work demonstrates an integrated strategy for converting fly ash into value-added carbonate materials while achieving CO2 mineralization, offering new insights into sustainable CCUS technologies.

Trajectory tracking in constrained waterway environments is challenging for unmanned surface vehicles (USVs) due to nonlinear dynamics, external disturbances, limited computational resources, and complex curved trajectories. To address these issues, this paper proposes a dynamic event-triggered model predictive control (DETMPC) framework for accurate and computationally efficient USV trajectory tracking. A dynamic event-triggered mechanism is developed to update the controller only when required by the actual system evolution, and a minimum safe measurement interval is introduced to reduce excessive state measurements. In addition, a shrinking-horizon strategy is incorporated to gradually shorten the prediction horizon during convergence, thereby reducing the online computational burden. Moreover, recursive feasibility of the optimization problem and closed-loop stability of the disturbed system are rigorously guaranteed without employing stabilizing terminal constraints. Simulation results in a representative virtual waterway environment show that the proposed method achieves accurate trajectory tracking with fewer optimization updates, lower measurement frequency, and improved computational efficiency. The maximum cross-track error is reduced by 39.16%, and the number of online optimizations is reduced by 93.24%.

The design of high-activity single-atom catalysts (SACs) toward two-electron oxygen reduction is dominated by regulating the adsorption energy of *OOH intermediates at active sites, whereas the critical factor of proton activity at the catalyst-electrolyte interface has received insufficient attention. Herein, an electrode-electrolyte synergistic strategy was employed to modulate the electronic structure of Pd single-atom sites via the construction of a Pd/CeO2-MXene heterostructure and hydrogen bond strength using cetyltrimethylammonium bromide (CTAB) additive. X-ray absorption spectroscopy (XAS) and density functional theory (DFT) calculations revealed that the real active sites are Pd single-atom sites anchored via Pd-O-Ce bonding, which significantly reduces the free energies of the key reaction steps (H2O→*OOH→H2O2). In situ attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) further verified that CTAB adsorbed at the reaction interface can enhance the hydrogen bond strength of interfacial water molecules, reduce the supply of interfacial *H species, and thereby effectively suppress H2O2 decomposition. As a result, the Pd/CeO2-MXene+CTAB system achieves a low electron transfer number of 2.02 and a high H2O2 selectivity of 98.8% at 0.5 V. This study provides a novel insight into the rational design of proton-coupled electrocatalysts through the integration of interfacial hydrogen bond engineering and single-atom catalysts.

Incorporating platinum (Pt) active species into metal-free covalent organic frameworks (COFs) that possess exceptional structural regularity, robust stability, and a local coordination environment provides inspiration for designing high-performance photocatalysts towards the hydrogen evolution reaction (HER). Nonetheless, rationally modulating metal coordination interactions in Pt-decorated COF photocatalysts, a key factor governing the hydrogen-evolving performance, is fundamentally challenging. Herein, we report a beta-ketoenamine-imine hybrid COF that achieves remarkably enhanced photocatalytic activity through an interfacial metal-coordination strategy. Compared with its conventional beta-ketoenamine counterpart (PaTp-3-NT), the modified PaTp-2-NT nanohybrids deliver an exceptional hydrogen evolution rate of 17.2 mmol & centerdot;g(-1)& centerdot;h(-1) at a low Pt loading. The adjacent & horbar;C & boxH;N & horbar; and & horbar;C & boxH;O chelating motifs in PaTp-2-NT constitute a bidentate coordination geometry that facilitates the precise anchoring of Pt species within the COF framework, yielding a specific Pt-impregnated COF hybrid photocatalyst (PaTp-2-NT@Pt). The modulation of metal-to-ligand charge-transfer (MLCT) pathways in the illuminated PaTp-2-NT@Pt is achieved by tailoring the local coordination environment from Pt (II) to N, O-chelated Pt/COF complexes, thereby promoting extensive electron delocalization across the pi-conjugated framework via d-pi* orbital hybridization. Advanced experimental studies and density functional theory (DFT) calculations further verify the structural evolution, coordination microenvironment, and also the catalytic mechanism.

Amid rising global demand for renewable energy and effective plastic waste management, adopting green methods to utilize plastic waste for chemicals is a win-win strategy. Constituting the largest amount of single-use plastic litter worldwide, cellulose diacetate (CDA) based waste cigarette filters urgently require sustainable valorization pathways. However, CDA photoconversion remains highly challenging due to substantial energy barriers for selective bond cleavage, inadequate radical generation capability, and inefficient charge-carrier separation. Herein we propose a strategy to efficiently obtain C2H4 through carbene-mediated CDA photoconversion by using a sulfur vacancy-regulated copper-gallium-zinc-sulfide (VS-CGZS) catalyst. VS-CGZS enhances the thermal effect of light and lowers the energy barrier for acetyl group (*CH3CO) desorption from CDA. VS reduces the adsorption energy of *CH3CO on VS-CGZS and facilitated :CH2 formation. Consumption of photogenerated holes via *CH3CO desorption and VS-enhanced carrier separation synergistically elevate the photogenerated electrons concentration for :CH2 coupling, thereby selectively triggering and boosting C2H4 yield. Therefore, we achieve a record-breaking 14.43 mmol·gcat-1 C2H4 for CDA photoconversion within 4 h, over 6 times exceeding previous reports on photoconverting plastic into C2H4. This work establishes a strategy for efficient ethylene production from photoconversion of cellulose diacetate and carves out a paradigm in solar-driven plastic valorization.

Covalent triazine frameworks (CTFs) represent an attractive family of metal-free visible light-responsive covalent organic frameworks (COFs), possessing promising characteristics such as large specific surface area, rich nitrogen content, permanent porosity, and high thermal and chemical stability for photocatalytic hydrogen production via water splitting. Nevertheless, the majority of CTFs are confronted with difficulty in chemical synthesis and generally suffer from low electric conductivity and severe photogenerated charge carrier recombination during photocatalytic hydrogen evolution reaction (HER). The hydrogen-evolving performance highly depends on the structure of pi-conjugated CTFs and the synthetic methods, and controlled synthesis of well-defined nano-structures is still highly challenging. In this work, we report the organic acid-catalyzed synthesis of porous CTF nanoarchitectures templated by mesoporous silica molecular sieve SBA-15 with a highly ordered hexagonal structure. The SBA-15 templated CTF-S2 nanorods exhibited a substantial increase in photocatalytic HER efficiency, with an impressive 14-fold enhancement compared to the micro-sized bulk CTF-1 (4.1 mu mol h-1). This remarkable improvement in the photocatalytic HER over SBA-templated CTF-S2 nanostructure is attributed to the extended visible light absorption, accelerated charge carrier transfer and the optimized band structure.

Excellent CO2 adsorption ability and fast photogenerated carriers' supply are vital conditions for efficient CO2 photoreduction. In this paper, Au localized surface plasmon resonance (LSPR) has been successfully applied in a R-CeO2/g-C3N4 S-scheme heterojunction photocatalyst for CO2 photoreduction. R-CeO2/Au/g-C3N4 (CAC-2) exhibited excellent CO2 photoreduction performance and great stability. The CO yield over CAC-2 is about 50.58 µmol·g-1·h-1 under UV-vis light irradiation, which is about 6.7 and 6.0 times higher than that of R-CeO2 and g-C3N4, respectively. FDTD simulation, DFT calculation and photoelectrochemical tests together prove the introduction of Au NPs not only enhances the photogenerated carriers' separation efficiency, but also decreases the formation energy barrier of the important intermediate *COOH, which is beneficial for the CO2 photoreduction to CO. N2/CO2 adsorption-desorption curves indicated that the CAC-2 ternary composite had the largest specific surface area and the best CO2 adsorption capacity. Meanwhile, DFT calculation confirmed that the reduction sites of the CAC-2 had the highest electron density, which can synergistically enhance the CO2 photoreduction activity. The improvement of photocatalytic performance can be attributed to the synergistic enhancement of Au LSPR effect and S-scheme heterojunction at the interface. Based on the in situ FTIR, in situ ESR, and 13C isotope tracer experiment, a potential LSPR effect-enhanced S-scheme heterojunction catalytic mechanism has been provided, which may represent a significant advancement in the field.

Cellulose diacetate (CDA) based cigarette filters currently are the largest amount of disposable plastic waste worldwide, however, disposal of waste CDA is challenging. This is mainly owing to the large energy barrier required for selective bond breaking in its irregular polymer structure, the limited activation ability of free radicals and low separation efficiency of photogenerated carriers. Herein, we propose a novel pathway to achieve a breakthrough C-2 product yield for CDA conversion by using Zn-modified CuGaS2/Ga2S3 (Zn-CGS/GS) as a photocatalyst. Zn-CGS/GS enhances the thermal effect of light while reducing energy barrier for radical (*CH3CO/*CH3) elimination from CDA. h+ consumption via radical dissociation as well as h(+)-e(-) separation strengthened by Zn-CGS/GS heterojunction interface, jointly increases e- concentration for C-C coupling. Thus, 9.2 % Zn-CGS/GS exhibited a record-breaking 18.74 mmol.g(cat)(-1) C-2 yield within 4 h. This work provides a novel approach for the resource photo-conversion of waste cigarette filters.

Urea-assisted water electrolysis is a significant and sustainable strategy to optimize electrolyte system to promote the efficiency of hydrogen producing in overall water splitting. Here we construct excellent catalysts (NiCoRu-X) by introducing Ru into reduced dual metal-organic frameworks (MOFs) via a mild chemical reduction method, which preserves multi hetero-interfaces that are spontaneously formed. Interestingly, excellent performances in urea oxidation reaction (UOR) can be observed on all NiCoRu-X samples but without obvious difference in the activity, while the optimal catalyst can be distinguished by testing their catalytic activity in hydrogen evolution reaction (HER). Dependent density functional theory (DFT) calculations are applied to identify the potential activity sites of different heterostructure in NiCoRu-X, and reveal that the hetero-interface promotes the formation of dynamic Ni3+ actives like NiOOH, which benefit for UOR. In the urea-assisted electrolytes, the reaction potential difference by coupling the LSV curves of HER and UOR is 155 mV lower than that in the electrolyte without urea at 20 mA cm- 2, and 70 mV lower than that in overall water splitting. It reaches a high faraday efficiency (FE) of 98.5 % at 2.0 V in urea-assistant water electrolysers, higher than that without urea assistant (92.9 %). This work highlights the possibility of using urea oxidation to decrease the reaction overpotential and to further improve the efficiency of producing hydrogen in overall water splitting by introducing urea in electrolyte system.