查看更多>>摘要：The electrochemical carbon dioxide reduction reaction (CO_2RR) represents a promising strategy for converting CO_2 into CO. Atomically dispersed transition metal sites have an exceptional ability to activate CO_2. However, the strong hybridization between the 3d orbitals of these transition metals and the 5σ or 2π* orbital of CO significantly impedes *CO desorption, thereby limiting the overall CO generation activity. In contrast, s-block metals, with diffuse 3s electron clouds, exhibit weaker interactions with *CO. Nevertheless, their practical application is hindered by the high energy barrier associated with the formation of the *COOH intermediate. To address these challenges, a fluorine(F)-tuned magnesium single-atom catalyst (Mg-SAC) is developed. Remarkably, this catalyst achieved a CO Faraday efficiency of 97.3% and a current density of 260.4 mA cm~(-2) at -0.4 V vs the reversible hydrogen electrode in a flow cell, surpassing the performance of most state-of-the-art SACs and transition metal catalysts reported in the literature. Mechanistic studies reveal that *CO desorption onMg sites is significantly easier compared to that on Fe and Co sites. Furthermore, the incorporation of F atoms modifies the electronic structure of the MgN4 sites, substantially lowering the energy barrier for the formation of the critical *COOH intermediate.
查看更多>>摘要：Friction accounts for up to 30% of global energy consumption, underscoring the urgent need for superlubricity in advanced materials. 2D electrides feature cationic layers separated by 2D confined anionic electrons. Ab initio calculations reveal that interlayer friction correlates with cationic charge and sliding-induced charge redistribution. Remarkably, the 2D electride Ba2N exhibits lower interlayer friction than graphene despite stronger interlayer adhesion, contradicting conventional tribological understanding. This anomaly stems from electron redistribution serving as the dominant energy dissipation pathway. Deep potential molecular dynamics (DPMD) simulations show that incommensurate twisted interfaces (2° < θ < 58°) in Ba2N achieve structural superlubricity by suppressing out-of-plane buckling and energy corrugation. Notably, a critical normal load of 2.3 GPa enables barrier-free sliding in commensurate Ba2N (θ = 0°), with an ultralow shear-to-load ratio of 0.001, suggesting superlubricity potential. Furthermore, electron doping effectively reduces interlayer friction by controllably modulating stacking energies. These findings establish 2D electrides as a transformative platform for energy-efficient tribology, enabling scalable superlubricity through twist engineering, load adaptation, or electrostatic gating. This work advances the fundamental understanding of electron-mediated friction, with Ba2N serving a model for cost-effective, high-performance material design.
查看更多>>摘要：Perovskite in situ exsolution is an effective approach for fabricating robust heterostructures with superior catalytic properties, but the concomitant phase transformation occurring in parent perovskite matrix often cause compromised structural integrity and diminished catalytic activity. Here a series of high-charge density Ca-doped Sr_(2-x)Ca_xFe_(1.3)Ni_(0.2)Mo_(0.5_O_(6-δ) (CaxSFNM, x ≤ 0.5) is synthesized, and treated them in reducing atmospheres to in situ exsolve FeNi3 nanoalloys (FeNi3@CaxSFNM). The phase structure progressively evolves during exsolution as Ca content decreases, among which FeNi3@Ca0.5SFNM preserves its double perovskite structure with maximal oxygen vacancy concentration, whereas other counterparts exhibit stepwise structural reconstruction. Moreover, increased oxygen vacancies strengthen their surface interactions with CO_2, conferring FeNi3@Ca0.5SFNM with exceptional CO_2 electrolysis performance, where a current density of 1.05 A cm~(-2) and a CO Faraday efficiency of 95.38%, coupled with a minimal decay rate of only 0.8 mA cm~(-2) h~(-1) during 200 h of test, are obtained at 850 ℃ and 1.5 V, surpassing others with varying phase transitions. Theoretical calculations reveal that relative to Sr~(2+), Ca~(2+) enhances electronic coupling of A-O-B sites and B 3d-O 2p orbital hybridization, ultimately reinforcing B-O bond covalency to suppress phase transition and oxygen vacancy loss upon exsolution.
查看更多>>摘要：As a promising photocatalyst for CO_2 conversion, graphitic carbon nitride (CN) suffers from limited visible-light absorption and rapid charge recombination. Here, a noble-metal-free plasmonic system, comprising titanium nitride (TiN) nanoparticle-decorated between CN nanolayers, functionalized with 2,2′-bipyridine-4,4′-dicarboxylic groups (dcbpy) is introduced. The CN-dcbpy-TiN hybrid exhibits activated dcbpy-induced substates, plasmonic features, and thus broadband light absorption, accompanied by elevated energy levels at the TiN-CN plasmonic Ohmic interface. Through steady-state and time-resolved photoluminescence, as well as transient absorption spectroscopy, it is shown that the dual-functionalization of dcbpy terminals and plasmonic TiN efficiently suppresses the exciton recombination and promotes internal electron transfer to the dcbpy-associated shallow-trapping sites. Moreover, plasmonic TiN enables ultrafast electron transfer (<400 fs) and generates long-lived active electrons via energetic high-lying electrons and a nanoheating effect. The optimized CN-dcbpy-TiN15 demonstrates a notable CO production rate of 1180 μmol g~(-1) h~(-1) under visible-light irradiation (λ > 420 nm) and an apparent quantum yield of 2.53% at 420 nm. This work develops a novel mechanism of "noble-metal-free plasmon-induced defect-state electron enhancement" that successfully addresses the trade-off between light absorption and thermodynamics/kinetics, offering new insights to resolve the trilemma of traditional photocatalysts-simultaneously achieving broad-spectrum responsiveness, high carrier energy, and long-lived charge separation.
查看更多>>摘要：Scalable and energy-efficient fabrication methods are essential for the practical deployment of solar-driven interfacial evaporator. Herein, a novel and scalable CO_2-puffing drying strategy is presented to construct high-performance biomass-based solar evaporator with hierarchical porous architectures. Compared to traditional freeze-drying, this method significantly reduces energy consumption and processing time while preserving mechanical integrity and enhancing pore interconnectivity. The resulting carbonized potato evaporator, further functionalized with poly (sodium 4-styrenesulfonate) (PNaSS), exhibits exceptional photothermal performance, achieving an evaporation rate of 3.46 kg∙m~(-2)∙h~(-1) and a solar-to-vapor conversion efficiency of 98.67% under 1 sun. The multiscale interconnected pore structure promotes rapid water transport, effective salt backflow, and thermal localization. Notably, the evaporator shows excellent salt resistance and long-term stability during cyclic operation and outdoor testing. This work offers a cost-effective and scalable pathway for producing bio-derived solar evaporator, providing new insights into sustainable freshwater harvesting and desalination technologies.
查看更多>>摘要：Although metal single atoms in photocatalysts can promote the CO_2 adsorption and reduction, it is still limited by the low valence state of metal single atoms. Here, S-Fe single-atom-loaded (S-Fe-hCN) nanosheets are synthesized by spark plasma sintering (SPS) and following S+ ion implantation. Benefiting from the mandatory nature of ion implantation technique, it not only reaches high content of S-doping, but also forms a high valence state of Fe and a special metal single-atom coordination structure, which greatly improves CO_2RR performance, and achieves 1100 times enhancement in CO yield with high yield of 110 μmol g~(-1) h~(-1), 100% CO selectivity, and a high quantum efficiency of 10.1% at 420 nm. EXAFS, in situ Mössbauer spectroscopy, and DFT calculations all reveal that S+ ion implantation constructs a Fe4+-N4S coordination structure, leading to the high electron transfer, which builds a stable CO_2-Fe-N4S adsorption state, opens the C═O double bond, and activates the O atom.
查看更多>>摘要：Nickel-iron-based sulfides have recently attracted considerable attention as promising candidates for water oxidation. However, the high concentration of chloride ions (Cl-) in seawater poses a major challenge, as they readily corrode active sites and significantly compromise long-term durability. Most nickel-iron-based sulfides suffer from poor stability under these conditions, particularly at high current densities, which greatly hinders their practical application in large-scale seawater electrolysis. In this study, an innovative iron and cobalt co-doped nickel sulfide (NiFeCoS) electrode is introduced, produced via a simple fabrication method, which effectively protects the active sites from Cl- attack during alkaline seawater oxidation, even under high current densities. The NiFeCoS catalyst exhibits remarkable stability, maintaining stable performance for over 148 h at a current density of 1 A cm~(-2) in alkaline seawater electrolytes. In an alkaline electrolyte, it achieves low overpotentials of 261, 312, and 342 mV to reach current densities of 100, 500, and 1000 mA cm~(-2). This research presents a novel approach for constructing NiFeCoS electrodes through a straightforward two-step synthesis process, offering a promising and efficient strategy for large-scale hydrogen production via seawater electrolysis.
查看更多>>摘要：Bioadhesives face significant challenges in achieving both wet tissue adhesion and deformation tolerance for bladder sealing. This study presents a "covalent/non-covalent" coupled bidirectional anchoring strategy to develop a high-performance protein-based Janus patch. The patch comprises a deformable hydrogel bottom layer (composed of renewable-source gelatin, anionic zein colloid, and genipin) and a bidirectional anchoring adhesive layer (composed of poly-lysine, anionic zein colloid, and genipin). The former ensures stress dissipation and anti-adhesion, while the latter enables initial strong wet adhesion to both the tissue and bottom layer via ionic interactions, followed by subsequent covalent anchoring at both the tissue-adhesive and hydrogel-adhesive interfaces. The underlying mechanism relies on the dynamic dissociation/reassociation of ionic bonds for exceptional energy dissipation and deformation tolerance, supplemented by permanent covalent anchoring that ensures long-term, robust interfacial adhesion. Consequently, the Janus patch exhibits superior bladder adhesion (132.5 J m~(-2)), high strain tolerance (>100%), and remarkable burst pressure resistance (108.1 cmH2O). In vivo/vitro tests confirm its reliable bladder adhesion, post-surgical anti-adhesion capability, exceptional biocompatibility, and automatic degradability, enabling effective bladder sealing and repair without post-surgical removal. This strategy overcomes key limitations of conventional bioadhesives, showing great promise for dynamic tissue sealing applications.
查看更多>>摘要：Constructing 3D Cu-based current collectors (CCs) is a promising strategy to stabilize Li metal anodes. However, the intrinsic lithiophobic nature of Cu hinders uniform Li diffusion and induces inhomogeneous Li deposition, whereas the insufficient understanding of stress evolution during Li deposition limits insights into its role in dendrite formation. Herein, a dual-gradient patterned Cu-Ag CC (PCA-CC) is designed with spatially ordered microstructures. The patterned architecture increases the electrode-electrolyte contact area and redistributes local current density through regularly aligned surface microgrooves. A gradient in lithiophilicity and conductivity directs Li nucleation, promoting uniform deposition and improved cycling stability. In addition, the ordered microgrooves provide a pathway for stress relaxation during Li plating, which helps suppress dendrite formation. As a result, the PCA-CC enables stable and durable electrochemical performance. Li/PCA-CC symmetric cells achieve long-term cycling for over 900 h at 1 mA cm~(-2) and 1 mAh cm~(-2). Furthermore, Li/PCA-CC | LFP full cells demonstrate excellent capacity retention and rate capability, maintaining stability across a wide range of rates. This study presents a scalable dual-gradient CC that integrates structural design, surface chemistry, and stress regulation to advance safer and high-performance Li metal batteries.
查看更多>>摘要：The electrocatalytic role of Ti_3C_2Tx MXene in U(VI) immobilization has remained largely unexplored. Herein, a binder-free electrode (TiMX/CNTCOOH) is designed and its exceptional performance in electrochemically U(VI) extraction under square-wave exchange (SWE) is demonstrated. The incorporation of carboxylated carbon nanotubes (CNT-COOH) as a rigid spacer not only enhances structural disorder but also exposes abundant undercoordinated Ti edge sites and induces bond stretching (Ti-O and O-H), further boosting intrinsic catalytic activity. This synergistic effect interaction lowers the energy barrier of the rate-determining step by 0.82 eV. Through integrated in situ Raman spectroscopy and density functional theory calculations, the dynamic U(VI)/U(V) transition is directly captured at Ti-active edge sites, representing the first mechanistic elucidation of MXene-based electrocatalysis for uranium. Consequently, the TiMX/CNT-COOH cathode achieves an impressive uranium extraction capacity of 1,1719.96 mg g~(-1) with excellent cycling stability. This work offers fundamental insights into the electrocatalytic mechanism and provides a strategic framework for designing large-scale electroactive materials for uranium recovery from wastewater.
NETL
NSTL
Wiley