Surface Chemistry Research Articles

Sculpting liquid metal stabilized interfaces: a gateway to liquid electronics.

Liquid electronics have potential applications in soft robotics, printed electronics, and healable electronics. The intrinsic shortcomings of solid-state electronics can be offset by liquid conductors. Alloys of gallium have emerged as transformative materials for liquid electronics owing to their intrinsic fluidity, conductivity, and low toxicity. However, sculpting liquid metal or its composites into a 3D architecture is a challenging task. To tackle this issue, herein, we explored the interfacial chemistry of metal ions and tannic acid (TA) complexation at a liquid-liquid interface. First, we established that an MIII-TA network at the liquid-liquid interface could structure liquid in liquid by jamming the interfacial film. The surface coverage of the droplet largely depends on the concentration of metal ions, oxidation state of metal ions and pH of the surrounding environment. Further extending the approach, we demonstrated that TA-functionalized gallium nanoparticles (Ga NPs) can also sculpt liquid droplets in the presence of transition metal ions. Finally, a mold-based free-standing 3D architecture is obtained using the interfacial reaction and interfacial crowding of a metal-phenolate network. Conductivity measurement reveals that these liquid constructs can be used for low-voltage electronic applications, thus opening the door for liquid electronics.

Influence of Material Properties on Surface Chemistry Induced Circular Dichroism in Halide Perovskite: Computational Insights.

The chirality transfer phenomenon is attractive for enhancing the optical functionality of nanomaterials by inducing sensitivity to the circular polarization states of photons. An underexplored aspect is how material properties of the achiral semiconductor impact the induced chiroptical signatures. Here we apply atomistic time-dependent density functional theory simulations to investigate the material properties that influence the chiroptical signatures of a lead halide perovskite nanocrystal with a chiral molecule bound to the surface. First, we find that both lattice disorder created by surface strain and halide substitution can increase the chiroptical response of the perovskite quantum dots by an order of magnitude. Both phenomena are attributed to a broadening of the density of the electronically excited states. Second, the intensity of the anisotropy spectra decreases with increasing dot size with a power law decay. Overall, these insights can be used to help guide experimental realization of highly resolvable polarized optical features in semiconducting nanomaterials.

Competitive Valerate Binding Enables RuO2-Mediated Butene Electrosynthesis in Water.

The (non)-Kolbe oxidation of valeric acid, sourced from a hydrolysis product of cellulose, provides a sustainable synthetic route to access value-added products, such as butene. An essential mechanistic step preceding product formation involves the oxidative and decarboxylative cleavage of a C-C bond. Yet, the role of the electrode surface in mediating this oxidative step remains an open question: the electron transfer can occur either via an inner-sphere or outer-sphere mechanism. Here, we report the electrochemical, in situ spectroscopic, computational, and reactivity studies of RuO2-mediated oxidative decarboxylation of valeric acid to butene in aqueous electrolytes. We find that carboxylates bind to RuO2 anode surfaces at potential values where decarboxylation products are observed. Our results are consistent with a reaction scheme where the competitive and catalytic oxygen evolution reaction (OER) is impeded by these bound carboxylate species while these species are inert toward butene formation. Our results implicate an outer-sphere electron transfer mechanism for decarboxylation where the surface chemistry of the RuO2 electrode serves to enable higher non-Kolbe reaction selectivity by suppressing the parasitic OER. Our findings delineate interfacial design principles for selective electrochemical systems that utilize water as the ultimate oxidant for sustainable decarboxylation.

Electrochemical Anion Sensing Using Conductive Metal-Organic Framework Nanocrystals with Confined Pores.

Anion sensing technology is motivated by the widespread and critical roles played by anions in biological systems and the environment. Electrochemical approaches comprise a major portion of this field but so far have relied on redox-active molecules appended to electrodes that often lack the ability to produce mixtures of distinct signatures from mixtures of different anions. Here, nanocrystalline films of the conductive metal-organic framework (MOF) Cr(1,2,3-triazolate)2 are used to differentiate anions based on size, which consequently affect the reversible oxidation of the MOF. During framework oxidation, the intercalation of larger charge-balancing anions (e.g., ClO4-, PF6-, and OTf-) gives rise to redox potentials shifted anodically by hundreds of mV due to the additional work of solvent reorganization and anion desolvation. Smaller anions (e.g., BF4-) may enter partially solvated, while larger ansions (e.g., OTf-) intercalate with complete desolvation. As a proof-of-concept, we leverage this "nanoconfinement" approach to report an electrochemical ClO4- sensor in aqueous media that is recyclable, reusable, and sensitive to sub-100-nM concentrations. Taken together, these results exemplify an unusual combination of distinct external versus internal surface chemistry in MOF nanocrystals and the interfacial chemistry they enable as a novel supramolecular approach for redox voltammetric anion sensing.

Aggregation and Sedimentation Stability of Nanoscale Zeolitic Imidazolate Framework (ZIF‐8) Nanocomposites for Antimicrobial Agent Delivery Applications

ABSTRACTThe applications of nanoscale zeolitic imidazolate frameworks (ZIF‐8) for antimicrobial drug delivery depend on the aqueous suspension stability of the ZIF‐8 which is influenced by their crystallinity, size, shape, aggregation, and surface chemistry. This study evaluated the stability of ZIF‐8 nanoparticles in terms of their aggregation and sedimentation characteristics. ZIF‐8 nanocomposites were synthesized with methanol via sonication at 30°C for 1 h. The effect of drying methods (oven drying at 80°C, and vacuum drying at 35°C), number of washing steps (0 = no wash, 1, 2, 3), and washing medium (washing with water and ethanol instead of methanol, and redispersion in water and ethanol) on the suspension stability was evaluated. The impact of added xanthan gum (XG) and poly‐L‐lysine (PL) as suspension media was also evaluated. ZIF‐8 nanoparticles were also synthesized using ethanol and suspended in PL. % transmittance and zeta potential were measured for freshly prepared ZIF‐8 suspensions in PL and after freeze‐drying and resuspending in water. Scanning electron microscopy (SEM), transmission electron microscopy (TEM), Fourier transform infrared spectroscopy (FTIR), and x‐ray diffraction (XRD) analysis were utilized for the assessment of the crystallinity, structure, and morphology of the samples. Antibacterial activity was evaluated by disc diffusion test against Escherichia coli. Dried methanol‐synthesized ZIF‐8 nanoparticles did not suspend in water; only the ZIF‐8 nanoparticles synthesized with reduced washing times and no drying treatment were resuspended in the water, XG and PL solutions. Instead, the ethanol‐synthesized ZIF‐8 nanoparticles were resuspended in water even after being washed three times and dried in a vacuum oven. SEM and TEM images and XRD patterns showed that alcohol can form well‐defined ZIF‐8 nanoparticles. FTIR spectra showed that ZIF‐8 had typical peaks of ZIF‐8 reported by others. Although particle size increased, the PL coating provided a 32.22% increase in zeta potential of ZIF‐8 nanoparticles from 36.25 to 47.93 mV (p < 0.05) and prevented aggregation and sedimentation of the nanoparticles without changing their morphology. All the tested ZIF‐8 nanoparticles showed antibacterial activity with the PL‐coated ZIF‐8 having the highest effect followed by the ZIF‐8 nanoparticles synthesized in ethanol.

Tailoring metal oxide nanozymes for biomedical applications: trends, limitations, and perceptions.

Nanomaterials with enzyme-like properties are known as 'nanozymes'. Nanozymes are preferred over natural enzymes due to their nanoscale characteristics and ease of tailoring of their physicochemical properties such as size, structure, composition, surface chemistry, crystal planes, oxygen vacancy, and surface valence state. Interestingly, nanozymes can be precisely controlled to improve their catalytic ability, stability, and specificity which is unattainable by natural enzymes. Therefore, tailor-made nanozymes are being favored over natural enzymes for a range of potential applications and better prospects. In this context, metal oxide nanoparticles with nanozyme-mimicking characteristics are exclusively being used in biomedical sectors and opening new avenues for future nanomedicine. Realising the importance of this emerging area, here, we discuss the mechanistic actions of metal oxide nanozymes along with their key characteristics which affect their enzymatic actions. Further, in this critical review, the recent progress towards the development of point-of-care (POC) diagnostic devices, cancer therapy, drug delivery, advanced antimicrobials/antibiofilm, dental caries, neurodegenerative diseases, and wound healing potential of metal oxide nanozymes is deliberated. The advantages of employing metal oxide nanozymes, their potential limitations in terms of nanotoxicity, and possible prospects for biomedical applications are also discussed with future recommendations.

Role of Cu Oxide and Cu Adatoms in the Reactivity of CO2 on Cu(110)

AbstractWe investigate the interaction of CO2 with metallic and oxidized Cu(110) surfaces using a combination of near‐ambient pressure scanning tunneling microscopy (NAP‐STM) and theoretical calculations. While the Cu(110) and full CuO films are inert, the interface between bare Cu(110) and the CuO film is observed to react instantly with CO2 at a 10 mbar pressure. The reaction is observed to proceed from the interfacial sites of CuO/Cu(110). During reaction with CO2, the CuO/Cu(110) interface releases Cu adatoms which combine with CO3 to produce a variety of added Cu−CO3 structures, whose stability depends on the gas pressure of CO2. A main implication for the reactivity of Cu(110) is that Cu adatoms and highly undercoordinated CuO segments are created on the Cu(110) surface through the interaction with CO2, which may act as reaction‐induced active sites. In the case of CO2 hydrogenation to methanol, our theoretical assessment of such sites indicates that their presence may significantly promote CH3OH formation. Our study thus implies that the CuO/Cu(110) interfacial system is highly dynamic in the presence of CO2, and it suggests a possible strong importance of reaction‐induced Cu and CuO sites for the surface chemistry of Cu(110) in CO2‐related catalysis.

Interfacial Decomposition Behaviour of Triethyl Phosphate‐Based Electrolytes for Lithium‐Ion Batteries

Triethyl phosphate (TEP) is a cheap, environmentally benign, and non‐flammable electrolyte solvent, whose implementation in lithium‐ion batteries is held back by its co‐intercalation into graphite anodes, resulting in exfoliation of the graphite structure. In this work, the electrode‐electrolyte interface behaviour of electrolytes containing up to 100% TEP was investigated and correlated to electrochemical performance. High capacity and stable cycling are maintained with up to 30% TEP in carbonate ester‐based electrolytes, but above this threshold the reversibility of Li+ intercalation into graphite drops sharply to almost zero. This represents a potential route to improved battery safety, while TEP can also improve safety indirectly by enabling the use of lithium bis(oxalato borate), a fluorine‐free salt with limited solubility in traditional electrolytes. To understand the poor performance at TEP concentrations of >30%, its solvation behaviour and interfacial reaction chemistry were studied. Nuclear magnetic resonance spectroscopy data confirms changes in the Li+ solvation shell above 30% TEP, while operando gas analysis indicates extensive gas evolution from TEP decomposition at the electrode above the threshold concentration, which is almost entirely absent below it. X‐ray photoelectron spectroscopy depth profiling of electrodes demonstrates poor passivation by the solid electrolyte interphase above 30% TEP and significant graphite exfoliation.

Temperature-Sensitive Sensors Modified with Poly(N-isopropylacrylamide): Enhancing Performance through Tailored Thermoresponsiveness

The development of temperature-sensitive sensors upgraded by poly(N-isopropylacrylamide) (PNIPAM) represents a significant stride in enhancing performance and tailoring thermoresponsiveness. In this study, an array of temperature-responsive electrochemical sensors modified with different PNIPAM-based copolymer films were fabricated via a “coating and grafting” two-step film-forming technique on screen-printed platinum electrodes (SPPEs). Chemical composition, grafting density, equilibrium swelling, surface wettability, surface morphology, amperometric response, cyclic voltammograms, and other properties were evaluated for the modified SPPEs, successively. The modified SPPEs exhibited significant changes in their properties depending on the preparation concentrations, but all the resulting sensors showed excellent stability and repeatability. The modified sensors demonstrated favorable sensitivity to hydrogen peroxide and L-ascorbic acid. Furthermore, notable temperature-induced variations in electrical signals were observed as the electrodes were subjected to temperature fluctuations above and below the lower critical solution temperature (LCST). The ability to reversibly respond to temperature variations, coupled with the tunability of PNIPAM’s thermoresponsive properties, opens up new possibilities for the design of sensors that can adapt to changing environments and optimize their performance accordingly.

Surface Chemistry of Cytosporone-B Incorporated in Models for Microbial Biomembranes as Langmuir Monolayers.

Cytosporone-B, a polyketide renowned for its antimicrobial properties, was integrated into Langmuir monolayers composed of dipalmitoylphosphoethanolamine (DPPE) and dioleoylphosphoethanolamine (DOPE) lipids, effectively emulating microbial cytoplasmic membranes. This compound exhibited an expansive influence on DPPE monolayers while inducing condensation in DOPE monolayers. This led to a notable reduction in the compressibility modulus for both lipids, with a more pronounced effect observed for DPPE. The heightened destabilization observed in DOPE monolayers subjected to biologically relevant pressures was particularly noteworthy, as evidenced by surface pressure-time curves at constant area. In-depth analysis using infrared spectroscopy at the air-water interface unveiled alterations in the alkyl chains of the lipids induced by cytosporone-B. This was further corroborated by surface potential measurements, indicating a heightened tilt in the acyl chains upon drug incorporation. Notably, these observed effects did not indicate an aggregating process induced by the drug. Overall, the distinctive impact of cytosporone-B on each lipid underscores the importance of understanding the nuanced effects of microbial drugs on membranes, whether in condensed or fluid states.

The interface between ice and alcohols analyzed by atomic force microscopy.

This study investigates the interface between ice and organic solvents using atomic force microscopy (AFM). Atomically flat ice surfaces were prepared and observed by AFM in 1-octanol, 1-hexanol, and 1-butanol. The results show differences in surface roughness influenced by the interaction of ice and alcohols. Young's modulus of ice was analyzed by force curve measurements, providing valuable insights into the properties of ice in liquid environments. The results showed the characteristics of the ice surface in different solvents, suggesting potential applications in understanding surface and interface phenomena associated with ice under realistic conditions.

Unveiling Atomic-Scaled Local Chemical Order of High-Entropy Intermetallic Catalyst for Alkyl-Substitution-Dependent Alkyne Semihydrogenation.

High-entropy intermetallic (HEI) nanocrystals, composed of multiple elements with an ordered structure, are of immense interest in heterogeneous catalysis due to their unique geometric and electronic structures and the cocktail effect. Despite tremendous efforts dedicated to regulating the metal composition and structures with advanced synthetic methodologies to improve the performance, the surface structure, and local chemical order of HEI and their correlation with activity at the atomic level remain obscure yet challenging. Herein, by determining the three-dimensional (3D) atomic structure of quinary PdFeCoNiCu (PdM) HEI using atomic-resolution electron tomography, we reveal that the local chemical order of HEI regulates the surface electronic structures, which further mediates the alkyl-substitution-dependent alkyne semihydrogenation. The 3D structures of HEI PdM nanocrystals feature an ordered (intermetallic) core enclosed by a disordered (solid-solution) shell rather than an ordered surface. The lattice mismatch between the core and shell results in apparent near-surface distortion. The chemical order of the intermetallic core increases with annealing temperature, driving the electron redistribution between Pd and M at the surface, but the surface geometrical (chemically disordered) configurations and compositions are essentially unchanged. We investigate the catalytic performance of HEI PdM with different local chemical orders toward semihydrogenation across a broad range of alkynes, finding that the electron density of surface Pd and the hindrance effect of alkyl substitutions on alkynes are two key factors regulating selective semihydrogenation. We anticipate that these findings on surface atomic structure will clarify the controversy regarding the geometric and/or electronic effects of HEI catalysts and inspire future studies on tuning local chemical order and surface engineering toward enhanced catalysts.

Weakly ionized gold nanoparticles amplify immunoassays for ultrasensitive point-of-care sensors.

Gold nanoparticle-based lateral flow immunoassays (AuNP LFIAs) are widely used point-of-care (POC) sensors for in vitro diagnostics. However, the sensitivity limitation of conventional AuNP LFIAs impedes the detection of trace biomarkers. Several studies have explored the size and shape factors of AuNPs and derivative nanohybrids, showing limited improvements or enhanced sensitivity at the cost of convenience and affordability. Here, we investigated surface chemistry on the sensitivity of AuNP LFIAs. By modifying surface ligands, a surface chemistry strategy involving weakly ionized AuNPs enables ultrasensitive naked-eye LFIAs (~100-fold enhanced sensitivity). We demonstrated how this surface chemistry-amplified immunoassay approach modulates nanointerfacial bindings to promote antibody adsorption and higher activity of adsorbed antibodies. This surface chemistry design eliminates complex nanosynthesis, auxiliary devices, or additional reagents while efficiently improving sensitivity with advantages: simplified fabrication process, excellent reproducibility and reliability, and ultrasensitivity toward various biomarkers. The surface chemistry using weakly ionized AuNPs represents a versatile approach for sensitizing POC sensors.

High-efficiency dysprosium-ion extraction enabled by a biomimetic nanofluidic channel

Biological ion channels exhibit high selectivity and permeability of ions because of their asymmetrical pore structures and surface chemistries. Here, we demonstrate a biomimetic nanofluidic channel (BNC) with an asymmetrical structure and glycyl-L-proline (GLP) -functionalization for ultrafast, selective, and unidirectional Dy3+ extraction over other lanthanide (Ln3+) ions with very similar electronic configurations. The selective extraction mainly depends on the amplified chemical affinity differences between the Ln3+ ions and GLPs in nanoconfinement. In particular, the conductivities of Ln3+ ions across the BNC even reach up to two orders of magnitude higher than in a bulk solution, and a high Dy3+/Nd3+ selectivity of approximately 60 could be achieved. The designed BNC can effectively extract Dy3+ ions with ultralow concentrations and thereby purify Nd3+ ions to an ultimate content of 99.8 wt.%, which contribute to the recycling of rare earth resources and environmental protection. Theoretical simulations reveal that the BNC preferentially binds to Dy3+ ion due to its highest affinity among Ln3+ ions in nanoconfinement, which attributes to the coupling of ion radius and coordination matching. These findings suggest that BNC-based ion selectivity system provides alternative routes to achieving highly efficient lanthanide separation.

Advancements of Glucose Monitoring Biosensor: Current State, Generations of Technological Progress, and Innovation Dynamics.

Glucose monitoring is essential for managing diabetes, and continuous glucose monitoring biosensors can offer real-time monitoring with little invasiveness. However, challenges remain in improving sensor accuracy, selectivity, and overall performance. This article aims to review current trends and recent advancements in glucose-monitoring biosensors while evaluating their benefits and limitations for diabetes monitoring. An analysis of current literature on transdermal glucose sensors was conducted, focusing on detection techniques, novel nanomaterials, and integrated sensor systems. Recent research has led to advancements in electrochemical, optical, electromagnetic, and sonochemical sensors for transdermal glucose detection. The use of novel nanomaterials and integrated sensor designs has improved sensitivity, selectivity, and accuracy. However, issues like calibration requirements, motion artifacts, and skin irritation persist. Transdermal glucose sensors show promise for non-invasive, convenient diabetes monitoring but require further enhancements to address limitations in accuracy, reliability, and biocompatibility. Continued research and innovation focusing on sensor materials, designs, and surface chemistry is needed to optimize biosensor performance and utility. The study offers a comprehensive analysis of the present status of technological advancement and highlights areas that need more research.

Unveiling Key Interface Characteristics of Ni/Yttria-Stabilized Zirconia Solid Oxide Cell Electrodes in H2O Electroreduction Using Operando X-ray Photoelectron Spectroscopy.

Nickel/yttria-stabilized zirconia (YSZ) composites are the most commonly used fuel electrodes for solid oxide cells. While microstructural changes of Ni/YSZ during operational conditions have been thoroughly investigated, there is limited knowledge regarding Ni/YSZ surface chemistry under working conditions. In this study, we examine the interaction between Ni/YSZ electrodes and water vapor under open circuit and polarization conditions, utilizing near ambient pressure soft and hard X-ray photoelectron spectroscopies. Miniature cells with conventional porous Ni/YSZ composite cermet cathodes were modified to facilitate the direct spectroscopic observation of the functional electrode's areas close to the interface with the YSZ electrolyte. The results highlight dynamic changes in the oxidation state and composition of Ni/YSZ under H2 and H2O atmospheres. We also quantify the accumulation of impurities on the electrode surface. Through adjustments in the pretreatment of the cell, the correlation between the nickel surface oxidation state and the cell's electrochemical performance during H2O electroreduction is established. It is unequivocally shown that nickel surface oxidation in H2O electrolysis favors NiO over Ni(OH)x, providing critical insights into the mechanism of Ni-phase redistribution within the electrode during long-term operation. Depth-dependent photoemission measurements, combined with theoretical quantitative simulations, reveal that NiO and Ni phases are uniformly mixed on the surface during H2O electrolysis. This differs from the conventional expectation of a NiO-shell/Ni-core configuration in gas phase oxidation. These findings provide crucial insights into the surface chemistry of Ni/YSZ electrodes under conditions relevant to H2O electrolysis, elucidating their impact on the electrochemical performance of the cell.

Insight into adsorption behaviors of shale oil in kerogen slit by molecular dynamics

Shale oil is predominantly stored in organic nanopores, with kerogen playing a pivotal role in its adsorption. This study utilizes molecular dynamics (MD) simulations to quantitatively investigate the adsorption behavior of multi-component shale oil within kerogen slits. Unlike previous studies that focused on single-component hydrocarbon fluids and simplified kerogen models to graphene, this research employs an authentic kerogen structure and a multi-component shale oil model, incorporating the effects of surface roughness. The research analyzes the interaction mechanisms and distribution patterns of light, medium, and heavy components within the pores. Additionally, it examines the effects of temperature, pore size, and wall surface physical and chemical properties on shale oil adsorption. Results indicate that strong adsorption between asphaltene and kerogen significantly reduces the width of the kerogen slits, inhibiting the adsorption of lighter components. The study introduces the concept of effective radius for kerogen slits and provides a quantitative analysis of the adsorption capacity of kerogen surfaces. Different kerogen surface roughness and chemical properties were compared to understand their influence on shale oil adsorption. Key findings show that with increasing temperature, the distribution of hydrocarbons becomes more uniform, with medium components showing the most significant response. Surface roughness of kerogen affects the adsorption capacity, although the component proportions remain consistent, while different chemical property surfaces influence selective adsorption and the overall adsorption amount of shale oil components. This research offers a deeper understanding of shale oil adsorption mechanisms and provides valuable insights for optimizing shale oil extraction and utilization.

Highly Selective Electrocatalytic CO2 Conversion to Tailored Products through Precise Regulation of Hydrogenation and C-C Coupling.

The electrochemical reduction reaction of carbon dioxide (CO2RR) into valuable products offers notable economic benefits and contributes to environmental sustainability. However, precisely controlling the reaction pathways and selectively converting key intermediates pose considerable challenges. In this study, our theoretical calculations reveal that the active sites with different states of copper atoms (1-3-5-7-9) play a pivotal role in the adsorption behavior of the *CHO critical intermediate. This behavior dictates the subsequent hydrogenation and coupling steps, ultimately influencing the formation of the desired products. Consequently, we designed two model electrocatalysts comprising Cu single atoms and particles supported on CeO2. This design enables controlled *CHO intermediate transformation through either hydrogenation with *H or coupling with *CO, leading to a highly selective CO2RR. Notably, our selective control strategy tunes the Faradaic efficiency from 61.1% for ethylene (C2H4) to 61.2% for methane (CH4). Additionally, the catalyst demonstrated a high current density and remarkable stability, exceeding 500 h of operation. This work not only provides efficient catalysts for selective CO2RR but also offers valuable insights into tailoring surface chemistry and designing catalysts for precise control over catalytic processes to achieve targeted product generation in CO2RR technology.

Amphiphilic Nanoscale Antifog Coatings: Improved Chemical Robustness by Continuous Assembly of Polymers.

Designing effective antifog coatings poses challenges in resisting physical and chemical damage, with persistent susceptibility to decomposition in aggressive environments. As their robustness is dictated by physicochemical structural features, precise control through unique fabrication strategies is crucial. To address this challenge, a novel method for crafting nanoscale antifog films with simultaneous directional growth and cross-linking is presented, utilizing solid-state continuous assembly of polymers via ring-opening metathesis polymerization (ssCAPROMP). A new amphiphilic copolymer (specified as macrocross-linker) is designed by incorporating polydimethylsiloxane, poly(2-(methacryloyloxy)ethyl) trimethylammonium chloride (PMETAC), and polymerizable norbornene (NB) pendant groups, allowing ssCAPROMP to produce antifog films under ambient conditions. This novel approach results in distinctive surface and molecular characteristics. Adjusting water-absorption and nanoscale assembly parameters produced ultra-thin (≤100nm) antifog films with enhanced durability, particularly against strong acidic and alkaline environments, surpassing commercial antifog glasses. Thickness loss analysis against external disturbances further validated the stable surface-tethered chemistries introduced through ssCAPROMP, even with the incorporation of minimal content of cross-linkable NB moieties (5mol%). Additionally, a potential zwitter-wettability mechanism elucidates antifog observations. This work establishes a unique avenue for exploring nanoengineered antifog coatings through facile and robust surface chemistries.

Regulation of Interfacial Chemistry Enabling High-Power Dual-Ion Batteries at Low Temperatures.

Interfacial chemistry plays a crucial role in determining the electrochemical properties of low-temperature rechargeable batteries. Although existing interface engineering has significantly improved the capacity of rechargeable batteries operating at low temperatures, challenges such as sharp voltage drops and poor high-rate discharge capabilities continue to limit their applications in extreme environments. In this study, an energy-level-adaptive design strategy for electrolytes to regulate interfacial chemistry in low-temperature Li||graphite dual-ion batteries (DIBs) is proposed. This strategy enables the construction of robust interphases with superior ion-transfer kinetics. On the graphite cathode, the design endues the cathode interface with solvent/anion-coupled interfacial chemistry, which yields an nitrogen/phosphor/sulfur/fluorin (N/P/S/F)-containing organic-rich interphase to boost anion-transfer kinetics and maintains excellent interfacial stability. On the Li metal anode, the anion-derived interfacial chemistry promotes the formation of an inorganic-dominant LiF-rich interphase, which effectively suppresses Li dendrite growth and improves the Li plating/stripping kinetics at low temperatures. Consequently, the DIBs can operate within a wide temperature range, spanning from -40 to 45°C. At -40°C, the DIB exhibits exceptional performance, delivering 97.4% of its room-temperature capacity at 1C and displaying an extraordinarily high-rate discharge capability with 62.3% capacity retention at 10C. This study demonstrates a feasible strategy for the development of high-power and low-temperature rechargeable batteries.