Elucidating the SO2 heterogeneous oxidation mechanism at the gas-liquid interface is critical for understanding haze formation. However, the dominant pathways and the oxidant's relative contributions remain ambiguous. This study developed a methodology that coupled a radical interfacial enrichment strategy with chemiluminescence (CL) detection, establishing a CL system capable of discriminating between the dissolved oxygen (DO) pathway and the non-DO oxidation pathway. By anchoring sorbic acid (SA)-functionalized Cr3+-doped ZnGa2O4 nanoparticles (ZGC NPs) at the interface of SO2 microbubbles, we constructed a highly efficient CL reaction interface with nanoscale characteristics. This design facilitated hydrogen-bond-driven spatial enrichment of SO2 and its radical intermediates at the gas-liquid interface. The radical-enriched interface induced a highly sensitive CL signal from the ZGC-SA-SO2 system, which displayed composite characteristics from both pathways. Deciphering the signals revealed that the heterogeneous oxidation mechanism of SO2 evolved dynamically with concentration. The dependence on the DO pathway decreased as the concentration increased. Additionally, the proposed method has been successfully implemented in the monitoring of automotive exhaust SO2 and the rapid assessment of food freshness. The generality of this approach was further demonstrated by the observable interfacial CL signals across various ZGC-type NPs-unsaturated fatty acid-SO2 systems. This work not only deciphers the dynamic, oxidant-dependent mechanism of SO2 oxidation but also establishes a universal platform for SO2 gas detection under mild conditions.
With the growing demand for highly efficient sensors capable of rapid and reliable detection of trap states in semiconductors, developing novel chemical and physical phenomena induced by trap states at nanomaterial interfaces has thus emerged as a critical technological field. Herein, we developed an innovative time-dependent chemiluminescence (CL) method for evaluating trap states in semiconductor materials. By leveraging the unique trap states of Cr3+-activated zinc gallate (ZGOC) semiconductors and the hydroxyl radical (·OH)-rich EDTA-Fe2+-H2O2 system, we achived rational manipulation of ·OH-triggered time-dependent near-infrared (NIR) CL induction. To extract high-information-density outputs from the CL response, ZGOC nanocrystals associated with different Cr3+-related trap states were precisely identified by a distinct CL "fingerprint" pattern and robust statistical analysis. Remarkably, the generalizability of this method was validated using mixed models containing two typical samples and other adjustable ZGOC systems. The developed CL probe for Cr3+-related trap state evaluation provides advantages such as cost-effectiveness, operational simplicity, and rapid response, offering a promising and innovative alternative to conventional trap state assessment methods.
High energy and power densities of lithium metal batteries (LMBs) attract continuing popular appeal, but extra requirements must be considered since disordered Li dendrites under violent Li fluxes pose challenges for flourishing LMB applications, especially for incompatible separators. In this research, a BPP@F-SiO2 composited separator is subtly prepared based on the two-step grafted SiO2 (F-SiO2) coating self-construction. F-SiO2 particles matched to lamellae sizes endow separators with centralized pore sizes. F-SiO2 coating self-construction on porous skeletons eliminates individual coating steps, which can simplify engineering equipment layouts and improve the actual manufacturing efficiency. Solvent-free and nonadhesive features avoid problems such as micropore blocking, thickness increase, and environmental pollution. Also, the F-SiO2 coating supplies extra Li+ for stabilizing the solid electrolyte interphase layer, homogenizing Li depositions, and acquiring remarkable electrochemical and battery performances for LMBs, which enable the BPP@F-SiO2 separator to be potentially applied in LMBs demanding sufficient security, high-capacity density, and fast charge technology. The proposed approach relies on current mainstream separator fabrication lines, which can achieve low-cost and large-scale production without developing extra production lines and lower practical application barriers of prospective LMBs.
[Purpose] This study explores user knowledge collaboration in open innovation communities, focusing on how interaction characteristics influence knowledge innovation through knowledge exchange. Based on social capital and knowledge creation theories, we analyze user interactions that facilitate knowledge flow and innovation. [Methods] Using Python-based natural language processing, we process 170,000 user interactions from the Huawei Pollen Club. A knowledge synergy model is built, transforming interaction features and knowledge exchange behaviors into measurable indicators. Stepwise regression and mediation analysis are applied. [Results] (1) Network centrality, structural holes, and relationship redundancy impact knowledge exchange and innovation. (2) Relationship redundancy follows an inverted U-shape, where moderate redundancy enhances knowledge creation, but excessive redundancy hinders it. [Innovations] (1) A user knowledge collaboration model is proposed. (2) NLP techniques enable large-scale knowledge extraction and provide strategic insights for managing innovation communities.
By 2030, China is projected to become a “super-aged” society, with individuals aged 65 and above comprising over 20
Literature reviews provide comprehensive overviews of research on a given topic, serving as a foundation for future studies and uncovering new insights by situating findings within a broader context. However, little research has examined these reviews as a collective body. The landscape of review studies on health information behavior and how they have evolved over time was explored. To achieve this, a review of reviews was conducted using a sample of 91 review studies identified through the Preferred Reporting Items for Systematic Reviews and Meta-Analyses flow diagram. The findings reveal that while some researchers are well-integrated into co-authorship networks, most authors tend to work independently when producing review studies. These reviews are widely dispersed across journals rather than concentrated in a few core outlets. Systematic reviews, purpose-specific reviews, and traditional reviews are the most commonly used types. These findings have practical implications for researchers aiming to produce high-quality review studies, and for journal editors, funding agencies, and policymakers seeking to trace and support the development of this field.
We developed a unique water droplet templating method to fabricate polymer films with three-dimensionally ordered porous structures. This technique is based on a polymer/solvent/H2O ternary system, and the key is to choose a volatile and hydrophobic solvent that is slightly miscible with H2O. With the fast evaporation of the solvent, water droplets separate from the casting solution and condense from the air to act as pore templates inside the film and on the surface, respectively. According to this law, nitrocellulose (NC) films were produced from the NC/methyl acetate (MA)/H2O system in which the solubility of H2O in MA is 8.1 wt %. By modulating the solution concentration (density) from 3% to 9% NC, the distribution of separated water droplets (pores) in the solution can be flexibly controlled from sinking to floating. On the other hand, substantial ordered honeycomb pores, originated from condensed water droplets, distribute uniformly on the surface of NC films. This water droplet templating technique can be extensively applied in various polymer films, providing an effective pathway to designing polymer films with a desirable porous structure and diverse functionalities.
PurposeDigital literacy has become a crucial personal competency in digital transformation across society, and its enhancement is increasingly recognized as an urgent issue.Design/methodology/approachThis study employs the grounded theory method of qualitative research, collecting data through semi-structured interviews, to explore older adults' digital literacy practices from a situated cognitive perspective, revealing that the acquisition, development, and application of digital literacy are strongly influenced by various situational factors.FindingsThematic, task, external, and internal situations affect digital behavioral intentions, acquisition strategies, digital analysis, and digital problem-solving, leading to diverse digital behavioral outcomes. The influence of composite situations on digital literacy can be summarized through three pathways: the endogenous motivation path of "wanting to" in terms of willingness, the cognitive level path of "can it" in terms of thinking, and the behavioral ability path of "can it work" in terms of operation.Originality/valueThis study outlines a situated acquisition framework for cultivating digital literacy: first, re-examining the situated attribute of the connotation and denotation of digital literacy from the perspective of situated cognition; second, promoting the acquisition and development of digital literacy through the suitability supply of digital resources and the cognitive transformation of individuals, focusing on both the external "affordance" of the environment and the internal motivation of individuals.
Traditional polyolefin separators used in lithium-ion batteries (LIBs) suffer from poor wettability with electrolytes, significantly hindering their application in high-energy density batteries. To address this issue, we developed an EVOH-coated polyethylene separator using a phase separation method. The modified separator retains mechanical properties such as tensile strength and puncture resistance similar to the base separator. The soft EVOH coating enhances the separator's ability to conform to the electrode under stress, improving contact and overall battery performance. Notably, the EVOH coating significantly enhances the separator's electrolyte wettability, resulting in an electrolyte uptake of 253%. The abundant hydroxyl groups within the coating improve the electrochemical performance, leading to enhanced discharge rate capacity and cycling stability. The lithium-ion transference number of the modified separator increased to 0.76. The straightforward preparation method and superior performance of the EVOH-coated separator suggest its promising application in high-performance LIBs.
Thermochromic VO2 has garnered widespread attention with unique optical regulation in the fields of smart windows. However, VO2 windows with persistent stability and optical tunability in an outdoor environment are still a challenge. This study presents a multifunctional VO2 film, including a thermochromic VO2/polymer layer with VO2 particles dispersed in a urea-polydimethylsiloxane (uPDMS) matrix and a smooth liquid-infused porous surface (SLIPS) layer with silicone oil filling in porous structures. Entrapping VO2 particles within the urea-polydimethylsiloxane net ensures thermochromic stability. The extensive hydrogen bonds between urea groups and highly mobile polydimethylsiloxane chains ensure the self-healing performance, while the upper SLIPS layer offers the self-cleaning performance. This bilayer composite film demonstrates excellent solar modulation ability (ΔTsol = 20.25%), adequate visible light transmittance (Tlum,c = 47.78%), a remarkable self-cleaning performance (RA = 8.9°), and notable self-healing abilities (healing rate = 88.48%). The research herein offers a reliable approach for fabricating stable smart energy-saving window films.
Background/Objectives: Online medical consultation (OMC) platforms have become an essential tool for facilitating communication between doctors and patients, providing an efficient way for patients to access healthcare services. However, research on the key drivers of patient satisfaction within this context remains limited. This study aims to identify and prioritize the key factors influencing patient satisfaction on OMC platforms, with a focus on the Chinese “Chunyu Doctor” app as a case study. Methods: Data from patient comments on the “Chunyu Doctor” app were collected and analyzed using grounded theory to identify the influencing factors of patient satisfaction. The decision-making trial and evaluation laboratory (DEMATEL) method was then applied to assess and prioritize the factors influencing patient satisfaction, identifying the key determinants from a complex set of potential influences. Results: The study identified 11 key factors out of 23 that significantly impact patient satisfaction. These factors include doctors provide professional treatment plans, doctors accurately understand patients’ concerns, doctors explain and advise on prescriptions, doctors personally respond, doctors provide comprehensive replies, cost-effectiveness, consultation fees, effectiveness of treatment outcomes, reasonableness of the doctors’ consultation process, avoidance of templated responses by doctors, and alignment of doctors responses with patient expectations. Conclusions: This study enriches the understanding of patient satisfaction in the context of online medical consultations. The findings offer theoretical insights for future research and provide practical implications for enhancing the management and development of OMC platforms, improving the quality of healthcare services, and boosting patient satisfaction.
The increasing demand for highly reliable sensors capable of anti-interference and sensitive detection of aerosol-associated hypochlorite (ClO-) drives progress in luminescence-based sensing technologies. Inspired by collective behavioral patterns in bird flocks, we developed a "bird-like flock" time-domain sensing method through the utilization of functional long afterglow nanomaterials (AGNPs) for ClO- detection. Particularly, by translating avian aggregation-separation-alignment behaviors into an algorithmic framework, we presented a new sensing mode based on simplifying time decay curves into interpretable temporal metrics. In light of dual-emission AGNPs with impressive luminescence performance, ClO--stimulated responsiveness, and derived metrics, our approach accurately distinguished ClO- concentrations down to 95 nM, resulting from the well-refined six temporal parameters. Furthermore, by integrating a portable aerosol generation device via pneumatic atomization and an aerosol-enriched hydrogel sensing matrix, we demonstrated that this time-domain analysis method maintained superior detection accuracy, outperforming traditional methods that often falter with complex water samples. This advancement paves the way for high-contrast sensing while enabling deeper exploration of atmospheric targets. Inspired by the dynamic evolution of avian flock behavior patterns, we developed a high-fidelity analytical method based on time-resolved long-afterglow spectral partitioning for qualitative and quantitative investigation of hypochlorite (ClO-) in atmospheric aerosols.
The efficient preparation of two-dimensional large-sized monolayer covalent organic framework (COF) nanosheets for highly permeable membranes has posed a long-standing challenge in the COF field. While the self-exfoliation of charged COFs represents a promising method for nanosheet production, its efficiency requires further enhancement. In this study, we present a novel finding that the presence of hydroxyl groups on the monomer significantly influences the self-exfoliation efficiency of charged COFs. Through precise regulation of hydroxyl group numbers on the monomers, we successfully achieved the efficient fabrication of large monolayer cationic COF nanosheets with impressive solubilities in common organic solvents. By virtue of their positive charge, COF monolayer nanosheets rapidly interacted with negatively charged monolayer graphene oxide (GO) in solution, facilitating their assembly into interlaced composite membranes through electrostatic interactions. The composite membranes benefited from the strong Coulombic attraction between the COF and GO nanosheets, leading to enhanced membrane stability, while the shielding effect of GO on the COF pores contributed to improved size sieving efficiency. This innovative strategy enabled the composite membranes to achieve highly selective separation of ReO4- and MoO42-, with a remarkable 100% interception rate for MoO42-.
Uneven separator porous construction inevitably raises lithium-ion migration barriers within the separator and thus limits overall lithium-ion battery (LIB) performance. In this research, serial LIB separators with various porous constructions were prepared precisely by adjusting the synchronous bidirectional drawing temperatures to confirm the bidirectional drawing modedetermined porous constructions and subsequent mechanical properties, thermal stability and electrochemical properties of separators. Crystal structure analyses, porous construction diagnoses, mechanical property characterizations and electrochemical tests reveal the competitive relationship between lamella slip and separation during the synchronous bidirectional drawing process. Lamella slip weakens at lower drawing temperatures, enhancing lamella separation and molecular chain rupture within amorphous regions. Therefore, a separator with broken fibrils presents optimized permeability and smoothed ion migration channels, but inferior mechanical properties and thermal stability. Excessive temperature highlights lamella slip, which damages the pore-forming process, worsens separator permeability and increases ion migration resistance. An appropriate drawing temperature of 100 degrees C maximally balances lamella slip and separation behaviors, retains intact fibrils and homogenized porous construction, which endows the separator with strengthened mechanical properties, isotropic thermal stability and optimized electrochemical performances. This study provides new insights for synchronous bidirectional drawing in practical separator fabrication and clarifies separator structure-determined LIB performances. (c) 2023 Society of Industrial Chemistry.
In light of deep tissue penetration and ultralow background, near-infrared (NIR) persistent luminescence (PersL) bioprobes have become powerful tools for bioapplications. However, the inhomogeneous signal attenuation may significantly limit its application for precise biosensing owing to tissue absorption and scattering. In this work, a PersL lifetime-based nanoplatform via deep learning was proposed for high-fidelity bioimaging and biosensing in vivo. The persistent luminescence imaging network (PLI-Net), which consisted of a 3D-deep convolutional neural network (3D-CNN) and the PersL imaging system, was logically constructed to accurately extract the lifetime feature from the profile of PersL intensity-based decay images. Significantly, the NIR PersL nanomaterials represented by Zn1+xGa2-2xSnxO4: 0.4 % Cr (ZGSO) were precisely adjusted over their lifetime, enabling the PersL lifetime-based imaging with high-contrast signals. Inspired by the adjustable and reliable PersL lifetime imaging of ZGSO NPs, a proof-of-concept PersL nanoplatform was further developed and showed exceptional analytical performance for hypochlorite detection via a luminescence resonance energy transfer process. Remarkably, on the merits of the dependable and anti-interference PersL lifetimes, this PersL lifetime-based nanoprobe provided highly sensitive and accurate imaging of both endogenous and exogenous hypochlorite. This breakthrough opened up a new way for the development of high-fidelity biosensing in complex matrix systems.
Polyolefin separators with worse porous structures and compatibilities mismatch the internal environment and deteriorate lithium-ion battery (LIB) combination properties. In this study, a sulfonated SiO2 (SSD) composited polypropylene separator (PP@SSD) is prepared to homogenize pore sizes and in situ-built SSD coatings on porous skeletons. Imported SSD uniformizes pore sizes owing to centralized interface distributions within casting films. Meanwhile, abundant cavitations enable the in situ SSD coating to facilely fix onto porous skeleton surfaces during separator fabrications, which feature simple techniques, low cost, environmental friendliness, and the capability for continuous fabrications. A sturdy SSD coating on the porous skeleton confines thermal shrinkages and offers a superior safety guarantee for LIBs. The abundant sulfonic acid groups of SSD endow PP@SSD with excellent electrolyte affinity, which lowers Li+ transfer barriers and optimizes interfacial compatibility. Therefore, assembled LIBs give the optimal C-rate capacity and cycling stability, holding a capacity retention of 82.7% after the 400th cycle at 0.5 C.
Developing robust electrocatalysts for efficient semi-hydrogenation of alkynes to markedly important alkenes is highly desirable in both research and industry areas. In this work, it is reported that robust palladium mesoporous nanospheres (Pd MSs) with electron-rich active sites perform perfectly as cathode electrocatalyst for electrochemical semi-hydrogenation of alkynes in water. In comparison to its counterparts, Pd MSs hold remarkable conversion (97%), superior selectivity (98%), good operation stability in selective semi-hydrogenation of p-aminophenylene. High performance is assigned to electron-rich Pd sites within mesopores that not only favor the formation of active H* but also accelerate the desorption of p-aminostyrene. Meanwhile, Pd MSs are also highly efficient in selective semi-hydrogenation of various terminal alkynes with different substituents. It is thus expected that robust Pd MSs can be demonstrated as an alternative catalyst design paradigm for other electrochemical hydrogenation reactions. Palladium mesoporous nanospheres are demonstrated as a robust and efficient electrocatalyst for alkyne semi-hydrogenation reactions in water. Thanks to the electron-rich sites in mesopores, this robust electrocatalyst discloses high conversion, remarkable alkenes selectivity, and superior operation stability in semi-hydrogenation of p-aminophenylene. image
Lithium metal batteries (LMBs) attract widespread attention under current high energy density developments. However, wild Li dendrite propagations owing to chaotic Li depositions raise challenges for LMB blossoming. Separators with specific demands thus should be involved when smoothly transferring into LMBs. In this research, a fascinating P(TPC@Lys-Li) separator is prepared by the turbulent interfacial polymerization and electrospinning to ingeniously clarify dependencies of Li+ transfer dynamics on double electric layer thickness (DELT) regulations within porous skeletons. P(TPC@Lys-Li) enables negatively charged porous skeleton surface and compresses DELT, which constructs high-efficiency Li+ fast-transfer channels on porous skeletons and accelerates Li+ transfer speed by 18.3 times. Especially, P(TPC@Lys-Li) supplies extra Li+ for stable formations of solid electrolyte interphase (SEI) layer, homogenizing nucleation and growth behaviors during Li depositions. Remarkable C-rate capacity and cycle stability thus arise for assembled LMBs, holding 87.2 % capacity retention after 700 cycles at 0.5C even under high cathode loading and lean electrolyte conditions. P(TPC@Lys-Li) also maintains constant physical scale and unabated mechanical strength even at elevated temperatures approaching 200 degrees C, which provides excellent battery security as LMBs encounter uncontrollable thermal runaway. Above attractive features enable P(TPC@Lys-Li) separator to be potentially applied in LMBs demanding sufficient security, high-capacity density, and fast charge technology.
To study the effect of molecular structure on ethylene-vinyl alcohol copolymer (EVOH) thermal stability during processing, EVOH samples with different molecular weights and comonomer distributions were prepared by solubility fractionation from two different commercial materials, and then, the structure features of samples were characterized by 1H-NMR, viscometry, differential scanning calorimetry, and, especially, successive self-nucleation and annealing. Their thermal stabilities were further analyzed by isothermal oxygen treatment and thermogravimetry. Attenuated total internal reflectance Fourier transform infrared spectroscopy and UV were used to obverse the structural changes in samples (the formation of chromogenic groups: CO and -CC-). According to the results of isothermal oxygen treatment at 200 degrees C, at the same ethylene content, low-molecular-weight samples have worse thermal stability, which were extremely easy to yellowing and form insoluble gel. To investigate the structure differences between the low-molecular-weight samples, it was found that long vinyl alcohol segments may not worsen the thermal stability in the conditions of the same ethylene content. But samples with a uniform distribution of ethylene segments and a certain length of ethylene segments will have better thermal stability, which makes it more difficult to form carbonyl even diketene conjugation structure. Ethylene-vinyl alcohol copolymer's different degradation degrees under 200 degrees C.image
Hydrogel actuators usually suffer from the poor mechanical property, which hinders their wide applications. In this study, we propose a tough bilayer hydrogel actuator that can respond quickly to temperature. The hydrogels are composed of poly(N-isopropylacylamide) (PNIPAM) layer and poly(acrylamide-co-acrylic acid) (P(AAm-co-AAc)) layer strengthened through Fe3+ complexation with carboxyl groups. By optimizing the PNIPAM content, the resulting bilayer hydrogel P(NIPAM0.9/AAm-co-AAc)-Fe3+ exhibits fast and large-amplitude bending and recovery in response to temperature. It also shows excellent mechanical properties with a tensile strength of 2.54 MPa, tensile modulus of 3.7 MPa, and toughness of 9.4 MJ/m(3), respectively. Besides, the multiple noncovalent interactions within the hydrogels, including Fe+-mediated coordination and hydrogen bonds, can serve as dynamic but stable associations, leading to a good self-healing ability. The bilayer hydrogel is further made into a gripper that can effectively and sensitively respond to temperature to capture and release an object, showing its potential application in artificial intelligent devices.