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The integration of chirality, specifically through the chirality-induced spin selectivity (CISS) effect, into electrocatalytic processes represents a pioneering approach for enhancing the efficiency of energy conversion and storage systems. This review delves into the burgeoning field of chiral electrocatalysis, elucidating the fundamental principles, historical development, theoretical underpinnings, and practical applications of the CISS effect across a spectrum of electrocatalytic reactions, including the oxygen evolution reaction (OER), oxygen reduction reaction (ORR), and hydrogen evolution reaction (HER). We explore the methodological advancements in inducing the CISS effect through structural and surface engineering and discuss various techniques for its measurement, from magnetic conductive atomic force microscopy (mc-AFM) to hydrogen peroxide titration. Furthermore, this review highlights the transformative potential of the CISS effect in addressing the key challenges of the NRR and CO2RR processes and in mitigating singlet oxygen formation in metal-air batteries, thereby improving their performance and durability. Through this comprehensive overview, we aim to underscore the significant role of incorporating chirality and spin polarization in advancing electrocatalytic technologies for sustainable energy applications.
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Ultrathin organic nanofibers (UTONFs) represent an emerging class of nanomaterials as they carry a set of favorable attributes, including ultrahigh specific surface area, lightweight, and mechanical flexibility, over inorganic counterparts, for use in biomedicine and nanotechnology. However, precise synthesis of uniform UTONFs (diameter ≤ 2 nm) with tailored functionalities remained challenging. Herein, we report robust multifunctional UTONFs using hydrophobic interaction-driven self-assembly of amphiphilic alternating peptoids containing hydrophobic photoresponsive azobenzene and hydrophilic hydroxyl moieties periodically arranged along the peptoid backbone. Notably, the as-crafted UTONFs are approximately 2 nm in diameter and tens of micrometers in length (an aspect ratio, AR, of â¼10000), exemplifying the UTONFs with the smallest diameter yielded via self-assembly. Intriguingly, UTONFs were disassembled into short-segmented nanofibers and controllably reassembled into UTONFs, resembling "step-growth polymerization". Photoisomerization of azobenzene moieties leads to reversible transformation between UTONFs and spherical micelles. Such meticulously engineered UTONFs demonstrate potential for catalysis, bioimaging, and antibacterial therapeutics. Our study highlights the significance of the rational design of amphiphiles containing alternating hydrophobic and hydrophilic moieties in constructing otherwise unattainable extremely thin UTONFs with ultrahigh AR and stimuli-responsive functionalities for energy and bionanotechnology.
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The growing global energy demand necessitates the development of renewable energy solutions to mitigate greenhouse gas emissions and air pollution. To efficiently utilize renewable yet intermittent energy sources such as solar and wind power, there is a critical need for large-scale energy storage systems (EES) with high electrochemical performance. While lithium-ion batteries (LIBs) have been successfully used for EES, the surging demand and price, coupled with limited supply of crucial metals like lithium and cobalt, raised concerns about future sustainability. In this context, potassium-ion batteries (PIBs) have emerged as promising alternatives to commercial LIBs. Leveraging the low cost of potassium resources, abundant natural reserves, and the similar chemical properties of lithium and potassium, PIBs exhibit excellent potassium ion transport kinetics in electrolytes. This review starts from the fundamental principles and structural regulation of PIBs, offering a comprehensive overview of their current research status. It covers cathode materials, anode materials, electrolytes, binders, and separators, combining insights from full battery performance, degradation mechanisms, in situ/ex situ characterization, and theoretical calculations. We anticipate that this review will inspire greater interest in the development of high-efficiency PIBs and pave the way for their future commercial applications.
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Nonalcoholic fatty liver disease (NAFLD) is a serious disease. There are no specific drugs for it, in part because of the lack of effective models to aid drug development. However, it has been shown that three-dimensional organoid culture systems can reproduce the organ structure and maintain the gene expression profile of the original tissue. Therefore, we aimed to construct NAFLD models from liver organoids for pharmacological and mechanism studies. We successfully observed morphological changes in normal liver tissue in mouse liver organoids with positive albumin (ALB) expression and potential for differentiation toward hepatocyte-like cells. The mRNA expression of the hepatocyte markers ALB and hepatocyte nuclear factor 4 alpha increased after liver organoid differentiation. We observed free fatty acid (FFA)-induced lipid accumulation in organoids with significant increases in alanine aminotransferase, aspartate aminotransferase, total bilirubin, and triglyceride levels. Moreover, FFA-induced inflammatory cytokines (interleukin-6, tumor necrosis factor-α, and nitric oxide) and fibrosis indicators (collagen type I α1 and laminin α1) were also increased. In addition, RNA sequencing results showed that the expression of key genes [nucleotide oligomerization domain-like receptor (NLR) family apoptosis inhibitory protein, interferon regulatory factor (IRF) 3, and IRF7] involved in NAFLD metabolic abnormalities and insulin resistance in the NLR signaling pathway was altered after FFA induction of the liver organoids. Finally, we found that JC2-11 and lanifibranor limited the FFA-induced increase in oil-red lipid droplets, liver damage, inflammation, and liver fibrosis. In conclusion, tissue structure, gene expression, and the response of mouse liver organoids to drugs can partially mimic in vivo liver tissue. Liver organoids can successfully construct NAFLD models for drug discovery research.
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Modelos Animais de Doenças , Fígado , Hepatopatia Gordurosa não Alcoólica , Organoides , Hepatopatia Gordurosa não Alcoólica/metabolismo , Hepatopatia Gordurosa não Alcoólica/patologia , Hepatopatia Gordurosa não Alcoólica/genética , Animais , Organoides/metabolismo , Organoides/efeitos dos fármacos , Organoides/patologia , Fígado/metabolismo , Fígado/patologia , Camundongos , Hepatócitos/metabolismo , Hepatócitos/efeitos dos fármacos , Hepatócitos/patologia , Camundongos Endogâmicos C57BL , Masculino , Diferenciação Celular/efeitos dos fármacos , Ácidos Graxos não Esterificados/farmacologia , Ácidos Graxos não Esterificados/metabolismo , Propionatos , ChalconasRESUMO
Photocatalysis offers a direct, yet robust, approach to eradicate pathogenic bacteria. However, the practical implementation of photocatalytic disinfection faces a significant challenge due to low-efficiency photogenerated carrier separation and transfer. Here, we present an effective approach to improve photocatalytic disinfection performance by exploiting the pyro-phototronic effect through a synergistic combination of pyroelectric properties and photocatalytic processes. A set of comprehensive studies reveals that the temperature fluctuation-induced pyroelectric field promotes photoexcited carrier separation and transfer and thus facilitates the generation of reactive oxygen species and ultimately enhances photocatalytic disinfection performance. It is worth highlighting that the constructed film demonstrated an exceptional antibacterial efficiency exceeding 95% against pathogenic bacteria under temperature fluctuations and light irradiation. Moreover, the versatile modulation role of the pyro-phototronic effect in boosting photocatalytic disinfection was corroborated. This work paves the way for improving photocatalytic disinfection efficiency by harnessing the synergistic potential of various inherent material properties.
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Batteries play a pivotal role in various electrochemical energy storage systems, functioning as essential components to enhance energy utilization efficiency and expedite the realization of energy and environmental sustainability. Zn-based batteries have attracted increasing attention as a promising alternative to lithium-ion batteries owing to their cost effectiveness, enhanced intrinsic safety, and favorable electrochemical performance. In this context, substantial endeavors have been dedicated to crafting and advancing high-performance Zn-based batteries. However, some challenges, including limited discharging capacity, low operating voltage, low energy density, short cycle life, and complicated energy storage mechanism, need to be addressed in order to render large-scale practical applications. In this review, we comprehensively present recent advances in designing high-performance Zn-based batteries and in elucidating energy storage mechanisms. First, various redox mechanisms in Zn-based batteries are systematically summarized, including insertion-type, conversion-type, coordination-type, and catalysis-type mechanisms. Subsequently, the design strategies aiming at enhancing the electrochemical performance of Zn-based batteries are underscored, focusing on several aspects, including output voltage, capacity, energy density, and cycle life. Finally, challenges and future prospects of Zn-based batteries are discussed.
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One-dimensional metal halide perovskites are among the most promising candidate materials for optoelectronic devices. However, the heterogeneity and fast degradation of perovskite nanowires (NWs) and nanorods (NRs) synthesized using conventional approaches impose a bottleneck for their optoelectronic applications. Recently, all-inorganic perovskite CsPbBr3 NRs with tailored dimensions, crafted using an amphiphilic bottlebrush-like block copolymer (BBCP) as nanoreactors, have demonstrated enhanced stabilities. Herein, we report the electronic investigation into these template-grown CsPbBr3 NRs using dielectric force microscopy (DFM), a contactless, nondestructive imaging technique. All freshly prepared CsPbBr3 NRs exhibited ambipolar behaviors for up to two months after sample synthesis. A transition from ambipolar to p-type behaviors occurred after two months, and nearly all NRs completed the transition within two weeks. Moreover, template-grown CsPbBr3 NRs displayed better nanoscale electronic homogeneity compared to their conventional counterparts. The improved electronic uniformity and nanoscale homogeneity place the template-grown CsPbBr3 NRs in a unique advantageous position for optoelectronic applications.
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Environmentally friendly crosslinked polymer networks feature degradable covalent or non-covalent bonds, with many of them manifesting dynamic characteristics. These attributes enable convenient degradation, facile reprocessibility, and self-healing capabilities. However, the inherent instability of these crosslinking bonds often compromises the mechanical properties of polymer networks, limiting their practical applications. In this context, environmentally friendly dual-crosslinking polymer networks (denoted EF-DCPNs) have emerged as promising alternatives to address this challenge. These materials effectively balance the need for high mechanical properties with the ability to degrade, recycle, and/or self-heal. Despite their promising potential, investigations into EF-DCPNs remain in their nascent stages, and several gaps and limitations persist. This Review provides a comprehensive overview of the synthesis, properties, and applications of recent progress in EF-DCPNs. Firstly, synthetic routes to a rich variety of EF-DCPNs possessing two distinct types of dynamic bonds (i.e., imine, disulfide, ester, hydrogen bond, coordination bond, and other bonds) are introduced. Subsequently, complex structure- and dynamic nature-dependent mechanical, thermal, and electrical properties of EF-DCPNs are discussed, followed by their exemplary applications in electronics and biotechnology. Finally, future research directions in this rapidly evolving field are outlined.
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Memristors offer a promising solution to address the performance and energy challenges faced by conventional von Neumann computer systems. Yet, stochastic ion migration in conductive filament often leads to an undesired performance tradeoff between memory window, retention, and endurance. Herein, a robust memristor based on oxygen-rich SnO2 nanoflowers switching medium, enabled by seed-mediated wet chemistry, to overcome the ion migration issue for enhanced analog in-memory computing is reported. Notably, the interplay between the oxygen vacancy (Vo) and Ag ions (Ag+) in the Ag/SnO2/p++-Si memristor can efficiently modulate the formation and abruption of conductive filaments, thereby resulting in a high on/off ratio (>106), long memory retention (10-year extrapolation), and low switching variability (SV = 6.85%). Multiple synaptic functions, such as paired-pulse facilitation, long-term potentiation/depression, and spike-time dependent plasticity, are demonstrated. Finally, facilitated by the symmetric analog weight updating and multiple conductance states, a high image recognition accuracy of ≥ 91.39% is achieved, substantiating its feasibility for analog in-memory computing. This study highlights the significance of synergistically modulating conductive filaments in optimizing performance trade-offs, balancing memory window, retention, and endurance, which demonstrates techniques for regulating ion migration, rendering them a promising approach for enabling cutting-edge neuromorphic applications.
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Durable superhydrophobic anti-erosion/anticorrosion coatings are highly demanded across various applications. However, achieving coatings with exceptional superhydrophobicity, mechanical strength, and corrosion resistance remains a grand challenge. Herein, a robust microstructure coating, inspired by the cylindrical structures situated on the surface of conch shell, for mitigating erosion and corrosion damages in gas transportation pipelines is reported. Specifically, citric acid monohydrate as a pore-forming agent is leveraged to create a porous structure between layers, effectively buffering the impact on the surface. As a result, the coating demonstrates remarkable wear resistance and water repellency. Importantly, even after abrasion by sandpaper and an erosion loop test, the resulting superhydrophobic surfaces retain the water repellency. The design strategy offers a promising route to manufacturing multifunctional materials with desired features and structural complexities, thereby enabling effective self-cleaning and antifouling abilities in harsh operating environments for an array of applications, including self-cleaning windows, antifouling coatings for medical devices, and anti-erosion/anticorrosion protection, among other areas.
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The growing demand for high energy storage materials has garnered substantial attention towards lead-free ferroelectric nanocrystals (NCs), such as BaTiO3 (BTO), for next-generation multilayer ceramic capacitors. Notably, it remains challenging to accurately measure the dielectric constant and polarization-electric field (P-E) hysteresis loop for BTO NCs. Herein, we report on nonlinear ferroelectric characteristics of BTO NCs via a polymer nanocomposite approach. Specifically, poly(vinyl pyrrolidone) (PVP)/BTO nanocomposite films of 3-10 µm thickness, containing 380 nm tetragonal-phased and 60 nm cubic-phased BTO NCs with uniform particle dispersion, were prepared. Theoretical deconvolution of the broad experimental P-E loops of the PVP/BTO NC composite films revealed three contributions, that is, the linear deformational polarization of the nanocomposites, the polarization of BTO NCs (Pp), and the polarization from strong particle-particle interactions. Using different mixing rules and nonlinear dielectric analysis, the overall dielectric constants of BTO NCs were obtained, from which the internal field in the BTO NCs (Ep) was estimated. Consequently, the Pp-Ep hysteresis loops were obtained for the BTO380 and BTO60 NCs. Interestingly, BTO380 exhibited square-shaped ferroelectric loops, whereas BTO60 displayed slim paraelectric loops. This work presents a robust and versatile route to extract the Pp-Ep loops of ferroelectric NCs from polymer/ceramic nanocomposites.
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The ability to pattern semiconducting conjugated polymers (CPs) and concurrently enable their highly oriented chains represents an important endeavor to render their high charge mobility for electronic devices. However, simple yet generalizable routes to CPs with such desirable characteristics are limited. Herein, we report a robust meniscus-assisted solution printing (MASP) strategy to craft arrays of donor-acceptor CP stripes and scrutinize the correlation between different stripes and their charge transport attributes. Specifically, the MASP constrains the CP solution to evaporate between two nearly parallel plates with a stationary upper plate and a mobile lower plate containing periodic photoresist (PR) microchannels. Orchestrating the MASP speed comparable to the CP crystal growth rate yields CP stripe arrays with highly aligned CP crystals, resulting in the highest carrier mobility. Notably, our MASP technique can conveniently pattern other CPs of interest. It stands out as a simple strategy to impart large-scale production of functional materials for a wide range of applications in optics, electronics, sensors, etc.
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The ability to create perovskite-based heterostructures with desirable charge transfer characteristics represents an important endeavor to render a set of perovskite materials and devices with tunable optoelectronic properties. However, due to similar material selection and band alignment in type-II and Z-scheme heterostructures, it remains challenging to obtain perovskite-based heterostructures with a favorable electron transfer pathway for photocatalysis. Herein, we report a robust tailoring of effective charge transfer pathway in perovskite-based heterostructures via a type-II to Z-scheme transformation for highly efficient and selective photocatalytic CO2 reduction. Specifically, CsPbBr3/TiO2 and CsPbBr3/Au/TiO2 heterostructures are synthesized and then investigated by ultrafast spectroscopy. Moreover, taking CsPbBr3/TiO2 and CsPbBr3/Au/TiO2 as examples, operando experiments and theoretical calculations confirm that the type-II heterostructure could be readily transformed into a Z-scheme heterostructure through establishing a low-resistance Ohmic contact, which indicates that a fast electron transfer pathway is crucial in Z-scheme construction, as further demonstrated by CsPbBr3/Ag/TiO2 and CsPbBr3/MoS2 heterostructures. In contrast to pristine CsPbBr3 and CsPbBr3/TiO2, the CsPbBr3/Au/TiO2 heterostructure exhibits 5.4- and 3.0-fold enhancement of electron consumption rate in photocatalytic CO2 reduction. DFT calculations and in situ diffuse reflectance infrared Fourier transform spectroscopy unveil that the superior CO selectivity is attributed to the lower energy of *CO desorption than that of hydrogenation to *HCO. This meticulous design sheds light on the modification of perovskite-based multifunctional materials and enlightens conscious optimization of semiconductor-based heterostructures with desirable charge transfer for catalysis and optoelectronic applications.
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3D raspberry-like core/satellite nanostructures were prepared by controlled surface functionalization of silica spheres using crosslinked poly(4-vinylpyridine) (P4VP) chains with known binding affinity for gold nanoparticles (AuNPs). The 3D SiO2-g-P(4VP-co-DVB)/AuNP nanoraspberries can be further transformed into 2D plasmonic nanoclusters by etching the silica core with hydrofluoric acid (HF). After the transformation, the interparticle distance between the AuNPs dramatically reduced from a 10 nm scale to sub 2 nm. Owing to the strong electromagnetic field generated by the plasmonic coupling between AuNPs in very close proximity, the established P(4VP-co-DVB)/AuNP nanoclusters provided strong and undisturbed Raman signals as a SERS substrate. In addition, benefiting from the stabilizing effect of the crosslinked P(4VP-co-DVB) network, the prepared SERS substrate has the advantages of good uniformity, stability and reproducibility, as well as strong SERS enhancement, endowing it with great potential for rapid and efficient SERS detection.
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Single-atom catalysts (SACs) hold immense promise in facilitating the rational use of metal resources and achieving atomic economy due to their exceptional atom-utilization efficiency and distinct characteristics. Despite the growing interest in SACs, only limited reviews have holistically summarized their advancements centering on performance metrics. In this review, first, a thorough overview on the research progress in SACs is presented from a performance perspective and the strategies, advancements, and intriguing approaches employed to enhance the critical attributes in SACs are discussed. Subsequently, a comprehensive summary and critical analysis of the electrochemical applications of SACs are provided, with a particular focus on their efficacy in the oxygen reduction reaction , oxygen evolution reaction, hydrogen evolution reaction , CO2 reduction reaction, and N2 reduction reaction . Finally, the outline future research directions on SACs by concentrating on performance-driven investigation, where potential areas for improvement are identified and promising avenues for further study are highlighted, addressing challenges to unlock the full potential of SACs as high-performance catalysts.
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Single-atom catalysts manifest nearly 100 % atom utilization efficiency, well-defined active sites, and high selectivity. However, their practical applications are hindered by a low atom loading density, uncontrollable location, and ambiguous interaction with the support, thereby posing challenges to maximizing their electrocatalytic performance. To address these limitations, the ability to arrange randomly dispersed single atoms into locally ordered single-atom catalysts (LO-SACs) substantially influences the electronic effect between reactive sites and the support, the synergistic interaction among neighboring single atoms, the bonding energy of intermediates with reactive sites and the complexity of the mechanism. As such, it dramatically promotes reaction kinetics, reduces the energy barrier of the reaction, improves the performance of the catalyst and simplifies the reaction mechanism. In this review, firstly, we introduce a variety of compelling characteristics of LO-SACs as electrocatalysts. Subsequently, the synthetic strategies, characterization methods and applications of LO-SACs in electrocatalysis are discussed. Finally, the future opportunities and challenges are elaborated to encourage further exploration in this rapidly evolving field.
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Iron-modified Ni(OH)2/NiSe2 enhances oxygen vacancies, expanding the electrochemically active surface area, which exhibiting superior selectivity and stability in urea oxidation reaction, outperforming pristine Ni(OH)2@NiSe2. It also demonstrates superior catalytic performance in the oxidation reactions of other small molecules.
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Background: Liver cancer, especially hepatocellular carcinoma (HCC), remains a significant global health challenge. Traditional prognostic indicators for HCC often fall short in providing comprehensive insights for individualized treatment. The integration of genomics and radiomics offers a promising avenue for enhancing the precision of HCC diagnosis and prognosis. Methods: From the Cancer Genome Atlas (TCGA) database, we categorized mRNA of HCC patients by Forkhead Box M1 (FOXM1) expression and performed univariate and multivariate studies to pinpoint autonomous HCC risk factors. We deployed subgroup, correlation, and interaction analyses to probe FOXM1's link with clinicopathological elements. The connection between FOXM1 and immune cells was evaluated using the CIBERSORTx database. The functions of FOXM1 were investigated through analyses of Gene Ontology (GO) and the Kyoto Encyclopedia of Genes and Genomes (KEGG). After filtering through TCGA and the Cancer Imaging Archive (TCIA) database, we employed dual-region computed tomography (CT) radiomics technology to noninvasively predict the mRNA expression of FOXM1 in HCC tissues. Radiomic features were extracted from both tumoral and peritumoral regions, and a radiomics score (RS) was derived. The performance and robustness of the constructed models were evaluated using 10-fold cross-validation. A radiomics nomogram was developed by incorporating RS and clinical variables from the TCGA database. The models' discriminative abilities were assessed using metrics such as the area under the curve (AUC) of the receiver operating characteristic curves (ROC) and precision-recall (PR) curves. Results: Our findings emphasized the overexpression of FOXM1 as a determinant of poor prognosis in HCC and illustrated its impact on immune cell infiltration. After selecting arterial phase CT, we chose 7 whole-tumor features and 3 features covering both the tumor and its surroundings to create WT and WP models for FOXM1 prediction. The WT model showed strong predictive capabilities for FOXM1 expression by PR curve. Conversely, the WP model did not demonstrate the good predictive ability. In our study, the radiomics score (RS) was derived from whole-tumor regions on CT images. The RS was significantly associated with FOXM1 expression, with an AUC of 0.918 in the training cohort and 0.837 in the validation cohort. Furthermore, the RS was correlated with oxidative stress genes and was integrated with clinical variables to develop a nomogram, which demonstrated good calibration and discrimination in predicting 12-, 36-, and 60-month survival probabilities. Additionally, bioinformatics analysis revealed FOXM1's potential role in shaping the immune microenvironment, with its expression linked to immune cell infiltration. Conclusion: This study highlights the potential of integrating FOXM1 expression and radiomics in understanding HCC's complexity. Our approach offers a new perspective in utilizing radiomics for non-invasive tumor characterization and suggests its potential in providing insights into molecular profiles. Further research is needed to validate these findings and explore their clinical implications in HCC management.
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The past decade has witnessed the great potential of Fe-based single-atom electrocatalysis in catalyzing oxygen reduction reaction (ORR). However, it remains a grand challenge to substantially improve their intrinsic activity and long-term stability in acidic electrolytes. Herein, we report a facile chemical vapor deposition strategy, by which high-density Fe atoms (3.97â wt%) are coordinated with square-planar para-positioned nitrogen and phosphorus atoms in a hierarchical carbon framework. The as-crafted atomically dispersed Fe catalyst (denoted Fe-SA/PNC) manifests an outstanding activity towards ORR over the entire pH range. Specifically, the half-wave potential of 0.92â V, 0.83â V, and 0.86â V vs. reversible hydrogen electrode (RHE) are attained in alkaline, neutral, and acidic electrolytes, respectively, representing the high performance among reported catalysts to date. Furthermore, after 30,000 durability cycles, the Fe-SA/PNC remains to be stable with no visible performance decay when tested in 0.1â M KOH and 0.5â M H2 SO4 , and only a minor negative shift of 40â mV detected in 0.1â M HClO4 , significantly outperforming commercial Pt/C counterpart. The coordination motif of Fe-SA/PNC is validated by density functional theory (DFT) calculations. This work provides atomic-level insight into improving the activity and stability of non-noble metal ORR catalysts, opening up an avenue to craft the desired single-atom electrocatalysts.
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Despite stunning progress in single-atom catalysis (SAC), it remains a grand challenge to yield a high loading of single atoms (SAs) anchored on substrates. Herein, we report a one-step laser-planting strategy to craft SAs of interest under an atmospheric temperature and pressure on various substrates including carbon, metals, and oxides. Laser pulses render concurrent creation of defects on the substrate and decomposition of precursors into monolithic metal SAs, which are immobilized on the as-produced defects via electronic interactions. Laser planting enables a high defect density, leading to a record-high loading of SAs of 41.8 wt %. Our strategy can also synthesize high-entropy SAs (HESAs) with the coexistence of multiple metal SAs, regardless of their distinct characteristics. An integrated experimental and theoretical study reveals that superior catalytic activity can be achieved when the distribution of metal atom content in HESAs resembles the distribution of their catalytic performance in a volcano plot of electrocatalysis. The noble-metal mass activity for a hydrogen evolution reaction within HESAs is 11-fold over that of commercial Pt/C. The laser-planting strategy is robust, opening up a simple and general route to attaining an array of low-cost, high-density SAs on diverse substrates under ambient conditions for electrochemical energy conversion.