Traditional statistical prediction methods on PM often focus on a single temporal or spatial dimension, with limited consideration for regional transport interactions among adjacent cities. To address this limitation, we propose a hybrid directed graph neural network method based on deep learning, which utilizes domain features to quantify the influence of neighboring cities and construct a directed graph. The model comprises a historical feature extraction module and a future transmission prediction module, and each module integrates a Graph Neural Network (GNN) and a Long Short-Term Memory Network (LSTM) for spatiotemporal encoding.
View Article and Find Full Text PDFThe internal rotation of triplet-generating molecules is detrimental to room temperature phosphorescence (RTP) radiation, and this rotation is usually mitigated by doping into rigid microenvironments. The chemical locking of internal rotation units in advance should be an effective strategy but is rarely studied in comparison. Herein, a triplet-generating molecule with two rotatable phenyls (DIA) was designed, synthesized, and then cyclized using two types of bonding bridges.
View Article and Find Full Text PDFConcentrated electrolytes based on lithium bis(fluorosulfonyl)imide (LiFSI) have been proposed as an effective Li-compatible electrolyte for anode-free lithium metal batteries (AFLMBs). However, these electrolytes suffer from severe aluminum corrosion at an elevated potential. To address this issue, we propose a binary ionic liquid (IL) electrolyte additive comprising the 1-methyl-1-butyl pyrrolidinium cation (Pyr), difluoro(oxalate)borate anion (DFOB), and difluorophosphate (POF) anion to mitigate the Li inventory loss and Al corrosion in 4 M LiFSI/DME electrolyte simultaneously.
View Article and Find Full Text PDFExploring glass materials beyond inorganic components represents a new direction in the development of artificial transparent materials. Inspired by the successes of polymeric and supramolecular glasses, we shifted our attention to the preparation of a transparent glass through the polymerization of low-molecular-weight monomers that are naturally tailored with noncovalent recognition motifs. In this work, an imidazolium unit bearing a vinyl group and a tetrafluoroborate counter anion was selected to construct an artificial glass.
View Article and Find Full Text PDFIonic gels are emerging as a promising solution for improving the functionality of electrochromic devices. They are increasingly drawing attention in the fields of electrochemistry and functional materials due to their potential to address issues associated with traditional liquid electrolytes, such as volatility, toxicity, and leakage. In extreme scenarios and/or the design of flexible devices, ionic gel electrolytes offer unique and invaluable advantages.
View Article and Find Full Text PDFHyper-crosslinked porous ionic polymers (HCPIPs) have garnered significant attention due to their unique ionic properties and high specific surface areas. However, the limited variety of monomers, low ionic density, and difficulty in functionalization restrict their development. Herein, a series of functionalized non-cationic HCPIPs with high ionic density are designed and directly synthesized an innovative and straightforward approach - anion (and cation) hyper-crosslinking of tetraphenylborate-based ionic liquids (ILs).
View Article and Find Full Text PDFIntegrating anodic biomass valorization with carbon dioxide electroreduction (CORR) can produce value-added chemicals on both the cathode and anode; however, anodic oxidation still suffers from high overpotential. Herein, a photothermal-assisted method was developed to reduce the potential of 5-hydroxymethyl furfural (HMF) electrooxidation. Capitalizing on the copious oxygen vacancies, defective CoO (D-CoO) exhibited a stronger photothermal effect, delivering a local temperature of 175.
View Article and Find Full Text PDFHigh-purity ethylene production from CO electroreduction (CORR) is a coveted, yet arduous feat because the product stream comprises a blend of unreacted CO, H and other off-target CO reduction products. Here we present an indirect reduction strategy for CO-to-ethylene conversion, one that employs 2-bromoethanol (Br-EO) as a mediator. Br-EO is initially generated from CORR and subsequently undergoes reduction to ethylene without the need for energy-intensive separation steps.
View Article and Find Full Text PDFSmart windows always respond to single stimuli, which cannot satisfy various needs in practical applications. Smart windows that integrate thermotropic, electrochromic and power-generating functions in one device is highly challenging yet important in satisfying on-demand light modulation and energy efficiency in practical applications. Herein, a thermoresponsive lower critical solution temperature (LCST) ion gel was fabricated a facile polymerization of butyl acrylate in a conventional ionic liquid to explore "all in one" smart windows.
View Article and Find Full Text PDFThe resistance of adhesives to organic solvents is of paramount importance in diverse industries. Unfortunately, many currently available adhesives exhibit either weak intermolecular chain interactions, resulting in insufficient resistance to organic solvents, or possess a permanent covalent crosslinked network, impeding recyclability. This study introduces an innovative approach to address this challenge by formulating zwitterionic poly(ionic liquid) (ZPIL) derivatives with robust dipole-dipole interactions, incorporating sulfonic anions and imidazolium cations.
View Article and Find Full Text PDFThe advancement of contemporary adhesives is often limited by the balancing act between cohesion and interfacial adhesion strength. This study explores an approach to overcome this trade-off by utilizing the spontaneous polymerization of a protic ionic liquid-based monomer obtained through the neutralization of 2-acrylamide-2-methyl propane sulfonic acid and hydroxylamine. The initiator-free polymerization process is carried out through a gradual increase in monomer concentration in aqueous solutions caused by solvent evaporation upon heating, which results in the in-situ formation of a tough and thin adhesive layer with a highly entangled polymeric network and an intimate interface contact between the adhesive and substrate.
View Article and Find Full Text PDFElectrochromic devices built with ionogel electrolytes are seen as a pivotal step toward the future of quasi-solid electrochromic devices, due to their striking properties like exceptional safety and high ionic conductivity. Yet, the poor mechanical strength of electrolyte of these devices remains a constraint that hampers their advancement. As a resolution, this research explores the use of a robust, transparent ionogel electrolyte, which is designed using an in situ microphase separation strategy.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
July 2024
In this study, Co/Ni-NC catalyst with hetero-diatomic Co/Ni active sites dispersed on nitrogen-doped carbon matrix is synthesized via the controlled pyrolysis of ZIF-8 containing Co and Ni compounds. Experimental characterizations and theoretical calculations reveal that Co and Ni are atomically and uniformly dispersed in pairs of CoN-NiN with an intersite distance ≈0.41 nm, and there is long-range d-d coupling between Co and Ni with more electron delocalization for higher bifunctional activity.
View Article and Find Full Text PDFExploring covalent triazine frameworks (CTFs) with high capacitative activity is highly desirable and challenging. Herein, the S-rich CTFs cathode is pioneeringly introduced in Zn-ion hybrid supercapacitors (ZSC), achieving outstanding capacity and energy density, and satisfactory anti-freezing flexibility. Specifically, the S-bridged CTFs are synthesized by a bifunctional template-catalytic strategy, where ZnCl serves as both the catalyst/solvent and in situ template to construct triazine frameworks with interconnected pores and layered gaps.
View Article and Find Full Text PDFThe in-tandem catalyst holds great promise for addressing the limitation of low *CO coverage on Cu-based materials for selective CH generation during CO electroreduction. However, the potential mismatch between the CO-formation catalyst and the favorable C-C coupling Cu catalyst represents a bottleneck in these types of electrocatalysts, resulting in low tandem efficiencies. In this study, we propose a robust solution to this problem by introducing a wide-CO generation-potential window nickel single atom catalyst (Ni SAC) supported on a Cu catalyst.
View Article and Find Full Text PDFACS Appl Mater Interfaces
October 2023
A brain-like neuromorphic computing system, as compared with traditional Von Neumann architecture, has broad application prospects in the fields of emerging artificial intelligence (AI) due to its high fault tolerance, excellent plasticity, and parallel computing capability. A neuromorphic visuosensory and memory system, an important branch of neuromorphic computing, is the basis for AI to perceive, process, and memorize optical information, now still suffering from nonlinearity of synaptic weight, crosstalk issues, and integration incompatibility, hindering the high-level training and inference accuracy. In this work, we propose a new optoelectronic neuromorphic architecture by integrating an electrochromic device and a perovskite photodetector.
View Article and Find Full Text PDFThe current development of single electrocatalyst with multifunctional applications in overall water splitting (OWS) and zinc-air batteries (ZABs) is crucial for sustainable energy conversion and storage systems. However, exploring new and efficient low-cost trifunctional electrocatalysts is still a significant challenge. Herein, the antiperovskite CuNCo prototype, that is proved to be highly efficient in oxygen evolution reaction but severe hydrogen evolution reaction (HER) performance, is endowed with optimum HER catalytic properties by in situ-derived interfacial engineering via incorporation of molybdenum (Mo).
View Article and Find Full Text PDFAngew Chem Int Ed Engl
September 2023
Balancing the activation of H O is crucial for highly selective CO electroreduction (CO RR), as the protonation steps of CO RR require fast H O dissociation kinetics, while suppressing hydrogen evolution (HER) demands slow H O reduction. We herein proposed one molecular engineering strategy to regulate the H O activation using aprotic organic small molecules with high Gutmann donor number as a solvation shell regulator. These organic molecules occupy the first solvation shell of K and accumulate in the electrical double layer, decreasing the H O density at the interface and the relative content of proton suppliers (free and coordinated H O), suppressing the HER.
View Article and Find Full Text PDFOrganic-doped polymers and room-temperature phosphorescence (RTP) mechanisms have been widely reported. However, RTP lifetimes >3 s are rare and RTP-enhancing strategies are incompletely understood. Herein, we demonstrate a rational molecular doping strategy to obtain ultralong-lived, yet bright RTP polymers.
View Article and Find Full Text PDFCarbon materials (CMs) hold immense potential for applications across a wide range of fields. However, current precursors often confront limitations such as low heteroatom content, poor solubility, or complicated preparation and post-treatment procedures. Our research has unveiled that protic ionic liquids and salts (PILs/PSs), generated from the neutralization of organic bases with protonic acids, can function as economical and versatile small-molecule carbon precursors.
View Article and Find Full Text PDFMain group single atom catalysts (SACs) are promising for CO electroreduction to CO by virtue of their ability in preventing the hydrogen evolution reaction and CO poisoning. Unfortunately, their delocalized orbitals reduce the CO activation to *COOH. Herein, an O doping strategy to localize electrons on p-orbitals through asymmetric coordination of Ca SAC sites (Ca-N O) is developed, thus enhancing the CO activation.
View Article and Find Full Text PDFAnodes based on silicon/carbon composites promise their commercial prospects for next-generation lithium ion batteries owing to their merits of high specific capacity, enhanced ionic and electronic conductivity, and excellent compatibility. Herein, a series of carbonaceous framework/Si composites are designed and prepared by rational waste utilization. N, P codoped foam-like porous carbon/Si composites (FPC@Si) and N, P codoped carbon coated Si composites (NPC@Si) are fabricated by utilizing expired milk powder as a carbon source with facile treatment methods.
View Article and Find Full Text PDFLung adenocarcinoma is the most common subtype of lung cancer clinically, with high mortality and poor prognosis. Cuproptosis present a newly discovered mode of cell death characterized by aggregation of fatty acylated proteins, depletion of iron-sulfur clusterin, triggering of HSP70, and induction of intracellular toxic oxidative stress. However, the impact of cuproptosis on lung adenocarcinoma development, prognosis, and treatment has not been elucidated.
View Article and Find Full Text PDFAtomically dispersed transition metals on carbon-based aromatic substrates are an emerging class of electrocatalysts for the electroreduction of CO. However, electron delocalization of the metal site with the carbon support via d-π conjugation strongly hinders CO activation at the active metal centers. Herein, we introduce a strategy to attenuate the d-π conjugation at single Ni atomic sites by functionalizing the support with cyano moieties.
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