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Heavy metal ion wastewater is a pressing and inescapable issue that is closely related to human health and ecological security due to its toxicity, carcinogenicity, and the unmanageable property of this type of wastewater. Metal-Organic Frameworks (MOFs) are a class of crystalline nanoporous materials with flexible designability and controllability, showing great potential in the field of adsorption and purification of heavy metals in wastewater. In this Perspective, we first discuss the harm of different heavy metal ions and briefly expound virtues of MOFs for pollutant adsorption. Then, we mainly summarize the recent advances in the construction of different metal-based MOFs (Zr-based, Zn-based, Co-based, Al-based, etc.) and their research progress in heavy metal ions adsorption. Furthermore, various types of MOF additives can often be effectively applied for heavy metal ion adsorption by functional modification or with other materials composition. Additionally, several commonly used adsorption kinetics and isotherm models are also detailed to help an in-depth understanding of the adsorption mechanism. Finally, the challenges and opportunities of MOFs for heavy metal ion adsorption are additionally discussed, and this review may provide new insight for other potential water purification applications.
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Visualizing the decision-making process is a key aspect of research regarding explainable arrhythmia recognition. This study proposed a visualized lead selection method to classify arrhythmia for multi-lead ECG signals. The proposed method has several advantages, as it uses a visualized approach to select effective leads, avoiding redundant leads and invalid information. It also captures the temporal dependencies of ECG signals and the complementary information between leads. The method deployed a lead activation heatmap (LA heatmap) based on a lead-wise network to select the proper 5 leads from 12-lead ECG heartbeats extracted from the public 2018 Chinese Physiological Signal Challenge database (CPSC 2018 DB), which were then fed into a ResBiTime network combining bidirectional long short-term memory (Bi-LSTM) networks and residual connections for a classification task of nine heartbeat categories (i.e., N, AF, I-AVB, RBBB, PAC, PVC, STD, LBBB, and STE). The results indicate an average precision of 93.25%, an average recall of 93.03%, an average F1-score of 0.9313, and that the proposed method can effectively extract additional information from ECG heartbeat data.
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Prognostic risk prediction is pivotal for clinicians to appraise the patient's esophageal squamous cell cancer (ESCC) progression status precisely and tailor individualized therapy treatment plans. Currently, CT-based multi-modal prognostic risk prediction methods have gradually attracted the attention of researchers for their universality, which is also able to be applied in scenarios of preoperative prognostic risk assessment in the early stages of cancer. However, much of the current work focuses only on CT images of the primary tumor, ignoring the important role that CT images of lymph nodes play in prognostic risk prediction. Additionally, it is important to consider and explore the inter-patient feature similarity in prognosis when developing models. To solve these problems, we proposed a novel multi-modal population-graph based framework leveraging CT images including primary tumor and lymph nodes combined with clinical, hematology, and radiomics data for ESCC prognostic risk prediction. A patient population graph was constructed to excavate the homogeneity and heterogeneity of inter-patient feature embedding. Moreover, a novel node-level multi-task joint loss was proposed for graph model optimization through a supervised-based task and an unsupervised-based task. Sufficient experimental results show that our model achieved state-of-the-art performance compared with other baseline models as well as the gold standard on discriminative ability, risk stratification, and clinical utility. The core code is available at https://github.com/wuchengyu123/MPGSurv.
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Membranes with ultrafast molecular separation ability in organic solvents can offer unprecedented opportunities for efficient and low-cost solvent recovery in industry. Herein, a graphene-like polymer carbon nitride nanosheet (PCNN) with a low-friction surface was applied as the main membrane building block to boost the ultrafast transport of the solvent. Meanwhile, inspired by the concept of "couple hardness with softness", soft and flexible graphene oxide (GO) was chosen to fix the random stack of the rigid PCNN and tailor the lamellar structure of the PCNN membrane. The optimal PCNN/GO lamellar membrane shows a remarkable methanol permeance of 435.5 L m-2 h-1 bar-1 (four times higher than that of the GO membrane) while maintaining a high rejection for reactive black (RB, 98.9% in ethanol). Molecular dynamics simulations were conducted to elucidate the ultrafast transport mechanism of the PCNN/GO membrane. This study reveals that PCNN is a promising building block for lamellar membranes and may open up new avenues for high-performance molecular separation membranes.
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The directional arrangement of H2O molecules can effectively regulate the ordered protons transfer to improve transport efficiency, which can be controlled by the interaction between materials and H2O. Herein, a strategy to build a stable hydration layer in metal-organic framework (MOF) platforms, in which hydrophilic centers that can manipulate H2O molecules are implanted into MOF cavities is presented. The rigid grid-Ni-MOF is selected as the supporting material due to the uniformly distributed cavities and rigid structures. The Ag0 possesses potential combination ability with the hydrophilic substances, so it is introduced into the MOF as hydration layer centers. Relying on the strong interaction between Ag0 and H2O, the H2O molecules can rearrange around Ag0 in the cavity, which is intuitively verified by DFT calculation and molecular dynamics simulation. The establishment of a hydration layer in Ag@Ni-MOF regulates the chemical properties of the material and gives the material excellent proton conduction performance, with a proton conductivity of 4.86 × 10-2 S cm-1.
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Aggregation of filler particles during the formation of mixed matrix membranes is difficult to avoid when filler loadings exceed a 10-15â wt %. Such agglomeration usually leads to poor membrane performance. In this work, using a ZIF-67 metal-organic framework (MOF) as filler along with surface modification of Ag4 tz4 to improve processability and selective olefin adsorption, we demonstrate that highly loaded with a very low agglomeration degree membranes can be synthesized displaying unmatched separation selectivity (39) for C3 H6 /C3 H8 mixtures and high permeability rates (99â Barrer), far surpassing previous reports in the literature. Through molecular dynamics simulation, the enhanced compatibility between ZIF-67 and polymer matrix with adding Ag4 tz4 was proven and the tendency in gas permeability and C3 H6 selectivity in the mixed matrix membranes (MMMs) were well explained. More importantly, the membrane showed a wide range of pressure and temperature resistance, together with remarkable long-term stability (>900â h). The modification method might help solve interface issues in MMMs and can be extended to the fabrication of other fillers to achieve high performance MMMs for gas separation.
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Nanosheets derived from two-dimensional covalent organic frameworks (2D COFs) are increasingly desirable in various fields. While breakthroughs in the chemical and physical delamination of 2D COFs are rising, precisely regulating the growth of the COF nanosheets has not been realized yet. Herein, we report an effective strategy of polymer-manipulated crystallization to accurately control the growth of COF nanosheets. Chemically asymmetric polyvinylpyrrolidone (PVP) is developed as the manipulator that selectively interacts with the aldehydes and (100) facet to induce anisotropic growth of COFs. The number of PVP constitutional units determines this specific interaction, leading to molecularly thin but thickness-controllable nanosheets with excellent dispersity. We process these nanosheets into robust A4-sized membranes for ultraselective molecular separation. The membrane intercalated with long-chain PVP demonstrates largely improved performance, surpassing the reported COF membranes. This work reports a strategy for anisotropically crystallizing 2D COFs to yield processable nanosheets toward practical applications.
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Vaccinium duclouxii, endemic to southwestern China, is a berry-producing shrub or small tree belonging to the Ericaceae family, with high nutritive, medicinal, and ornamental value, abundant germplasm resources, and good edible properties. In addition, V. duclouxii exhibits strong tolerance to adverse environmental conditions, making it a promising candidate for research and offering wide-ranging possibilities for utilization. However, the lack of V. duclouxii genome sequence has hampered its development and utilization. Here, a high-quality telomere-to-telomere genome sequence of V. duclouxii was de novo assembled and annotated. All of 12 chromosomes were assembled into gap-free single contigs, providing the highest integrity and quality assembly reported so far for blueberry. The V. duclouxii genome is 573.67 Mb, which encodes 41 953 protein-coding genes. Combining transcriptomics and metabolomics analyses, we have uncovered the molecular mechanisms involved in sugar and acid accumulation and anthocyanin biosynthesis in V. duclouxii. This provides essential molecular information for further research on the quality of V. duclouxii. Moreover, the high-quality telomere-to-telomere assembly of the V. duclouxii genome will provide insights into the genomic evolution of Vaccinium and support advancements in blueberry genetics and molecular breeding.
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Ceramic membranes have been increasingly employed in water treatment owing to their merits such as high-stability, anti-oxidation, long lifespan and environmental friendliness. The application of ceramic membranes mainly focuses on microfiltration and ultrafiltration processes, and some precise separation can be achieved by introducing novel porous materials with superior selectivity. Recently, metal-organic frameworks (MOFs) have developed a wide spectrum of applications in the fields of the environment, energy, water treatment and gas separation due to the diversity and tunable advantages of metal clusters and organic ligands. Although the issue of water stability in MOF materials inhibits the development of MOF membranes in water treatment, researchers still overcome many obstacles to advance the application of MOF membranes in water treatment processes. To the best of our knowledge, there is still a lack of a reviews on the development process and prospects of ceramic-based MOF membranes for water treatment. Therefore, in this review, we mainly summarize the fabrication method for ceramic-based MOF membranes and their application in water treatment, such as water/salt separation, pollutant separation, heavy metal separation, etc. Following this, based on the high structural, thermal and chemical stability of ceramic substrates, and the high controllability of MOF materials, the superiority and insufficient use of ceramic-based MOF membranes in the field of water treatment are critically discussed.
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Solar-driven interfacial evaporation harnessing solar energy on a water surface provides a sustainable and economic means to efficiently capture freshwater from nontraditional water sources. Endowed with a hierarchical porous structure and mechanical stability, wood-based evaporators represent a renewable alternative to petroleum-based materials. Nonetheless, incidental inferiorities of a low evaporation rate and weak interfacial strength are challenging to overcome. Herein, we propose the usage of chemically stable coordination polymers (Ni-dithiooxamidato, Ni-DTA) as hydrophilic photothermal nanomaterials for the molecular design of robust wood-based evaporators with improved performance. In situ synthesis of Ni-DTA onto the channel wall of balsawood provides sufficient photothermal domains that localize the converted energy for facilitated interfacial evaporation. A rational control of methanol/dimethylformamide ratios enables the coexistence of 1D-nanofibers and 0D-nanoparticles, endowing Balsa-NiDTA with a high evaporation rate of 2.75 kg m-2 h-1 and an energy efficiency of 82% under one-sun illumination. Experimental and simulation results reveal that Ni-DTA polymers with strong hydration ability decrease the equivalent evaporation enthalpy induced by decreased H-bonding density of water molecules near the evaporation interface. The Balsa-NiDTA evaporator showed a high chemical stability, mainly due to the robust Ni-S/Ni-N bonds and the superior cellulose affinity of Ni-DTA. Furthermore, the Balsa-NiDTA evaporator shows an excellent antibacterial activity and low oil-fouling propensity. This work presents a facile and mild strategy to design chemically stable wood-based evaporators, contributing to highly efficient and sustainable solar desalination under harsh conditions.
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Membranes with ultrapermeability for CO2 are desired for future large-scale carbon capture projects, because of their excellent separative productivity and economic efficiency. Herein, we demonstrate that a membrane with ultrapermeability for CO2 can be constructed by combining N/O para-doped noble carbons, C2NxO1-x, with high-permeability polymer PIM-1. The optimal PIM-1/C2NxO1-x membranes exhibit superior CO2 permeability (22110 Barrer) with a CO2/N2 selectivity of 15.5, and an unprecedented CO2 permeability of 37272 Barrer can be obtained after a PEG activation treatment, far surpassing the 2008 upper bound. Both broad experiments and molecular dynamics simulations reveal that the numerous ordered polar channels of C2NxO1-x and their excellent compatibility with PIM-1 are responsible for the superior CO2 separation performance of the membrane. Although this is the first study on C2N-type gas separation membranes, the outstanding results indicate that noble carbon building blocks may pave a new avenue to advance high-performance CO2 separation membranes.
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Covalent organic frameworks (COFs) have showcased great potential in diverse applications such as separation and catalysis, where mass transfer confined in their pore channels plays a significant role. However, anisotropic orientation usually occurs in polycrystalline COFs, and perpendicular alignment of COF pore channels is ultimately desired to maximize their performance. Herein, we demonstrate a strategy, solvent vapor annealing, to reorient COF pore channels from anisotropic orientation to perpendicular alignment. COF thin films are first synthesized to have flexible N-H bonds in their skeletons, thus having structural mobility to enable molecular rearrangement. A solvent with low relative permittivity and a conjugated structure is then identified to have a strong affinity toward the COFs, allowing its vapor to easily penetrate into the COF interlayers. The solvent vapor weakens the π-π interaction and consequently allows the COF monolayers to dissociate. The COF monolayers undergo a reorientation process that converts from random stacking into the face-on stacking fashion, in which the through COF pores are perpendicularly aligned. The aligned COF film exhibits high separation precision toward ions featuring a size difference down to 2 Å, which is 8 times higher than that of the anisotropically oriented counterpart. This work opens up an avenue for COF orientation regulation by solvent vapor annealing and reveals the essential role of the perpendicular alignment of COF pore channels to enable precision separations.
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BACKGROUND AND OBJECTIVE: Automatic recognition of wearable dynamic electrocardiographic (ECG) signals is a difficult problem in biomedical signal processing. However, with the widespread use of long-range ambulatory ECG, a large number of real-time ECG signals are generated in the clinic, and it is very difficult for clinicians to perform timely atrial fibrillation (AF) diagnosis. Therefore, developing a new AF diagnosis algorithm can relieve the pressure on the healthcare system and improve the efficiency of AF screening. METHODS: In this study, a self-complementary attentional convolutional neural network (SCCNN) was designed to accurately identify AF in wearable dynamic ECG signals. First, a 1D ECG signal was converted into a 2D ECG matrix using the proposed Z-shaped signal reconstruction method. Then, a 2D convolutional network was used to extract shallow information from adjacent sampling points at close distances and interval sampling points at distant distances in the ECG signal. The self-complementary attention mechanism (SCNet) was used to focus and fuse channel information with spatial information. Finally, fused feature sequences were used to detect AF. RESULTS: The accuracies of the proposed method on the three public databases were 99.79%, 95.51%, and 98.80%. The AUC values were 99.79%, 95.51%, and 98.77%, respectively. The sensitivity on the clinical database was as high as 99.62%. CONCLUSIONS: These results show that the proposed method can accurately identify AF and has good generalization.
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Fibrilação Atrial , Humanos , Fibrilação Atrial/diagnóstico , Eletrocardiografia/métodos , Redes Neurais de Computação , Algoritmos , Eletrocardiografia AmbulatorialRESUMO
One scalable and facile dip-coating approach was utilized to construct a thin CO2-selection layer of Pebax/PEGDA-MXene on a hollow fiber PVDF substrate. An interlayer spacing of 3.59 Å was rationally designed and precisely controlled for the MXene stacks in the coated layer, allowing efficient separation of the CO2 (3.3 Å) from N2 (3.6 Å) and CH4 (3.8 Å). In addition, CO2-philic nanodomains in the separation layer were constructed by grafting PEGDA into MXene interlayers, which enhanced the CO2 affinity through the MXene interlayers, while non-CO2-philic nanodomains could promote CO2 transport due to the low resistance. The membrane could exhibit optimal separation performance with a CO2 permeance of 765.5 GPU, a CO2/N2 selectivity of 54.5, and a CO2/CH4 selectivity of 66.2, overcoming the 2008 Robeson upper bounds limitation. Overall, this facile approach endows a precise controlled molecular sieving MXene membrane for superior CO2 separation, which could be applied for interlayer spacing control of other 2D materials during membrane construction.
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The application of membrane-based separation processes for propylene/propane (C3 H6 /C3 H8 ) is extremely promising and attractive as it is poised to reduce the high operation cost of the established low temperature distillation process, but major challenges remain in achieving high gas selectivity/permeability and long-term membrane stability. Herein, a C3 H6 facilitated transport membrane using trisilver pyrazolate (Ag3 pz3 ) as a carrier filler is reported, which is uniformly dispersed in a polymer of intrinsic microporosity (PIM-1) matrix at the molecular level (≈15 nm), verified by several analytical techniques, including 3D-reconstructed focused ion beam scanning electron microscropy (FIB-SEM) tomography. The π-acidic Ag3 pz3 combines preferentially with π-basic C3 H6 , which is confirmed by density functional theory calculations showing that the silver ions in Ag3 pz3 form a reversible π complex with C3 H6 , endowing the membranes with superior C3 H6 affinity. The resulting membranes exhibit superior stability, C3 H6 /C3 H8 selectivity as high as ≈200 and excellent C3 H6 permeability of 306 Barrer, surpassing the upper bound selectivity/permeability performance line of polymeric membranes. This work provides a conceptually new approach of using coordinatively unsaturated 0D complexes as fillers in mixed matrix membranes, which can accomplish olefin/alkane separation with high performance.
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Detecting atrial fibrillation (AF) of short single-lead electrocardiogram (ECG) with low signal-to-noise ratio (SNR) is a key of the wearable heart monitoring system. This study proposed an AF detection method based on feature fusion to identify AF rhythm (A) from other three categories of ECG recordings, that is, normal rhythm (N), other rhythm (O), and noisy (â¼) ECG recordings. So, the four categories, that is, N, A, O, and â¼ were identified from the database provided by PhysioNet/CinC Challenge 2017. The proposed method first unified the 9 to 60 seconds unbalanced ECG recordings into 30 s segments by copying, cutting, and symmetry. Then, 24 artificial features including waveform features, interval features, frequency-domain features, and nonlinear feature were extracted relying on prior knowledge. Meanwhile, a 13-layer one-dimensional convolutional neural network (1-D CNN) was constructed to yield 38 abstract features. Finally, 24 artificial features and 38 abstract features were fused to yield the feature matrix. Random forest was employed to classify the ECG recordings. In this study, the mean accuracy (Acc) of the four categories reached 0.857. The F 1 of N, A, and O reached 0.837. The results exhibited the proposed method had relatively satisfactory performance for identifying AF from short single-lead ECG recordings with low SNR.
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Fibrilação Atrial , Humanos , Fibrilação Atrial/diagnóstico , Razão Sinal-Ruído , Processamento de Sinais Assistido por Computador , Redes Neurais de Computação , Monitorização Fisiológica , Eletrocardiografia/métodos , AlgoritmosRESUMO
Thin film nanocomposite (TFN) membranes have proven their unrivaled value, as they can combine the advantages of different materials and furnish membranes with improved selectivity and permeability. The development of TFN membranes has been severely limited by the poor dispersion of the nanoparticles and the weak adhesion between the nanoparticles and the polymer matrix. In this study, to address the poor dispersion of nanoparticles in TFN membranes, we proposed a new combination of m-ZIF-8 and m-HNTs, wherein the ZIF-8 and HNTs were modified with poly (sodium p-styrenesulfonate) to enhance their dispersion in water. Furthermore, the hydropathic properties of the membranes can be well controlled by adjusting the content of m-ZIF-8 and m-HNTs. A series of modified m-ZIF-8/m-HNT/PAN membranes were prepared to modulate the dye/salt separation performance of TFN membranes. The experimental results showed that our m-ZIF-8/m-HNT/PAN membranes can elevate the water flux significantly up to 42.6 L m-2 h-1 MPa-1, together with a high rejection of Reactive Red 49 (more than 80%). In particular, the optimized NFM-7.5 membrane that contained 7.5 mg of HNTs and 2.5 mg of ZIF-8 showed a 97.1% rejection of Reactive Red 49 and 21.3% retention of NaCl.
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Microporous organic nanotubes (MONs) hold considerable promise for designing molecular-sieving membranes because of their high microporosity, customizable chemical functionalities, and favorable polymer affinity. Herein, we report the use of MONs derived from covalent organic frameworks to engineer 15-nm-thick microporous membranes via interfacial polymerization (IP). The incorporation of a highly porous and interpenetrated MON layer on the membrane before the IP reaction leads to the formation of polyamide membranes with Turing structure, enhanced microporosity, and reduced thickness. The MON-modified membranes achieve a remarkable water permeability of 41.7 L m-2 h-1 bar-1 and high retention of boron (78.0%) and phosphorus (96.8%) at alkaline conditions (pH 10), surpassing those of reported nanofiltration membranes. Molecular simulations reveal that introducing the MONs not only reduces the amine molecule diffusion toward the organic phase boundary but also increases membrane porosity and the density of water molecules around the membrane pores. This MON-regulated IP strategy provides guidelines for creating high-permeability membranes for precise nanofiltration.
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BACKGROUND: Safe and effective analgesia strategy remains one of the priorities for pediatric inguinal hernia treatment. AIM: To explore safety and efficacy of dexmededomidine monotherapy for postoperative analgesia in children who received laparoscopic unilateral internal inguinal ring ligation. METHODS: This randomized single-center controlled trial included 390 children (aged 1-3 years, ASA grade I-II), randomly divided into a dexmededomidine group (D group), a dexmededomidine + sufentanil group (DS group), and a sufentanil group (S group). The primary endpoint was percentage of children with the Face, Legs, Activity, Cry, and Consolability (FLACC) score ≤ 3 points 2 h after surgery. RESULTS: The comparisons of the FLACC scores at 2, 4, 6, 8, 12, and 24 h were not significantly different among the three groups (P > 0.05). The sedative effects in the D group were significantly better than those in the S group (P > 0.05), but not significantly different from those in the DS group. The incidence of nausea and vomiting was significantly lower in the D group than in the S group and DS group (P > 0.05). CONCLUSION: Analgesic effects of dexmededomidine monotherapy are comparable to those of sufentanil alone or in combination with dexmededomidine for children who underwent laparoscopic unilateral internal inguinal ring ligation, with better sedative effects and a lower incidence of adverse events.
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Trade-off between permeability and nanometer-level selectivity is an inherent shortcoming of membrane-based separation of molecules, while most highly porous materials with high adsorption capacity lack solution processability and stability for achieving adsorption-based molecule separation. We hereby report a hydrophilic amidoxime modified polymer of intrinsic microporosity (AOPIM-1) as a membrane adsorption material to selectively adsorb and separate small organic molecules from water with ultrahigh processing capacity. The membrane adsorption capacity for Rhodamine B reaches 26.114 g m-2, 10-1000 times higher than previously reported adsorptive membranes. Meanwhile, the membrane achieves >99.9% removal of various nano-sized organic molecules with water flux 2 orders of magnitude higher than typical pressure-driven membranes of similar rejections. This work confirms the feasibility of microporous polymers for membrane adsorption with high capacity, and provides the possibility of adsorptive membranes for molecular separation.