Construction of Hydration Layer for Proton Transport by Implanting the Hydrophilic Center Ag0 in Nickel Metal-Organic Frameworks.

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.

Rational Design of MXene Hollow Fiber Membranes for Gas Separations.

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.

Uniformly Distributed Mixed Matrix Membranes via a Solution Processable Strategy for Propylene/Propane Separation.

Aggregation of filler particles during the formation of mixed matrix membranes is difficult to avoid when filler loadings exceed a 10-15 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 (99 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 (>900 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.

Perpendicular Alignment of Covalent Organic Framework (COF) Pore Channels by Solvent Vapor Annealing.

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.

Comparing performance of iterative and non-iterative algorithms on various feature schemes for arrhythmia analysis.

To evaluate the performance of the classic machine learning algorithms and the effectiveness of various features, the iterative algorithms (i.e., support vector machine (SVM), and least-squares SVM (LS-SVM)) and non-iterative algorithms (i.e., random forest (RF) and naive bayes (NB)) for six feature schemes were performed to classify the ECG recordings. The ECG recordings were initially filtered with a 0.1 Hz - 12 Hz band pass filter. Then 80 features, including 48 time domain, 18 frequency domain, 12 time-frequency and two principle component analysis (PCA) features, were extracted to construct six feature schemes. The RF, SVM, LS-SVM and NB were employed to discern a binary-classification task (i.e., normal and AF ECG recordings) and a tri- classification task (i.e., the normal, AF and ST change ECG recordings) for the six feature schemes. The results revealed that time domain, frequency domain features and PCA features can provide relatively reliable feature combinations to the RF and SVM. In addition, the RF yielded the highest F1-scores (0.8908 and 0.7535) for the binary-classification task and the tri-classification task than the SVM, LS-SVM and NB.

Flexible and Robust Three-Dimensional Covalent Organic Framework Membranes for Precise Separations under Extreme Conditions.

Membranes based on covalent organic frameworks (COFs) have demonstrated huge potential to resolve the long-standing bottlenecks in separation fields due to their structural and functional attributes. Herein, a three-dimensional COF featuring interpenetrated apertures, 3D-OH-COF, is rationally synthesized on polyimide supports to generate flexible, robust membranes. The resultant 3D-OH-COF presents excellent crystallinity, prominent porosity, and exceptional solvent resistance, enabling the produced membrane a sharp and durable selectivity to small molecules in water and organic solvents. Impressively, the membrane also exhibits excellent flexibility and robustness as verified by the well-maintained performances after serious bending and solvent soaking under elevated temperatures. We further chemically convert 3D-OH-COF into the carboxyl-decorated 3D-COOH-COF by a postsynthetic strategy. The 3D-COOH-COF retains high crystallinity, and the converted membrane receives a remarkable capture ability for targeted multivalent ions over other competing ions. This study exploits a viable avenue to produce practical 3D COF membranes toward ultimate separations under extreme conditions.

Preparing Two-Dimensional Ordered Li0.33 La0.557 TiO3 Crystal in Interlayer Channel of Thin Laminar Inorganic Solid-State Electrolyte towards Ultrafast Li+ Transfer.

Inorganic superionic conductor holds great promise for high-performance all-solid-state lithium batteries. However, the ionic conductivity of traditional inorganic solid electrolytes (ISEs) is always unsatisfactory owing to the grain boundary resistance and large thickness. Here, a 13 µm-thick laminar framework with ≈1.3 nm interlayer channels is fabricated by self-assembling rigid, hydrophilic vermiculite (Vr) nanosheets. Then, Li0.33 La0.557 TiO3 (LLTO) precursors are impregnated in interlayer channels and afterwards in situ sintered to large-size, oriented, and defect-free LLTO crystal. We demonstrate that the confinement effect permits ordered arrangement of LLTO crystal along the c-axis (the fastest Li+ transfer direction), permitting the resultant 15 µm-thick Vr-LLTO electrolyte an ionic conductivity of 8.22×10-5  S cm-1 and conductance of 87.2 mS at 30 °C. These values are several times' higher than that of traditional LLTO-based electrolytes. Moreover, Vr-LLTO electrolyte has a compressive modulus of 1.24 GPa. Excellent cycling performance is demonstrated with all-solid-state Li/LiFePO4 battery.

Ultrafast Ion Sieving from Honeycomb-like Polyamide Membranes Formed Using Porous Protein Assemblies.

Despite the commercial success of thin film composite polyamide membranes, further improvements to the water permeation of polyamide membranes without degradation in product water quality remain a great challenge. Herein, we report the fabrication of an interfacially polymerized polyamide nanofiltration membrane with a novel 3D honeycomb-like spatial structure, which is formed from a tobacco mosaic virus (TMV) porous protein nanosheet-coated microfiltration membrane support. TMV nanosheets with uniform pores and appropriate hydrophilicity deposited inside the support membrane pores facilitate the construction of a localized water-oil reaction interface with evenly distributed monomers and guide the formation of a defect-free polyamide layer with a spatial structure that copies the geometry of the membrane cavities. Such a 3D morphology possesses ultrahigh specific surface area, leading to unprecedented membrane water permeance as high as 84 L m-2 h-1 bar-1, high MgSO4 rejection of 98%, and monovalent/divalent ion sieving selectivity up to 89.

The Brassica napus GATA transcription factor BnA5.ZML1 is a stigma compatibility factor.

Self-incompatibility (SI) is a genetic mechanism that rejects self-pollen and thus prevents inbreeding in some hermaphroditic angiosperms. In the Brassicaceae, SI involves a pollen-stigma recognition system controlled by a single locus known as the S locus, which consists of two highly polymorphic genes that encode S-locus cysteine-rich protein (SCR) and S-receptor kinase (SRK). When self-pollen lands on the stigma, the S-haplotype-specific interaction between SCR and SRK triggers SI. Here, we show that the GATA transcription factor BnA5.ZML1 suppresses SI responses in Brassica napus and is induced after compatible pollination. The loss-of-function mutant bna5.zml1 displays reduced self-compatibility. In contrast, overexpression of BnA5.ZML1 in self-incompatible stigmas leads to a partial breakdown of SI responses, suggesting that BnA5.ZML1 is a stigmatic compatibility factor. Furthermore, the expression levels of SRK and ARC1 are up-regulated in bna5.zml1 mutants, and they are down-regulated in BnA5.ZML1 overexpressing lines. SRK affects the cellular localization of BnA5.ZML1 through direct protein-protein interaction. Overall, our findings highlight the fundamental role of BnA5.ZML1 in SI responses in B. napus, establishing a direct interaction between BnA5.ZML1 and SRK in this process.

Improving poly-(γ-glutamic acid) production from a glutamic acid-independent strain from inulin substrate by consolidated bioprocessing.

To excavate the application of Jerusalem artichoke on poly(γ-glutamic acid) (γ-PGA) production, a γ-PGA producing strain Bacillus amyloliquefaciens NX-2S154 was obtained through atmospheric and room temperature plasma mutagenesis, which produced 14.83 ± 0.31 g/L of γ-PGA in batch fermentation with raw inulin extract. Simultaneous saccharification and fermentation (SSF) by adding commercial inulinase were further investigated for γ-PGA fermentation. Results showed SSF could eliminate the ineffective utilization of inulin while avoiding inhibition effect of high concentration substrate, which made γ-PGA concentration reach 18.54 ± 0.39 g/L with the process being shortened by 17%. Finally, an immobilized column for reducing inulinase cost was introduced to γ-PGA production. Repeated batch cultures showed the novel bioreactor exhibited higher stability and simplicity and gave average γ-PGA concentration and productivity of 19.40 ± 0.37 g/L and 0.27 ± 0.008 g/L/h, respectively. This work proposes a productive method for efficient γ-PGA production using Jerusalem artichoke feedstock.

A novel IL-1RA-PEP fusion protein alleviates blood-brain barrier disruption after ischemia-reperfusion in male rats.

BACKGROUND: Current options to treat clinical relapse in inflammatory central nervous system (CNS) conditions such as cerebral ischemia-reperfusion injury are limited, and agents that are more effective are required. Disruption of the blood-brain barrier is an early feature of lesion formation that correlates with clinical exacerbation and facilitates the entry of inflammatory medium and inflammatory cells. Interleukin-1 receptor antagonist (IL-1RA) is a naturally occurring anti-inflammatory antagonist of the interleukin-1 (IL-1) family. The broad-spectrum anti-inflammatory effects of IL-1RA have been investigated against various forms of neuroinflammation. However, the effect of IL-1RA on blood-brain barrier disruption following ischemia-reperfusion has not been reported. METHODS: In this study, we investigated the effects of IL-1RA and a novel protein (IL-1RA-PEP) that was fused to IL-1RA with a cell penetrating peptide, on blood-brain barrier integrity, in male rats subjected to transient middle cerebral artery occlusion. RESULTS: After intravenous administration, IL-1RA-PEP (50 mg/kg) penetrated cerebral tissues more effectively than IL-1RA. Moreover, it preserved blood-brain barrier integrity, attenuated changes in expression and localization of tight junction proteins and matrix metalloproteinases, and enhanced angiogenesis in ischemic brain tissue. Further study suggested that the effects of IL-1RA-PEP on preserving blood-brain barrier integrity might be closely correlated with the p65/NF-κB pathway, as evidenced by the effects of the inhibitor JSH-23. CONCLUSIONS: Collectively, our results demonstrated that IL-1RA-PEP could effectively penetrate the brain of rats with middle cerebral artery occlusion and ameliorate blood-brain barrier disruption. This finding might represent its novel therapeutic potential in the treatment of the cerebral ischemia-reperfusion injury.

[Complexity Analysis of Physiological Signals Using Encoding Lempel-Ziv Algorithm].

To distinguish the randomness and chaos characteristics of physiological signals and to keep its performance independent of the signal length and parameters are the key judgement of performance of a complexity algorithm.We proposed an encoding Lempel-Ziv(LZ)complexity algorithm to try to explicitly discern between the randomness and chaos characteristics of signals.Our study also compared the effects of length of time series,the sensitivity to dynamical properties change of time series and quantifying the complexity between gauss noise and 1/f pink noise ELZ with those from classic LZ(CLZ),multi-state LZ(MLZ),sample entropy(SampEn)and permutation entropy(PE).The experimental results showed ELZ could not only distinguish the randomness and chaos characteristics of time series on all time length(i.e.100,500,5 000),but also reflected exactly that the complexity of gauss noise was lower than that of pink noise,and responded change of dynamic characteristics of time series in time.The congestive heart failure(CHF)RR Interval database and the normal sinus rhythm(NSR)RR Interval database created by Massachusetts Institute of Technology(MIT)and Boston Beth Israel Hospital(BIH)were used as real data in our study.The results revealed that the ELZ could show the complexity of congestive heart failure which was lower than that of normal sinus rhythm during all lengths of time series(P<0.01),and the ELZ algorithm had better generalization ability and was independent of length of time series.

Formation of Ultrathin, Continuous Metal-Organic Framework Membranes on Flexible Polymer Substrates.

Metal-organic framework (MOF) materials have an enormous potential in separation applications, but to realize their potential as semipermeable membranes they need to be assembled into thin continuous macroscopic films for fabrication into devices. By using a facile immersion technique, we prepared ultrathin, continuous zeolitic imidazolate framework (ZIF-8) membranes on titania-functionalized porous polymeric supports. The coherent ZIF-8 layer was surprisingly flexible and adhered well to the support, and the composite membrane could sustain bending and elongation. The membranes exhibited molecular sieving behavior, close to the theoretical permeability of ZIF-8, with hydrogen permeance up to 201×10(-7)  mol m(-2) s(-1) Pa(-1) and an ideal H2 /CO2 selectivity of 7:1. This approach offers significant opportunities to exploit the unique properties of MOFs in the fabrication of separation and sensing devices.

Using Lempel-Ziv Complexity to Assess ECG Signal Quality.

The poor quality of wireless electrocardiography (ECG) recordings can lead to misdiagnosis and waste of medical resources. This study presents an interpretation of Lempel-Ziv (LZ) complexity in terms of ECG quality assessment, and verifies its performance on real ECG signals. Firstly, LZ complexities for typical signals, namely high-frequency (HF) noise, low-frequency (LF) noise, power-line (PL) noise, impulse (IM) noise, clean artificial ECG signals, and ECG signals with various types of noise added (ECG plus HF, LF, PL, and IM noise, respectively) were analyzed. Then, the effects of noise, signal length, and signal-to-noise ratio (SNR) on the LZ complexity of ECG signals were analyzed. The simulation results show that LZ complexity for HF noise was obviously different from those for PL and LF noise. The LZ value can be used to determine the presence of HF noise. ECG plus HF noise had the highest LZ values. Other types of noise had low LZ values. Signal lengths of over 40 s had only a small effect on LZ values. The LZ values for ECG plus all types of noise increased monotonically with decreasing SNR except for LF and PL noise. For the test of real ECG signals plus three types of noise, namely muscle artefacts (MAs), baseline wander (BW), and electrode motion (EM) artefacts, LZ complexity varied obviously with increasing MA but not for BW and EM noise. This study demonstrates that LZ complexity is sensitive to noise level (especially for HF noise) and can thus be a valuable reference index for the assessment of ECG signal quality.

Visualized Lead Selection for Arrhythmia Classification Based on a Lead Activation Heatmap Using Multi-Lead ECGs.

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.

A Novel Multi-modal Population-graph based Framework for Patients of Esophageal Squamous Cell Cancer Prognostic Risk Prediction.

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.

Polymer carbon nitride nanosheet-based lamellar membranes inspired by "couple hardness with softness" for ultrafast molecular separation in organic solvents.

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.

Preparation and antibacterial property of PES/AgNO3 three-bore hollow fiber ultrafiltration membranes.

In this study, a three-bore polyethersulfone (PES) hollow fiber ultrafiltration (UF) membrane with antibacterial properties was prepared by phase inversion, using PES as the membrane material, N,N-dimethylacetamide (DMAC) as solvent, polyvinylpyrrolidone (PVP) and AgNO3 as additives. The silver particles were detected by X-ray photoelectron spectroscopy. The effect of AgNO3 content on the antibacterial properties and separation performance was studied in detail. The membranes showed good antibacterial activity against Escherichia coli after adding AgNO3 and the antibacterial rate of PES/AgNO3 UF membrane with AgNO3 content of 1 wt% could reach 99.9% after running for 48 hours. Moreover, the bovine serum albumin solution filtration results indicated that the PES/AgNO3 membranes had a certain degree of antifouling performance. Therefore, three-bore PES/AgNO3 membranes have a potential application to reduce both bacterial and organic fouling in water treatment.

A Mini Review of Ceramic-Based MOF Membranes for Water Treatment.

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.

When Coordination Polymers Meet Wood: From Molecular Design toward Sustainable Solar Desalination.

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.