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1.
J Am Chem Soc ; 2024 Jun 06.
Artigo em Inglês | MEDLINE | ID: mdl-38842082

RESUMO

Biological ion channels exhibit switchable cation transport with ultrahigh selectivity for efficient energy conversion, such as Ca2+-activated TRPM4 channels tuned by cation-π interactions, but achieving an analogous highly selective function is challenging in artificial nanochannels. Here, we design a TRPM4-inspired cation-selective nanochannel (CN) assembled by two poly(ether sulfone)s, respectively, with sulfonate acid and indole moieties, which act as cation-selective activators to manage Na+/Cl- selectivity via ionic and cation-π interactions. The cation selectivity of CNs can be activated by Na+, and thereby the Na+ transference number significantly improves from 0.720 to 0.982 (Na+/Cl- selectivity ratio from 2.6 to 54.6) under a 50-fold salinity gradient, surpassing the K+ transference number (0.886) and Li+ transference number (0.900). The TRPM4-inspired nanochannel membrane enabled a maximum output power density of 5.7 W m-2 for salinity-gradient power harvesting. Moreover, a record energy conversion efficiency of up to 46.5% is provided, superior to most nanochannel membranes (below 30%). This work proposes a novel strategy to biomimetic nanochannels for highly selective cation transport and high-efficiency salinity-gradient energy conversion.

2.
Small ; : e2401264, 2024 Apr 18.
Artigo em Inglês | MEDLINE | ID: mdl-38634249

RESUMO

Biological photo-responsive ion channels play important roles in the important metabolic processes of living beings. To mimic the unique functions of biological prototypes, the transition metal dichalcogenides, owing to their excellent mechanical, electrical, and optical properties, are already used for artificial intelligent channel constructions. However, there remain challenges to building artificial bio-semiconductor nanochannels with finely tuned band gaps for accurately simulating or regulating ion transport. Here, two well-designed peptides are employed for the WS2 nanosheets functionalization with the sequences of PFPFPFPFC and DFDFDFDFC (PFC and DFC; P: proline, D: aspartate, and F: phenylalanine) through cysteine (Cys, C) linker, and an asymmetric peptide-WS2 membrane (AP-WS2M) could be obtained via self-assembly of peptide-WS2 nanosheets. The AP-WS2M could realize the photo-driven anti-gradient ion transport and vis-light enhanced osmotic energy conversion by well-designed working patterns. The photo-driven ion transport mechanism stems from a built-in photovoltaic motive force with the help of formed type II band alignment between the PFC-WS2 and DFC-WS2. As a result, the ions would be driven across the channels of the membrane for different applications. The proposed system provides an effective solution for building photo-driven biomimetic 2D bio-semiconductor ion channels, which could be extensively applied in the fields of drug delivery, desalination, and energy conversion.

3.
ACS Cent Sci ; 10(2): 469-476, 2024 Feb 28.
Artigo em Inglês | MEDLINE | ID: mdl-38435527

RESUMO

With the rapid development of the lithium ion battery industry, emerging lithium (Li) enrichment in nature has attracted ever-growing attention due to the biotoxicity of high Li levels. To date, fast lithium ion (Li+) detection remains urgent but is limited by the selectivity, sensitivity, and stability of conventional technologies based on passive response processes. In nature, archaeal plasma membrane ion exchangers (NCLX_Mj) exhibit Li+-gated multi/monovalent ion transport behavior, activated by different stimuli. Inspired by NCLX_Mj, we design a pH-controlled biomimetic Li+-responsive solid-state nanochannel system for on-demand Li+ detection using 2-(2-hydroxyphenyl)benzoxazole (HPBO) units as Li+ recognition groups. Pristine HPBO is not reactive to Li+, whereas negatively charged HPBO enables specific Li+ coordination under alkaline conditions to decrease the ion exchange capacity of nanochannels. On-demand Li+ detection is achieved by monitoring the decline in currents, thereby ensuring precise and stable Li+ recognition (>0.1 mM) in the toxic range of Li+ concentration (>1.5 mM) for human beings. This work provides a new approach to constructing Li+ detection nanodevices and has potential for applications of Li-related industries and medical services.

4.
Chem Sci ; 15(12): 4538-4546, 2024 Mar 20.
Artigo em Inglês | MEDLINE | ID: mdl-38516083

RESUMO

Oceans and salt lakes contain vast amounts of uranium. Uranium recovery from natural water not only copes with radioactive pollution in water but also can sustain the fuel supply for nuclear power. The adsorption-assisted electrochemical processes offer a promising route for efficient uranium extraction. However, competitive hydrogen evolution greatly reduces the extraction capacity and the stability of electrode materials with electrocatalytic activity. In this study, we got inspiration from the biomineralisation of marine bacteria under high salinity and biomimetically regulated the electrochemical process to avoid the undesired deposition of metal hydroxides. The uranium uptake capacity can be increased by more than 20% without extra energy input. In natural seawater, the designed membrane electrode exhibits an impressive extraction capacity of 48.04 mg-U per g-COF within 21 days (2.29 mg-U per g-COF per day). Furthermore, in salt lake brine with much higher salinity, the membrane can extract as much uranium as 75.72 mg-U per g-COF after 32 days (2.37 mg-U per g-COF per day). This study provides a general basis for the performance optimisation of uranium capture electrodes, which is beneficial for sustainable access to nuclear energy sources from natural water systems.

5.
Sci Adv ; 10(11): eadj7867, 2024 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-38478611

RESUMO

The voltage-gated ion channels, also known as ionic transistors, play substantial roles in biological systems and ion-ion selective separation. However, implementing the ultrafast switchable capabilities and polarity switching of ionic transistors remains a challenge. Here, we report a nanofluidic ionic transistor based on carbon nanotubes, which exhibits an on/off ratio of 104 at operational gate voltage as low as 1 V. By controlling the morphology of carbon nanotubes, both unipolar and ambipolar ionic transistors are realized, and their on/off ratio can be further improved by introducing an Al2O3 dielectric layer. Meanwhile, this ionic transistor enables the polarity switching between p-type and n-type by controlled surface properties of carbon nanotubes. The implementation of constructing ionic circuits based on ionic transistors is demonstrated, which enables the creation of NOT, NAND, and NOR logic gates. The ionic transistors are expected to have profound implications for low-energy consumption computing devices and brain-machine interfacing.

6.
World J Gastrointest Surg ; 16(2): 289-306, 2024 Feb 27.
Artigo em Inglês | MEDLINE | ID: mdl-38463362

RESUMO

BACKGROUND: Phospholipase A2 (PLA2) enzymes are pivotal in various biological processes, such as lipid mediator production, membrane remodeling, bioenergetics, and maintaining the body surface barrier. Notably, these enzymes play a significant role in the development of diverse tumors. AIM: To systematically and comprehensively explore the expression of the PLA2 family genes and their potential implications in cholangiocarcinoma (CCA). METHODS: We conducted an analysis of five CCA datasets from The Cancer Genome Atlas and the Gene Expression Omnibus. The study identified differentially expressed genes between tumor tissues and adjacent normal tissues, with a focus on PLA2G2A and PLA2G12B. Gene Set Enrichment Analysis was utilized to pinpoint associated pathways. Moreover, relevant hub genes and microRNAs for PLA2G2A and PLA2G12B were predicted, and their correlation with the prognosis of CCA was evaluated. RESULTS: PLA2G2A and PLA2G12B were discerned as differentially expressed in CCA, manifesting significant variations in expression levels in urine and serum between CCA patients and healthy individuals. Elevated expression of PLA2G2A was correlated with poorer overall survival in CCA patients. Additionally, the study delineated pathways and miRNAs associated with these genes. CONCLUSION: Our findings suggest that PLA2G2A and PLA2G12B may serve as novel potential diagnostic and prognostic markers for CCA. The increased levels of these genes in biological fluids could be employed as non-invasive markers for CCA, and their expression levels are indicative of prognosis, underscoring their potential utility in clinical settings.

7.
Chem Soc Rev ; 53(6): 2972-3001, 2024 Mar 18.
Artigo em Inglês | MEDLINE | ID: mdl-38345093

RESUMO

Nanofluidic channels with tailored ion transport dynamics are usually used as channels for ion transport, to enable high-performance ion regulation behaviors. The rational construction of nanofluidics and the introduction of external fields are of vital significance to the advancement and development of these ion transport properties. Focusing on the recent advances of nanofluidics, in this review, various dimensional nanomaterials and their derived homogeneous/heterogeneous nanofluidics are first briefly introduced. Then we discuss the basic principles and properties of ion transport in nanofluidics. As the major part of this review, we focus on recent progress in ion transport in nanofluidics regulated by external physical fields (electric field, light, heat, pressure, etc.) and chemical fields (pH, concentration gradient, chemical reaction, etc.), and reveal the advantages and ion regulation mechanisms of each type. Moreover, the representative applications of these nanofluidic channels in sensing, ionic devices, energy conversion, and other areas are summarized. Finally, the major challenges that need to be addressed in this research field and the future perspective of nanofluidics development and practical applications are briefly illustrated.

9.
Adv Mater ; 36(6): e2308639, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-37923399

RESUMO

The quasi-solid electrolytes (QSEs) attract extensive attention due to their improved ion transport properties and high stability, which is synergistically based on tunable functional groups and confined solvent molecules among the polymetric networks. However, the trade-off effect between the polymer content and ionic conductivity exists in QSEs, limiting their rate performance. In this work, the epitaxial polymerization strategy is used to build the gradient hydrogel networks (GHNs) covalently fixed on zinc anode. Then, it is revealed that the asymmetric distribution of negative charges benefits GHNs with fast and selective ionic transport properties, realizing a higher Zn2+ transference number of 0.65 than that (0.52) for homogeneous hydrogel networks (HHNs) with the same polymer content. Meanwhile, the high-density networks formed at Zn/GHNs interface can efficiently immobilize free water molecules and homogenize the Zn2+ flux, greatly inhibiting the water-involved parasitic reactions and dendrite growth. Thus, the GHNs enable dendrite-free stripping/plating over 1000 h at 8 mA cm-2 and 1 mAh cm-2 in a Zn||Zn symmetric cell, as well as the evidently prolonged cycles in various full cells. This work will shed light on asymmetric engineering of ion transport channels in advanced quasi-solid battery systems to achieve high energy and safety.

10.
Angew Chem Int Ed Engl ; 63(7): e202317361, 2024 Feb 12.
Artigo em Inglês | MEDLINE | ID: mdl-38116868

RESUMO

Numerous reported bioinspired osmotic energy conversion systems employing cation-/anion-selective membranes and solutions with different salinity are actually far from the biological counterpart. The iso-osmotic power generator with the specific ionic permselective channels (e.g., K+ or Na+ channels) which just allow specific ions to get across and iso-osmotic solutions still remain challenges. Inspired by nature, we report a bioinspired K+ -channel by employing a K+ selective ligand, 1,1,1-tris{[(2'-benzylaminoformyl)phenoxy]methyl}ethane (BMP) and graphene oxide membrane. Specifically, the K+ and Na+ selectivity of the prepared system could reach up to ≈17.8, and the molecular dynamics simulation revealed that the excellent permselectivity of K+ mainly stemmed from the formed suitable channel size. Thus, we assembled the K+ -selective iso-osmotic power generator (KSIPG) with the power density up to ≈15.1 mW/m2 between equal concentration solutions, which is higher than traditional charge-selective osmotic power generator (CSOPG). The proposed strategy has well shown the realizable approach to construct single-ion selective channels-based highly efficient iso-osmotic energy conversion systems and would surely inspire new applications in other fields, including self-powered systems and medical materials, etc.

11.
Small ; : e2308277, 2023 Dec 03.
Artigo em Inglês | MEDLINE | ID: mdl-38044301

RESUMO

Bioinspired two-dimensional (2D) nanofluidic systems for photo-induced ion transport have attracted great attention, as they open a new pathway to enabling light-to-ionic energy conversion. However, there is still a great challenge in achieving a satisfactory performance. It is noticed that organic solar cells (OSCs, light-harvesting device based on photovoltaic effect) commonly require hole/electron transport layer materials (TLMs), PEDOT:PSS (PE) and PDINN (PD), respectively, to promote the energy conversion. Inspired by such a strategy, an artificial proton pump by coupling a nanofluidic system with TLMs is proposed, in which the PE- and PD-functionalized tungsten disulfide (WS2 ) multilayers construct a heterogeneous membrane, realizing an excellent output power of ≈1.13 nW. The proton transport is fine-regulated due to the TLMs-engineered band structure of WS2 . Clearly, the incorporating TLMs of OSCs into 2D nanofluidic systems offers a feasible and promising approach for band edge engineering and promoting the light-to-ionic energy conversion.

12.
ACS Sens ; 8(9): 3428-3434, 2023 09 22.
Artigo em Inglês | MEDLINE | ID: mdl-37552848

RESUMO

Pesticides have caused concerns about food safety due to their residual effects in vegetables and fruits. Imidacloprid, as the frequently used neonicotinoid pesticide, could harm cardiovascular and respiratory function and cause reproductive toxicity in humans. Therefore, reliable methods for portable, selective, and rapid detection are desirable to develop. Herein, we report a neuron-inspired nanofluidic biosensor based on a tyrosine-modified artificial nanochannel for sensitively detecting imidacloprid. The functional tyrosine is modified on the outer surface of porous anodic aluminum oxide to rapidly capture imidacloprid through π-π interactions and hydrogen bonds. The integrated nanofluidic biosensor has a wide concentration range from 10-8 to 10-4 g/mL with an ultralow detection limit of 6.28 × 10-9 g/mL, which outperforms the state-of-the-art sensors. This work provides a new perspective on detecting imidacloprid residues as well as other hazardous pesticide residues in environmental and food samples.


Assuntos
Técnicas Biossensoriais , Resíduos de Praguicidas , Praguicidas , Humanos , Neonicotinoides/análise , Praguicidas/análise , Resíduos de Praguicidas/análise , Técnicas Biossensoriais/métodos
13.
Entropy (Basel) ; 25(7)2023 Jul 04.
Artigo em Inglês | MEDLINE | ID: mdl-37509967

RESUMO

Quantum adiabatic shortcut technology provides a technique to accelerate the quantum adiabatic process and has been widely used in various fields of quantum information processing. In this work, we proposed a two-level quantum shortcut adiabatic passage model. Then, exploiting the nuclear magnetic resonance, we experimentally simulated the dynamics of quantum shortcut adiabatic passage using the water molecules.

14.
Chem Commun (Camb) ; 59(61): 9384-9387, 2023 Jul 27.
Artigo em Inglês | MEDLINE | ID: mdl-37434494

RESUMO

A biomimetic hierarchical membrane consisting of ZIF-8 and MXene with controllable morphology could be fabricated by the facile electrochemical deposition method, well-realizing Li+/Mg2+ sieving. This membrane could work stably in real brine with perm-selectivity of Li+/Mg2+ up to 47.4.

15.
J Hazard Mater ; 458: 131978, 2023 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-37399726

RESUMO

Crystalline porous covalent frameworks (COFs) have been considered as a platform for uranium extraction from seawater and nuclear waste. However, the role of rigid skeleton and atomically precise structures of COFs is often ignored in the design of defined binding configuration. Here, a COF with an optimized relative position of two bidentate ligands realizes full potential in uranium extraction. Compared with the para-chelating groups, the optimized ortho-chelating groups with oriented adjacent phenolic hydroxyl groups on the rigid skeleton endow an additional uranyl binding site, thereby increasing the total number of binding sites up to 150%. Experimental and theoretical results indicate that the uranyl capture is greatly improved via the energetically favored multi-site configuration and the adsorption capacity reaches up to 640 mg g-1, which exceeds that of most reported COF-based adsorbents with chemical coordination mechanism in uranium aqueous solution. This ligand engineering strategy can efficiently advance the fundamental understanding of designing the sorbent systems for extraction and remediation technology.

16.
Turk Neurosurg ; 33(4): 556-567, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-37309626

RESUMO

AIM: To optimize the Spontaneous intracerebral hemorrhage (sICH) early hematoma expansion prediction scoring table to adopt appropriate clinical treatment plans and improve the prognosis of sICH patients. MATERIAL AND METHODS: A total of 150 patients with sICH were enrolled, and 44 had early hematoma expansion. According to the selection and exclusion criteria, the study subjects were screened, their NCCT characteristic signs and clinical data were analyzed statistically. The established prediction score was applied to the follow-up study cohort to conduct a pilot study, and the t-test and ROC curve were used to evaluate its predictive ability. RESULTS: Statistical analysis found that initial hematoma volume, GCS score, and NCCT special signs were independent risk factors for early hematoma expansion after sICH (p < 0.05). Thus, a score table was established. Subjects with ≥10 were divided into high-risk group, 6-8 comprised the medium-risk group, and ≤4 were divided into low-risk group. Among 17 patients with acute sICH, 7 developed early hematoma enlargement. The prediction accuracy was 92.41% in the low-risk group, 98.06% in the medium-risk group, and 84.61% in the high-risk group. CONCLUSION: This optimized prediction score table based on the special signs of NCCT shows the high prediction accuracy of sICH early hematoma.


Assuntos
Hemorragia Cerebral , Tomografia Computadorizada por Raios X , Humanos , Seguimentos , Projetos Piloto , Tomografia Computadorizada por Raios X/efeitos adversos , Hemorragia Cerebral/complicações , Hemorragia Cerebral/diagnóstico por imagem , Hematoma/diagnóstico por imagem , Hematoma/etiologia , Hipertrofia/complicações , Estudos Retrospectivos
17.
Nanomicro Lett ; 15(1): 130, 2023 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-37209189

RESUMO

The global carbon neutrality strategy brings a wave of rechargeable lithium-ion batteries technique development and induces an ever-growing consumption and demand for lithium (Li). Among all the Li exploitation, extracting Li from spent LIBs would be a strategic and perspective approach, especially with the low energy consumption and eco-friendly membrane separation method. However, current membrane separation systems mainly focus on monotonous membrane design and structure optimization, and rarely further consider the coordination of inherent structure and applied external field, resulting in limited ion transport. Here, we propose a heterogeneous nanofluidic membrane as a platform for coupling multi-external fields (i.e., light-induced heat, electrical, and concentration gradient fields) to construct the multi-field-coupled synergistic ion transport system (MSITS) for Li-ion extraction from spent LIBs. The Li flux of the MSITS reaches 367.4 mmol m-2 h-1, even higher than the sum flux of those applied individual fields, reflecting synergistic enhancement for ion transport of the multi-field-coupled effect. Benefiting from the adaptation of membrane structure and multi-external fields, the proposed system exhibits ultrahigh selectivity with a Li+/Co2+ factor of 216,412, outperforming previous reports. MSITS based on nanofluidic membrane proves to be a promising ion transport strategy, as it could accelerate ion transmembrane transport and alleviate the ion concentration polarization effect. This work demonstrated a collaborative system equipped with an optimized membrane for high-efficient Li extraction, providing an expanded strategy to investigate the other membrane-based applications of their common similarities in core concepts.

18.
Opt Express ; 31(9): 14008-14026, 2023 Apr 24.
Artigo em Inglês | MEDLINE | ID: mdl-37157274

RESUMO

Low-light images always suffer from dim overall brightness, low contrast, and low dynamic ranges, thus result in image degradation. In this paper, we propose an effective method for low-light image enhancement based on the just-noticeable-difference (JND) and the optimal contrast-tone mapping (OCTM) models. First, the guided filter decomposes the original images into base and detail images. After this filtering, detail images are processed based on the visual masking model to enhance details effectively. At the same time, the brightness of base images is adjusted based on the JND and OCTM models. Finally, we propose a new method to generate a sequence of artificial images to adjust the brightness of the output, which has a better performance in image detail preservation compared with other single-input algorithms. Experiments have demonstrated that the proposed method not only achieves low-light image enhancement, but also outperforms state-of-the-art methods qualitatively and quantitatively.

19.
Angew Chem Int Ed Engl ; 62(23): e202302938, 2023 Jun 05.
Artigo em Inglês | MEDLINE | ID: mdl-37029469

RESUMO

Nanofluidic reverse electrodialysis provides an attractive way to harvest osmotic energy. However, most attention was paid to monotonous membrane structure optimization to promote selective ion transport, while the role of external fields and relevant mechanisms are rarely explored. Here, we demonstrate a Kevlar-toughened tungsten disulfide (WS2 ) composite membrane with bioinspired serosa-mimetic structures as an efficient osmotic energy generator coupling light. As a result, the output power could be up to 16.43 W m-2 under irradiation, outperforming traditional two-dimensional (2D) membranes. Both the experiment and simulation uncover that the generated photothermal and photoelectronic effects could synergistically promote the confined ion transport process. In addition, this membrane also possesses great anti-fouling properties, endowing its practical application. This work paves new avenues for sustainable power generation by coupling solar energy.

20.
Angew Chem Int Ed Engl ; 62(18): e202300167, 2023 Apr 24.
Artigo em Inglês | MEDLINE | ID: mdl-36882908

RESUMO

Biological proton channels play important roles in the delicate metabolism process, and have led to great interest in mimicking selective proton transport. Herein, we designed a bioinspired proton transport membrane by incorporating flexible 14-crown-4 (14C4) units into rigid frameworks of polyimine films by an interfacial Schiff base reaction. The Young's modulus of the membrane reaches about 8.2 GPa. The 14C4 units could grab water, thereby forming hydrogen bond-water networks and acting as jumping sites to lower the energy barrier of proton transport. The molecular chains present a vertical orientation to the membrane, and the ions travel between the quasi-planar molecular sheets. Furthermore, the 14C4 moieties could bond alkali ions through host-guest interactions. Thus, the ion conductance follows H+ ≫K+ >Na+ >Li+ , and an ultrahigh selectivity of H+ /Li+ (ca. 215) is obtained. This study provides an effective avenue for developing ion-selective membranes by embedding macrocycle motifs with inherent cavities.

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