Hypertension significantly increases the risk of cardiovascular diseases and seriously affects people’s health. The incidence of hypertension is rising rapidly in the world and hypertension has become a significant factor influencing the global average life expectancy. The diagnosis of hypertension is generally fulfilled by measuring diastolic and systolic blood pressure, but it is insufficient to differentiate essential hypertension from secondary hypertension, so it is crucial to identifying the cause of hypertension by detecting biomarkers in plasma. In clinical practice, five plasma biomarkers are utilized for diagnosing hypertension, and the detection tasks of a large number of cases have raised increasing demands for cost-effective, efficient, speedy, and diverse methods, which makes many traditional diagnostic technologies inadequate for meeting the needs of clinical diagnosis. The nanomaterial-based detection techniques have frequently attained the qualities of quick reaction, low cost, straightforward operation, high sensitivity, and strong specificity in recent years with the advancement of nanotechnology, so they have great potential for early and rapid diagnosis. In this review, we will introduce the characteristics and drawbacks of current clinical detection methods for hypertension screening, the principles and advancements of nanotechnology-based detection methods, as well as their potentials for clinical application.
Collecting green hydrogen (H2) from water splitting driven by renewable energy is a new competition to implement the construction of H2 energy industry and promote new economic growth for global governments. The common strategy to enhance the efficiency of H2 production is to reduce the potential of electrolytic cell that is the mainstream way to prepare efficient electrocatalysts. Layered double hydroxides (LDHs) are one of the most active electrocatalysts with adjustable active sites in contemporary research. In this review, we discuss the recent advanced progress of LDHs for hydrogen evolution reaction (HER) on cathode and oxygen evolution reaction (OER) or organic oxidation on anode and emphasize the influence of LDHs structure regulation in water electrolysis process (HER/OER) as well as the current development status of organic oxidation catalyzed by active oxygen species on anode. Finally, we propose the current challenges of LDHs in electrocatalysis and prospect their developing tendency and further application.
Layered double hydroxide (LDH) is regarded as an advanced platform material in catalysis and attracts vast attrition recently. As a kind of two-dimensional layered material, it exhibits great advantages including cation-tunability in layer, lattice limitation, topological transformation, ion exchange and intercalation characteristics. It also can be used as building blocks for composite catalytic materials. Over 100 years, a large number of works have been accomplished and researchers made great progress on investigating the LDH-based catalytic materials. In this review, we summarize representative achievements and significant progress in recent years, which mainly include constructing high entropy catalytic material, high dispersion/stability and interfacial supported catalytic material, composite catalytic materials and nano-reactor based on LDH. Furthermore, through collecting the excellent works, we conclude the future development potential of LDH and provide a perspective.
In this review, we delve into the intricate regulation of the tumor microenvironment (TME) under malignant conditions and explore the transformative potential of nanoscale metal-organic frameworks (nMOFs) in the realm of sonodynamic therapy (SDT). The TME serves as a dynamic milieu influencing tumor progression and therapeutic response, presenting formidable challenges, such as hypoxia, acidity, excess hydrogen peroxide, high expression of glutathione, and immunosuppression. Utilizing the exceptional attributes of nMOFs, including their tunable structures and biocompatibility, holds immense promise for enhancing SDT efficacy and reshaping the TME landscape. By integrating nMOFs with SDT, researchers aim to assemble multiple functionalities in a single platform that enhance tumor cell eradication while counteracting unfavorable TME conditions and immune resistance. The potential of nMOFs to revolutionize tumor therapies by precisely targeting TME and overcoming therapeutic barriers is underscored by an in-depth analysis of recent breakthroughs in the use of nMOFs-based sonosensitizers to remodulate TME to amplify the efficacy of SDT.
Carbon nanobelts (CNBs) with aesthetically appealing molecular structures and outstanding physical properties have attracted more and more attentions from the scientific community due to their potential applications in synthetic materials, host-guest chemistry, optoelectronics, and so on. The synthesis of CNBs at different stages was overviewed and some representative breakthroughs and advances in synthetic strategies were highlighted and discussed. The key issue for the synthesis of CNBs is how to construct curved structures with high strain energy. We not only proposed a few unconventional CNBs as the promising target molecules, but also pointed out the bottom-up synthesis of conjugated tubular segments of carbon nanotubes sharing similar properties as carbon nanotubes is the next focus in this emerging area.
Cyclic GMP-AMP (cGAMP) synthase (cGAS) plays a pivotal role in the innate immune system. As the primary DNA sensor in cells, cGAS binds to dsDNA in the cytoplasm and forms cGAS-DNA liquid-liquid phase separation (LLPS) and activates its catalytic activity. This activation triggers the cGAS-stimulator of interferon genes (STING) signaling pathway, establishing an efficient system for pathogen detection. Beyond pathogen surveillance, cGAS performs a diverse range of roles, involved in inflammatory response, metabolic homeostasis, DNA damage repair, and cell death. These biological functions regulate cellular physiological homeostasis and influence the occurrence and development of diseases. This review provides an overview of the structure, localization, and intracellular biological functions of the cGAS-STING signaling pathway and cGAS-DNA LLPS. Furthermore, we discuss their contribution to the development of tumors, autoimmune diseases, and inflammatory diseases and highlight the innovative strategies in modulating cGAS activity, either through activation or inhibition, as a promising therapeutic approach.
With the rapid development of industrialization, it is inevitable to produce solid wastes in the fields of energy petrochemical industry. However, the storage and utilization of these solid wastes have become a considerable challenge. Due to the main element composition of these solid wastes including silicon and aluminum, it has attracted extensive attention for synthesizing zeolites. This review summarized the properties of major solid wastes including coal fly ash, coal gangue, spent fluid catalytic cracking (FCC) catalyst, lithium slag, bauxite residue, and waste glass. Then, the preparation of LTA, FAU, ZSM-5, SSZ-13, Beta, and MOR zeolites from these solid wastes were introduced. Finally, the current challenges and perspectives were discussed.
Developing easily accessible deep-red/near-infrared circularly polarized emitters for practical organic light-emitting diodes remains a significant challenge. Here, a practical strategy has been proposed for developing deep-red circularly polarized delayed fluorescent emitters based on a novel chiral acceptor platform. By changing triphenylamine (TPA) substitution position from para to meta, R/S-M-TBBTCN demonstrated thermally activated delayed fluorescence (TADF) properties with a delayed lifetime of 6.6 µs that R/S-P-TBBTCN doesn’t have. Furthermore, R/S-M-TBBTCN showed a 65 nm red-shift in emission and a 10-fold enhancement in asymmetry factor (g lum), compared with R/S-P-TBBTCN. The solution-processed nondoped circularly polarized organic light-emitting diodes (CP-OLEDs) based on R-M-TBBTCN display deep-red emission and 2.2% external quantum efficiency.
Driven by renewable or excess electrical energy, electrochemical CO2 reduction reaction (eCO2RR) represents a promising carbon-neutral approach to generating valuable low-carbon fuels by consuming CO2 and H2O. C2+ products are one of the most economically valuable products among the reduction species of eCO2RR, but there are still some challenges, such as low selectivity or low current density. In this work, we showed that a copper-based metal-azolate framework (MAF), denoted as MAF-203, exhibits the high performance of eCO2RR to yield C2+ products with the Faradaic efficiency (C2+) of 52.5% and a current density of 660 mA/cm2 at −1.2 V vs. RHE in a flow cell device under alkaline condition. Controlled experiment, in situ infrared spectroscopy and the density functional theory (DFT) calculations showed that the electron donating effect of methyl substituents on organic ligands of the copper-based MAF could enhance the ligand field and activation of key intermediates (*CO and *CHO species), thus promoting the coupling of *CO and *CHO for yielding C2+ products.
The hierarchical assemblies of precise nanoparticles (NPs) have created materials with emergent properties and functionalities. However, the complex assemblies remain unclear at a precise scale. Here, we show the hierarchical self-assembly of atomically precise gold nanoclusters (Au NCs) with molecular rotor-based ligands (MRL), featuring a double-layer surface. Compared to two other types of monolayer-protected (MLP) Au NCs, the significantly reduced surface density for MRL Au NCs profoundly influences their assembly behavior within the lattice. Furthermore, the long length of rotor-based ligands and the rotational freedom of the phenyl-rings of rotor-based ligands also facilitate the assembly of NCs. Our works elucidate the hierarchical assembly on a precise scale, suggesting that the rotor-based ligand’s strategy offers promising potential for designing well-defined and more complex structures in supercrystals.
One-step harvest of high-purity methane (CH4) from ternary propane/ethane/methane (C3H8/C2H6/CH4) mixtures remains a desirable yet challenging goal for natural gas purification. However, adsorbents either suffer from high capacity and selectivity, or are caught in a dilemma of scalable synthesis. Herein, we demonstrate a scalable pillar layered metal-organic framework Ni-MOF for highly efficient one-step CH4 purification. Ni-MOF exhibits high C2H6 and C3H8 uptakes of 83.3 and 86.1 cm3/g at 298 K and 100 kPa and remarkable C2H6/CH4 (50/50, volume ratio, 21.5) and C3H8/CH4 (50/50, volume ratio, 212.0) selectivities. Notably, high C2H6 (42.2 cm3/g at 10 kPa) and C3H8 (64.7 cm3/g at 5 kPa) capacities in the low-pressure region at 298 K were realized on Ni-MOF, suggesting the strong affinities of Ni-MOF towards C2H6 and C3H8. Furthermore, the dynamic breakthrough experiments revealed that purifying CH4 from natural gas in one-step can be achieved in Ni-MOF with high-purity (>99.8%) and productivity (346.0 cm3/g). Most significantly, the production of Ni-MOF can be scalably synthesized at room temperature, rendering it promising potential for industrial application. The combined advantages of exceptional separation performance, scalability, and cycle stability of Ni-MOF pave the way for one-step CH4 purification from natural gas.
The construction of heterogeneous frustrated Lewis pairs (FLPs) catalysts is crucial for realizing highly efficient and recyclable pyridines catalytic hydrogenation. In this work, we prepared a recyclable heterogenous FLPs catalyst CMP-BF with conjugated microporous polymer CMP-ethynyl as the support via self-catalyzed 1,1-carboboration reaction with commercial Lewis acid B(C6F5)3. The as-synthesized CMP-BF demonstrates superior heterogenous catalytic hydrogenation performance (conversion>99%), and considerable stability (84% conversion after three cycles) in recyclable hydrogenation of 2,6-phenylpyridine. This work provides insights into the fabrication and catalytic application of recyclable heterogenous FLP catalysts.
Representing the next-generation technology in lithium-ion batteries, lithium-sulfur (Li-S) batteries offer increased specific energy without relying on scarce metals like nickel and cobalt, but suffer from a low practical specific energy due to poor conductivity and a short lifespan due to the shuttle effect of polysulfides. Balancing the confinement of polysulfides and the transport of lithium ions requires highly elaborate modifiers for separators. Hollow multi-shelled structures (HoMSs) show promise as hierarchical mesostructures for separators, offering multiple shell layers and internal cavities that effectively inhibit polysulfide shuttle. Thoughtful design of these structures is crucial to address these challenges effectively. In this study, nitrogen-doped carbon HoMS (NC HoMS) was created using polymer templates through a precisely controlled polymerization process. Batteries featuring NC HoMS-modified separators exhibit improved capacity and cycling stability in comparison to those utilizing commercial separators. Especially, triple-shelled NC HoMS strikes a balance in polysulfide containment and lithium ion transport. Featuring a sulfur loading of 6.34 mg/cm2, the Li-S battery can consistently complete 100 charge-discharge cycles, starting with a discharge capacity of 966.4 mA·h/g with a 75.8% capacity retention rate. NC HoMS holds potential as the separator modifier in addressing the polysulfide shuttle problem and facilitating the Li-ion transportation for advanced Li-S batteries.
Thienoacenes is one of most important groups of semiconducting materials due to the high stability and superior mobility. However, there are scarce studies on the emission properties of thienoacenes to date. Herein, we synthesized fluorinated and chlorinated dibenzo[d,d’]thieno[3,2-b;4,5-b’]dithiophenes (DBTDTs) derivatives F6-DBTDT and Cl6-DBTDT by sulfoxide cyclization, significantly lowering the energy levels relative to the parent compound DBTDT. According to single crystal structure analysis, F6-DBTDT molecules adopt one-dimensional slipped stacking with close π-π interactions of 3.43 Å (1 Å=0.1 nm), which is different from the parent compound DBTDT with herringbone stacking motif. Interestingly, the halogenated DBTDT derivatives exhibit enhanced emission properties both in solution and in the solid state, opening up possiblities to improve photoluminescence of thienoacences by halogenation.
Hollow zeolite microspheres have recently attracted much attention for their applications in catalysis, microreactors and biomedicine. Herein, we present hierarchically structured zeolite ZSM-5 microspheres with unique, abundant macropores that allow more efficient use for catalysis. The hierarchically macroporous zeolite ZSM-5 microspheres are synthesized under the assistance of water/oil emulsions and using polystyrene nanospheres as templates. The zeolite microsphere is assembled by uniform hollow zeolite nanospheres. Their large inner cavities and thin zeolite shells lead to smaller diffusion channel and higher improved accessibility to active sites, contributing to high catalytic performance in the catalytic conversion of benzyl alcohol in mesitylene. Such novel zeolite microspheres with impressive performance will be applied to numerous other industrial catalytic reactions.
Recently, the rapid development of non-fullerene acceptors (NFAs) has laid the foundation for performance improvements in near-infrared (NIR) organic photodetectors (OPDs). However, reducing the bandgap of NFAs to achieve strong absorption in the shorter-wave region usually leads to increased dark current density (J d) and decreased responsivity (R), severely limiting the detectivity (D*) of NIR-OPDs. To date, it remains challenging to manipulate the J d of NIR-OPDs through rational structure engineering of NFAs. Herein, three NIR-NFAs, namely bis(2-decyltetradecyl)4,4′-(2′,7′-di-tert-butylspiro[cyclopenta[2,1-b:3,4-b′]dithiophene-4,9′-fluorene]-2,6-diyl)bis(6-(((Z)-1-(dicyanomethylene)-5,6-difluoro-3-oxo-1,3-dihydro-2H-inden-2-ylidene)methyl)thieno[3,4-b]thiophene-2-carboxylate) (TSIC-4F), bis(2-decyltetradecyl)6,6′-(2′,7′-di-tert-butylspiro[cyclopenta[2,1-b:3,4-b′]dithiophene-4,9′-fluorene]-2,6-diyl)bis(4-(((Z)-1-(dicyanomethylene)-5,6-difluoro-3-oxo-1,3-dihydro-2H-inden-2-ylidene)methyl)thieno[3,4-b]thiophene-2-carboxylate) (STIC-4F), and 2,2′-((2Z,2′Z)-(((2′,7′-di-tert-butylspiro[cyclopenta [2,1-b:3,4-b′]dithiophene-4,9′-fluorene]-2,6-diyl)bis(2,3-bis(5-(2-butyloctyl)thiophen-2-yl)thieno[3,4-b]pyrazine-7,5-diyl))bis(metha-neylylidene))bis(5,6-difluoro-3-oxo-2,3-dihydro-1H-indene-2,1-diylidene))dimalononitrile (TPIC-4F), were designed using the thieno[3,4-b]thiophene (TT) and thieno[3,4-b]pyrazine (TPy) derivatives as the π-bridge. Owing to the intramolecular S-S and S-N interactions, STIC-4F and TPIC-4F exhibited smaller backbone distortions than TSIC-4F. A significantly red-shifted absorption with a peak at 1015 nm was observed in TPIC-4F film, larger than that (ca. 960 nm) for TSIC-4F and STIC-4F films. Moreover, OPDs operating in a photovoltaic mode were successfully fabricated, and TPIC-4F-based OPDs achieved the lowest J d of 3.18×10−8 A/cm2 at −0.1 V. Impressively, although TPIC-4F-based OPDs exhibited the lowest R, higher shot-noise-limited specific detectivity (D sh*) in 1000–1200 nm could be achieved due to its lowest J d. This study underscored the effectiveness of optimizing the π-bridge structure of NFAs to suppress J d, ultimately attaining higher D sh* in the NIR region.
Sodium gluconate (SG) is reported as an electrolyte additive for rechargeable aqueous zinc batteries. The SG addition is proposed to modulate the nucleation overpotential and plating behaviors of Zn by forming a shielding buffer layer because of the adsorption priority and large steric hindrance effect, which contributes to limited rampant Zn2+ diffusion and mitigated hydrogen evolution and corrosion. With the introduction of 30 mmol/L SG in 2 mol/L ZnSO4 electrolyte, the Zn anode harvests a reversible cycling of 1200 h at 5 mA/cm2 and a high average Coulombic efficiency of Zn plating/stripping (99.6%). Full cells coupling Zn anode with V2O5·1.6H2O or polyaniline cathode far surpass the SG additivefree batteries in terms of cycle stability and rate capability. This work provides an inspiration for design of a high-effective and low-cost electrolyte additive towards Zn-based energy storage devices.
Unsaturated ketones are typical oxygenated volatile organic compounds (OVOCs) with high reactivity, and are important precursors in air pollution. The sources of OVOCs are complex and include direct emissions and secondary oxidation formation of VOCs in the atmosphere. 2-Cyclohexen-1-one is a widespread substance, and is derived from the industrial catalytic oxidation of cyclohexene. In this paper, we investigated the rate constants of the chemical reactions of 2-cyclohexen-1-one with NO3 radicals, which is (7.25±0.29)×10−15 cm3·molecule−1·s−1 at 298 K and under 1 atm (1 atm=101325Pa). It supplemented the kinetics of NO3 radicals database, and revealed its effects in the nighttime atmosphere. In addition, the reaction products of 2-cyclohexen-1-one with NO3 radicals were detected by Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS), which revealed a series of nitrate esters in the composition of the secondary organic aerosol (SOA), which may reduce atmospheric visibility. Finally, the possible pathways for the generation of the products were developed.
Solid oxide electrolysis cells (SOECs) provide a promising way for converting renewable energy into chemical fuels. Traditionally, NiO/CGO (nickel-gadolinium doped ceria) cermet has shown its excellent properties in ionic and electronic conductivity under reducing conditions. Herein, we developed a novel 1D NiO/CGO cathode through a cerium metal-organic framework (MOF) derived process. The cathode’s 1D nanostructure integrated with a microchannel scaffold facilitates enhanced mass transport, providing vertically aligned pathways for CO2 and H2O diffusion. Additionally, the 1D framework increases the number of interfacial sites and reduces ion diffusion distances, thereby simplifying electron/ion transport. Consequently, this advanced cathode achieved a significant breakthrough in SOEC performance, maintaining efficient CO2 and H2O electrolysis at an extraordinary current density of 1.41 A/cm2 at 1.5 V and excellent stability over 24 h at 850 °C. The enhanced performance of this newly developed cathode not only achieves a remarkable 100% improvement compared to those of NiO/CGO cathodes with varying geometrical configurations but also surpasses those of commercial NiO/CGO catalysts by an outstanding 40% when tested under identical conditions. The development of the 1D NiO/CGO enhances the efficiency and durability of ceramic cathodes for CO2 and H2O co-electrolysis in SOECs and improves the scalability and effectiveness of SOECs in renewable energy applications.
A new acentric galloborate (GBO) [H2dab][GaB5O10] (1, 1,4-dab: 1,4-diaminobutane) has been synthesized under solvothermal conditions. The alternation of 4,4-connected GaO4 and B5O10 cluster build up the 3D [GaB5O10] n 2n− uninodal framework, which contains three pairs of helical channels with 8-member ring (MR) and 7-MR apertures, respectively. Compound 1 exhibits a moderate second harmonic generation (SHG) response of 1.8 times that of KH2PO4 (KDP), indicating its potential application in UV regions. The acentric uninodal framework in compound 1 represents a new type of zeolitic framework in the GBOs’ family.
PtCo nanoalloys (NAs) deposited on carbon black are emerging as robust electrocatalysts for addressing the sluggish kinetic issue of oxygen reduction reaction (ORR). However, developing a simple and low-cost method to synthesize PtCo/C with excellent performance is still a great challenge. In this work, a one-pot method was used to successfully obtain the PtCo NAs on commercial carbon supports of acetylene black and Ketjenblack ECP600JD, respectively. Compared with those grown on Ketjenblack ECP600JD, the PtCo NAs grown on acetylene black exhibited higher electrochemical surface area (ECSA) and mass activity (MA), which may be attributed to the different particle sizes of PtCo NAs, distinct hydrophilicity, electroconductivity and charge distribution between the carbon supports and PtCo NAs. Our study provides valuable insights into the optimal design of carbon-supported ORR electrocatalysts with exceptional activity and durability.