Latest ArticlesFor large-scale energy storage devices, all-solid-state sodium-ion batteries (SIBs) have been revered for the abundant resources, low cost, safety performance and a wide operating temperature range. Na-ion solid-state electrolytes (Na-ion SSEs) are the critical parts and mostly determine the electrochemical performance of SIBs. Among the studied ones, inorganic Na-ion SSEs stand out for their good safety performance and high ionic conductivity. In this review, we outline the research progress of inorganic SSEs in SIBs based on the perspectives of crystal structure, performance optimization, synthesis methods, all-solid-state SIBs, interface modification and related characterization techniques. We hope to provide some ideas for the design of future high-performance Na-ion SSEs.
Molecular catalysts can effectively steer the electrocatalytic acetylene semihydrogenation into ethylene, but realizing high Faradaic efficiency (FE) at industrial current densities remains a challenge. Herein, we report a ligand engineering strategy that utilizes polymeric N-heterocyclic carbene (NHC) as a hydrophobic ligand to modulate the microenvironment of Cu sites. This polymeric NHC imparts appropriate hydrophobic properties for the chelated Cu sites, thereby moderating the H2O transport and enabling easy access of acetylene. Consequently, the polymeric NHC chelated Cu exhibits an FEethylene of ~97% at a current density of 500 mA/cm2 in a flow cell. Particularly in a zero-gap reactor, the FEethylene consistently exceeds 86% across current densities from 100 mA/cm2 to 400 mA/cm2, reaching an optimal FEethylene of 98% at 200 mA/cm2 and achieving durable operation for 155 h at 100 mA/cm2. This work provides a promising paradigm to regulate the microenvironment of molecular catalysts for improving electrocatalytic performances under industrial current densities.
Aryl-ether bonds are facile to attack by oxidizing radicals, thus stimulating the exploitation of ether-free polymers as proton exchange membranes (PEMs) for the long-lasting operation of fuel cells. In this study, a novel class of PEMs derived from all-carbon fluorinated backbone polymers containing sulfide-linked alkyl sulfonic acid side chains have been developed through a straightforward and effective synthetic procedure. The sulfide-linked alkyl sulfonate groups were tethered to the poly(triphenylene pentafluorophenyl) backbone through a quantified and site-specific para-fluoro-thiol click reaction. Owing to the existence of obvious phase separation morphology between hydrophobic main chain and hydrophilic sulfonate groups in the side chains, resulting PEMs demonstrated favorable proton conductivity of 142.5 mS/cm at 80 ℃, while maintaining excellent dimensional stability with an in-plane swelling ratio of <17% as well as a through-plane swelling ratio of <25%. They also exhibit elevated thermal decomposition temperatures (Td5% exceeding 300 ℃) alongside high tensile strength (>50 MPa). Furthermore, the ether-free full-carbon fluorinated main chain and the -S- group in the side chain, which serves as an effective free-radical scavenger, providing good chemical stability during Fenton's test. The PEMs achieved a maximum power density of 407 mW/cm2 in a single H2/air fuel cell, and an open-circuit voltage decline rate of 0.275 mV/h in a durability test at 30% RH and 80 ℃. Concurrently, the hydrogen crossover current density is only 1/3 of that of Nafion 212. These findings reveal that the resulted PEMs display considerable antioxidative properties along with commendable performance, with prospective applications in proton exchange membrane fuel cells.
Single-molecule junctions are building blocks for constructing molecular devices. However, intermolecular interactions like winding bring additional interference among the surrounding molecules, which inhibits the intrinsic coherent transport through single-molecule junctions. Here, we employed a nanocavity (dimethoxypillar[5]arene, DMP[5]), which is analogous to electric cables, to confine the conformation of flexible chains (1,8-diaminooctane, DAO) via host-guest interaction. Single-molecule conductance measurements indicate that the conductance of DAO encapsulated with DMP[5] is as high as that of pure DAO, as reproduced by theoretical simulations. Intriguingly, the molecular lengths of the DAO encapsulated with DMP[5] increase from 1.13 nm to 1.46 nm compared with the pure DAO, indicating that DMP[5] keeps DAO upright-standing via the confinement effect. This work provides a new strategy to decouple the intermolecular interaction by employing an insulating sheath, enabling the high-density integration of single-molecule devices.
Enhancing the corrosion resistance of carriers within Fenton-like systems and inhibiting the migration and aggregation of single atoms in reaction environments are essential for maintaining both high activity and stability at catalytic sites, thus meeting fundamental requirements for practical application. The Fenton-like process of activating various strong oxidants by silicon-based single atom catalysts (SACs) prepared based on silicon-based materials (mesoporous silica, silicon-based minerals, and organosilicon materials) has unique advantages such as structural stability (especially important under strong oxidation conditions) and environmental protection. In this paper, the preparation strategies for the silicon-based SACs were assessed first, and the structural characteristics of various silicon-based SACs are systematically discussed, their application process and mechanism in Fenton-like process to achieve water purification are investigated, and the progress of Fenton-like process in density functional theory (DFT) of silicon-based derived single atom catalysts is summarized. In this paper, the preparation strategies and applications of silicon-based derived SACs are analyzed in depth, and their oxidation activities and pathways to different pollutants in water are reviewed. In addition, this paper also summarizes the device design and application of silicon-based derived SACs, and prospects the future development of silicon-based SACs in Fenton-like applications.
Rapid carrier recombination and slow charge transfer dynamics have significantly reduced the performance of photocatalytic hydrogen production. Construction of heterojunctions via utilizing the sulfur-edge and metal-edge sites of metal sulfide semiconductor for improving photocatalytic activity remains a significant challenge. Herein, a novel ZnIn2S4/MnS S-scheme heterojunction was prepared by hydrothermal synthesis to accelerate charge carrier transfer for efficient photocatalysis. Notably, ZnIn2S4/MnS exhibited excellent photocatalytic hydrogen evolution activity (7.95 mmol g−1 h−1) under visible light irradiation (≥420 nm), up to 4.7 times higher than that of pure ZnIn2S4. Additionally, cycling experiments showed that ZM-2 remained high stability after four cycles. Density-functional theory (DFT) calculations and in situ XPS results confirm the formation of S-scheme heterojunction, indicating that the tight interfacial contact between ZnIn2S4 and MnS with the presence of Mn-S bonds (the unsaturated Mn edges of MnS and the uncoordinated S atoms in the edge of ZnIn2S4) promoted faster charge transfer. Besides, the unsaturated S atom on the surface of MnS is an active site with strong H+ binding ability, which can effectively reduce the overpotential or activation barrier for hydrogen evolution. This study illustrates the critical influence of the interfacial Mn-S bond on the ZnIn2S4/MnS S-scheme heterojunction to achieve efficient photocatalytic hydrogen production and provides relevant guidance for carrying out rational structural/interfacial modulation.
Protein damage repair and prevention are important objectives in skin care industry. Skin protein damage or modifications such as glycation, carbonylation or oxidation, have a significant impact on its function, therefore directly influencing various skin functions or properties including skin appearance. However, there is a lack of comprehensive methods to visualize and assess the protein damage. In this article, we present a three-channel imaging approach to simultaneously visualize and quantitatively evaluate protein oxidation, protein glycation and carbonylation in a full-thickness skin model. We successfully visualized and quantified the impact of the multiple stimuli (ultraviolet radiation A (UVA) and/or methylglyoxal) as well as treatment effect of positive control (vitamins C and E) with this method. Our findings indicate that multiple stimuli exhibit synergistic effects on protein damage. Furthermore, we evaluated a unique combination of skin care ingredients which demonstrated an excellent efficacy in resisting protein damage. Further research revealed that three ingredients of the combination upregulate autophagy in cells, which may contribute to remove damaged proteins and maintain protein quality homeostasis. This method provides a holistic assessment of protein damages and can be employed to evaluate the impact of various stimuli or to assess the efficacy of skin care ingredients in mitigating such damage.
Organic semiconductor materials have demonstrated extensive potential in the field of gas sensors due to the advantages including designable chemical structure, tunable physical and chemical properties. Through density functional theory (DFT) calculations, researchers can investigate gas sensing mechanisms, optimize, and predict the electronic structures and response characteristics of these materials, and thereby identify candidate materials with promising gas sensing applications for targeted design. This review concentrates on three primary applications of DFT technology in the realm of organic semiconductor-based gas sensors: (1) Investigating the sensing mechanisms by analyzing the interactions between gas molecules and sensing materials through DFT, (2) simulating the dynamic responses of gas molecules, which involves the behavior on the sensing interface using DFT combined with other computational methods to explore adsorption and diffusion processes, and (3) exploring and designing sensitive materials by employing DFT for screening and predicting chemical structures, thereby developing new sensing materials with exceptional performance. Furthermore, this review examines current research outcomes and anticipates the extensive application prospects of DFT technology in the domain of organic semiconductor-based gas sensors. These efforts are expected to provide valuable insights for further in-depth exploration of DFT applications in sensor technology, thereby fostering significant advancements and innovations in the field.
Quantum dots (QDs), a type of nanoscale semiconductor material with unique optical and electrical properties like adjustable emission and high photoluminescence quantum yields, are suitable for applications in optoelectronics. However, QDs are typically degraded under humid and high-temperature circumstances, greatly limiting their practical value. Coating the QD surface with an inorganic silica layer is a feasible method for improving stability and endurance in a variety of applications. This paper comprehensively reviews silica coating methodologies on QD surfaces and explores their applications in optoelectronic domains. Firstly, the paper provides mainstream silica coating approaches, which can be divided into two categories: in-situ hydrolysis of silylating reagents on QD surfaces and template techniques for encapsulation QDs. Subsequently, the recent applications of the silica-coated QDs on optoelectronic fields including light-emitting diodes, solar cells, photodetectors were discussed. Finally, it reviews recent advances in silica-coated QD technology and prospects for future applications.
Mitochondria are crucial organelles responsible for maintaining cell growth, and their homeostasis is closely linked to pH regulation. Physiologically, mitochondria exhibit a weakly alkaline state (pH~8.0). However, when subjected to stress stimuli that cause damage, cells initiate the process of mitophagy, resulting in mitochondrial acidification. Therefore, monitoring changes in mitochondrial pH to comprehend the physiological processes associated with mitophagy is essential. In this study, we developed an asymmetric pentamethine cyanine dye Cy5.5-H-CyN as a probe for continuous monitoring of mitophagy in living cells. By incorporating an azaindole structure into the dye molecule, a ratiometric fluorescence response was achieved that is specifically responsive to pH variations while preserving its ability to target mitochondria and emit near-infrared fluorescence. Through various methods inducing mitophagy, Cy5.5-H-CyN was employed to determine mitochondrial pH quantitatively, demonstrating its suitability as an ideal probe for continuous monitoring of mitophagy in living cells.
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