Latest ArticlesThe poor interfacial contact is one of the biggest challenges that solid-state lithium batteries suffer from. Reducing the solid-state electrolyte surface energy by transforming the interface from lithiophobic to lithiophilic is effective to promote the interfacial contact, but electronic conductive interphases usually increase the risk of electron attack, thus leading to uncontrollable Li dendrite growth. Herein, we propose a self-assembled thermodynamic stable LiI interphase to simultaneously improve the interfacial contact between the garnet electrolyte Li7La3Zr2O12 (LLZO) and Li anode, and prohibit the electron attack. The direct contact between LLZO and Li and the high temperature Li melting process was ascribed to Zr4+ reduction, which facilitated Li dendrite formation and propagation. With the modification of the high lithiophilic I2 thin film, the area specific interfacial resistance of LLZO/Li was reduced from 1525 Ω/cm2 to 57 Ω/cm2. More importantly, LLZO was protected from being reduced due to the outstanding electronic insulativity of the LiI interphase, which leaded to a high critical current density of 1.2/7.0 mA/cm2 in the time/capacity-constant modes, respectively.
Developing narrow-bandgap organic semiconductors is important to facilitate the advancement of organic photovoltaics (OPVs). Herein, two near-infrared non-fused ring acceptors (NIR NFRAs), PTBFTT-F and PTBFTT-Cl have been developed with A-πA-πD-D-πD-πA-A non-fused structures. It is revealed that the introduction of electron deficient π-bridge (πA) and multiple intramolecular noncovalent interactions effectively retained the structural planarity and intramolecular charge transfer of NFRAs, extending strong NIR photon absorption up to 950 nm. Further, the chlorinated acceptor, with the enlarged π-surface compared to the fluorinated counterpart, promoted not only molecular stacking in solid, but also the desirable photochemical stability in ambient, which are helpful to thereby improve the exciton and charge dynamics for the corresponding OPVs. Overall, this work provides valuable insights into the design of NIR organic semiconductors.
Coordination complex of a copper cyanurate (Cu(Ⅱ)-CA) was transformed into coordination polymers upon the stimulus of extra Cu(Ⅱ) through "directed Ostwald ripening". By increasing the molar ratio of Cu(Ⅱ) to CA, we obtained two coordination polymers with selective coordination sites: Cu(Ⅱ)-κN(HCA)κN-Cu(Ⅱ) and Cu(Ⅱ)-κN(HCA)κO-Cu(Ⅱ), which display disparate magnetic interactions.
Humans have relied on biomass for survival and development since the Stone Age. All aspects of human needs for materials are covered by tools, fuel, and buildings. Nowadays, metals and petroleum-based materials are widely used in highly developed industries. Unfortunately, environmental contamination and the loss of natural resources have led to the reemergence of biomass resources as efficient and sustainable energy sources. Notably, simple and direct applications can no longer meet the demand for functionalization, high performance of materials and construction materials. Therefore, it is imperative to modify biomass and combine its utilisation to produce functionalization and high performance materials. For example, construction materials with superior mechanical properties and water resistance can be produced by reinforcing fibres to facilitate crosslinking. Water-oil separation or adsorption effects of hydrogels and aerogels are determined by the porosity and lightness of biomass, biocomposite conductor is prepared by chimaeric conductive material. Here, we review the approaches that have been taken to devise an environmentally friendly yet fully recyclable and sustainable functionalised biocomposites from biomass and its potential directions for future research.
Electrolyte design is essential for stabilizing lithium metal anodes and localized high-concentration electrolyte (LHCE) is a promising one. However, the state-of-the-art LHCE remains insufficient to ensure long-cycling lithium metal anodes. Herein, regulating the solvation structure of lithium ions in LHCE by weakening the solvating power of diluents is proposed for improving LHCE performance. A diluent, 1,1,2,2,3,3,4,4-octafluoro-5-(1,1,2,2-tetrafluoroethoxy) pentane (OFE), with weaker solvating power is introduced to increase the proportion of aggregates (an anion interacts with more than two lithium ions, AGG-n) in electrolyte compared with the commonly used 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether (TTE). The decomposition of AGG-n in OFE-based LHCE intensifies the formation of anion-derived solid electrolyte interphase and improves the uniformity of lithium deposition. Lithium metal batteries with OFE-based LHCE deliver a superior lifespan of 190 cycles compared with 90 cycles of TTE-based LHCE under demanding conditions. Furthermore, a pouch cell with OFE-based LHCE delivers a specific energy of 417 Wh/kg and undergoes 49 cycles. This work provides guidance for designing high-performance electrolytes for lithium metal batteries.
The electric field-induced irreversible domain wall motion results in a ferroelectric (FE) hysteresis. In antiferroelectrics (AFEs), the irreversible phase transition is the main reason for the hysteresis effects, which plays an important role in energy storage performance. Compared to the well-demonstrated FE hysteresis, the structural mechanism of the hysteresis in AFE is not well understood. In this work, the underlying correlation between structure and the hysteresis effect is unveiled in Pb(Zr, Sn, Ti)O3 AFE system by using in-situ electrical biasing synchrotron X-ray diffraction. It is found that the AFE with a canting dipole configuration, which shows a continuous polarization rotation under the electric field, tends to have a small hysteresis effect. It presents a negligible phase transition, a small axis ratio, and electric field-induced lattice changing, small domain switching. All these features together lead to a slim hysteresis loop and a high energy storage efficiency. These results offer a deep insight into the structure-hysteresis relationship of AFEs and are helpful for the design of energy storage material.
In the physiological environment, nanoparticles (NPs) interact with proteins to form a protein-rich layer on the surface which is called "protein corona". Understanding and analyzing the formation process of protein corona and protein corona-nanoparticles is of great significance for biological related nano research. Many separation techniques have been used to analyze the composition of protein corona, but in situ analysis of protein corona is still absent. With the development of detection technology, sum frequency generation (SFG) is an effective instrument to analyze the surface protein structure and dynamic changes of protein corona in situ. In this work the molecular mechanism and surface structure effect of the interaction between nanoparticles with surface protein corona (S-NPP) and phospholipid membrane were studied. When S-NPP interacts with phospholipid membrane, the bond affinity network formed by the binding water can stabilize S-NPP around the lipid bilayer. In this process, S-NPP can be found wrapped in the hydration shell. This ultimately leads to a more moderate interaction between particles and phospholipid membrane.
Rechargeable aluminum batteries with multi-electron reaction have a high theoretical capacity for next generation of energy storage devices. However, the diffusion mechanism and intrinsic property of Al insertion into MnO2 are not clear. Hence, based on the first-principles calculations, key influencing factors of slow Al-ions diffusion are narrow pathways, unstable Al-O bonds and Mn3+ type polaron have been identified by investigating four types of δ-MnO2 (O3, O'3, P2 and T1). Although Al insert into δ-MnO2 leads to a decrease in the spacing of the Mn-Mn layer, P2 type MnO2 keeps the long (spacious pathways) and stable (2.007–2.030 Å) Al-O bonds resulting in the lower energy barrier of Al diffusion of 0.56 eV. By eliminated the influence of Mn3+ (low concentration of Al insertion), the energy barrier of Al migration achieves 0.19 eV in P2 type, confirming the obviously effect of Mn3+ polaron. On the contrary, although the T1 type MnO2 has the sluggish of Al-ions diffusion, the larger interlayer spacing of Mn-Mn layer, causing by H2O could assist Al-ions diffusion. Furthermore, it is worth to notice that the multilayer δ-MnO2 achieves multi-electron reaction of 3|e|. Considering the requirement of high energy density, the average voltage of P2 (1.76 V) is not an obstacle for application as cathode in RABs. These discover suggest that layered MnO2 should keep more P2-type structure in the synthesis of materials and increase the interlayer spacing of Mn-Mn layer for providing technical support of RABs in large-scale energy storage.
Photoacoustic agents combining photodynamic therapy (PDT) and photothermal therapy (PTT) functions have emerged as potent theranostic agents for combating cancer. The molecular approaches for enhancing the near-infrared (NIR)-absorption and maximizing non-radiative energy transfer are essential for effective photoacoustic imaging (PAI) and therapy applications. In addition, such molecules with high specificity and affinity to cancer cells are urgently needed, which would further decrease the side effect during treatments. In this study, we applied a heavy-atom engineering strategy and introduced p-aminophenol, -thio, and -seleno moieties into NIR heptamethine cyanine (Cy7) skeleton (Cy7-X-NH2, X = O, S, Se) to significantly increase photothermal conversion efficiency for PTT and promote intersystem crossing for PDT. Additionally, we designed a series of nitroreductase (NTR)-activated photoacoustic probes (Cy7-X-NO2, X = O, S, Se), and target hypoxic tumors with NTR overexpression. Our prostate cancer targeting probe, Cy7-Se-NO2-KUE, exhibited specific tumor photoacoustic signals and effective tumor killing through outstanding synergistic PTT/PDT in vivo. These findings highlighted a versatile strategy for cancer photoacoustic diagnosis and enhanced phototherapy.
Microchannels enable the fast and efficient mixing of multiphase fluids. In this study, a millimeter-scale three-dimensional (3D) circular cyclone-type microreactor was designed for the mixing. The flow characteristics and mixing intensity were simulated by computational fluid dynamics simulations at a flow rate range of 12–96 mL/min using a water/ethyl acetate system. In the 3D variable-diameter structure, the microreactor induced paired opposite vortices and abruptly changed the local pressure to achieve a stable turbulent effect within the theoretical range of laminar flow. Tracer injection simulations indicated that sufficient mixing units successfully promote fluid dispersion. Diazo-coupling experiments showed a segregation index of XS = 0. 00,039 within a residence time of 9 s. Extraction experiments on the n-butanol/succinic acid/water system showed that the 3D circular cyclone-type microreactor achieved 100% extraction efficiency (E) in 4.25 s, and the overall volume mass transfer coefficient (KLa) reached 0.05–1.5 s-1 in 12–96 mL/min. The isolated yield of the phase transfer alkylation and oxidation reactions in the 3D circular cyclone-type microreactor achieved 99% within 36 s, which was superior to the coil microreactor and batch reactor.
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