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131.
Covalent organic frameworks (COFs) are proposed as promising candidates for engineering advanced molecular sieving membranes due to their precise pore sizes, modifiable pore environment, and superior stability. However, COFs are insoluble in common solvents and do not melt at high temperatures, which presents a great challenge for the fabrication of COF-based membranes (COFMs). Herein, for the first time, a new synthetic strategy is reported to prepare continuous and intact self-standing COFMs, including 2D N-COF membrane and 3D COF-300 membrane. Both COFMs show excellent selectivity of H2/CO2 mixed gas (13.8 for N-COF membrane and 11 for COF-300 membrane), and especially ultrahigh H2 permeance (4319 GPU for N-COF membrane and 5160 GPU for COF-300 membrane), which is superior to those of COFMs reported so far. It should be noted that the overall separation performance of self-standing COFMs exceeds the Robeson upper bound. Furthermore, a theoretical study based on Grand Canonical Monte Carlo (GCMC) simulation is performed to explain the excellent separation of H2/CO2 through COFMs. Thus, this facile preparation method will provide a broad prospect for the development of self-standing COFMs with highly efficient H2 purification.  相似文献   
132.
Balancing the contradictory relationship between thermoelectric parameters, such as effective mass and carrier mobility, is a challenge to optimize thermoelectric performance. Herein, the exceptional thermoelectric performance is realized in GeTe through collaboratively optimizing the carrier and phonon transport via stepwise alloying Pb and CuSbSe2. The formation energy of Ge vacancy is efficiently bolstered by alloying Pb, which reduces carrier density and carrier scattering to maintain superior carrier mobility in GeTe. Additionally, CuSbSe2, acting as an n-type dopant, further modulates carrier density and validly equilibrates carrier mobility and effective mass. Accordingly, the promising power factor of 45 µW cm−1 K−2 is achieved at 723 K. Meanwhile, point defects are found to significantly suppress phonons transport to descend lattice thermal conductivity by Pb and CuSbSe2 alloying, which barely impacts the carrier mobility. A combination with superior carrier mobility and lower lattice thermal conductivity, a maximum ZT of 2.2 is attained in Ge0.925Pb0.075Cu0.005Sb0.005TeSe0.01, which corresponds to a 100% promotion compared with that of intrinsic GeTe. This study provides a new indicator for optimizing carrier and phonon transport properties by balancing interrelated thermoelectric parameters.  相似文献   
133.
Tomographic volumetric bioprinting (VBP) enables fast photofabrication of cell-laden hydrogel constructs in one step, addressing the limitations of conventional layer-by-layer additive manufacturing. However, existing biomaterials that fulfill the physicochemical requirements of VBP are limited to gelatin-based photoresins of high polymer concentrations. The printed microenvironments are predominantly static and stiff, lacking sufficient capacity to support 3D cell growth. Here a dynamic resin based on thiol–ene photo-clickable polyvinyl alcohol (PVA) and thermo-sensitive sacrificial gelatin for fast VBP of functional ultrasoft cell-laden hydrogel constructs within 7–15 s is reported. Using gelatin allows VBP of permissive hydrogels with low PVA contents of 1.5%, providing a stress-relaxing environment for fast cell spreading, 3D osteogenic differentiation of embedded human mesenchymal stem cells and matrix mineralization. Additionally, site-specific immobilization of molecules-of-interest inside a PVA hydrogel is achieved by 3D tomographic thiol–ene photopatterning. This technique may enable spatiotemporal control of cell-material interactions and guides in vitro tissue formation using programmed cell-friendly light. Altogether, this study introduces a synthetic dynamic photoresin enabling fast VBP of functional ultrasoft hydrogel constructs with well-defined physicochemical properties and high efficiency.  相似文献   
134.
Li-rich layered oxides (LLOs) have been considered as the most promising cathode materials for achieving high energy density Li-ion batteries. However, they suffer from continuous voltage decay during cycling, which seriously shortens the lifespan of the battery in practical applications. This review comprehensively elaborates and summarizes the state-of-the-art of the research in this field. It is started from the proposed mechanism of voltage decay that refers to the phase transition, microscopic defects, and oxygen redox or release. Furthermore, several strategies to mitigate the voltage decay of LLOs from different scales, such as surface modification, elemental doping, regulation of components, control of defect, and morphology design are summarized. Finally, a systematic outlook on the real root of voltage decay is provided, and more importantly, a potential solution to voltage recovery from electrochemistry. Based on this progress, some effective strategies with multiple scales will be feasible to create the conditions for their commercialization in the future.  相似文献   
135.
Anode-free batteries can maximize the energy density but their development is hindered by a lack of Li-rich cathodes for compensating the irreversible Li loss. Li2S cathode is particularly appealing to this desire due to 2.6–4.7 folds more Li content and 4.2–6.8 times higher capacity than conventional intercalation cathodes. But its practical application is hindered by poor stability against moisture attacking in the air. Herein, a facile expendable polymer sheathing strategy toward air-stable Li2S cathodes with high capacities for developing high-performance quasi-solid-state anode-free batteries without risk of cell leakage is reported. Tight protection by dense polymer barrier dramatically prolongs the lifetime of Li2S cathode by 2,000 times at least in the air. Such air-stable Li2S cathode allows for high compatibility of anode-free battery production with commercial schemes. More attractively, the polymer protective layer can in situ transform to multifunctional gel polymer electrolyte for releasing ionic pathways and enhancing cell performance by inhibiting LiPS loss and smoothing Li plating. With air-stable Li2S cathode, the quasi-solid-state anode-free cells are assembled in ambient environment to deliver superb volumetric energy density of 1093 Wh L−1. This study may shed new light to push the commercialization of high-energy and reliable anode-free batteries forward.  相似文献   
136.
Construction of high efficiency and stable Li metal anodes is extremely vital to the breakthrough of Li metal batteries. In this study, for the first time, groundbreaking in situ plasma interphase engineering is reported to construct high-quality lithium halides-dominated solid electrolyte interphase layer on Li metal to stabilize & protect the anode. Typically, SF6 plasma-induced sulfured and fluorinated interphase (SFI) is composed of LiF and Li2S, interwoven with each other to form a consecutive solid electrolyte interphase. Simultaneously, brand-new vertical Co fibers (diameter: ≈5 µm) scaffold is designed via a facile magnetic-field-assisted hydrothermal method to collaborate with plasma-enhanced Li metal anodes (SFI@Li/Co). The Co fibers scaffold accommodates active Li with mechanical integrity and decreases local current density with good lithiophilicity and low geometric tortuosity, supported by DFT calculations and COMSOL Multiphysics simulation. Consequently, the assembled symmetric cells with SFI@Li/Co anodes exhibit superior stability over 525 h with a small voltage hysteresis (125 mV at 5 mA cm−2) and improved Coulombic efficiency (99.7%), much better than the counterparts. Enhanced electrochemical performance is also demonstrated in full cells with commercial cathodes and SFI@Li/Co anode. The research offers a new route to develop advanced alkali metal anodes for energy storage.  相似文献   
137.
High current carrying capacity and high conductivity are two important indicators for materials used in microscale electronics and inverters. However, it is challenging to obtain high conductivity and high current carrying capacity at the same time since high conductivity requires a weakly bonded system to provide free electrons, while high current carrying capacity requires a strongly bonded system. In this paper, CuI@SWCNT networks by filling the single-walled carbon nanotubes (SWCNTs) with CuI is ingeniously prepared. CuI@SWCNT shows good stability due to the confinement protection of SWCNTs. Through the host-guest hybridization, CuI@SWCNT networks exhibit a current carrying capacity of 2.04 × 107 A cm−2 and a conductivity of 31.67 kS m−1. Their current carrying capacity and conductivity are significantly improved compared with SWCNT. The Kelvin probe force microscopy measurements show a drop of surface potential energy after SWCNT filled with CuI, indicating that the CuI guest molecules regulate the position of the Fermi level of SWCNTs, increasing carrier concentration, achieving high conductivity and high current carrying capacity. This study offers ideas and solutions for the regulation of high-performance carbon tube networks, which hold great promise for future applications in carbon-based electronic devices.  相似文献   
138.
A tunable circularly polarized square patch antenna with parasitic elements is designed for a wide frequency tuning range and high gain characteristics. The proposed antenna is constructed by one main patch and four semi-elliptic parasitic units. By loading four varactor diodes and adjusting their capacitance values, the tunable feature is performed to reallocate the corresponding working frequency. Moreover, the diagonal corners of the antenna are cut and loaded with varactor diodes, which provide the appropriate perturbation between the two orthogonality modes of the antenna, so as to ensure the circular polarization characteristic in the entire operating tuning band. The experimental results demonstrate that the reflection coefficient and axial ratio are less than −13 dB and 3 dB, respectively. The proposed antenna features a relatively wide continuously tuning range of 24% within 1.9-2.3 GHz and a stable gain of over 7 dBi with a radiation efficiency of above 85%.  相似文献   
139.
In this study, a series of donor–acceptor–donor (D-A-D) type small molecules based on the fluorene and diphenylethenyl enamine units, which are distinguished by different acceptors, as holetransporting materials (HTMs) for perovskite solar cells is presented. The incorporation of the malononitrile acceptor units is found to be beneficial for not only carrier transportation but also defects passivation via Pb–N interactions. The highest power conversion efficiency of over 22% is achieved on cells based on V1359, which is higher than that of spiro-OMeTAD under identical conditions. This st shows that HTMs prepared via simplified synthetic routes are not only a low-cost alternative to spiro-OMeTAD but also outperform in efficiency and stability state-of-art materials obtained via expensive cross-coupling methods.  相似文献   
140.
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