Notes

A-Site Impact on the particular Corrosion Means of Sn-Halide Perovskite: First-Principles Data.
More importantly, a universal facile strategy of H-bonding-dominating construction of MPc-involved heterojunctions is successfully established.Memory devices have been advanced so much, but still it is highly required to find stable and reliable materials with low-power consumption. Halide perovskites (HPs) have been recently adopted for memory application since they have advantages of fast switching based on ionic motion in crystal structure. However, HPs also suffer from poor stability, so it is necessary to improve the stability of HPs. In this regard, combined first-principles screening and experimental verification are performed to design HPs that have high environmental stability and low-operating voltage for memory devices. First-principles screening identifies 2D layered AB2X5 structure as the best candidate switching layer for memory devices, because it has lower formation energy and defect formation energy than 3D ABX3 or other layered structures (A3B2X7, A2BX4). To verify results, all-inorganic 2D layered CsPb2Br5 is synthesized and used in memory devices. The memory devices that use CsPb2Br5 show much better stability and lower operating voltages than devices that use CsPbBr3. These findings are expected to provide new opportunity to design materials for reliable device applications based on calculation, screening, and experimental verification.Simultaneously achieving high efficiency and high durability in perovskite solar cells is a critical step toward the commercialization of this technology. Inverted perovskite photovoltaic (IP-PV) cells incorporating robust and low levelized-cost-of-energy (LCOE) buffer layers are supposed to be a promising solution to this target. However, insufficient inventory of materials for back-electrode buffers substantially limits the development of IP-PV. Herein, a composite consisting of 1D cation-doped TiO2 brookite nanorod (NR) embedded by 0D fullerene is investigated as a top modification buffer for IP-PV. The cathode buffer is constructed by introducing fullerene to fill the interstitial space of the TiO2 NR matrix. Meanwhile, cations of transition metal Co or Fe are doped into the TiO2 NR to further tune the electronic property. Such a top buffer exhibits multifold advantages, including improved film uniformity, enhanced electron extraction and transfer ability, better energy level matching with perovskite, and stronger moisture resistance. Correspondingly, the resultant IP-PV displays an efficiency exceeding 22% with a 22-fold prolonged working lifetime. The strategy not only provides an essential addition to the material inventory for top electron buffers by introducing the 0D1D composite concept, but also opens a new avenue to optimize perovskite PVs with desirable properties.Colloidal liquid crystals (LCs) formed by nanoparticles hold great promise for creating new structures and topologies. However, achieving highly ordered hierarchical architectures and stable topological configurations is extremely challenging, mainly due to the liquid-like fluidity of colloidal LCs in nature. Herein, an innovative synchronous nanofluidic rectification (SNR) technique for generating ultralong graphene oxide (GO) liquid crystal (GOLC) fibers with hierarchical core-skin architectures is presented, in which the GO sheet assemblies and hydrogel skin formation are synchronous. The SNR technique conceptually follows two design principles horizontal polymer-flow promotes the rapid planar alignment of GO sheets and drives the chiral-reversing of cholesteric GOLCs, and in situ formed hydrogel skin affords some protection against environmental impact to maintain stable topological configurations. Importantly, the dried fibers retain the smooth surface and ordered internal structures, achieving high mechanical strength and flexibility. The linear and circular polarization potential of GOLC fibers are demonstrated for optical sensing and recognition. This work may open an avenue toward the scalable manufacture of uniform and robust, yet highly anisotropic, fiber-shaped functional materials with complex internal architectures.Polysaccharides are a class of carbohydrates that play pivotal roles in living systems such as being chemical messengers in many vital biological pathways. However, the complexity and heterogeneity of these natural structures have posed daunting challenges on their production, characterization, evaluation, and applications. While there have been various types of synthetic skeletons that could mimic some biological aspects of polysaccharides, a safer and more easily accessed system is still desired to avoid the unnatural components and difficulties in modifying the structures. In this work, conveniently accessible self-assembling glycopeptide conjugates are developed, where the natural O-glycosidic linkages and phosphoryl modifications assist the self-assembly and concurrently reduce the risk of toxicity. The generated nanoparticles in aqueous solution offer a multivalent display of structurally controllable carbohydrates as mimics of polysaccharides, among which a mannosylated version exhibits immunostimulatory effects in both cellular assays and vaccination of mice. The obtained results demonstrate the potential of this glycopeptide conjugate-derived platform in exploiting the intriguing properties of carbohydrates in a more structurally maneuverable fashion.A breakthrough utilizing an anionic redox reaction (O2-/On-) for charge compensation has led to the development of high-energy cathode materials in sodium-ion batteries. However, its reaction results in a large voltage hysteresis due to the structural degradation arising from an oxygen loss. Herein, an interesting P2-type Mn-based compound exhibits a distinct two-phase behavior preserving a high-potential anionic redox (≈4.2 V vs Na+/Na) even during the subsequent cycling. Through a systematic series of experimental characterizations and theoretical calculations, the anionic redox reaction originating from O 2p-electron and the reversible unmixing of Na-rich and Na-poor phases are confirmed in detail. In light of the combined study, a critical role of the anion-redox-induced two-phase reaction in the positive-negative point of view is demonstrated, suggesting a rational design principle considering the phase separation and lattice mismatch. Furthermore, these results provide an exciting approach for utilizing the high-voltage feature in Mn-based layered cathode materials that are charge-compensated by an anionic redox reaction.Biohybrid microswimmers exploit the swimming and navigation of a motile microorganism to target and deliver cargo molecules in a wide range of biomedical applications. #link# Medical biohybrid microswimmers suffer from low manufacturing yields, which would significantly limit their potential applications. In the present study, a biohybrid design strategy is reported, where a thin and soft uniform coating layer is noncovalently assembled around a motile microorganism. link2 Chlamydomonas reinhardtii (a single-cell green alga) is used in the design as a biological model microorganism along with polymer-nanoparticle matrix as the synthetic component, reaching a manufacturing efficiency of ≈90%. Natural biopolymer chitosan is used as a binder to efficiently coat the cell wall of the microalgae with nanoparticles. The soft surface coating does not impair the viability and phototactic ability of the microalgae, and allows further engineering to accommodate biomedical cargo molecules. Furthermore, by conjugating the nanoparticles embedded in the thin coating with chemotherapeutic doxorubicin by a photocleavable linker, on-demand delivery of drugs to tumor cells is reported as a proof-of-concept biomedical demonstration. The high-throughput strategy can pave the way for the next-generation generation microrobotic swarms for future medical active cargo delivery tasks.Continual precision actuations with nanoscale resolution over large ranges have extensive requirements in advanced intelligent manufacturing and precise surgical robots. To produce continual nanostep motion, conventionally, multiple pairs of piezo-actuators are employed to operate in inchworm principle under complex three- or four-phase timing signal drive. Inspired by the idea of ordered structures with functional units, a much simpler nanostep piezoelectric actuator consisting of (2 × 2) arrayed, cofired multilayer piezoceramic actuation units is developed, which operates in an artificially generated quasi shear mode (AGQSM) that is missing in natural piezoelectric ceramics. Under only one-phase square-wave voltage drive, the actuator can produce a stable, continual nanostep motion in two ways at nonresonant frequencies, and the obtained minimum step displacement is as low as 7 nm in open control, indicating its potential application as a precise finger or knife actuator in surgical robots. This work is of great guiding significance for future actuator designs using the methodology of ordered structure with piezoceramic actuation units and AGQSM.Compartmentalized microfluidic platforms are an invaluable tool in neuroscience research. However, harnessing the full potential of this technology remains hindered by the lack of a simple fabrication approach for the creation of intricate device architectures with high-aspect ratio features. Here, a hybrid additive manufacturing approach is presented for the fabrication of open-well compartmentalized neural devices that provides larger freedom of device design, removes the need for manual postprocessing, and allows an increase in the biocompatibility of the system. Suitability of the method for multimaterial integration allows to tailor the device architecture for the long-term maintenance of healthy human stem-cell derived neurons and astrocytes, spanning at least 40 days. Leveraging fast-prototyping capabilities at both micro and macroscale, a proof-of-principle human in vitro model of the nigrostriatal pathway is created. link3 By presenting a route for novel materials and unique architectures in microfluidic systems, the method provides new possibilities in biological research beyond neuroscience applications.Solvent additives are known to modify the morphology of bulk heterojunction active layers to achieve high efficiency organic solar cells. However, the knowledge about the influence of solvent additives on the morphology degradation is limited. Hence, in operando grazing-incidence small and wide angle X-ray scattering (GISAXS and GIWAXS) measurements are applied on a series of PffBT4T-2ODPC71BM-based solar cells prepared without and with solvent additives. Raltitrexed fabricated without a solvent additive, with 1,8-diiodoctane (DIO), and with o-chlorobenzaldehyde (CBA) additive show differences in the device degradation and changes in the morphology and crystallinity of the active layers. The mesoscale morphology changes are correlated with the decay of the short-circuit current Jsc and the evolution of crystalline grain sizes is codependent with the decay of open-circuit voltage Voc. Without additive, the loss in Jsc dominates the degradation, whereas with solvent additive (DIO and CBA) the loss in Voc rules the degradation. CBA addition increases the overall device stability as compared to DIO or absence of additive.
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