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Ternary copolymerization is a cost‐effective and time‐saving approach to improve device performance and batch stability of polymer donors. However, the structure of the ternary polymer donor obtained by the traditional one‐pot polymerization is vague due to the different monomer reaction order, which has a great influence on the absorption, crystallization, molecular stacking, and device performance. Therefore, it is necessary to obtain terpolymers with definite structures, and systematically study the differences in device properties of polymers with different sequence structures. Herein, three terpolymers D1, D2, and D3 are developed. Random copolymer D3 is obtained via the traditional one‐pot method while alternating copolymer donor D1 and block copolymer D2 are synthesized by stepwise polymerization. Because the block copolymer D2 possess periodic sequence distribution and retains the excellent properties of the two polymer matrix very well, the D2‐based device shows enhanced tightened π‐face‐on molecular stacking, distinguished efficient exciton dissociation, and decreased energy loss. As a result, the D2:L8‐BO‐based polymer solar cells achieve one of a record power conversion efficiency of 19.03%. The work demonstrates changing the sequence structure of the polymers to synthesize well‐defined structures polymer donors not only maintains the features of polymer matrix, but also combines the advantages of ternary copolymerization. [ABSTRACT FROM AUTHOR]

High‐performance bio‐based fibers have unique advantages in biocompatibility for biomedical applications, such as sutures, hernia patches, and blood vessels. Herein, strong and tough biofibers based on regenerated silk fibroins (RSFs) are designed by a dual‐crosslinking strategy and prepared continuously in situ via a single‐channel microfluidic device. During the wet spinning process, covalent bonds between tyrosines are introduced by photo crosslinking and coordination interactions of Zn2+ ions with serines are built between RSFs, forming a dual‐crosslinked, and inter‐connected network and effectively improving the mechanical performances of RSF fibers. By optimizing the wet spinning parameters and applying an optimal post‐stretching treatment, dual‐crosslinked RSF fibers exhibit an excellent tensile strength of 891 MPa, a remarkable Young's modulus of 15.0 GPa, a large tensile strain of 20.1%, and an outstanding toughness of 114 MJ m−3, which are superior to other regenerated biofibers. In addition to the outstanding mechanical performances, dual‐crosslinked RSF fibers also possess excellent temperature adaptability, fatigue resistance, biocompatibility, and biodegradability, making them ideal candidates for biomedical applications. In vivo tests of dual‐crosslinked RSF fibers as sutures demonstrate a good wound healing performance with smaller scar and lower inflammation. [ABSTRACT FROM AUTHOR]

Electrochemically converting waste nitrate (NO3−) into ammonia (NH3) is a green route for both wastewater treatment and high‐value‐added ammonia generation. However, the NO3−‐to‐NH3 reaction involves multistep electron transfer and complex intermediates, making it a grand challenge to drive efficient NO3− electroreduction with high NH3 selectivity. Herein, an in‐operando electrochemically synthesized Cu2O/NiO heterostructure electrocatalyst is proven for efficient NH3 electrosynthesis. In situ Raman spectroscopy reveals that the obtained Cu2O/NiO, induced by the electrochemistry‐driven phase conversion, is the real active phase. This electronically coupled phase can modulate the interfacial charge distribution, dramatically lower the overpotential in the rate‐determining step and thus requiring lower energy input to proceed with the NH3 electrosynthesis. The orbital hybridization calculations further identify that Cu2O is beneficial for NO3− adsorption, and NiO could promote the desorption of NH3, forming an excellent tandem electrocatalyst. Such a tandem system leads to NH3 Faradaic efficiency of 95.6%, a super‐high NH3 selectivity of 88.5% at −0.2 V versus RHE, surpassing most of the NH3 electrosynthesis catalysts at an ultralow reaction voltage. [ABSTRACT FROM AUTHOR]

Halide perovskites are potential next‐generation optoelectronic devices. However, the film quality of this charming material fabricated by the conventional spin‐coating method is far from satisfactory, significantly affecting the optoelectronic devices' performance. Here, one facile slow‐evaporating solvent (SE) method is demonstrated to synthesize high‐quality organic–inorganic halide perovskite films. Compared with the conventional spin coating method, the films fabricated by this SE method show much higher crystallinity, oriented lattice, smoother surface morphology, and lower trap density. Besides, the photodetector manufactured by the SE method‐based film also performs much better than the ones by the spin‐coating method. Importantly, this universal method can be applied to different organic–inorganic halide perovskites, such as Dion–Jacobson (DJ) type and Ruddlesden–Popper type 2D halide perovskites and conventional 3D halide perovskites. This work gives an effective solution to improve the quality of the DJ‐type halide perovskites, which endows the halide perovskites with a more practical chance to be commercialized cosmically. [ABSTRACT FROM AUTHOR]

Alloying the active metal with a second metal is an effective way to tailor the adsorption of reaction intermediates through an ensemble effect. Herein, based on theoretical calculations validating that the ensemble sites composed of Ag and Pd atoms could reduce the energy gap for *COOH and *CO intermediates generated during electrocatalytic CO2 reduction reaction (eCO2RR) by either weakening the CO adsorption or enhancing the COOH adsorption, a strategy to produce AgPd alloy nanoparticles with fine sizes for synergizing the ensemble effect and size leverage toward high CO faradaic efficiency in eCO2RR is reported. In particular, the AgPd alloy nanoparticles at an optimized Ag/Pd atomic ratio of 35/65 affords a maximum CO faradaic efficiency of 98.9% and a CO partial current density of 5.1 mA cm−2 at the potential of −0.8 V (vs RHE) with satisfactory durability of up to 25 h, outperforming those of most Pd‐based electrocatalysts recently reported and demonstrating great potential for further application in producing CO via eCO2RR at ambient conditions. [ABSTRACT FROM AUTHOR]

Photo‐electrochemical (PEC) water splitting is a promising method for converting solar energy into clean energy, but the mechanism of improving PEC efficiency through the interfacial contact and defect strategy remains highly controversial. Herein, reduced graphene oxide (rGO) and oxygen vacancies are introduced into α‐Fe2O3 nanorod (NR) arrays using a simple spin‐coating method and acid treatment. The resultant oxygen vacancy–α‐Fe2O3/rGO‐integrated system exhibits a higher photocurrent, four times than the pristine α‐Fe2O3. It is well evidenced that the electronic interface interaction between α‐Fe2O3 and rGO is boosted with the oxygen vacancies, facilitating electron transfer from α‐Fe2O3 to rGO. Moreover, the oxygen vacancies not only create interband states in α‐Fe2O3 that can trap photogenerated holes and thus facilitate charge separation but significantly also strengthen the adsorption of oxidative intermediates and reduce the energy barrier of rate‐determining step during oxygen evolution reaction (OER). This study demonstrates an rGO–oxygen vacancy synergistic interfacial contact and defect modification approach to design semiconducting photocatalysts for high‐efficiency solar energy capture and conversion. The generated principle is expected to be extendable to another material system. [ABSTRACT FROM AUTHOR]

Abstract: Erasable electrical conductive domain walls in an insulating ferroelectric matrix provide novel functionalities for applications in logic and memory devices. The crux of such success requires sufficiently high wall currents to drive high‐speed and high‐power nanodevices. This work provides an appealing strategy to increase the current by two orders of magnitude through the careful selection of current flowing paths along the charged walls. The dense walls come into form through the hierarchical evolution of the 71°, 109°, and 180° domains of epitaxial BiFeO3 films in a planar‐geometry ferroelectric resistance‐switching memory cell. The engineered films grown on SrTiO3 and GdScO3 substrates allow the observation of detailed local configurations and the evolution of the different domain types using vector piezo‐force microscopy. The higher local electrical conductivity near the charged domain walls is identified by conductive atomic‐force microscopy. It is shown that 180° domain reversal proceeds by three‐step 71° rotations of the pristine domains. Surprisingly, a maximum current of ≈300 nA is observed for current paths along charge‐uncompensated head‐to‐head hierarchical domain walls connecting the two electrodes on the film surface. Furthermore, the achievable current level can be conveniently controlled by varying the relative directions of the initial polarization and the applied field. [ABSTRACT FROM AUTHOR]

Two coordination complex emitters as well as host materials Be(PPI)2 and Zn(PPI)2 (PPI = 2-(1-phenyl-1 H-phenanthro[9,10- d]imidazol-2-yl)phenol) are designed, synthesized, and characterized. The incorporation of the metal atom leads to a twisted conformation and rigid molecular structure, which improve the thermal stability of Be(PPI)2 and Zn(PPI)2 with high Td and Tg at around 475 and 217 °C, respectively. The introduction of the electron-donating phenol group results in the emission color shifting to the deep-blue region and the emission maximum appears at around 429 nm. This molecular design strategy ensures that the highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) HOMO and LUMO of Be(PPI)2 and Zn(PPI)2 localize on the different moieties of the molecules. Therefore, the two complexes have an ambipolar transport property and a small singlet-triplet splitting of 0.35 eV for Be(PPI)2 and 0.21 eV for Zn(PPI)2. An undoped deep-blue fluorescent organic light-emitting device (OLED) that uses Be(PPI)2 as emitter exhibits a maximum power efficiency of 2.5 lm W−1 with the CIE coordinates of (0.15, 0.09), which are very close to the National Television Standards Committee (NTSC) blue standard (CIE: 0.14, 0.08). Green and red phosphorescent OLEDs (PhOLEDs) that use Be(PPI)2 and Zn(PPI)2 as host materials show high performance. Highest power efficiencies of 67.5 lm W−1 for green PhOLEDs and 21.7 lm W−1 for red PhOLEDs are achieved. In addition, the Be(PPI)2-based devices show low-efficiency roll-off behavior, which is attributed to the more balanced carrier-transport property of Be(PPI)2. [ABSTRACT FROM AUTHOR]

Nanocarriers are essential for targeted and enhanced drug delivery. However, the use of toxic solvent and the complex of chemical functionalization have seriously limited their clinical translation. Here, a one‐step strategy is developed to direct the self‐assembly of biocompatible core‐shell nanocapsules with tunable surface functionality by microfluidics. Upon rapid mixing and solvent exchange of ethanol with water in a microfluidic device, drug, oil, polymer, and polymer‐PEG‐function co‐precipitate and self‐assemble into core‐shell nanocapsules with desired surface functionality as driven by energy minimization. The prepared PCL‐PEG‐FA core‐shell nanocapsules demonstrate a high encapsulation efficiency and loading capacity and exhibit excellent tumor‐targeting drug delivery performances both in vitro and in vivo via the binding of functional group on the nanocapsule surface with corresponding receptor on the tumor cell membrane. The immune activation in the tumor microenvironment is investigated in detail by flow cytometry and multiplex immunohistochemistry staining to reveal the underlying mechanism for enhanced anti‐tumor performances. The developed strategy is green, facile, versatile, scalable and offers a promising platform for the design of advanced nanocarriers with hierarchical structure and desired function for enhanced drug delivery. [ABSTRACT FROM AUTHOR]

Solution‐processed oxide thin films are actively pursued as hole‐injection layers (HILs) in quantum‐dot light‐emitting diodes (QLEDs), aiming to improve operational stability. However, device performance is largely limited by inefficient hole injection at the interfaces of the oxide HILs and high‐ionization‐potential organic hole‐transporting layers. Solution‐processed NiOx films with a high and stable work function of ≈5.7 eV achieved by a simple and facile surface‐modification strategy are presented. QLEDs based on the surface‐modified NiOx HILs show driving voltages of 2.1 and 3.3 V to reach 1000 and 10 000 cd m−2, respectively, both of which are the lowest among all solution‐processed LEDs and vacuum‐deposited OLEDs. The device exhibits a T95 operational lifetime of ≈2500 h at an initial brightness of 1000 cd m−2, meeting the commercialization requirements for display applications. The results highlight the potential of solution‐processed oxide HILs for achieving efficient‐driven and long‐lifetime QLEDs. [ABSTRACT FROM AUTHOR]