Postdeposition halide exchange has been a popular strategy for tuning the emission wavelength of metal halide perovskites and is particularly attractive in achieving deep-blue perovskite light-emitting diodes (PeLEDs), where the quality of the emissive layer is largely limited by the low solubility of chlorides in perovskite precursor solution. In this work, the halide exchange strategy is examined for deep-blue PeLEDs, with a focus on understanding the role of the organic cations of the halide salt (i.e., the chloride source for ion exchange) in modifying the properties of the perovskite films and consequently the PeLED performances. By comparatively investigating the treatment effects of two model systems, namely phenethylammonium chloride and 2,2-diphenylethylammonium chloride (DPEACl), it is found that although the two chlorides produce highly similar photoluminescence properties of the perovskite films, they create different landscapes for current flow in the PeLEDs. In particular, the bulky branch-structured DPEA cations exhibit minimal disturbance to the perovskite grains while providing highly effective inter-grain void filling and thus leakage current blocking, leading to 3D perovskite-based PeLEDs with a record high peak external quantum efficiency of 6.4% at 462 nm. The study highlights the importance of organic cation selection in the halide exchange processes for PeLEDs.

Aqueous zinc-ion batteries (AZIBs) are expected to be an attractive alternative in advanced energy storage devices due to large abundance and dependable security. Nevertheless, the undesirable energy density and operating voltage still hinder the development of AZIBs, which is intimately associated with the fundamental properties of the cathode. In this work, polyvinylpyrrolidone (PVP) intercalated Mn0.07VOx (PVP-MnVO) with a large interlayer spacing of 13.5 Å (against 12.5 Å for MnVO) synthesized by a facile hydrothermal method is adopted for the cathode in AZIBs. The experimental results demonstrate that PVP-MnVO with expanded interlayer spacing provides beneficial channels for the rapid diffusion of Zn2+, resulting in a high discharge capacity of 402 mAh g−1 at 0.1 A g−1, superior to that of MnVO (275 mAh g−1 at 0.1 A g−1). Meanwhile, the PVP molecule remains in the layer structure as a binder/pillar, which can maintain its structural integrity well during the charging/discharging process. Consequently, PVP-MnVO cathode exhibits superior rate capability and cycling stability (89% retention after 4300 cycles at 10 A g−1) compared to that of MnVO (≈51% retention over 500 cycles at 2 A g−1). This work proposes a new approach to optimize the performance of vanadium-based electrode materials in AZIBs.

Lithium–sulfur batteries (LSBs) as a next-generation promising energy storage device have a great potential commercial application due to their high specific capacity and energy density. However, it is still a challenge to real-time monitor the evolution process of polysulfides during the LSBs discharge process. Herein, an in situ electrochemical-fluorescence technology is developed to measure the fluorescence intensity change of cadmium sulfide quantum dots (CdS QDs) during the LSBs discharge process in real-time, which could monitor the evolution process of polysulfides. First, the real-time fluorescent spectrum and confocal fluorescence imaging of discharge processes for LSBs with CdS QDs are integrally illustrated. Furthermore, the fluorescence spectra and imaging results show that CdS QDs could immobilize polysulfides through bonding with polysulfides to improve the LSB device performance. This in situ electrochemical-fluorescence technology provides a new in situ and real-time-monitor method for better understanding the working mechanism of LSBs.

A multi-engine highly integrated microrobot, which is a Janus hemispherical shell structure composed of Pt and α-Fe2O3, is successfully developed. The microrobot can be efficiently driven and flexibly regulated by five stimuli, including an optical field, an acoustic field, magnetic field, an electric field, and chemical fuel. In addition, no matter which way it is driven by, the direction can be effectively controlled through the magnetic field regulation. Furthermore, this microrobot can also utilize magnetic or acoustic fields to achieve excellent aggregation control and swarm movement. Finally, this study demonstrates that the microrobots’ propulsion can be effectively synergistically enhanced through the simultaneous action of two driving mechanisms, which can greatly improve the performance of the motor in applications, such as pollutant degradation. This multi-engine, highly integrated microrobot not only can adapt to more complex environments and has a wider application range, better application prospects, but also provides important ideas for designing future advanced micro/nanorobots.

Recent developments in the design and synthesis of more and more sophisticated organic building blocks with controlled structures and physical properties, combined with the emergence of novel assembly modes and nanofabrication methods, make it possible to tailor unprecedented structurally complex porous systems with precise multiscale control over their architectures and functions. By tuning their porosity from the nanoscale to microscale, a wide range of functional materials can be assembled, including open frameworks and micro/nanoscaffold architectures. During the last two decades, significant progress is made on the generation and optimization of advanced porous systems, resulting in high-performance multifunctional scaffold materials and novel device configurations. In this perspective, a critical analysis is provided of the most effective methods for imparting controlled physical and chemical properties to multifunctional porous skeletons. The future research directions that underscore the role of skeleton structures with varying physical dimensions, from molecular-level open frameworks (100 nm), are discussed. The limitations, challenges, and opportunities for potential applications of these multifunctional and multidimensional material systems are also evaluated in particular by addressing the greatest challenges that the society has to face.

Two-dimensional transition metal carbide/nitrides (MXenes) have recently received extensive attention due to their diverse material types and versatile structures, large-scale production, and excellent properties. MXene sheets possess abundant hydrophilic functional groups on their surface, which enable them to be assembled into macroscopic fibers or compounded with other functional materials to produce composite fibers. This review aims to provide a comprehensive analysis of MXene fibers in terms of their fabrication, structure, properties, and recent applications as flexible and wearable electronics. The review will discuss the principles of different methods used to synthesize MXene fibers and analyze the characteristics of the as-synthesized fibers, with a particular focus on the wet spinning method. The fundamental relationships between the microstructure of MXene fibers and their resulting mechanical and electrical properties will be explored. Furthermore, the review will elaborate on the progress made in MXene-based fibers in the rapidly growing field of wearable electronics applications, provide insights into future development of MXene fiber materials and propose solutions to the challenges facing practical applications.

Polymer-based magnetic particles have been widely used for the separation of biological samples including nucleic acids, proteins, virus, and cells. Existing magnetic particles are almost prepared by coating polymers on magnetic nanoparticles (NPs). However, this strategy usually encounters the problem of poor magnetic NPs loading capacity. Here, a series of nanofractal magnetic particles (nanoFMPs) synthesized by a strategy of mediator monomer regulated emulsion interfacial polymerization is presented, which allows effective magnetic NPs loading and show efficient nucleic acid separation performance. The mediator monomers facilitate the dispersion of magnetic NPs in internal phase to achieve higher loading, and the hydrophilic monomers use electrostatic interactions to form surface nanofractal structures with functional groups. Compared with magnetic particles without nanofractal structure, nanoFMPs exhibit a higher nucleic acid extraction capability. This strategy offers an effective and versatile way for the synthesis of nanoFMPs toward efficient separation in various fields from clinical diagnosis to food safety and environmental monitoring.

Electrochemical reduction of oxygen into hydrogen peroxide in an acidic medium offers an energy-efficient and green H2O2 synthesis as an alternative to the energy-intensive anthraquinone process. Unfortunately, high overpotential, low production rates, and fierce competition from traditional four-electron reduction limit it. In this study, a metalloenzyme-like active structure is mimicked in carbon-based single-atom electrocatalysts for oxygen reduction to H2O2. Using a carbonization strategy, the primary electronic structure of the metal center with nitrogen and oxygen coordination is modulated, followed by epoxy oxygen functionalities close to the metal active sites. In an acidic medium, CoNOC active structures proceed with greater than 98% H2O2 selectivity (2e−/2H+) rather than CoNC active sites that are selective to H2O (4e−/4H+). Among all MNOC (M = Fe, Co, Mn, and Ni) single-atom electrocatalysts, the CoNOC is the most selective (> 98%) for H2O2 production, with a mass activity of 10 A g−1 at 0.60 V vs. RHE. X-ray absorption spectroscopy is used to identify the formation of unsymmetrical MNOC active structures. Experimental results are also compared to density functional theory calculations, which revealed that the structure-activity relationship of the epoxy-surrounded CoNOC active structure reaches optimum (ΔG*OOH) binding energies for high selectivity.

The fabrication of high quality nanophotonic surfaces for integration in optoelectronic devices remains a challenge because of the complexity and cost of top–down nanofabrication strategies. Combining colloidal synthesis with templated self-assembly emerged as an appealing low-cost solution. However, it still faces several obstacles before integration in devices can become a reality. This is mostly due to the difficulty in assembling small nanoparticles (<50 nm) in complex nanopatterns with a high yield. In this study, a reliable methodology is proposed to fabricate printable nanopatterns with an aspect ratio varying from 1 to 10 and a lateral resolution of 30 nm via nanocube assembly and epitaxy. Investigating templated assembly via capillary forces, a new regime was identified that was used to assemble 30–40 nm nanocubes in a patterned polydimethylsiloxane template with a high yield for both Au and Ag with multiple particles per trap. This new method relies on the generation and control of an accumulation zone at the contact line that is thin as opposed to dense, displaying higher versatility. This is in contrast with conventional wisdom, identifying a dense accumulation zone as a requirement for high-yield assembly. In addition, different formulations are proposed that can be used for the colloidal dispersion, showing that the standard water-surfactant solutions can be replaced by surfactant-free ethanol solutions, with good assembly yield. This allows to minimize the presence of surfactants that can affect electronic properties. Finally, it is shown that the obtained nanocube arrays can be transformed into continuous monocrystalline nanopatterns via nanocube epitaxy at near ambient temperature, and transferred to different substrates via contact printing. This approach opens new doors to the templated assembly of small colloids and could find potential applications in various optoelectronic devices ranging from solar cells to light-emitting diodes and displays.

Bionic robotics and actuators have made dramatic advancements in structural design, material preparation, and application owing to the richness of nature and innovative material design. Appropriate and ingenious sources of bio-inspiration can stimulate a large number of different bionic systems. After millennia of survival and evolutionary exploration, the mere existence of life confirms that nature is constantly moving in an evolutionary direction of optimization and improvement. To this end, bio-inspired robots and actuators can be constructed for the completion of a variety of artificial design instructions and requirements. In this article, the advances in bio-inspired materials for robotics and actuators with the sources of bio-inspiration are reviewed. The specific sources of inspiration in bionic systems and corresponding bio-inspired applications are summarized first. Then the basic functions of materials in bio-inspired robots and actuators is discussed. Moreover, a principle of matching biomaterials is creatively suggested. Furthermore, the implementation of biological information extraction is discussed, and the preparation methods of bionic materials are reclassified. Finally, the challenges and potential opportunities involved in finding sources of bio-inspiration and materials for robotics and actuators in the future is discussed.

Flexible piezoelectric energy harvesters (PEHs) have gained substantial attention owing to their wearability, breathability, and sustainable self-powered supply. However, existing film PEHs cannot identify forces in different bending directions, limiting their applications in wearable electronics and artificial intelligence. This study constructs a fabric PEH for the first time by introducing piezoelectric anisotropic BaTi2O5 nanorods (BT2-nr) into piezoelectric polyvinylidene fluoride (PVDF) nanofibers with a bi-oriented architecture, in which BT2-nr uniformly aligns in the PVDF nanofiber during electrospinning. The dual-orientation feature endows the flexible PEH with anisotropy, which can sensitively identify the forces at different bending directions (e.g., bent vertically, parallelly, or twisted by 45° along the fiber orientations). Simultaneously, the composite PVDF/BT2 PEH containing 15 wt.% BT2-nr delivers an optimal piezoelectric output of 31.2 V with a high sensitivity of 5.22 V N−1. The developed anisotropic PEH can be used as a self-powered pressure sensor for multimodal intelligent biomonitoring of human movement. This study provides a feasible strategy for fabricating self-powered flexible PEHs with high electromechanical conversion efficiency and multifunctionality for wearable piezoelectric pressure sensors.

Wearable Electronic Devices

Inside Front Cover

The current polymerase chain reactions-based nucleic acid tests for large-scale infectious disease diagnosis are always lab-dependent and generate large amounts of highly infectious plastic waste. Direct non-linear acoustic driven of microdroplets provide an ideal platform for contactless spatial and temporal manipulation of liquid samples. Here, a strategy to programmable-manipulate microdroplets using potential pressure well for contactless trace detection is conceptualized and designed. On such contactless modulation platform, up to seventy-two piezoelectric transducers are precisely self-focusing single-axis arranged and controlled, which can generate dynamic pressure nodes for effectively contact-free manipulating microdroplets without vessel contamination. In addition, the patterned microdroplet array can act as contactless microreactor and allow multiple trace samples (1–5 µL) biochemical analysis, and the ultrasonic vortex can also accelerate non-equilibrium chemical reactions such as recombinase polymerase amplification (RPA). The results of fluorescence detection indicated that such programmable modulated microdroplet achieved contactless trace nucleic acid detection with a sensitivity of 0.21 copy µL−1 in only 6–14 min, which is 30.3–43.3% shorter than the conventional RPA approach. Such a programmable containerless microdroplet platform can be used for toxic, hazardous, or infectious samples sensing, opening up new avenues for developing future fully automated detection systems.

Over the past few decades, organic–inorganic halide perovskites (OIHPs) as novel photocatalyst materials have attracted intensive attention for an impressive variety of photocatalytic applications due to their excellent photophysical (chemical) properties. Regarding practical application and future commercialization, the air–water stability and photocatalytic performance of OIHPs need to be further improved. Accordingly, studying modification strategies and interfacial interaction mechanisms is crucial. In this review, the current progress in the development and photocatalytic fundamentals of OIHPs is summarized. Furthermore, the structural modification strategies of OIHPs, including dimensionality control, heterojunction design, encapsulation techniques, and so on for the enhancement of charge-carrier transfer and the enlargement of long-term stability, are elucidated. Subsequently, the interfacial mechanisms and charge-carrier dynamics of OIHPs during the photocatalytic process are systematically specified and classified via diverse photophysical and electrochemical characterization methods, such as time-resolved photoluminescence measurements, ultrafast transient absorption spectroscopy, electrochemical impedance spectroscopy measurements, transient photocurrent densities, and so forth. Eventually, various photocatalytic applications of OIHPs, including hydrogen evolution, CO2 reduction, pollutant degradation, and photocatalytic conversion of organic matter.

During rheumatoid arthritis (RA) development, over-produced proinflammatory cytokines represented by tumor necrosis factor-α (TNF-α) and reactive oxygen species (ROS) represented by H2O2 form a self-promoted cycle to exacerbate the synovial inflammation and tissue damage. Herein, biomimetic nanocomplexes (NCs) reversibly cloaked with macrophage membrane (RM) are developed for effective RA management via dual scavenging of TNF-α and ROS. To construct the NCs, membrane-penetrating, helical polypeptide first condenses TNF-α siRNA (siTNF-α) and forms the cationic inner core, which further adsorbs catalase (CAT) via electrostatic interaction followed by surface coating with RM. The membrane-coated NCs enable prolonged blood circulation and active joint accumulation after systemic administration in Zymosan A-induced arthritis mice. In the oxidative microenvironment of joints, CAT degrades H2O2 to produce O2 bubbles, which shed off the outer membrane layer to expose the positively charged inner core, thus facilitating effective intracellular delivery into macrophages. siRNA-mediated TNF-α silencing and CAT-mediated H2O2 scavenging then cooperate to inhibit inflammation and alleviate oxidative stress, remodeling the osteomicroenvironment and fostering tissue repair. This study provides an enlightened strategy to resolve the blood circulation/cell internalization dilemma of cell membrane-coated nanosystems, and it renders a promising modality for RA treatment.

Incontrovertibly there is an increasing demand for the development of benign inks suitable for fabrication of high-performing perovskite-based thin film functional layers. Nevertheless, most reported perovskite precursors rely on the use of highly toxic solvents such as acetonitrile, 2-methoxyethanol, dimethylformamide, and many others. Hence, there is a strong imperative for the development of novel and greener inks, which will facilitate smoother commercialization of technologies based on functional perovskite films. Therefore, four perovskite precursors are studied, some of which consist of up to 90% ethanol. All inks are developed to fulfill the requirements of a high-throughput deposition compatible with roll-to-roll techniques at room temperature, assisted by an air knife for instant solvent removal. Two of the inks are particularly suitable for the fabrication of high-quality and densely packed multi-crystalline (CH3NH3)PbI3 layers, as confirmed by numerous nanoscale spectroscopic and material characterization techniques. Additionally, large-area photoluminescence (PL) imaging is demonstrated to improve the quality of the deposited perovskite films, with a route to enhance deposition uniformity when upscaling for manufacture. The genuine potential of the developed greener perovskite inks is demonstrated with the fabrication of solar cells with power conversion efficiencies above 19.5%.

For devices encountering long-term stability challenges, a precise evaluation of degradation is of paramount importance. However, methods for comprehensively elucidating the degradation mechanisms in devices, particularly those undergoing dynamic chemical and mechanical changes during operation, such as batteries, are limited. Here, a method is presented using operando computed tomography combined with X-ray absorption near-edge structure spectroscopy (CT-XANES) that can directly track the evolution of the 3D distribution of the local capacity loss in battery electrodes during (dis)charge cycles, thereby enabling a five-dimensional (the 3D spatial coordinates, time, and chemical state) analysis of the degradation. This paper demonstrates that the method can quantify the spatiotemporal dynamics of the local capacity degradation within an electrode during cycling, which has been truncated by existing bulk techniques, and correlate it with the overall electrode performance degradation. Furthermore, the method demonstrates its capability to uncover the correlation among observed local capacity degradation within electrodes, reaction history during past (dis)charge cycles, and electrode microstructure. The method thus provides critical insights into the identification of degradation factors that are not available through existing methods, and therefore, will contribute to the development of batteries with long-term stability.

Among the materials for the negative electrodes in Li-ion batteries, oxides capable of reacting with Li+ via intercalation/conversion/alloying are extremely interesting due to their high specific capacities but suffer from poor mechanical stability. A new way to design nanocomposites based on the (Ti/Sn)O2 system is the partial oxidation of the tin-containing MAX phase of Ti3Al(1-x)SnxO2 composition. Exploiting this strategy, this work develops composite electrodes of (Ti/Sn)O2 and MAX phase capable of withstanding over 600 cycles in half cells with charge efficiencies higher than 99.5% and specific capacities comparable to those of graphite and higher than lithium titanate (Li4Ti5O12) or MXenes electrodes. These unprecedented electrochemical performances are also demonstrated at full cell level in the presence of a low cobalt content layered oxide and explained through an accurate chemical, morphological, and structural investigation which reveals the intimate contact between the MAX phase and the oxide particles. During the oxidation process, electroactive nanoparticles of TiO2 and Ti(1-y)SnyO2 nucleate on the surface of the unreacted MAX phase which therefore acts both as a conductive agent and as a buffer to preserve the mechanical integrity of the oxide during the lithiation and delithiation cycles.

Implantable electronic devices can realize real-time and reliable health monitoring, diagnosis, and treatment of human body, which are expected to overcome important bottlenecks in the biomedical field. However, the commonly used energy supply devices for them are implantable batteries based on conventional rigid device design with toxic components, which both mechanically and biologically mismatch soft biological tissues. Therefore, the development of highly soft, safe, and implantable tissue-matchable flexible batteries is of great significance and urgency for implantable bioelectronics. In this work, the recent advances of tissue-matchable and implantable flexible batteries are overviewed, focusing on the design strategies of electrodes/batteries and their biomedical applications. The mechanical flexibility, biocompatibility, and electrochemical performance in vitro and in vivo of these flexible electrodes/batteries are then discussed. Finally, perspectives are provided on the current challenges and possible directions of this field in the future.