http://onlinelibrary.wiley.com/rss/journal/10.1002/(ISSN)1521-4095

CD93-Targeted Microbubbles

In article number 2310421, Qiuyang Li, Lijun Yuan, and co-workers develop a novel ultrasound contrast microbubble for evaluation of immune status through molecular imaging of endothelial CD93 expression. High levels of CD93 in tumor vasculature correlate well with immune cell infiltration deficiency, and ultrasound imaging of CD93 with MMRN2-modified microbubbles holds as a promising strategy to assess the anti-tumor immune response.

Mesoporous Metal Oxides

In article number 2311809 by Hong Chul Moon, Taesung Kim, Jin Kon Kim, and co-workers, a new synthetic approach for mesoporous metal oxides by exploiting synergistic effect of thermal activation and plasma is introduced. This synthetic method can be universally applied to various mesoporous metal oxides and can even be directly applied to the synthesis on a plastic substrate. This approach is expected to pave the way for a wide range of flexible electronics.

Functional Amyloids

Functional amyloid is produced in many different organisms where they serve a range of mainly structural purposes. Their exceptional stability and ready availability has formed the basis for many biotechnological applications which are highlighted in article number 2312823 by Huabing Wang, Daniel E. Otzen, and co-workers.

Mechanically Strengthened Aerogels

In article number 2307772, Vinayak G. Parale, Kazuyoshi Kanamori, Hyung-Ho Park, and co-workers summarize the state-of-the art developments of mechanically strengthened aerogels through multi-scale, multi-compositional, and multidimensional approaches. The discussed aerogel production methods enable great improvements in the properties of aerogels, considerably expanding their scope for future colonization of Mars.

Hydrothermal Carbonization of Biomass

In article number 2307412, Hui Zhou, Maria-Magdalena Titirici, and co-workers systematically review the progress of hydrothermal carbonization of biomass for sustainable carbon materials with an interdisciplinary perspective, which could potentially expand the landscape of biomass-based carbon materials and simultaneously contribute to climate change mitigation through carbon negative emissions.

On-Skin Electronics

In article number 2308831, Hao Wu, Yutian Liu, and co-workers develop on-skin patches with polyaspartic acid-modified dopamine/ethyl-based ionic liquid hydrogel to capture electromyography signals. Triggered by a one-step electric field treatment, the hydrogel realizes rapid, wide-range adhesion regulation and enhanced mechanical performance. Hydrogel devices can establish intimate device/skin interfaces or ensure benign removal while achieving precise diagnoses of nerve injuries.

Magnetoelectric Paper

In article number 2311154 by Myoung Hoon Song, Chaenyung Cha, Jiyun Kim, and co-workers, a flexible, biodegradable, and wireless bioelectronic paper is developed showing significant scalability, design flexibility, and rapid customizability through simple paper crafting techniques such as origami and kirigami.

Microrobots

In article number 2310084, Salvador Pané, Minsoo Kim, Hao Ye, and co-workers introduce microrobotic superstructures comprising a magnetic gelatin composite chassis threaded with iron helical micromachines. Magnetic inputs can be used to navigate the superstructure (gradients) and also dissolve the chassis through magnetic hyperthermia, thereby releasing the micromachines to navigate through narrow channels. The capability of these micromachines to disassemble on-command to access narrower conduits enhances the microrobots' multifunctionality.

It has already been ≈90 years since the first development of aerogels, and many researchers have devoted tremendous efforts to enhance their mechanical properties, which is yet completely achieved. This review presents multiscale, multicompositional and multidimensional strategies, resulting from flexible synthesis techniques for 0D–1D, 0D–2D, 1D–2D, and 0D–1D–2D combined aerogels.

In recent decades, aerogels have attracted tremendous attention in academia and industry as a class of lightweight and porous multifunctional nanomaterial. Despite their wide application range, the low mechanical durability hinders their processing and handling, particularly in applications requiring complex physical structures. “Mechanically strengthened aerogels” have emerged as a potential solution to address this drawback. Since the first report on aerogels in 1931, various modified synthesis processes have been introduced in the last few decades to enhance the aerogel mechanical strength, further advancing their multifunctional scope. This review summarizes the state-of-the-art developments of mechanically strengthened aerogels through multicompositional and multidimensional approaches. Furthermore, new trends and future directions for as prevailed commercialization of aerogels as plastic materials are discussed.

Versatile nitrogen-centered redox-active organic materials, including electrochemical performance and reaction mechanism, are discussed individually. The challenges, solutions, and perspectives are also proposed in this review.

Versatile nitrogen-centered organic redox-active molecules have gained significant attention in alkali metal-ion batteries (AMIBs) due to their low cost, low toxicity, and ease of preparation. Specially, their multiple reaction categories (anion/cation insertion types of reaction) and higher operating voltage, when compared to traditional conjugated carbonyl materials, underscore their promising prospects. However, the high solubility of nitrogen-centered redox active materials in organic electrolyte and their low electronic conductivity contribute to inferior cycling performance, sluggish reaction kinetics, and limited rate capability. This review provides a detailed overview of nitrogen-centered redox-active materials, encompassing their redox chemistry, solutions to overcome shortcomings, characterization of charge storage mechanisms, and recent progress. Additionally, prospects and directions are proposed for future investigations. It is anticipated that this review will stimulate further exploration of underlying mechanisms and interface chemistry through in situ characterization techniques, thereby promoting the practical application of nitrogen-centered redox-active materials in AMIBs.

Ternary copper (Cu) halides are promising candidates for replacing toxic lead halides in the field of perovskite light-emitting diodes (LEDs) toward practical applications. However, the electroluminescent performance of Cu halide-based LEDs remains a great challenge due to the presence of serious nonradiative recombination and inefficient charge transport in Cu halide emitters. Here, we report the rational design of host-guest [dppb]2Cu2I2 (dppb denotes 1,2-bis[diphenylphosphino]benzene) emitters and its utility in fabricating efficient Cu halide-based green LEDs that show a high external quantum efficiency (EQE) of 13.39%. The host-guest [dppb]2Cu2I2 emitters with mCP (1,3-Bis(N-carbazolyl)benzene) host demonstrate a significant improvement of carrier radiative recombination efficiency, with the photoluminescence quantum yield increased by nearly 10 times, which is rooted in the efficient energy transfer and type-I energy level alignment between [dppb]2Cu2I2 and mCP. Moreover, the charge-transporting mCP host can rise the carrier mobility of [dppb]2Cu2I2 films, thereby enhancing the charge transport and recombination. More importantly, this strategy enables a large-area prototype LED with a record-breaking area up to 81 cm2, along with a decent EQE of 10.02% and uniform luminance. We believe these results represent an encouraging stepping stone to bring Cu halide-based LEDs from the laboratory towards to commercial lighting and displays panels.

This article is protected by copyright. All rights reserved

Self-healing microelectronics are needed for costly applications with limited or without access. They are needed in fields such as space exploration to increase lifetime and decrease both costs and the environmental impact. While advanced self-healing mechanisms for polymers are numerous, practical ways for self-healing in metal films have yet to be found. A concept for an autonomous intrinsic self-healing metallic film system was developed, allowing the healing of cracks in metallic films on flexible substrates. The concept relies on stabilizing metastable thin films with high mixing enthalpy via segregation barriers. This allows the films to possess autonomous intrinsic self-healing capabilities triggered by cracking at temperatures not detrimental to flexible microelectronics. The effect will be shown on metastable Mo1-xAgx thin films, stabilized via a Mo segregation barrier. Without a segregation barrier, the system is known to exhibit spontaneous Ag particle formation on the surface. This property was controlled and directed to heal cracks and partially restore the electro-mechanical properties of the multilayer system. This mechanism opens up the field of self-healing thin metallic films that could profoundly impact the design of future microelectronics.

This article is protected by copyright. All rights reserved

The interface between electrodes and neural tissues plays a pivotal role in determining the efficacy and fidelity of neural activity recording and modulation. While considerable efforts have been made to improve the electrode-tissue interface, the majority of studies have primarily concentrated on the development of biocompatible neural electrodes through abiotic materials and structural engineering. In this study, we present an approach that seamlessly integrates abiotic and biotic engineering principles into the electrode-tissue interface. Specifically, we combine ultraflexible neural electrodes with short hairpin RNAs (shRNAs) designed to silence the expression of endogenous genes within neural tissues. Our system facilitates shRNA-mediated knockdown of PTEN and PTBP1, two essential genes associated in neural survival/growth and neurogenesis, within specific cell populations located at the electrode-tissue interface. Additionally, we demonstrate that the downregulation of PTEN in neurons can result in an enlargement of neuronal cell bodies at the electrode-tissue interface. Furthermore, our system enables long-term monitoring of neuronal activities following PTEN knockdown in a mouse model of Parkinson's disease and traumatic brain injury. Our system provides a versatile approach for genetically engineering the electrode-tissue interface with unparalleled precision, paving the way for the development of regenerative electronics and next-generation brain-machine interfaces.

This article is protected by copyright. All rights reserved

Fine-tuning nucleation and growth of colloidal liquid crystalline (LC) droplets, also known as tactoids, is highly desirable in both fundamental science and technological applications. However, the tactoid structure results from the trade-off between thermodynamics and non-equilibrium kinetics effects, and controlling liquid-liquid crystalline phase separation (LLCPS) in these systems is still work in progress. Here we introduce a single-step strategy to obtain a rich palette of morphologies for tactoids formed via nucleation and growth within an initially isotropic phase exposed to a gradient of depletants. We show the simultaneous appearance of rich LC structures along the depleting potential gradient, where the position of each LC structure is correlated with the magnitude of the depleting potential. Changing the size (nanoparticles) or the nature (polymers) of the depleting agent provides additional, precise control over the resulting LC structures through a size-selective mechanism, where the depletant may be found both within and outside the LC droplets. The use of depletion gradients from depletants of varying size and nature offers a powerful toolbox to manipulation, templating, imaging and understanding heterogeneous colloidal LC structures.

This article is protected by copyright. All rights reserved

Photocatalytic CO2 reduction to high-value-added C2+ products presents significant challenges, which is attributed to the slow kinetics of multi-e − CO2 photoreduction and the high thermodynamic barrier for C−C coupling. Incorporating redox-active Co2+/Ni2+ cations into lead halide photocatalysts has high potentials to improve carrier transport and introduce charge polarized bimetallic sites, addressing the kinetic and thermodynamic issues, respectively. In this study, we have developed a coordination-driven synthetic strategy to introduce 3d transition metals into the interlamellar region of layered organolead iodides with atomic precision. The resultant bimetallic halide hybrids exhibit selective photoreduction of CO2 to C2H5OH using H2O vapor at the evolution rates of 24.9∼31.4 μmol g–1 h–1 and high selectivity of 89.5∼93.6%, while pristine layered lead iodide yields only C1 products. Band structure calculations and photoluminescence studies indicate that the interlayer Co2+/Ni2+ species greatly contribute to the frontier orbitals and enhance exciton dissociation into free carriers, facilitating carrier transport between adjacent lead iodide layers. In addition, Bader charge distribution calculations and in situ experimental spectroscopic studies reveal that the asymmetric Ni−O−Pb bimetallic catalytic sites exhibit intrinsic charge polarization, promoting C−C coupling and leading to the formation of the key *OC−CHO intermediate.

This article is protected by copyright. All rights reserved

DNA double-strand breaks (DSBs) yield highly determines radiotherapy efficacy. However, improving the inherent radiosensitivity of tumour DNA to promote radiation-induced DSBs remains a challenge. Using theoretical and experimental models, we discover the underexplored impact of Z-DNA conformations on radiosensitivity, yielding higher DSBs than other DNA conformations. Thereout, we propose a radiosensitization strategy focused on inducing Z-DNA conformation, utilizing CBL@HfO2 nanocapsules loaded with a Z-DNA inducer CBL0137. A hollow mesoporous HfO2 (HM-HfO2) acts as a delivery and an energy depositor to promote Z-DNA breakage. The nanocapsule permits the smart DSBs accelerator that triggers its radiosensitization with irradiation stimulation. Impressively, the CBL@HfO2 facilitates the B-Z DNA conformational transition, augmenting DSBs about 4-fold stronger than irradiation alone, generating significant tumour suppression with a 30% cure rate. The approach enables DSBs augmentation by improving the inherent radiosensitivity of DNA. As such, it opens up an era of Z-DNA conformation manipulation in radiotherapy.

This article is protected by copyright. All rights reserved

Photopyroptosis is an emerging research branch of photodynamic therapy (PDT), whereas there remains a lack of molecular structural principles to fabricate photosensitivers for triggering a highly efficient pyroptosis. Herein, we propose a general and rational structural design principle to implement this hypothesis. The principle relies on the clamping of cationic moieties (e.g., pyridinium, imidazolium) onto one photosensitive core to facilitate a considerable mitochondrial targeting (both of the inner and the outer membranes) of the molecules, thus maximizing the photogenerated reactive oxygen species (ROS) at the specific site to trigger the gasdermin E-mediated pyroptosis. Through this design, the pyroptotic trigger can be achieved in a minimum of 10 seconds of irradiation with a substantially low light dosage (0.4 J/cm2), compared to relevant work reported (up to 60 J/cm2). Moreover, immunotherapy with high tumor inhibition efficiency was realized by applying the synthetic molecules alone. This structural paradigm is valuable for deepening the understanding of PDT (especially the mitochondrial-targeted PDT) from the perspective of pyroptosis, towards the future development of the state-of-the-art form of PDT.

This article is protected by copyright. All rights reserved

Depression is one of the most common mental illnesses and is a well-known risk factor for suicide, characterized by low overall efficacy (< 50%) and high relapse rate (40%). A rapid and objective approach for screening and prognosis of depression is highly desirable but still awaits further development. Herein, we present a high-performance metabolite-based assay to aid the diagnosis and therapeutic evaluation of depression by developing a vacancy-engineered cobalt oxide (Vo-Co3O4) assisted laser desorption/ionization mass spectrometer platform. The nanoparticles with optimal vacancy achieve a signal enhancement (up to 20 folds than the commercialized products), characterized by favorable charge transfer and increased photothermal conversion. The optimized Vo-Co3O4 allows for a direct and robust record of plasma metabolic fingerprints (PMFs). Through machine learning of PMFs, high-performance depression diagnosis is achieved, with the areas under the curve (AUC) of 0.941–0.980 and an accuracy of over 92%. Further, a simplified diagnostic panel for depression is established, with a desirable AUC value of 0.933. Finally, we quantify proline levels in a follow-up cohort of depressive patients, highlighting the potential of metabolite quantification in the therapeutic evaluation of depression. Our work promotes the progression of advanced matrixes and brings insights into the management of depression.

This article is protected by copyright. All rights reserved

The in vivo fate of chemotherapeutic drugs plays a vital role in helping the understanding of the therapeutic outcome, side effects, and the mechanism of action. However, the lack of imaging abilities of most drugs, tedious labelling processes, and premature leakage of imaging agents currently result in loss of fidelity between the drugs and any imaging signals. Herein, an unique amphiphilic polymer was created by copolymerization of a NIR-II fluorophore drug tracer (T) and an anticancer Pt(IV) prodrug (D) of cisplatin in a hand-holding manner into one polymer chain for the first time. The obtained PolyplatinDT was capable of delivering the drugs and the fluorophores concomitantly at a precise D/T ratio, thereby resulting in tracking the platinum drugs and even readout of them in real-time via NIR-II fluorescence imaging both in vitro and in vivo. PolyplatinDT could self-assemble into nanoparticles, referred to as NanoplatinDT. Furthermore, a caspase-3 cleavable peptide with quenched FRET pairs that serves as an apoptosis protein reporter was attached to NanoplatinDT, resulting in NanoplatinDTR that were capable of simultaneously tracking platinum drugs with NIR-II fluorescence and evaluating the therapeutic efficacy with the apoptosis reporters. The strong correlations between the fluorescence intensity of the NIR-II fluorophores and 5′-FAM, and the Pt levels were investigated both in vitro and in vivo with NanoplatinDTR, enabling a quantitative readout of the platinum levels and feasible evaluation of treatment efficacy. Overall, we reported here the design of the first theranostic polymer with anticancer drugs, drug tracers, and drug efficacy reporters that could work in concert to provide possible insight into the drug fate and mechanism of action in vitro and in vivo.

This article is protected by copyright. All rights reserved

Seawater batteries that directly utilize natural seawater as electrolytes are ideal sustainable aqueous devices with high safety, exceedingly low cost, and environmental friendliness. However, the present seawater batteries are either primary batteries or rechargeable half-seawater/half-nonaqueous batteries because of the lack of suitable anode working in seawater. Here, we demonstrate a unique lattice engineering to unlock the electrochemically inert anatase TiO2 anode to be highly active for the reversible uptake of multiple cations (Na+, Mg2+, and Ca2+) in aqueous electrolytes. Density functional theory calculations and in-situ Raman further reveal the origin of the unprecedented charge storage behaviors, which can be attributed to the significant reduction of the cations diffusion barrier within the lattice, i.e., from 1.5 eV to 0.4 eV. As a result, the capacities of anatase TiO2 with 2.4% lattice expansion are ca. 100 times higher than the routine one in natural seawater, and ca. 200 times higher in aqueous Na+ electrolyte. The finding should significantly advance aqueous seawater energy storage devices closer to practical applications.

This article is protected by copyright. All rights reserved