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

Bioengineering

In article number 2303196, Twan Lammers, Horst Fischer, Fabian Kiessling, and co-workers establish mesoscopic 3D vascularized tumors in perfusable bioreactors to mimic the onset of metastasis in vitro. The “High Tide” cover art exemplifies how a tumor spheroid triggers bioprinted endothelium's angiogenesis, akin to the moon's effect on the sea, resulting in high tides.

Single-Atom Catalysts

In article number 2307991, Nuria López, Javier Pérez-Ramírez, Sharon Mitchell, and co-workers introduce open-access, machine-learning image analysis tools that can readily discriminate metal center organization in single-atom heterogeneous catalysts. The standardized approach rapidly detects features, including the fraction, size, and geometry of metal clusters present, offering valuable insights for confirming synthesis quality and advancing precision catalyst design.

Borophene-Based Heterostructures

In article number 2307591, Jia Zhang, Haibo Li, Jin Zhang, Wei Ma, and co-workers demonstrate the photoexcited carrier dynamics in borophene-based heterostructures. The diverse borophenes exhibit distinct and selective carrier transfer behaviors with an ultrafast timescale, enabling efficient charge separation and opening doors to potential applications in optoelectronic and photovoltaic devices.

Bismuth Oxides

In article number 2306205, Eric D. Wachsman, Kang Taek Lee, and co-workers report outstandingly conductive and stable bismuth oxides through a rational triple-doping strategy. The developed bismuth oxides show ≈140 times higher conductivity than YSZ for 1000 h at 600 °C. Designed low-temperature solid oxide electrochemical cells, utilizing the bismuth oxides, exhibit exceptional performances in both fuel cell (2.02 W cm−2) and electrolysis modes (0.95 A cm−2 at 1.3 V) at 600 °C.

Insulin–Dendrimer Nanocomplexes

In article number 2308965, Matthew J. Webber and co-workers present a new strategy to deliver insulin, from synergistic interactions between the insulin protein and a branched synthetic carrier, achieving nanoscale complex formation upon injection. The complexes are solubilized in response to changes in glucose level in order to correct the symptoms of diabetes in real time, with function lasting for at least a week.

Interfacial solar vapor generation (SVG) exhibits considerable potential to mitigate the global freshwater crisis for water and energy sustainability. Here, interfacial engineering of solar evaporators and devices design principles of SVG capable of efficient solar-to-thermal conversion, along with high-yielding liquid clean water is reviewed. The challenges and future opportunities are also discussed for fostering SVG economic and commercial applications.

Continuously increasing demand for the life-critical water resource induces severe global water shortages. It is imperative to advance effective, economic, and environmentally sustainable strategies to augment clean water supply. The present work reviews recent reports on the interfacial engineering to devices design of solar vapor generation (SVG) system for boosting the viability of drinkable water harvesting. Particular emphasis is placed on the basic principles associated with the interfacial engineering of solar evaporators capable of efficient solar-to-thermal conversion and resulting freshwater vapor via eliminating pollutants from quality-impaired water sources. The critical configurations manufacturing of the devices for fast condensation is then highlighted to harvest potable liquid water. Fundamental and practical challenges, along with prospects for the targeted materials architecture and devices modifications of SVG system are also outlined, aiming to provide future directions and inspiring critical research efforts in this emerging and exciting field.

This review article presents a comprehensive survey of the latest developments in near-infrared (NIR) light harvesting strategies, with a particular focus on the emerging field of two-photon excitation NIR photocatalysis. The emphasis is on the unique benefits offered by NIR light and two-photon excitation when compared to UV–visible irradiation and one-photon excitation.

Efficient utilization of sunlight in photocatalysis is widely recognized as a promising solution for addressing the growing energy demand and environmental issues resulting from fossil fuel consumption. Recently, there have been significant developments in various near-infrared (NIR) light-harvesting systems for artificial photosynthesis and photocatalytic environmental remediation. This review provides an overview of the most recent advancements in the utilization of NIR light through the creation of novel nanostructured materials and molecular photosensitizers, as well as modulating strategies to enhance the photocatalytic processes. A special focus is given to the emerging two-photon excitation NIR photocatalysis. The unique features and limitations of different systems are critically evaluated. In particular, it highlights the advantages of utilizing NIR light and two-photon excitation compared to UV–visible irradiation and one-photon excitation. Ongoing challenges and potential solutions for the future exploration of NIR light-responsive materials are also discussed.

The CO2 reduction electrolytic cells based on electrolyte flow system (flow cells) have shown great potential for industrial devices. An overview of design and optimization of flow cells for C2+ product is presented with a perspective to achieve their industrial applications in the near future.

Electrocatalytic CO2 reduction into value-added fuels and chemicals by renewable electric energy is one of the important strategies to address global energy shortage and carbon emission. Though the classical H-type electrolytic cell can quickly screen high-efficiency catalysts, the low current density and limited CO2 mass transfer process essentially impede its industrial applications. The electrolytic cells based on electrolyte flow system (flow cells) have shown great potential for industrial devices, due to higher current density, improved local CO2 concentration, and better mass transfer efficiency. The design and optimization of flow cells are of great significance to further accelerate the industrialization of electrocatalytic CO2 reduction reaction (CO2RR). In this review, the progress of flow cells for CO2RR to C2+ products is concerned. Firstly, the main events in the development of the flow cells for CO2RR are outlined. Second, the main design principles of CO2RR to C2+ products, the architectures, and types of flow cells are summarized. Third, the main strategies for optimizing flow cells to generate C2+ products are reviewed in detail, including cathode, anode, ion exchange membrane, and electrolyte. Finally, the preliminary attempts, challenges, and the research prospects of flow cells for industrial CO2RR toward C2+ products are discussed.

Many metal–organic frameworks consist of nodes such as Zr6O8 connected by organic linkers. Hydroxyl groups are present in various forms on the nodes, characterized by infrared and NMR spectroscopies. They have contrasting reactivities, and many play central roles in catalysis, with terminal hydroxyl groups being among the most reactive.

Among the most stable metal–organic frameworks (MOFs) are those incorporating nodes that are metal oxide clusters with frames such as Zr6O8. This review is a summary of the structure, bonding, and reactivity of MOF node hydroxyl groups, emphasizing those bonded to nodes containing aluminum and zirconium ions. Hydroxyl groups are often present on these nodes, sometimes balancing the charges of the metal ions. They arise during MOF syntheses in aqueous media or in post-synthesis treatments. They are identified with infrared and 1H nuclear magnetic resonance spectroscopies and characterized by their reactivities with polar compounds such as alcohols. Terminal OH, paired µ2-OH, and aqua groups on nodes are catalytic sites in numerous reactions. Relatively unreactive hydroxyl groups (such as isolated µ2-OH groups) may replace reactive groups and inhibit catalysis; some node hydroxyl groups (e.g., µ3-OH) are mere spectators in catalysis. There are similarities between MOF node hydroxyl groups and those on the surfaces of bulk metal oxides, zeolites, and enzymes, but the comparisons are mostly inexact, and much remains to be understood about MOF node hydroxyl group chemistry. It is posited that understanding and controlling this chemistry will lead to tailored MOFs and improved adsorbents and catalysts.

The poor reversibility of zinc anodes hampers the development of rechargeable alkaline zinc-based batteries due to dendrite formation, passivation, corrosion, and hydrogen evolution. In this review, optimization strategies including 3D structures, protective layers, alloying, additives, separators, and charge protocols, are suggested and summarized to overcome the challenges associated with Zn anodes and fully unlock their potential in alkaline zinc-based batteries.

Rechargeable alkaline zinc-based batteries (ZBBs) have attracted extensive research attention due to their advantages of low cost, high specific energy, and high safety. Although the investigation of cathodes for alkaline secondary ZBBs has reached a relatively advanced stage, the exploration of zinc anodes is still in its infancy. Zinc anodes in alkaline electrolytes encounter challenges such as dendrite formation, passivation, corrosion during periods of cell inactivity, and hydrogen evolution during cycling, thereby limiting their rechargeability and storability. Drawing upon the latest research on zinc anodes, six fundamental strategies that encompass a wide range of aspects are identified and categorized, from electrode modifications and electrolytes to charge protocols. Specifically, these strategies include 3D structures, coatings, alloying, additives, separators, and charge protocols. They serve as an insight summary of the current research progress on zinc anodes. Additionally, the complementary nature of these strategies allows for flexible combinations, enabling further enhancement of the overall performance of zinc anodes. Finally, several future directions for the advancement of practical alkaline Zn anode are proposed. This comprehensive review not only consolidates the existing knowledge but also paves the way for broader research opportunities in the pursuit of high-performance alkaline zinc anodes.

This review highlightsrecent progress in the field of nanoelectronics utilizing metal-insulatortransition (MIT) behaviors in Mott insulators. It covers a wide range oftopics, from the microscopic interactions in condensed matter systems to themacroscopic device functionalities by various external stimuli. This review servesas an overview and a comprehensive understanding of the design of next-generation MIT-based nanoelectronics.

Metal–insulator transition (MIT) coupled with an ultrafast, significant, and reversible resistive change in Mott insulators has attracted tremendous interest for investigation into next-generation electronic and optoelectronic devices, as well as a fundamental understanding of condensed matter systems. Although the mechanism of MIT in Mott insulators is still controversial, great efforts have been made to understand and modulate MIT behavior for various electronic and optoelectronic applications. In this review, recent progress in the field of nanoelectronics utilizing MIT is highlighted. A brief introduction to the physics of MIT and its underlying mechanisms is begun. After discussing the MIT behaviors of various Mott insulators, recent advances in the design and fabrication of nanoelectronics devices based on MIT, including memories, gas sensors, photodetectors, logic circuits, and artificial neural networks are described. Finally, an outlook on the development and future applications of nanoelectronics utilizing MIT is provided. This review can serve as an overview and a comprehensive understanding of the design of MIT-based nanoelectronics for future electronic and optoelectronic devices.

Relieving inflammation via scavenging toxic reactive oxygen species (ROS) during the acute phase of spinal cord injury (SCI) has been proved to be an effective strategy to mitigate secondary spinal cord injury and improve recovery of motor function. However, commonly used corticosteroid anti-inflammatory drugs such as methylprednisolone show adverse side effects which may induce gastrointestinal bleeding, femoral head necrosis and an increased risk of wound infection. Fortunately, hydrogen (H2), featuring selective antioxidant performance, easy penetrability and excellent biosafety, is being extensively investigated as a potential anti-inflammatory therapeutic gas for the treatment of SCI. In this work, by a facile in situ growth approach of gold nanoparticles (AuNPs) on the piezoelectric BaTiO3, a particulate nanocomposite with Schottky heterojunction (Au@BT) has been synthesized, which can generate H2 continuously by catalyzing H+ reduction through piezoelectric catalysis. Furthermore, theoretical calculations were employed to reveal the piezoelectric catalytic mechanism of Au@BT. Transcriptomics analysis and nontargeted large-scale metabolomic analysis reveal that the deeper mechanism of the neuroprotective effect of H2 therapy based on Au@BT + US. The as-prepared Au@BT nanoparticles have been first explored as a flexible hydrogen gas generator for efficient anti-inflammatory and pro-repair application for SCI therapy. This study highlights a promising prospect of nanocatalytic medicine for disease treatments by catalyzing H2 production, thus offering a significant alternative to conventional approaches against refractory spinal cord injury.

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Female sterilization via fallopian tube ligation is a common procedure. However, after the operation, over 10% of women seek re-fertilization, which is frequently unsuccessful. In addition, there is evidence that fallopian tubes contribute to the spread of endometriotic tissue as they serve as channels for proinflammatory media entering the abdominal cavity via retrograde menstruation. Here, we present stimuli-degradable hydrogel implants for the functional, biocompatible, and reversible occlusion of fallopian tubes. The hydrogel implants, designed with customized swelling properties, mechanically occlude fallopian tubes in a high-performance manner with burst pressures reaching 255–558 mmHg, exceeding normal abdominal pressures (95 mmHg). Their damage-free removal can be achieved within 30 minutes using near-visible UV light or a glutathione solution, employing a method akin to standard fallopian tube perfusion diagnostics. We demonstrate ultrasound-guided implant placement using a clinical hysteroscope in a human-scale uterus model and biocompatibility in a porcine in vivo model. Importantly, the prevention of live sperm as well as endometrial cell passage through blocked fallopian tubes is demonstrated. Overall, we present a multifunctional system that constitutes a possible means of on-demand, reversible contraception along with the first ever mechanical approach to abdominal endometriosis prevention and treatment.

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Rapid-acting, convenient, and broadly applicable medical materials are in high demand for the treatment of extensive and intricate tissue injuries in extremely medical scarcity environment, such as battlefields, wilderness, and traffic accidents. Conventional biomaterials fail to meet all the high criteria simultaneously for emergency management. Here, we have designed a multifunctional hydrogel system capable of rapid gelation and in situ spraying, addressing clinical challenges related to hemostasis, barrier establishment, support, and subsequent therapeutic treatment of irregular, complex and urgent injured tissues. This hydrogel can be fast formed in less than 0.5-second under ultraviolet initiation. The precursor maintains an impressively low viscosity of 0.018 Pa·s, while the hydrogel demonstrates a storage modulus of 0.65 MPa, achieving the delicate balance between sprayable fluidity and the mechanical strength requirements in practice, allowing flexible customization of the hydrogel system for differentiated handling and treatment of various tissues. Notably, the interactions between the component of this hydrogel and the cell surface protein confer upon its inherently bioactive functionalities such as osteogenesis, anti-inflammation, and angiogenesis. This research endeavored to provide new insights and designs into emergency management and complex tissue injuries treatment.

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Thermochromism, the change in color of a material with temperature, is the fundamental basis of optical thermometry. A longstanding challenge in realizing sensitive optical thermometers for widespread use is identifying materials with pronounced thermometric optical performance in the visible range. To this end, we demonstrate that single crystals of indium selenium iodide (InSeI), a 1D van der Waals (vdW) solid consisting of weakly-bound helical chains, exhibit considerable visible range thermochromism. We show a strong temperature-dependent optical band edge absorption shift ranging from 450 to 530 nm (2.8 to 2.3 eV) over a 380 K temperature range with an experimental (dEg/dT)max value extracted to be 1.26 × 10−3 eV K−1. This value appreciably lies above most dense conventional semiconductors in the visible range and is comparable to soft lattice solids. We further sought to understand the origin of this unusually sensitive thermochromic behavior and found that it arises from strong electron-phonon interactions and anharmonic phonons that significantly broaden band edges and lower the Eg with increasing temperature. Our identification of structural signatures resulting to sensitive thermochromism in exfoliable 1D vdW crystals opens avenues in discovering low-dimensional solids with strong temperature-dependent optical response across broad spectral windows, dimensionalities, and nanoscale size regimes.

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Following the success of dendritic cell (DC) vaccine, cell-based tumor vaccine shows its promise as a vaccination strategy. Except for DC cells, targeting other immune cells, especially myeloid cells are expected to address currently unmet clinical needs (e.g., tumor types, safety issues such as cytokine storms, and therapeutic benefits). Here, we show that an in situ injected macroporous myeloid cell adoptive scaffold (MAS) not only actively delivers antigens (Ags) that are triggered by scaffold-infiltrating cell surface thiol groups but also releases granulocyte–macrophage colony-stimulating factor (GM-CSF) and other adjuvant combos. Consequently, this promotes cell differentiation, activation, and migration from the produced monocyte and DC vaccines (MASVax) to stimulate antitumor T-cell immunity. Neoantigen-based MASVax combined with immune checkpoint blockade (ICB) induces rejection of established tumors and long-term immune protection. The combined depletion of immunosuppressive myeloid cells further enhanced the efficacy of MASVax, indicating the potential of myeloid cell-based therapies for immune enhancement and normalization treatment of cancer.

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Cellular energetics plays an important role in tissue regeneration, and the enhanced metabolic activity of delivered stem cells can accelerate tissue repair and regeneration. However, conventional hydrogels with limited network cell adaptability restrict cell–cell interactions and cell metabolic activities. In this work, we showed that a cell-adaptable hydrogel with high network dynamics enhanced the glucose uptake and fatty acid β-oxidation (FAO) of encapsulated human mesenchymal stem cells (hMSCs) compared with a hydrogel with low network dynamics. We further showed that the hMSCs encapsulated in the dynamic hydrogels exhibited increased TCA cycle activity, oxidative phosphorylation (OXPHOS) and ATP biosynthesis via an E-cadherin- and AMPK-dependent mechanism. The in vivo evaluation further showed that the delivery of MSCs by the dynamic hydrogel enhanced in situ bone regeneration in an animal model. We believe that our findings provide critical insights into the impact of stem cell–biomaterial interactions on cellular metabolic energetics and the underlying mechanisms.

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Solid-state potassium metal batteries (SPMBs) are promising candidates for the next generation of energy storage systems for their low cost, safety, and high energy density. However, full SPMBs have not yet been reported due to the K dendrites, interfacial incompatibility, and limited availability of suitable solid-state electrolytes. Here, we present stable SPMBs using a new iodinated solid polymer electrolyte (ISPE). The functional ions reconstruct ion transport channels, providing efficient potassium ion transport. ISPE shows a combination of high ionic conductivity, superior interfacial compatibility, and electrochemical stability. In-situ alloying and iodinated interlayer increase K metal compatibility for prolonged cycling with low polarization. Moreover, the ISPE enables SPMBs with Prussian blue cathode stable operation at a high voltage of 4.5 V, a superior rate capability, and long-term cycling over 3,000 cycles (4.2 V versus K+/K) with an ultra-high coulombic efficiency of 99.94%. More importantly, a classic solid-state potassium metal pouch cell achieved 4.2 V stable cycling over 800 cycles with an high retention of 93.6%, presenting a new development strategy for secure and high-performance rechargeable solid-state potassium metal batteries.

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Accurate structure control in dissipative assemblies is vital for precise biological functions. However, the accuracy and functionality of current artificial dissipative assembly are far from this objective. Herein, we introduce a novel approach by harnessing complex chemical reaction networks (CRN) rooted in coordination chemistry to create well-defined dissipative assemblies. We designed atomically-precise Cu nanocluster (CuNCs), specifically Cu11(μ9-Cl)(μ3-Cl)3L6Cl clusters (L = 4-methyl-piperazine-1-carbodithioate). Cu(I)-ligand ratio change and dynamic Cu(I)-Cu(I) metallophilic/coordination interactions enable the reorganization of CuNCs into metastable CuL2, finally converting into the equilibrium [CuL·Y]Cl complexes (Y = MeCN or H2O) via Cu(I) oxidation/reorganization and ligand exchange process. Upon adding fuels (ascorbic acid, AA), the system goes further dissipative cycles. We observed that the encapsulated/bridging halide ions exert a subtle influence on the optical properties of CuNCs and topological changes of polymeric networks when integrating CuNCs as crosslink sites. CuNCs duration and switch period could be controlled by varying the ions, AA concentration, O2 pressure and pH. The unique Cu(I)-Cu(I) metallophilic and coordination interactions provide a versatile toolbox for designing delicate life-like materials, paving the way for tailored dissipative assemblies with precise structures and functionalities. Furthermore, these CuNCs can be employed as modular units within polymers for materials mechanics or functionalization studies, expanding their potential applications.

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Lithium (Li) metal batteries (LMBs) are considered the most promising high-energy-density electrochemical energy storage devices of the next generation. However, the unstable solid-electrolyte interphase (SEI) derived from electrolytes usually lead to high impedance, Li dendrites growth and poor cyclability. Herein, the ferroelectric BaTiO3 with orderly arranged dipoles (BTOV) is integrated on the polypropylene separator as a functional layer. Detailed characterizations and theoretical calculations indicate that surface oxygen vacancies (OVs) drive the phase transition of BaTiO3 materials and promote the ordered arrangement of dipoles. The strong dipole moments in BTOV can adsorb TFSI− and NO3 − anions selectively and promote their preferential reduction to form a SEI film enriched with inorganic LiF and LiNxOy species, thus facilitating the rapid transfer of Li+ and restraining the growth of Li dendrites. As a result, the Li-Li cell with the BTOV functional layer exhibit enhanced Li plating/stripping cycling with an ultra-long life of over 7000 hours at 0.5 mA cm−2/1.0 mAh cm−2. And the LiFePO4 || Li (50 μm) full cells display excellent cycling performance exceeding 1760 cycles and superior rate performance. This work provides a new perspective for regulating the SEI chemistry by introducing ordered dipoles to control the distribution and reaction of anions.

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