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

Cu2-xTe electrodes are disclosed in acidic multivalent-ion batteries for the first time to achieve a high capacity of up to 409 mAh g−1 and a long cycling lifespan of 40 000 cycles. Composite in situ X-ray diffraction measurements and spectroscopic analyses show that the synergistic copper-ion/proton electrolyte environment ensures stable reversible storage of copper-ions and prevents potential material oxidation.

Acidic batteries permit a reliable energy supply at low temperatures with low cost and intrinsic safety, yet the development of stable acid-resistant electrodes with high capacity and a reliable lifespan is still challenging. Herein, nonstoichiometric copper telluride (Cu2-xTe) nanosheets are first explored as high-performance electrodes for acidic batteries to provide a stable capacity release of 409 mAh g−1 with a record-breaking lifespan of 40 000 cycles and excellent kinetics, enabling operation at a high current density of 20 A g−1. In contrast to the inherent perception of corrosive destruction of electrode materials by strongly acidic environments, the electrolyte environment enriched with copper ions and hydrogen ions synergistically stabilizes the Cu2-xTe electrode and drives reversible multielectron transfer asymmetric deep conversion, which is confirmed by in situ synchrotron X-ray diffraction, X-ray absorption spectroscopy, first-principal calculations, and composite electrochemical characterization. Therefore, Cu2-xTe provides an impressive accumulation capacity of over 4764 Ah g−1, exceeding that of most acidic batteries, and works well at −20 °C. High-performance Cu2-xTe electrodes also promote the establishment of Cu2-xTe//Mn2O3 and Cu2-xTe//Fe acidic full cells enabling stable operation at room temperature and low temperature, offering promising opportunities for electrode progress in advanced acidic batteries.

Biocompatible, low-bandgap conjugated polymer nanosheets are interfaced with non-photosynthetic and non-genetic engineered Escherichia coli for solar hydrogen production using near-infrared light. The rationally designed polymer nanosheets play a crucial role in harnessing the broad solar spectrum and injecting photo-generated electrons into bacteria, thereby enhancing hydrogen production.

The efficient conversion of solar energy into clean hydrogen fuel presents a promising pathway for sustainable energy production. However, utilizing the full solar spectrum, particularly the near-infrared (NIR) region, remains underexplored in photosynthetic biohybrid systems. In this study, biocompatible, low-bandgap conjugated polymer nanosheets (PyTT-tBAL-HAB) are developed to integrate with non-photosynthetic, non-genetically engineered Escherichia coli (E. coli) for enhanced solar-driven biological hydrogen production. The PyTT-tBAL-HAB nanosheets exhibit unique NIR light absorption properties. Integrating these nanosheets with E. coli facilitates efficient electron transfer, resulting in a 1.96-fold increase in hydrogen production rate under NIR light. Consequently, this photosynthetic biohybrid system achieves a quantum efficiency of 18.36% at 940 nm. This study demonstrates the potential of using low-bandgap conjugated polymer nanosheets as advanced photosensitizers in semi-artificial photosynthetic systems, offering a robust platform for the effective utilization of the solar spectrum.

A strategy for azepination-induced frontier molecular orbital (FMO) delocalization of multiple resonance (MR) emitters is proposed to construct long-wavelength MR materials. Organic light-emitting diode based on m-PAz-BNCz exhibits excellent electroluminescence performances with Commission Internationale de L'Eclairage coordinates of (0.26, 0.70) and a maximum external quantum efficiency of 36.2%.

Developing diversified construction strategies for high-color-purity and efficient multiple resonance thermally activated delayed fluorescence (MR-TADF) materials is a major strategic demand to meet the requirements of ultra-high-definition organic light-emitting diode (OLED) displays, posing a significant challenge to the design and synthesis of emitters at the molecular level. Herein, a strategy is proposed for azepination-induced frontier molecular orbital (FMO) delocalization of MR emitters, that is, embedding azepine into the prototype molecule BNCz can effectively improve the π-conjugation degree and extend the FMO delocalization, thereby constructing a series of long-wavelength MR-TADF materials with narrowband emission. Through an intramolecular Scholl reaction, these target molecules with an azepine-embedded core are afforded by one-fold heptagonal cyclization of BNCz core and the phenyl ring attached to (aromatic amine-substituted) aryl precursor. They all exhibit efficient green emission around 520 nm and narrow full-widths at half-maximum (FWHMs) of ≤ 37 nm in toluene. OLEDs employing these emitters show excellent electroluminescence (EL) performances, among which m-PAz-BNCz-based OLED exhibits the optimal EL performances with a peak of 528 nm, a FWHM of 37 nm, Commission Internationale de L'Eclairage (CIE) coordinates of (0.26, 0.70), and a maximum external quantum efficiency (EQE) of 36.2%.

A lanthanide Eu(II) complex is demonstrated as an emitter in light-emitting electrochemical cells (LECs) for the first time. The bis[hydrotris(3-tert-butylpyrazolyl)borate]europium(II) complex based LEC achieved a record-breaking external quantum efficiency of 19.8% with Commission Internationale de L'Eclairage coordinates of (0.12, 0.18).

Light-emitting electrochemical cells (LECs) have good prospects in the solid-state lighting field due to their simple single-layer structure and low manufacturing cost. However, the lack of high-efficiency blue LECs limits their development and further application. To solve this problem, many luminescent materials with various mechanisms such as fluorescence, phosphorescence, and thermally-activated delayed fluorescence are studied as emitters in LECs. Besides these materials, herein lanthanide europium(II) (Eu(II)) complex with d-f transition is demonstrated as a new type of emitter for LECs. In detail, a blue emitting Eu(II) complex bis[hydrotris(3-tert-butylpyrazolyl)borate]europium(II) is dispersed into 9-(3-(triphenylsilyl)phenyl)-9H-3,9′-bicarbazole host and tetrahexylammonium tetrafluoroborate electrolyte to make a blend film, which attains a high photoluminescence quantum yield of ≈100%. The LEC using the blend film as an active layer achieves a blue emission with Commission Internationale de L'Eclairage coordinates of (0.12, 0.18) and a record-breaking external quantum efficiency of 19.8%, corresponding to an exciton utilization efficiency of ≈100%. This work reveals that Eu(II) complex with d-f transition is a promising emitter toward high-performance blue LECs, which can inspire further research on Eu(II) complex based LECs.

The Cd–S co-alloying-induced microstructural evolution enables high-performance Sb2Te3-based thermoelectrics. Subsequently, an innovative full-scale Bi–Sb–Te segmented power generator is fabricated, extending the operational range of conventional Bi2Te3-based modules from 500 to 650 K and achieving an exceptional efficiency of 9.3% under a distinct ΔT = 350 K. Notably, it exhibits remarkable stability after 80-cycle thermal shock and 160-h thermal durability, highlighting great potential for low-grade waste heat recovery.

Thermoelectric (TE) technology offers a promising solution for waste heat recovery, particularly in applications involving abundant low-grade heat (<650 K). However, for over half a century, TE power generators have predominantly relied on Bi2Te3 alloys with limited efficiencies below 7%. Herein, Cd and S are doped into Sb2Te3 to promote microstructural regulation characterized by dense twin boundaries and dislocations, resulting in a 45% reduction of lattice thermal conductivity at 300 K. Combined with the optimized density-of-states effective mass and expanded band gap, the Cd0.04Sb1.96Te2.94S0.06 sample attains a peak ZT of 1.1 at 650 K and an average ZT of 1.0 from 500 to 650 K, while exhibiting remarkable compressive and bending strengths of 197 and 56 MPa. Most importantly, a well-designed, homogeneous segmented TE power generator, constructed entirely from Bi–Sb–Te alloys, achieves a remarkable efficiency of 9.3% under a temperature gradient of 350 K, as certified by third-party validation. This work provides new insights into extending the operation temperature of Bi2Te3, demonstrating great potential for low-grade waste heat harvest.

Cellulose triacetate-based binder with broad compatibility, high ionic conductivity, and superior binding strength has been successfully designed and validated through its application in high-voltage polyanionic cathodes (Na3V2(PO4)2O2F), layered oxide cathodes (NaNi1/3Fe1/3Mn1/3O2), and tunnel-type oxide cathodes (Na0.61[Mn0.27Fe0.34Ti0.39]O2). This work presents a sustainable and effective strategy for achieving high-performance sodium-ion batteries.

Binders play a pivotal role in the performance of sodium-ion battery (SIB) cathodes, but traditional binders often struggle to balance broad compatibility, high ionic conductivity, superior binding strength, and environmental sustainability. In this study, a universal cellulose triacetate (TAC)-based binder (TAC-MMT) composed of TAC and natural montmorillonite (MMT) is designed to facilitate rapid Na+ transport pathways and establish a robust hydrogen-bonding network. This innovative TAC-MMT binder features a unique chemical structure that achieves high ionic conductivity through a self-enrichment and fast-transport mechanism, while its superior binding strength is attributed to hydrogen-bonding crosslinks between proton acceptors (C═O) in TAC and proton donors (−OH) in MMT. More importantly, the outstanding solubility and film-forming properties of TAC-MMT contribute to stable electrode protection and broad compatibility with high-voltage SIB cathodes. Benefiting from these advantages, the Na3V2(PO4)2O2F (NVPOF) electrodes with the TAC-MMT binder demonstrate exceptional performance, including a high capacity retention of 95.2% over 500 cycles at 5C and a rapid rate response of up to 15C. The versatility of the TAC-MMT binder is further confirmed with high-voltage NaNi1/3Fe1/3Mn1/3O2 and Na0.61[Mn0.27Fe0.34Ti0.39]O2 cathodes. This study highlights the potential of biomass-based binders as a sustainable and effective solution for advancing high-performance sodium-ion batteries.

This review provides a comprehensive analysis of engineering modification strategies for ruthenium (Ru)-based catalysts, highlighting their critical role in optimizing electronic structures and surface properties to enhance electrocatalytic conversion. Furthermore, it emphasizes the integration of multiple engineering strategies aimed at improving catalytic performance, while also addressing key commercialization challenges.

Electrochemical conversion has been regarded as an ideal technology for achieving clean and sustainable energy, showing significant promise in addressing the increasingly serious energy crisis and environmental pollution. Ru-containing electrocatalysts (RUCE) outperform other precious metals due to elevated intrinsic activity and superior cost-effectiveness, developing into a promising candidate for electrochemical conversion reactions. A significant challenge in the field of catalyst discovery lies in its heavy reliance on empirical methods, rather than approaches that are rooted in rational design principles. This review first concentrates on the catalytically active sites and critical factors governing catalytic activity and performance durability. Then, a comprehensive summary of multifunctional modification strategies ranging from nanoscale to atomic scale is explored to control the structure and improve the performance. By unveiling the roles of each component in the modified RUCE at the atomic level, their intrinsic active sites are identified and discussed to establish the structure-performance relationship of the catalysts. Finally, the challenges and perspectives of Ru-based materials for electrochemical hydrogen, oxygen, and nitrogen conversion reactions are presented to inspire further efforts toward understanding RUCE to meet the ever-growing demand in the future.

A Bi-based catalyst is developed via the electrochemical transformation of bismuth-oxide composites, inducing enhanced lattice strain to optimize catalytic performance. At an applied potential of −0.76 V versus RHE, the catalyst exhibits outstanding efficiency in glycine electrosynthesis, achieving a Faradaic efficiency (FE) of 79.1% and a record-high glycine concentration of 0.17 m, significantly outperforming conventional Bi-based systems. Moreover, the introduction of glycolaldehyde and hydroxylamine as reactants further elevate the glycine FE to 91.3%, with an impressive production rate of 2433.3 µmol h−1 under identical conditions.

Glycine plays a crucial role in various industrial and daily applications. However, traditional synthesis methods are often associated with high toxicity, energy intensity, and inefficiency. This study introduces an efficient and eco-friendly method for synthesizing glycine via the reductive coupling of oxalic acid and nitrate using a Bi metal catalyst, enhanced by lattice strain from Bi and oxide composites undergoing electrochemical transformation. At an applied potential of −0.76 V versus the reversible hydrogen electrode (RHE), the Bi catalyst achieves an impressive glycine Faradaic efficiency (FE) of 79.1%, yielding a record concentration of 0.17 m, substantially higher than conventional Bi-based systems. Furthermore, the introduction of glycolaldehyde and hydroxylamine as reactants raise the glycine FE to 91.3% with a production rate of 2433.3 µmol h−1 under identical conditions. Electrochemical analysis and theoretical calculations demonstrate that lattice expansion notably boosts glycine synthesis by facilitating NH2OH formation and promoting the efficient reduction of oxime intermediates. These results underscore the significance of lattice engineering in enhancing active site performance and accelerating reaction kinetics, offering a sustainable and efficient alternative to traditional glycine synthesis methods.

A heavy-metal removal battery is designed, which displays the capacity of simultaneous heavy-metal ion adsorption and electricity generation. In such battery, the heavy-metal ion adsorption is driven by the potential difference between adsorption electrodes and metal electrodes. Furthermore, a chemical oxidation strategy is developed to desorb heavy-metal ions from adsorption electrodes, achieving the recycling of the electrodes.

The heavy-metal ion in wastewater is a great threat to the health of both humans and ecosystems. The common heavy-metal ion removal strategies usually suffer from energy consumption and poor recyclability. Herein, a heavy-metal removal battery is designed by constructing a two-chamber configuration. Such battery displays the capacity of simultaneous heavy-metal ion adsorption and electricity output, where heavy-metal ion adsorption is driven by the potential difference between adsorption electrodes and metal electrodes, and electricity is generated continuously during the adsorption process. Significantly, various heavy-metal ions (e.g., Mn2+, Co2+, Ni2+, Zn2+, Cr3+ and Pb2+ ions) can be removed due to the large lattice spacing of active materials in adsorption electrodes, displaying the universality of adsorbing heavy-metal ions from wastewater. In addition, an environmental-friendly chemical oxidation strategy is developed to desorb heavy-metal ions from adsorption electrodes, which not only produces high-quality metal salts, but also reduces the toxicity of sludge in the case of secondary pollution. Impressively, these heavy-metal removal batteries can be easily scaled up and integrated to extend the heavy-metal ion adsorption ability and voltage/current output. This work proves a creative approach for simultaneous heavy-metal ion removal and electricity generation from wastewater.

The TOC illustrates Cs₃Cu₂Br₅, Cs₃Cu₂Cl₅, and double perovskite suspensions, the 3D-printed “MIZZOU” text under 325 nm laser excitation, the corresponding emission spectra of the color conversion layer, and the CIE 1976 (u', v') color space of the fabricated white LED.

Metal halide perovskites and their derivatives have emerged as highly promising materials for next-generation optoelectronic devices, owing to their intrinsic defect tolerance and exceptional electrical and optical properties. Among these, lead-free copper(I)-based halide perovskite derivatives, Cs₃Cu₂X₅ (X = Cl, Br, I) (CHPs), have garnered significant attention as environmentally friendly and stable alternatives to lead-based perovskites. In this study, a cost-effective and sustainable synthesis route for Cs₃Cu₂Cl₅ and Cs₃Cu₂Br₅ powders is developed, which exhibit strong green (≈526 nm) and blue (≈458 nm) emissions, and achieve remarkable photoluminescence quantum yields (PLQYs) of 100% and 92%, respectively. Cs₃Cu₂X₅ (X = Cl, Br) powders are incorporated into 3D-printed structures, exhibiting excellent transparency and color stability. Furthermore, white LEDs are fabricated by using the green-emitting Cs₃Cu₂Cl₅ and blue-emitting Cs₃Cu₂Br₅ and a yellow-emitting double perovskite (PLQY≈ 73%), resulting in devices with an exceptionally high color rendering index (CRI) of up to 98 and tunable correlated color temperatures (CCTs) ranging from 3864 to 9677 K, closely mimicking natural white light. Beyond solid-state lighting, the superior optical performance and stability of Cs₃Cu₂X₅ (X = Cl, Br) powders open new avenues for their application in photovoltaics and other optoelectronic devices.

Mesoporous core@shell Cu2O/Cu@PdCu nanozymes are demonstrated as efficient tandem electrocatalyst for highly selective NH3 electrosynthesis from NO3 − at fairly positive potentials. Meanwhile, this enzyme-like electrocatalyst performs perfectly in the two-electrode coupling system for cathode NO3 −-to-NH3 and anode ethanol oxidation in a more energy-efficient manner.

Electrocatalytic tandem nitrate reduction to ammonia (NO3 −-to-NH3) offers a promising pathway for energy and environmental sustainability. Although considerable efforts have been presented to modulate the reaction pathways for enhanced NO3 −-to-NH3 electrocatalysis, these advances often require relatively high overpotentials to balance yield rate and selectivity of NH3, resulting in a remarkable energy inefficiency. Inspired by enzyme catalysis in nature, herein a tandem enzyme-like electrocatalyst is designed consisting of a core of Cu2O/Cu heterojunction surrounded by mesoporous PdCu shell (Cu2O/Cu@mesoPdCu) that accelerated NO3 −-to-NH3 electrocatalysis in positive potentials. Impressively, Cu2O/Cu@mesoPdCu nanozymes hold superior performance for robust NH3 electrosynthesis in a fairly positive potential of 0.10 V (versus reversible hydrogen electrode), having Faraday efficiency of 96.2%, yield rate of 13.3 mg h−1 mg−1, and half-cell energy efficiency of 46.0%. Kinetic studies, in situ spectra and density functional theory calculations revealed that Cu2O/Cu core preferentially adsorbed NO3 − and further reduced to *NO2, while active hydrogen radicals enriched on PdCu shell promoted multistep hydrodeoxygenation of *NO2 to NH3 within “semi-closed” mesoporous microenvironment, both of which synergistically enabled tandem electrocatalysis in positive potentials. Moreover, this enzyme-like electrocatalyst disclosed better NO3 −-to-NH3 performance in a more energy-efficient manner when coupling with more thermodynamically favorable ethanol oxidation reaction.

Residue-free 2D materials with exceptional cleanliness and high quality are achieved using van der Waals interaction-based fabrication and manipulation techniques, completely free from polymers and solvents. Precise manipulation enables the construction of vdW heterostructures with controlled alignment, expanding the potential of 2D materials for next-generation electronic and optoelectronic devices.

2D materials have garnered considerable attention due to their distinctive properties, prompting diverse applications across various domains. Beyond their inherent qualities, the significance of 2D materials extends into the fabrication processes that can lead to the degradation of intrinsic performance through undesirable mechanical defects and surface contaminations. Herein, a novel fabrication technique to achieve residue-free 2D materials using van der Waals (vdW) interactions, primarily employing molybdenum disulfide (MoS2) is proposed. Optical and electrical characterizations confirm the absence of residues, mechanical defects, oxidation, and strain, along with a prominent field-effect mobility of up to 60 cm2 V−1 s−1 and an on/off ratio of ≈108. Furthermore, the utilization of residue-free material as a stamp enables various manipulations of flakes transferred on substrates in advance, including pick-up and release, stacking, exfoliation, wiping-out, flipping, and smoothing-out processes. Additionally, the manipulation techniques also facilitate the fabrication of vdW heterostructures with precise positioning and the desired stacking order. In this regard, the feasibility of applying this method to hexagonal boron nitride and graphite is demonstrated. It is expected that this method will offer a versatile and effective approach to enhancing the qualities of 2D material-based electronic and optoelectronic devices.

A universal strategy for constructing ultrasensitive self-powered sensing materials with dual-gradient heterojunctions is developed through the induction of anionic and cationic polymer gradient distribution under direct current electric field.

The hydrogel ionic diode is regarded as a promising self-powered sensor, capable of harvesting energy from low-frequency stimuli human motions and converting it into electrical signals. However, the sensitivity of the reported conventional bilayer hydrogel ionic diodes are relatively low, due to the single heterojunction interface and high interface resistance, making it challenging to meet the demands of high-precision sensing. Here, a universal method for fabricating dual-gradient hydrogel ionic diodes without bilayer structure through the induction of anionic and cationic polymer gradient distribution via a direct current electric field is developed. Due to the dual-gradient distribution, numerous heterogeneous microstructures (i.e., microdiodes) with low interface resistance are formed in the bulk phase of hydrogel, and these series-connected microdiodes demonstrate a significantly increase in open circuit voltage in response to mechanical pressure. The dual-gradient hydrogel ionic diode exhibits ultra-high sensitivity (1247.3 mV/MPa) and ultralow detection limit (0.8 Pa), enabling the smart prosthetic hand to non-destructive grasp ultrasoft tofu. This work is expected to pave the way for novel high-precision self-powered sensors in intelligent wearable electronics.

A novel highly biocompatible organic phosphorescent HOF nanoscintillators (BPT-HOF@PEG) is designed and engineered to enhance X-PDT for unresectable HCC treatment. Precise tumor localization capability of SRT and effective X-ray energy absorbing and transferring capability of BPT-HOF@PEG endowing BPT-HOF@PEG-mediated X-PDT approach with significant HCC therapeutic potential. Therefore, phosphorescent HOF-based X-PDT is an ideal alternative therapy for patients with unresectable HCC.

X-ray induced photodynamic therapy (X-PDT) leverages penetrating X-ray to generate singlet oxygen (1O2) for treating deep-seated tumors. However, conventional X-PDT typically relies on heavy metal inorganic scintillators and organic photosensitizers to produce 1O2, which presents challenges related to toxicity and energy conversion efficiency. In this study, highly biocompatible organic phosphorescent nanoscintillators based on hydrogen-bonded organic frameworks (HOF) are designed and engineered, termed BPT-HOF@PEG, to enhance X-PDT in hepatocellular carcinoma (HCC) treatment. BPT-HOF@PEG functions simultaneously as both scintillator and photosensitizer, effectively absorbing and transferring X-ray energy to generate abundant 1O2. Both in vitro and in vivo investigations demonstrate that internalized BPT-HOF@PEG efficiently produces significant quantities of 1O2 upon X-ray irradiation. Additionally, X-ray exposure directly inflicts DNA damage, and the synergistic effects of these mechanisms result in pronounced cell death and substantial tumor growth inhibition, with a significant inhibition rate of up to 90.4% in vivo assessments. RNA sequencing analyses reveal that X-PDT induces apoptosis in Hepa1-6 cells while inhibiting cell proliferation, culminating in tumor cell death. Therefore, this work highlights the considerable potential of efficient phosphorescent HOF nanoscintillators-based X-PDT as a promising therapeutic approach for HCC, providing a highly effective alternative with negligible toxicity for patients with unresectable tumors.

Atomic-Scale Polarization

In article number 2420510, Walid A. Daoud and colleagues report an atomic-scale polarization-functionalized Mn3O4-based catalyst for vanadium redox flow battery, where the role of vacancy-induced local polarization on vanadium redox reactions is investigated. The findings shed light on the fundamental rules governing the utility and evolution of vacancies in transition metal oxide electrocatalysts, thereby moving a step closer toward their deployment in a wide range of sustainable energy storage schemes.

Cancer Cell Detection

In article number 2412738, Zihan Zhao, Guangwei Hu, Xumin Ding, and co-workers report a method that employs a multiplexed THz metachip with high sensitivity to capture rich spectral signatures of human cancer cells and maps them in a three-dimensional spatial coordinate. The experimental detection success rate reaches 93.33%, providing a novel path for early cancer screening technology.

Hybrid Organic–Inorganic MXenes

This cross-sectional STEM image captures the wave-like rippling observed in an organic-inorganic hybrid 2D MXene. Here, these ripples, often referred to as Ripplocations, are formed when the organic surface groups are exposed to the electron beam. Ripplocations are a fundamental defect in layered materials and may play a key role in how the material responds to stress and external conditions. More details can be found in article number 2411669 by Francisco Lagunas, Robert F. Klie, and co-workers.

X-Ray Induced Photodynamic Therapy

A novel biocompatible organic phosphorescent HOF nanoscintillator (BPT-HOF@PEG) was fabricated to enhance X-ray induced photodynamic therapy (X-PDT) for treating unresectable hepatocellular carcinoma (HCC). The precise tumor localization ability of stereotactic radiotherapy, along with the efficient X-ray energy absorption and transfer properties of BPT-HOF@PEG, provides significant therapeutic potential for HCC treatment, making this phosphorescent HOF-based X-PDT a promising alternative for patients with unresectable HCC. More details can be found in article number 2417001 by Feng Shen, Huijing Xiang, Yu Chen, Tian Yang, and co-workers.