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Energy Environ. Sci., 2025, Accepted Manuscript
DOI: 10.1039/D4EE05264A, PaperQin Wang, Yiming Zhang, Meng Yao, Kang Li, Lv Xu, Haitao Zhang, Xiaopeng Wang, Yun Zhang
The utilization of high-capacity lithium-rich layered oxide (LRLO) in lithium-ion batteries is hampered by its severe interface reactions and poor interface dynamics. Herein, an OG gate (OG) is constructed on...
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Soft-actuated cuff electrodes (SACE) for bidirectional peripheral interfaces enable minimal and secure contact to the nerve through fluid injection-based soft actuation. A 3D bent structure can grasp and securely contact the nerves with only a little pressure (<1.21 gram-force). The SACE can achieve negligible damage to the nerve during recording of sensory and motor feedback signals with superior SNR and neuromodulation for long-term studies.

Abstract

Neural interfaces with embedded electrical functions, such as cuff electrodes, are essential for monitoring and stimulating peripheral nerves. Still, several challenges remain with cuff electrodes because sutured devices can damage the nerve by high pressure and the secured contact of electrodes with the nerve is hard to accomplish, which however is essential in maintaining electrical performance. Here, a sutureless soft-actuated cuff electrodes (SACE) that can envelop the nerve conveniently by creating a bent shape controlled upon fluid injection, is introduced. Moreover, fluid injection protrudes part of the device where electrodes are formed, thereby achieving minimized, soft but secure contact between the electrodes and the nerve. In vivo results demonstrate the successful recording and stimulation of peripheral nerves over time up to 6 weeks. While securing contact with the nerve, the implanted electrodes can preserve the nerve intact with no reduction in blood flow, thereby indicating only minimal compressive force applied to the nerve. The SACE is expected to be a promising tool for recording and stimulation of peripheral nerves toward bidirectional neuroprostheses.

A novel UV-induced two-step thiol-ene “click chemistry” is introduced for the tailorable fluorescent perovskite quantum dots (T-PQDs). A protective shell is formed around the PQDs in the first step, while chemical cross-linking between PQD and thiol-ene polymer occurs in the second step. The T-PQDs offer high efficiency, stability, and processability, facilitating their multiform manufacturing for a wide range of applications.

Abstract

In practical applications, fluorescent perovskite quantum dots (PQDs) must exhibit high efficiency, stability, and processibility. So far, it remains a challenge to synthesize PQDs with stable dispersibility in tailorable monomers both before and after photocuring. In this work, a novel strategy of UV-induced two-step thiol-ene “click chemistry” is proposed to prepare PQDs with these attributes. The first step aims to epitaxially grow a shell around the PQD core to ensure stable dispersibility in a thiol-ene monomer solution. The second step is to achieve stable dispersibility in the photocured thiol-ene matrixes for multiform manufacturing processes. The tailorable PQDs (T-PQDs) not only have the highest photoluminescence quantum yield (PLQY) to ≈100% for green emission and over 96% for red emission, but also exhibit remarkable stability under severe conditions, including “double 85” aging, water exposure, and mechanical stress. Moreover, their exceptional processability allows for various processing techniques, including slot-die coating, inkjet printing, direct-laser writing, UV-light 3D printing, nanoimprinting, and spin coating. The high efficiency and stability of T-PQDs facilitate their multiform manufacturing for a wide range of applications.

In this study, bi-confinement effects arising from a highly cross-linked polymer network and rigid Al₂O₃ matrix are exploited to achieve ultra-stable carbonized polymer dots (CPDs). The obtained CPDs@Al2O3 composite demonstrates exceptional long-term stability in various solvents and high photoluminescence emission thermotolerance up to 500 K for 150 h, representing the best performance of carbon dots under harsh conditions reported to date.

Abstract

Carbon dots are emerging luminescent nanomaterials that have drawn considerable attention due to their abundance, environmental friendliness, and customizable optical properties. However, their susceptibility to temperature-induced vibrational exciton changes and the tendency to thermal quenching of emission have hindered their practical applications. Here, a method is reported for achieving high-temperature photoluminescence carbonized polymer dots (CPDs) through a bi-confinement approach that involves a highly cross-linked polymer network and a rigid Al2O3 matrix. As the temperature increased from 303 to 500 K, the fluorescence and phosphorescence emission intensities of CPDs@Al2O3 remained virtually unchanged, with the emission duration exceeding 150 h at 500 K. Additionally, CPDs@Al2O3 composites with different degrees of carbonization exhibit dynamic excitation-dependent photoluminescence properties, which can be patterned for multiple information encryption application. This work provides a concept for designing stable and luminous CPDs under harsh conditions, thus expanding their potential application range.

A stretchable multimodal photonic sensor capable of simultaneously detecting and discriminating strain deformations, temperature, and sweat pH is developed for on-skin health monitoring. By integrating multiple sensing mechanisms in a single hydrogel-coated PDMS optical fiber (HPOF) at distinct wavelengths, the device achieves simultaneous monitoring of heartbeat, respiration, body temperature, and sweat pH of a person in real-time with negligible crosstalk.

Abstract

Stretchable sensors that can conformally interface with the skins for wearable and real-time monitoring of skin deformations, temperature, and sweat biomarkers offer critical insights for early disease prediction and diagnosis. Integration of multiple modalities in a single stretchable sensor to simultaneously detect these stimuli would provide a more comprehensive understanding of human physiology, which, however, has yet to be achieved. Here, this work reports, for the first time, a stretchable multimodal photonic sensor capable of simultaneously detecting and discriminating strain deformations, temperature, and sweat pH. The multimodal sensing abilities are enabled by realization of multiple sensing mechanisms in a hydrogel-coated polydimethylsiloxane (PDMS) optical fiber (HPOF), featured with high flexibility, stretchability, and biocompatibility. The integrated mechanisms are designed to operate at distinct wavelengths to facilitate stimuli decoupling and employ a ratiometric detection strategy for improved robustness and accuracy. To simplify sensor interrogation, spectrally-resolved multiband emissions are generated upon the excitation of a single-wavelength laser, utilizing upconversion luminescence (UCL) and radiative energy transfer (RET) processes. As proof of concept, this work demonstrates the feasibility of simultaneous monitoring of the heartbeat, respiration, body temperature, and sweat pH of a person in real-time, with only a single sensor.

Advanced Materials, Volume 37, Issue 5, February 5, 2025.

Wetting-Induced Process

The wetting-induced interconnected reentrant geometry (WING) process enables the large-scale fabrication of multifunctional re-entrant microcavity surfaces, representing a significant technological advancement. Utilizing capillary action in a scalable roll-to-roll printing technique, it produces surfaces with exceptional liquid repellency while maintaining microstructures under external forces. This process offers a cost-effective and high throughput solution for various applications, such as anti-icing, anti-fouling, and particle capture. More details can be found in article number 2411064 by Seok Kim, Young Tae Cho, and co-workers.

Recyclable Polyimide Composite Aerogels

In article number 2411599 by Wim J. Malfait, Qinghua Zhang, Shanyu Zhao, and co-workers, a molecular design strategy was employed to facilitate the formation and controlled disassembly of high-performance, recyclable polyimide composite aerogels. The innovative “aerogel-in”aerogel" structure exhibits a highly porous, interpenetrating architecture with complete disaggregation capabilities. This composite showcases exceptional resistance to extreme conditions, spanning from ultra-low temperatures of −196 °C to ultra-high environments of 800 °C, providing a groundbreaking and sustainable solution for next-generation thermal protection materials.

Single-Cell Exosome

The background shows a microwell array chip with a light beam symbolizing photothermal technology for single-cell isolation. A magnified view highlights exosome secretion by a purple cell. Multicolored markers identify different exosomes. More details can be found in article number 2411259 by Lin Han and co-workers.

Polymorphing Hydrogels – Sculpting with Light

Polymorphing hydrogels can be reshaped on demand by shining light on specific areas. These hydrogels incorporate photo-reactive DNA cross-links, whose lengths are reversibly controlled by UV or visible light. Under UV illumination, the cross-links shorten, causing the hydrogel to contract, while exposure to visible light restores their original length. The image symbolizes this process by depicting a “VIS”ible man and “UV”men working together to sculpt the material. More details can be found in article number 2414648 by Eunjin Choi, Yeongjae Choi, and co-workers.

Perovskite Quantum Dots

Inspired by the hedgehog, the fluorescent perovskite quantum dots (PQDs) with a defending layer are designed via using thiol-ene “click chemistry”. Benefiting from the high colloidal dispersion of PQDs in the photo-curable matrixes, the PQDs offer high efficiency, stability, and processability, facilitating their multiform manufacturing for a wide range of applications, even for underwater displays. More details can be found in article number 2411453 by Zuliang Du and co-workers.

Organic Electronics

Record ion mobility and conductivities are revealed within a nanoscopic interfacial superhighway of an organic mixed ionic-electronic conductor. Fast ion transport can be controlled by hydrophobicity of molecules local to this channel, effectively gating ion access to the superhighway. This mechanism is used in a novel chemical sensing device which detects the dynamics of a local, buried chemical reaction. More details can be found in article number 2406281 by Tamanna Khan, Terry McAfee, Thomas J. Ferron, Awwad Alotaibi, and Brian A. Collins.

Soft-Actuated Cuff Electrodes

A sutureless, soft-actuated cuff electrodes (SACE) device envelops a nerve by itself upon fluid injection into part of the device made of soft and expandable polymeric structures. Three-dimensionally protruded part of the device ensures soft, minimal but secure contact between electrodes and nerve, resulting in superior performance in signal recording. More details can be found in article number 2409942 by Sohee Kim and co-workers.

This review examines the critical role of multi-scale hierarchical structures, from molecular to macro levels, in optimizing light harvesting and photothermal efficiency in solar steam generation (SSG) systems. By tailoring materials and structures to enhance light absorption, manage thermal properties, and support effective water transport, these integrated designs advance solar-thermal desalination as a sustainable solution to water scarcity.

Abstract

Solar steam generation (SSG) presents a promising approach to addressing the global water crisis. Central to SSG is solar photothermal conversion that requires efficient light harvesting and management. Hierarchical structures with multi-scale light management are therefore crucial for SSG. At the molecular and sub-nanoscale levels, materials are fine-tuned for broadband light absorption. Advancing to the nano- and microscale, structures are tailored to enhance light harvesting through internal reflections, scattering, and diverse confinement effects. At the macroscopic level, light capture is optimized through rationally designed device geometries, configurations, and arrangements of solar absorber materials. While the performance of SSG relies on various factors including heat transport, physicochemical interactions at the water/air and material/water interfaces, salt dynamics, etc., efficient light capture and utilization holds a predominant role because sunlight is the sole energy source. This review focuses on the critical, yet often underestimated, role of hierarchical light harvesting/management at different dimensional scales in SSG. By correlating light management with the structure-property relationships, the recent advances in SSG are discussed, shedding light on the current challenges and possible future trends and opportunities in this domain.

The review explores the potential of Li-rich Mn-based (LRM) cathodes in next-generation lithium-ion and all-solid-state batteries, addressing their challenges, and degradation mechanisms, and proposing strategies for improvement and future research directions.

Abstract

Li-rich Mn-based (LRM) cathode materials, characterized by their high specific capacity (>250 mAh g−¹) and cost-effectiveness, represent promising candidates for next-generation lithium-ion batteries. However, their commercial application is hindered by rapid capacity degradation and voltage fading, which can be attributed to transition metal migration, lattice oxygen release, and the toxicity of Mn ions to the anode solid electrolyte interphase (SEI). Recently, the application of LRM cathode in all-solid-state batteries (ASSBs) has garnered significant interest, as this approach eliminates the liquid electrolyte, thereby suppressing transition metal crosstalk and solid–liquid interfacial side reactions. This review first examines the historical development, crystal structure, and mechanisms underlying the high capacity of LRM cathode materials. It then introduces the current challenges facing LRM cathode and the associated degradation mechanisms and proposes solutions to these issues. Additionally, it summarizes recent research on LRM materials in ASSBs and suggests strategies for improvement. Finally, the review discusses future research directions for LRM cathode materials, including optimized material design, bulk doping, surface coating, developing novel solid electrolytes, and interface engineering. This review aims to provide further insights and new perspectives on applying LRM cathode materials in ASSBs.

This review offers an in-depth overview of the state-of-the-art advances in the Ru-based electrocatalysts for NO x reduction to NH3, covering the mechanism, design, and applications. Additionally, the review presents the primary challenges relevant to relatively high cost, complex reaction mechanism, and serious hydrogen evolution, as well as the critical perspectives on the fronter of this exciting research area.

Abstract

Ammonia (NH3) is widely recognized as a crucial raw material for nitrogen-based fertilizer production and eco-friendly hydrogen-rich fuels. Currently, the Haber–Bosch process still dominates the worldwide industrial NH3 production, which consumes substantial energy and contributes to enormous CO2 emission. As an alternative NH3 synthesis route, electrocatalytic reduction of NO x species (NO3 −, NO2 −, and NO) to NH3 has gained considerable attention due to its advantages such as flexibility, low power consumption, sustainability, and environmental friendliness. This review timely summarizes an updated and critical survey of mechanism, design, and application of Ru-based electrocatalysts for NO x reduction. First, the reason why the Ru-based catalysts are good choice for NO x reduction to NH3 is presented. Second, the reaction mechanism of NO x over Ru-based materials is succinctly summarized. Third, several typical in situ characterization techniques, theoretical calculations, and kinetics analysis are examined. Subsequently, the construction of each classification of the Ru-based electrocatalysts according to the size of particles and compositions is critically reviewed. Apart from these, examples are given on the applications in the production of valuable chemicals and Zn−NO x batteries. Finally, this review concludes with a summary highlighting the main practical challenges relevant to selectivity and efficiency in the broad range of NO x concentrations and the high currents, as well as the critical perspectives on the fronter of this exciting research area.

Cancer immunotherapy holds significant promise for improving cancer treatment, yet the low response rate remains a substantial challenge. It is crucial to gain a deep understanding of tumor-targeted catalytic materials to enhance targeting precision and therapeutic outcomes. This review focuses on recent advances in these materials and their role in improving catalytic immunotherapy, paving the way for next-generation cancer therapy.

Abstract

Cancer immunotherapy holds significant promise for improving cancer treatment efficacy; however, the low response rate remains a considerable challenge. To overcome this limitation, advanced catalytic materials offer potential in augmenting catalytic immunotherapy by modulating the immunosuppressive tumor microenvironment (TME) through precise biochemical reactions. Achieving optimal targeting precision and therapeutic efficacy necessitates a thorough understanding of the properties and underlying mechanisms of tumor-targeted catalytic materials. This review provides a comprehensive and systematic overview of recent advancements in tumor-targeted catalytic materials and their critical role in enhancing catalytic immunotherapy. It highlights the types of catalytic reactions, the construction strategies of catalytic materials, and their fundamental mechanisms for tumor targeting, including passive, bioactive, stimuli-responsive, and biomimetic targeting approaches. Furthermore, this review outlines various tumor-specific targeting strategies, encompassing tumor tissue, tumor cell, exogenous stimuli-responsive, TME-responsive, and cellular TME targeting strategies. Finally, the discussion addresses the challenges and future perspectives for transitioning catalytic materials into clinical applications, offering insights that pave the way for next-generation cancer therapies and provide substantial benefits to patients in clinical settings.

This review article systematically explores the recent advances in the membrane processes for lithium cycling and recovery, offering the first correlation between these technologies and technology readiness levels, unveiling the fundamentals for the lithium separation, and providing insights into the future design of membrane materials from both academic and industrial perspectives.

Abstract

Rapid uptake of lithium-centric technology, e.g., electric vehicles and large-scale energy storage, is increasing the demand for efficient technologies for lithium extraction from aqueous sources. Among various lithium-extraction technologies, membrane processes hold great promise due to energy efficiency and flexible operation in a continuous process with potential commercial viability. However, membrane separators face challenges such as the extraction efficiency due to the limited selectivity toward lithium relative to other species. Low selectivity can be ascribed to the uncontrollable selective channels and inefficient exclusion functions. However, recent selectivity enhancements for other membrane applications, such as in gas separation and energy storage, suggest that this may also be possible for lithium extraction. This review article focuses on the innovations in the membrane chemistries based on rational design following separation principles and unveiling the theories behind enhanced selectivity. Furthermore, recent progress in membrane-based lithium extraction technologies is summarized with the emphasis on inorganic, organic, and composite materials. The challenges and opportunities for developing the next generation of selective membranes for lithium recovery are also pointed out.

Electrical manipulation of spins by spin Hall current from heavy metals facilitates the implementation of multifunctional spintronic devices. This work reports direct evidence of spin current generation in ferromagnets via observation of efficient current-induced switching of noncollinear antiferromagnet Mn3Sn in Mn3Sn/ferromagnet structure. The further realization of field-free switching suggests the ferromagnets could function as more versatile spin sources.

Abstract

The ability to electrically manipulate spin states in magnetic materials is essential for the advancement of energy-efficient spintronic device, which is typically achieved in systems composed of a spin source and a magnetic target, where the magnetic state of the target is altered by a charge current. While theories suggest that ferromagnets could function as more versatile spin sources, direct experimental studies involving only the spin source and target layers have been lacking. Here electrical manipulation of spin states in noncolinear antiferromagnet Mn3Sn using ferromagnets (Ni, Fe, NiFe, CoFeB) as the spin sources is reported. Both field-free switching and switching with an assistive field are achieved in Mn3Sn/ferromagnet bilayers, where the switching polarity correlates with the sign of anomalous Hall effect of the ferromagnets. The experimental findings can be accounted for by the presence of spin currents arising from spin-dependent scattering within the ferromagnets. This finding provides valuable insights into the underlying mechanisms of spin-conversion in ferromagnets, offering an alternative spin source for novel technological applications.

This study introduces AZBX (AZn₂BO₃X₂) as a quasi-vdW layered dielectric for 2D semiconductor devices, offering a wide bandgap (≈5.6 eV) and high dielectric constant (κ = 13.5). KZBB/MoS₂ FETs demonstrate excellent performance, including steep subthreshold swing, high on/off ratio, minimal hysteresis, and low leakage, highlighting AZBX's potential for advanced 2D electronics.

Abstract

The development of dielectrics with atomic planes and van der Waals (vdW) interfaces is essential for enhancing the performance of 2D devices. However, vdW dielectrics often have smaller bandgaps compared to traditional 3D dielectrics, limiting their options. This study introduces AZBX (AZn₂BO₃X₂, where A = K or Rb, X = Cl or Br), a nonlinear deep-ultraviolet optical crystal, as a quasi-vdW layered dielectric ideal for 2D electronic devices. Focusing on KZBB, it's excellent dielectric properties, including a wide bandgap, high dielectric constant (high-κ), and smooth interfaces are demonstrated. When used as the top gate dielectric in a KZBB/MoS₂ field-effect transistor (FET) with MoS₂ channels and graphene contacts, the device exhibits outstanding performance, with a steep subthreshold swing (≈ 73 mV dec−1), high on/off ratio (≈ 10⁷), negligible hysteresis (0–8 mV), and stable, low leakage current (≈10⁻⁷ A cm− 2) before breakdown. This work expands the 2D material and dielectric landscape and highlights the strong potential of AZBX as high-performance dielectrics.