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

In this work, by synergistically modulating carrier dynamics, both the separation efficiency and the quantity of electrons and holes transferred to ferroelectrics are optimized in parallel. As a result, the highest apparent quantum yield (AQY) of 5.78% at 365 nm for overall water splitting among ferroelectric materials is achieved and reported to date.

Ferroelectric materials, known for their non-inversion symmetry, show promise as photocatalysts due to their unique asymmetric charge separation, which separates hydrogen and oxygen evolution sites. However, the strong depolarized field induces a relaxed surface structure, which in turn directly leads to slow hole charge transfer dynamics, hindering their efficiency in water splitting. In this study, a fundamental breakthrough in dramatically enhancing the overall water-splitting activity is presented, through the synergistically regulating of the surface behaviors of photogenerated carriers, resulting in nearly perfect parallel dynamics and balanced amounts. By depositing atomic layers of TiO2 onto the surface of PbTiO3, surface vacancies are effectively passivated, significantly prolonging the hole lifetime from 10−6 to 10−3 s. Spatially resolved transient photovoltage spectroscopy showed that improved hole dynamics led to a 180° phase shift between photogenerated electrons and holes, indicating nearly identical extraction dynamics. Notably, hole and electron concentrations increased to equivalent levels. This leads to a nearly 578-fold increment in the apparent quantum yield, resulting in significantly increased overall water-splitting rates, with a quantum yield of 5.78% at 365 nm. The strategy is also effective with Al2O3 and SiO2, demonstrating its versatility across varied materials, providing a valuable method for creating high-performance ferroelectric photocatalysts.

This work fabricates abundant vacancy defects on the MXene surface for anchoring neighboring metal single atoms, to construct atomically dispersed sub-metallene (Pd ADSM) on the nanoscale. Pd ADSM combines the advantages of 2D structures, single atoms, and metal bonds, which makes it excellent and active in alkaline hydrogen evolution reactions and room-temperature hydrogen sensing.

Despite the metal coordination and single-atom catalyst (SAC) have been extensively investigated in surface science over the past decade, their overall activity in involving multi-step reactions remains unsatisfactory owing to the metal bond and single atom being irreconcilable. Here, a stable atomically dispersed Pd sub-metallene (Pd ADSM) layer supported on the 2D MXene (Mo2TiC2) is reported, which combines the advantages of 2D structures, single atoms, and metal bonds. Pd ADSM shows covalent structures along the z-coordination and highly coordinated metal bonds in the 2D direction. During the alkaline hydrogen evolution reaction (HER), Pd ADSM shows 7- and 112-times higher mass activity than the SAC (Pd SAC) and commercial Pt/C at the overpotential of −108 mV, respectively. Operando characterizations and theoretical calculations reveal that the Pd─Pd interface not only makes the adsorbed water form a flexible hydrogen-bonded skeleton closer to the catalytic center but also reduces the energy barrier for the HER rate-determining step. Moreover, the moderate adsorption energy of Pd─Pd bonds in ADSM can rapidly activate, dissociate, and desorb hydrogen molecules at room temperature, resulting in record-high hydrogen sensing performances (Response time, Recovery time, and Sensitivity for 100 ppm H2 are 4.8, 1.6 s, and 43.5%, respectively).

The 3D self-assembled SiO2@SiO2/C nanorods crosslinked nitrogen-doped carbon fiber (SSA/NCF) networks are prepared by electrostatic spinning to promote the preferential deposition of (101) crystalline surfaces to obtain dense and flat zinc anodes. Uniform zinc ion transport and enhanced ion transfer kinetics are also achieved toward flexible, binder-free, and high-performance APLs.

Owing to the low redox potential, abundant nature, and widespread availability, aqueous zinc-ion batteries (AZIBs) have attracted extensive investigation. Nevertheless, the commercialization of the batteries is severely hindered by negative side reactions, catastrophic dendrite growth, and uneven Zn2+ diffusion. Here, 3D self-assembled necklace-like nanofibers are developed by a simple electrospinning technique, in which SiO2@SiO2/C nanospheres are sequentially aligned on interconnected nitrogen/carbon networks (SSA/NCF) to achieve binder-free, high-performance, and dendrite-free growth of APLs. The design structure combines excellent interfacial ion transfer, corrosion resistance, and unique planar deposition regulation. The protective layer of SSA/NCF paper exhibits a high affinity for Zn2+, thereby reducing the nucleation barrier of Zn2+ and ensuring a more homogeneous Zn deposit. More importantly, this multifunctional interfacial layer induces preferential crystalline (101) oriented electroplating growth and promotes oriented dense Zn deposition. Consequently, the SSA/NCF paper layer endowed the cell with remarkable cycling stability, achieving an extended cycle life of 3000 h at 5 mA cm−2/1.25 mAh cm−2. This study offers novel insights into the development of high-performance zinc anodes.

A mesoporous-dominant carbon nanoreactor is designed with dimensions in the range of 15–43 nm with edge-rich defective atomic Zn sites. The crystal size and pore diameter of this carbon nanoreactors can be precisely adjusted to enable tunable mass diffusion pathways and porosities. The hydrophobic nature of 25 nm nanoreactors maximizes the nonkinetic advantages of active site exposure and rapid O2 mass transfer at the triple-phase interface.

High-active nonplatinum group metal oxygen reduction reaction (ORR) catalysts have great potential to improve fuel cell and metal–air battery performance due to their efficiency and cost-effectiveness. However, a fundamental understanding of their size-dependent structure–performance relationships remain elusive. Here a mesoporous-dominant carbon nanoreactor with dimensions in the range of 15–43 nm with edge-rich defective atomic Zn sites is designed. The crystal size and pore diameter of this carbon nanoreactors can be precisely adjusted to enable tunable mass diffusion pathways and porosities. Importantly, the hydrophobic nature of 25 nm nanoreactors maximizes the nonkinetic advantages of active site exposure and rapid O2 mass transfer at the triple-phase interface. The developed Zn-N-P/NPC catalysts delivers outstanding alkaline and acidic ORR performance with half-wave potentials of 0.92 and 0.80 V, respectively, as well as excellent zinc–air battery performance with charge/discharge over 400 h under 20 mA cm−2. X-ray absorption spectroscopy and theoretical calculations indicate that the enhanced ORR catalytic activity of Zn-N-P/NPC stems from the introduction of P atoms and edge carbon defects effectively exciting the localized electronic asymmetric distribution of Zn species. The findings provide new perspectives on the size effect of porous carbon supports for the development of efficient cathodes catalysts with multifunctionality.

This study presents a novel approach room-temperature ultrasound assisted atomic ordering method using to fabricate multi-grained NiPt nanoalloys with an intermetallic Ni3Pt5 phase. The resulting catalyst exhibits state-of-the-art durability and activity in all operational condition of proton exchange membrane fuel cells. Structural and electrochemical analyses reveal direct the role of atomic ordering in mitigating metal dissolution, ensuring long-term stability.

Rational design of catalytic nanomaterials is essential for developing high-performance fuel cell catalysts. However, structural degradation and elemental dissolution during operation pose significant challenges to achieving long-term stability. Herein, the development of multi-grained NiPt nanocatalysts featuring an atomically ordered Ni3Pt5 phase within intragrain is reported. Ultrasound-assisted synthesis facilitates atomic transposition by supplying sufficient diffusion energy along grain boundaries, enabling unprecedented phase formation. The Ni3Pt5 embedded nanocatalysts exhibit outstanding proton exchange membrane fuel cell performance under both light-duty and heavy-duty vehicle conditions, with significantly reduced Ni dissolution. Under light-duty vehicle conditions, the catalyst achieves a mass activity of 0.94 A mgPt −1 and a 421 mA cm−2 current density (@ 0.8 V in air), retaining 78% of its initial mass activity after long-term operation. Under heavy-duty vehicle conditions, the multi-grained nanocrystal demonstrates only an 8% decrease in Pt utilization, a 5% power loss, and a 13 mV voltage drop, surpassing U.S. Department of Energy (DOE) durability targets. This study underscores the critical role of the atomically ordered Ni3Pt5 phase in stabilizing multi-grained NiPt nanocrystals, enhancing both durability and catalytic activity. These findings establish Ni3Pt5 embedded nanocatalysts as promising candidate for next-generation PEMFC applications, addressing key challenges in long-term operation.

Liquid Metal Photothermal Actuators

In article number 2416991, Xingyou Tian, Xian Zhang, and co-workers present a novel design for programmable liquid metal photothermal actuators using laser etching, overcoming the trade-off between load-carrying capacity and response speed. Featuring high stability, rapid oscillation, and robust performance, these actuators show promise in advanced robotics, enabling versatile smart devices like photothermally actuated robotic dogs for diverse terrains.

Potassium-Ion Batteries

In article number 2502894, Shaoming Huang, Wei Zhang, and co-workers reveal a novel self-catalytic conversion reaction mechanism of N-doped CoTe2 composites (N-CoTe2/LTTC) incorporating 3D low-tortuosity tunneling structure, self-catalytic N-Co bonds, and heterojunction. Acting as the anode in potassium-ion batteries, the N-CoTe2/LTTC composite accelerates the catalytic conversion kinetics of potassium polytellurides (K5Te3 and K2Te) and achieves an ultralong-lifespan potassium storage performance over 25000 cycles.

3-D Printable Living Hydrogels

The cover depicts the creation of a miniaturized and portable bio-battery using living hydrogels containing electroactive microorganisms. The electricity generated by this device can be utilized to stimulate neutrons, allowing for precise control over bioelectrical stimulation and physiological blood pressure signals. In article number 2419249, Xinyu Wang, Renheng Wang, Zhiyuan Liu, Chao Zhong, and co-workers represent a pivotal advancement towards engineered living energy materials. Cover image designed by Lei Chen.

Dew Water Harvesting by Laser Micropatterning

A metallic surface micropatterned with a laser achieves self-cooling capacity when it faces the night sky thanks to its enhanced infrared emissivity, which triggers water condensation similar to natural dew on leaves. The patterned microgrooves promote condensation as a continuous film rather than dispersed droplets, enabling an efficient and autonomous harvesting of dew water. More details ban be found in article number 2419472 by Pablo Pou-Álvarez and co-workers.

The capillary-driven 3D open fluidic networks (OFNs), composed of connected polyhedral frames, enable precise, programmable, and versatile manipulation of unary, binary, and multiple continuous flows in both spatial and temporal dimensions. OFNs represent a significant leap beyond conventional microfluidics, unlocking new possibilities for selective metallization, programmable mixing, spatiotemporal control of multi-step reactions, and enhanced mass and heat transfer.

Human civilization hinges on the capability to manipulate continuous flows. However, continuous flows are often regulated in closed-pipe configurations to address their instability, isolating the flows from the environment and considerably restricting their functionality. Manipulating continuous flows in open systems remains challenging. Here, capillary-driven 3D open fluidic networks (OFNs) composed of connected polyhedral frames are reported. Each frame acts as a fluid chamber with free interfaces that enable fluid entry and exit; the connecting rods function as valves, allowing precise control over the direction, velocity, and path of the flow. The OFNs seamlessly adapt to various fluid systems, enabling precise 3D manipulation of multiple flows. Leveraging these distinctive features, a series of applications, including selective metallization, programmable mixing and diagnostics, and spatiotemporal control of multi-step reactions, are achieved. The OFNs’ free fluid interfaces also facilitate controlled drug release and efficient heat exchange. These versatile OFNs will significantly advance technological innovations in engineering, microfluidics, interfacial chemistry, and biomedicine.

This study uses a structurally fixed conjugation molecule as a precursor. It efficiently forms carbon core states of carbon dots. This approach optimizes the control over the conjugated domain size of the carbon core. It also significantly enhances the synthetic efficiency of CDs and the tunability of the optical properties.

Room-temperature phosphorescent (RTP) materials hold significant potential for applications in lighting, anti-counterfeiting, and multi-level information encryption. However, regulating RTP emission wavelengths, especially shifting into the red spectral region, remains challenging due to the spin-forbidden transitions of triplet-state excitons and non-radiative decay. To address this issue, carbon dots (CDs) with different conjugated domain sizes and phosphorescent potential are designed and synthesized. The CDs are then encapsulated in polyacrylamide (PAM), resulting in multicolored RTP emission ranging from cyan to red (465–635 nm), with cyan and red phosphorescence exceeding 10 s and 2 s, respectively. The mechanism suggests that the enhanced conjugation effect leads to energy level splitting and strengthened electron coupling, which lowers the energy gap between singlet and triplet excitons, ultimately causing a redshift in the phosphorescent emission wavelength. Meanwhile, the introduction of hydrogen bonding protects the excited state of the electrons, suppresses non-radiative transitions, and induces RTP in the CDs. These materials are applied in multi-level information encryption and time-delayed LED illumination, offering novel strategies for high-security technologies and advanced optical devices.

A gradient doping strategy based on vapor deposition is proposed, which effectively reduces the crystallization rate at the bottom layer, promotes uniform crystallization, and applies pre-compressive stress to the surface of the perovskite film, thereby effectively alleviating the residual stress and achieving a PCE of 23.0% for p-i-n PSCs with vapor-deposited perovskite.

Vapor-deposited p-i-n perovskite solar cells (PSCs) present key advantages such as low cost, excellent stability, low-temperature fabrication, and compatibility with tandem architectures, positioning them as strong contenders for industrial-scale solar applications. However, their power conversion efficiency (PCE) remains lower than that of n-i-p architectures. Herein, a gradient doping strategy to alleviate the stress in vapor-deposited perovskite films is introduced. Gradient chloride doping in the perovskite precursor film effectively slows the crystallization rate at the bottom layer, facilitating uniform crystallization and mitigating residual strain. This method yielded high-quality perovskite films, achieving a PCE of 23.0% for p-i-n PSCs with vapor-deposited perovskite and 21.43% for entirely vapor-deposited PSCs. Additionally, the devices demonstrates outstanding stability, showing negligible performance degradation over 1600 h of nitrogen storage and maintaining 87.3% of their initial PCE after 500 h of maximum power point tracking under 1-sun equivalent illumination at 70% relative humidity. The gradient doping strategy provides valuable insights for advancing large-area and perovskite-textured silicon tandem solar cells.

A Bi/Mg-based hybrid interphase protective layer is formed on the Mg foil via an in situ quasi-solid−solid redox reaction. Magnesiophilic components enhance Mg ion transfer, desolvation, and nucleation kinetics, whereas magnesiophobic species confer passivation-free and corrosion-resistant properties. Consequently, the smooth anode-electrolyte interphase facilitates homogeneous charge/ion distribution, promoting a highly reversible Mg plating/stripping process.

Magnesium (Mg) is a promising anode material for magnesium metal batteries (MMBs) owing to its high specific capacity, excellent safety profile, and abundant availability. However, pristine Mg anodes suffer from uneven plating/stripping and surface passivation/corrosion, limiting the safety and cycling stability of MMBs. This study introduces a Bi/Mg-based hybrid interphase protective layer on Mg foil (denoted Bi-Mg@Mg) through an in situ quasi-solid–solid redox reaction by immersing the foil in a bismuth oxybromide suspension. The resulting interphase layer consists of magnesiophilic components (Bi metal and Bi2Mg3 alloy) and magnesiophobic species (MgO, MgBr2, and BiBr3). These components synergistically enhance the desolvation, nucleation, and deposition kinetics, mitigate side reactions, and promote uniform electric field and ion flux distributions. As a result, the Bi-Mg@Mg electrodes exhibit superior Mg plating/stripping reversibility, maintaining stable performance for over 4100 h in the all-phenyl complex electrolyte and 2900 h in the Mg(TFSI)2 electrolyte, significantly outperforming pristine Mg electrodes. Furthermore, full cells paired with Mo6S8 and S cathodes demonstrate excellent capacities, rate capabilities, and long lifespans, highlighting the exceptional electrochemical performance of the Bi-Mg@Mg anode. This study offers a promising strategy for developing highly reversible Mg anodes, paving the way for practical long-cycle MMBs.

Biomechanical-to-electrical energy conversion devices are uniquely suited for self-driven physiological information monitoring and powering human–computer interaction systems. These devices based on micro-/nanoarchitectured inorganic dielectric materials (MNIDMs) have shown ultrahigh electromechanical performance and thus great potential for practical deployment. This review constructs a nexus among MNIDMs and all kinds of biomechanical-to-electrical energy conversion nanogenerators in terms of material development.

Biomechanical-to-electrical energy conversion technology rapidly developed with the emergence of nanogenerators (NGs) in 2006, which proves promising in distributed energy management for the Internet of Things, self-powered sensing, and human–computer interaction. Recently, researchers have increasingly integrated inorganic dielectric materials (IDMs) and micro-/nanoarchitectures into various types of NGs (i.e., triboelectric, piezoelectric, and flexoelectric NGs). This strategy significantly enhances the electrical performance, enabling near-theoretical energy harvesting capability and precise multiple physiological information detection. However, because micro-/nanoarchitectured IDMs function differently in each type of NG, numerous studies have focused on a single NG type and lack a unified perspective on their role across all types of biomechanical energy NGs. In this review, from an overall theoretical root of NGs, the performance enhancement mechanisms and effects of designs of IDMs coupling micro-/nanoarchitectures of various kinds of biomechanical energy NGs are systematically summarized. Next, advanced applications in human energy scavenging and physiological signal sensing are delved into. Finally, challenges and rational guidelines for designing future devices are discussed. This work provides researchers with in-depth insight into the development of high-performance personalized high-entropy power supplies and sensor networks via biomechanical-to-electrical energy conversion technologies based on IDMs coupling micro-/nanoarchitectures.

This research explores lipid nanoparticles (LNPs) for enhancing mRNA delivery to the central nervous system via intrathecal injection. By chemically engineering brain-targeting small molecules into ionizable lipids (BLs), the developed BLNPs effectively facilitate mRNA delivery across the brain. Intrathecal administration of Cas9 mRNA/sgRNA using the lead BLNP achieves significant gene editing in the brain with minimal off-target effects.

Lipid nanoparticle-messenger RNA formulations have garnered significant attention for their therapeutic potential in infectious diseases, cancer and genetic disorders. However, effective mRNA delivery to the central nervous system (CNS) remains a formidable challenge. To overcome this limitation, a class of brain-targeting lipids (BLs) is developed by incorporating brain-targeting small molecules with amino lipids and formulated them with helper lipids to generate brain-targeting lipid nanoparticles (BLNPs) for mRNA delivery. Screening studies led to a lead formulation, TD5 BLNPs, outperforming FDA-approved DLin-MC3-DMA LNPs in delivering mRNA to the brain upon intrathecal injection. Specifically, a single intrathecal injection of TD5 BLNP-GFP mRNA led to GFP expression in 29.6% of neurons and 38.1% of astrocytes across the brain. In an Ai14 mouse model, TD5 BLNP-Cre recombinase mRNA treatment induced tdTomato expression in ≈30% of neurons and 40% of astrocytes across major brain regions. Notably, delivery of Cas9 mRNA/sgRNA complex using TD5 BLNPs achieved effective genome editing in the brain. Additionally, TD5 BLNPs showed comparable safety profiles to MC3 LNPs, indicating promising biocompatibility. Overall, this TD5 BLNP formulation effectively delivers mRNA to brain tissues via intrathecal injection and facilitates efficient expression in both neurons and astrocytes, presenting a potential strategy for treating CNS diseases.

A rational design of skeleton-homologous nanoparticles for highly efficient and high-contrast theranostics is reported. The nanoparticles synchronously exhibit thermally activated delayed fluorescence (40 µs) and generate multiple ROS, enabling TRI-guided PDT, where TRI eliminates the background noise and guides PDT accurately.

Although photoluminescence imaging-guided photodynamic therapy (PDT) is promising for theranostics, it easily suffers from tissue autofluorescence and PDT photoproducts. To develop time-resolved imaging (TRI)-guided PDT with long-lived emission pathways, like thermally activated delayed fluorescence (TADF), is urgent but challenging, because of the triplet competition between radiative transition and reactive oxygen species (ROS) production. Herein, skeleton-homologous nanoparticles are designed and constructed to address this dilemma, thereby achieving in vivo TRI-guided PDT for the first time. This system is formed with a lipophilic TADF core (as a TRI probe) encapsulated by an amphiphilic photosensitizer shell (as the corona exposed to oxygen for PDT), both of which are derived from the same donor–acceptor skeleton to minimize phase separation in the single entity, and enable the same long-wavelength photoexcitation for TRI and PDT. The chloropropylamine group is helpful for endoplasmic reticulum targeting to enhance PDT upon minimizing the ROS transmission path. Synchronously, the TADF core exhibits a delayed fluorescence of 40 µs for a clear TRI. The NPs are eventually applied in vivo with a high signal-to-background ratio (45.25) and outstanding PDT effects in a mouse model of deep-seated kidney cancer. Such a material design is beneficial for developing high-efficient and high-contrast theranostic approaches.

Atomically dispersed Co−Ru dimer catalyst synthesized by a confined pyrolysis strategy shows the orbital coupling effect derived from the atomic pair, which could reduce energy barrier of lithium polysulfides conversion and Li2S dissociation, thus accelerating the catalytic kinetics and achieving the enhanced Li−S battery performance.

The sluggish sulfur redox reaction in lithium−sulfur (Li−S) batteries triggers the development of highly active electrocatalysts for accelerating the polysulfides conversion kinetics. Rational design of catalysts with satisfactory active sites and high atom utilization toward multistep sulfur-based conversion is much desired but remains challenging. Here, it is shown that the well-designed Co−Ru dimer sites confined on carbon matrix could effectively manipulate the sulfur-involved conversion reactions and thus improve Li−S batteries performance. The orbital coupling of Co−Ru dimer induces the orbital regulation for the atomic pair, resulting the favored lithium polysulfides adsorption strength and lowed conversion energy barrier, as confirmed by systematic electrochemical characterizations and theoretical calculation. Besides, the intrinsic catalytic activity of Ru from Co–Ru moiety also accelerates the Li2S dissociation reaction. Taken together, the as-constructed Co–Ru dimer sites render the Li−S battery with excellent performance, delivering energy density of 468 Wh kg−1 of total assembled pouch cell. This study offers a rational design of catalysts for boosting the catalytic performance in Li−S batteries.

A full-color pixel with only a single perovskite photodiode is presented. By integrating multiple photoresponse mechanisms into one device, spectral information is encoded directly into its impedance characteristics. Machine learning-based reconstruction enables accurate color retrieval without the need for additional optical components or modulation. The RGB reconstruction error is kept below 2%.

Photodetectors typically provide only 1D information about light intensity. Even the most basic color sensing requires external optical components, such as integrated filters. This limitation of information richness has only been overcome in recent years at the cost of spatial inefficiencies in multidetector integration designs or challenges in precisely controlling in situ modulation in single-detector designs. Acquiring high-dimensional color information with a single photodetector without external components, integration, or modulation remains a significant challenge that is aimed to resolve in this work. Due to the differences in carrier excitation by photons of varying energies, the simultaneous introduction of both electronic and ionic photoconductivity mechanisms enables the spectral characteristics of the unknown exciting light to be embedded within the impedance features of the device. By extracting impedance spectra and using machine learning-based reconstruction, a full-color pixel is achieved for the first time with just a single photodetector.

Unique oxygen-deficient, hybrid phased titanates are leveraged to achieve nanoconfinement of ammonia borane (AB) via a distinctive one-end-anchored docking (OEAD) mechanism. This approach enables sustained H2 release while mitigating the detrimental reaction between AB and hydrogen peroxide in pathological conditions. The released H2, in synergy with magnesium ions, effectively promotes innervated-vascularized bone regeneration in a diabetic model.

Despite its potential in hydrogen (H2) therapy, ammonia borane (AB) has limited biomedical applications due to its uncontrolled hydrolysis rate and potential to cause cytotoxicity. Existing material-based delivery strategies focus on accelerating AB hydrolysis for H2 production, hence exacerbating these issues. A new nanoconfinement strategy is reported, which loads AB onto oxygen-deficient, hybrid-phased titanate nanocrystals on implant surfaces through a unique one-end-anchored docking (OEAD) mechanism. This nanoconfinement strategy effectively restricts the release of AB molecules, allowing only water molecules to infiltrate the interlayer space for slow hydrolysis and sustained H2 release. This significantly prolongs the duration of H2 release and effectively circumvents the cytotoxicity associated with AB interacting with hydrogen peroxide (H2O2) in the inflammatory microenvironment. In vitro and in vivo have shown that sustained H2 release from the implant surface effectively alleviates diabetes-related oxidative stress, and combined with the release of magnesium ions (Mg2+) synergistically promotes innervated-vascularized bone regeneration.