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

A new kind of “crosslinked hetero-chain polymeric CEI” (CHP-CEI) is particularly tailored for LRMO cathode. This CHP-CEI is homogeneous and shows a balanced combination of high robustness, flexibility, and mechanical energy dissipation ability, which can not be achieved by conventional additives. Therefore, the cracking of LRMO cathode, gas release, and transition metal dissolution are largely mitigated during cycling at aggressive voltages.

The lithium-rich manganese-based layered oxide (LRMO) cathode shows grar promise for high-energy density and environment-friendly batteries due to its cation and anion redox. However, it suffers from continuous electrolyte consumption and capacity decay, especially at high mass loadings (>10 mg cm−2). Conventional electrolyte/interphase strategies fail to address the structural characteristics of LRMO, limiting its practical application. Here, we reveal the specific requirements for cathode electrolyte interphase (CEI) of LRMO and accordingly design a non-fluorinated additive, 2,4,6-trivinyl-2,4,6-trimethylcyclotrisiloxane (TVTMS). TVTMS could form a crosslinked hetero-chain polymeric CEI (CHP-CEI) through ring-opening polymerization and ethylene group crosslinking, offering a unique balance of high robustness, flexibility, and mechanical energy dissipation, which could not be achieved by conventional additives. Therefore, the cracking of LRMO cathode, gas release and transition metal dissolution were effectively mitigated. It should be noted that, for the first time to our knowledge, we employed the single-particle aerosol mass spectrometry (SPAMS) to study CEI components, especially the organic/polymer species. The Li|LRMO cells based on CHP-CEI display a lifespan >825 cycles with remained capacity of 204 mAh g−1 and the cells with high-loading cathode (12 mg cm−2) achieve stable cycling >145 cycles with 80% capacity retention, which surpasses the performance of previously reported electrolytes.

Light-induced membraneless organelles (MLOs) are formed in artificial cells upon light irradiation. The enrichment of iNOS+ in MLOs increases the production rate of NO 3.2 times of that without MLOs. Artificial cells containing light-induced MLOs are utilized to treat melanoma efficiently.

Membraneless organelles (MLOs) formed by liquid–liquid phase separation exhibit diverse important biofunctions in cells. The construction of artificial cells containing MLOs with enhanced complexity and functions is still challenging. Here a light-responsive protein, Cry2olig-IDRs, is designed and purified to form MLOs upon light (488 nm) irradiation. They are capable of rapidly recruiting positively charged inducible nitric oxide synthase (iNOS+) from surroundings to regulate its activity for NO production. NO-artificial cells are constructed by encapsulating Cry2olig-IDRs and iNOS+ into giant unilamellar vesicles, which are capable of rapid production of NO with high concentration due to the formation of MLOs upon light irradiation. NO-artificial cells are confirmed to possess the ability for melanoma tumor therapy in mice. These findings provide an efficient method for remotely regulating enzyme activity inside artificial cells, paving the path to build more sophisticated artificial cells for their biomedical applications.

A vaccine (Bif-OVA-Ocur) is designed to target gut-associated lymphoid tissues, promoting the maturation of dendritic cells (DCs) and the expansion of cytotoxic T lymphocytes (CTLs) at mucosal sites. This targeted approach strengthens both mucosal and systemic immunes responses. These immune responses enable the immune system to specifically recognize and destroy tumor cells, thereby inhibiting tumor growth and progression.

Gut-associated lymphoid tissue (GALT) possesses a highly specialized immune system and is rational as a foothold for oral tumor vaccines. Here, a noninvasive oral vaccine (Bif-OVA-Ocur) is designed to engage GALT, inducing both intestinal mucosal and systemic immunity for tumor therapeutics. The vaccine uses Bifidobacterium (Bif) as a delivery vehicle for tumor antigen peptides, which are coated with antigen peptides (OVA) and oxidized curdlan (Ocur) in a layer-by-layer (LBL) manner. Upon oral administration, Bif-OVA-Ocur is efficiently directed to Peyer's patches (PPs) in the intestines and further presented to antigen-presenting cells (APCs), which then migrate to the mesenteric lymph nodes (MLNs) to evoke specific T cell responses. In mouse models, Bif-OVA-Ocur effectively boosts the production of secretory immunoglobin A (SIgA) and promotes a strong mucosal and systemic immune response, leading to significant tumor suppression and resistance to tumor challenges. Importantly, the vaccine shows no systemic toxicity. This approach to harnessing the intestinal mucosal immune system offers valuable insights for the development of other non-invasive oral vaccines and therapeutic agents.

Two enantiomeric pairs of alloy clusters composed of two Pt2Ag4 monomer are synthesized. Chiral structural transformations occurred in response to solvent stimuli, concomitant with high-contrast chiroptical switching. By manipulation of such chiral clusters, a chiral cubic lattice with high-efficiency circularly polarized luminescence is achieved. Further, the application in the information encryptions is explored.

Establishing atom-precise and controllable self-assembly of metal clusters to achieve high-efficiency circularly polarized luminescence (CPL) is especially fascinating, yet it creates considerable challenges. Here, two enantiomeric pairs of dimer clusters R/S-Pt4Ag8-green and R/S-Pt4Ag8-orange composed of two octahedral Pt2Ag4 monomers through Pt–Pt bonds are constructed, which show a 28-fold increase in photoluminescence quantum yield (PLQY) compared with the reported monomer in solution. The solid-state chiral dimer R/S-Pt4Ag8-orange shows a PLQY of 87% without an aggregation-caused quenching effect. The intercluster distances and arrangements of the chiral cluster can be modulated through the ligand configuration and solvent stimuli, giving rise to the reversible transformations between chiral single crystals, concomitant with high-contrast optical/chiroptical switching. Additionally, by further assembling chiral Pt-Ag clusters with Ag+, a chiral 3D cubic lattice with high-efficiency red-emitting CPL is achieved. Furthermore, high-efficiency luminescence, intrinsic chirality, and the adjustable assembly behaviors of these chiral cluster assemblies bestow them with excellent smart CPL switching properties. This work opens a new avenue for high-efficiency CPL-active metal clusters by regulating metal-metal interactions.

Porous carbons with tunable pore sizes are synthesized to investigate the impact of pore size on charge storage in Zn-ion hybrid capacitors. An unusual multi-stage charge storage mechanism is revealed, involving a transition from capacitive Zn2+ ion storage to faradaic Had adsorption on the carbon surface, providing new insights into Zn-ion electrochemistry.

Zn-ion hybrid capacitors (ZIHCs) are promising high-power energy storage devices. However, the underlying charge storage mechanisms, especially the influence of proton storage, remain poorly understood. Herein, the model porous carbons are synthesized having similar specific surface areas (SSAs) and surface chemistry but different pore sizes. They highlight the role of supermicropores and small mesopores (0.86–4 nm) enabling a high capacity of 198 mAh g−1 (capacitance of 446 F g−1), while larger mesopores (4–13 nm) significantly enhance cycling stability, exceeding 0.6 million cycles. Electrochemical studies, including EQCM analysis, reveal a 4-stage charge-storage process under cathodic polarization, comprising adsorption and desolvation of hydrated Zn2+ ions, followed by water reduction, catalyzed by Zn2+, and formation of Had. The rising pH leads to the formation of insoluble zinc hydroxysulfate hydrates (ZHS). Depending on the pore architecture, the precipitation of ZHS has different effects on the overall stability of cycling. The study overall: (i) presents a simplified method for pore control in carbon synthesis; (ii) discuss the effect of pore size on charge storage and cycling stability in respect of ZHS formation; (iii) sheds light on the charge storage mechanism indicating the important contribution of cation effect known from electrocatalysis on faradaic charge storage mechanism.

A machine learning procedure combined with an artificial intelligence (AI) model are used to accelerate the generation of ammonium ligands (ALs) in 2D perovskites. The relationship between the carrier transport barrier and the structure of ALs is explored. Utilizing the AI-designed ALs significantly enhances the carrier transport of the 2D perovskites, leading to high-efficiency and stable 2D/3D perovskite solar cells.

The 2D/3D heterojunction perovskite solar cells (PSCs) exhibit remarkable stability, but the quantum well in the 2D perovskite capping layer hinders the carrier transport, thereby lowering the power conversion efficiency (PCE). The relationship between the transport barrier and the complex structure of ammonium ligands (ALs) is currently poorly understood, thus leading to the one-sided approach and inefficient process in the development of 2D perovskite. Here, a machine learning procedure is established to comprehensively explore the relationship and combined it with an artificial intelligence (AI) model based on reinforcement learning algorithm to accelerate the generation of ALs. Finally, the AI-designed ALs improved the carrier transport performance of the 2D perovskite capping layer, and we achieved a certified PCE of 26.12% in inverted PSCs. The devices retained 96.79% of the initial PCE after 2000 h operation in maximum power point tracking under 1-sun illumination at 85°C.

This study develops a light-responsive liposome Lip-CuRA that synergizes photothermal therapy (CuS/980 nm) with dual NLGN3 regulation: RuBi-GABA/UCNPs suppress NLGN3 synthesis via Cl⁻ channels, while GI254023X inhibits ADAM10-mediated release. In glioma models, this strategy blocks PI3K/Wnt pathways, reduces stemness, and prolongs survival through combined neuromodulation-photothermal effects.

Neuronal activity is shown to potentiate glioma initiation, progression, and/or metastasis. A key mechanism in neural regulation of brain cancer involves the activity-dependent cleavage and release of the synaptic adhesion molecule neuroligin-3 (NLGN3). Here, this report describes the preparation of optogenetics-like liposome Lip-CuRA, which is used to regulate the content of NLGN3 in neurons and mediate phototherapy in cancer cells. Lip-CuRA contains upconversion nanoparticles encapsulating CuS (CuS@PUCNPs), a visible light-activated neurotransmitter prodrug RuBi-GABA, and a disintegrin and metalloproteinase (ADAM10) inhibitors GI254023X. Upon 980 nm laser irradiation, the photothermal conversion of CuS not only induces tumor cell apoptosis, but also destroys liposome structure, releasing Rubi-GABA and GI254023X. The UCNPs convert the 980 nm laser into 540 nm, activating RuBi-GABA into GABA. GABA selectively opens Cl⁻ channels in nerve cells, reducing the expression of NLGN3 and the degree of axonal connections. GI254023X inhibits the activity of the ADAM10 enzyme on the nerve surface, reducing the release of NLGN3, thereby blocking the transmission of proliferation and stemness signals. In the GL261-luc orthotopic glioma model, C6-luc orthotopic glioma model, and glioma patient-derived xenograft (PDX) model, Lip-CuRA effectively inhibits tumor recurrence, reduces glioma stemness, and extends survival through a synergistic photothermal and NLGN3-regulating therapy.

Graphene-skinned alumina fiber fabric (GAFF) with widely tunable electrical and electromagnetic properties is developed by graphene chemical vapor deposition (CVD) on each fiber in alumina fiber fabric (AFF). GAFF offers broad tunability in sheet resistance, electrothermal capability, as well as electromagnetic reflectivity and transmissivity. GAFF with widely tunable multifunction promises significant advancements in diverse applications in modern electronics and instrumentation.

As electronics and instrumentation grow increasingly complex, multifunctional materials are essential for simplifying designs. Electrothermal and electromagnetic functions are commonly used, typically supplied by separate materials. Integrating them into a single material can reduce components and miniaturize systems. Meanwhile, materials with widely tunable electrical and electromagnetic properties are needed to meet diverse application requirements, from electromagnetic waves transmitting to shielding, and electric heating across a wide temperature range. Graphene-skinned alumina fiber fabric (GAFF) with widely tunable electrical and electromagnetic properties is developed by graphene chemical vapor deposition (CVD) on each fiber in alumina fiber fabric (AFF). GAFF offers broad tunability in sheet resistance (1–10 000 Ω·sq−1), electrothermal capability (up to ≈1400 °C), as well as electromagnetic reflectivity (≈0.003 to ≈0.91) and transmissivity (≈0.98 to ≈0.0001) by adjusting graphene thickness and AFF pore size. Mass production of GAFFs in various specifications is realized, enabling diverse applications. Heating-shielding-integrated device (GAFF-HS) featuring high electromagnetic reflectivity and low transmissivity, and heating-transmitting-compatible device (GAFF-HT) with low electromagnetic reflectivity and high transmissivity, are both fabricated to target distinct applications: electrothermal anti-/de-icing for electromagnetic interference shielding systems and radar systems, respectively. GAFF with widely tunable multifunction promises significant advancements in diverse applications in modern electronics and instrumentation.

This research proposes self-powered difunctional flexible chemosensors by using a specially designed smart adaptable ion-introduced hydrogel to address the issue of single perception function in wearable devices, which can be highly sensitive and crosstalk-free to accurately assess oxygen and humidity levels in different states, and is expected to be widely used in the fields of safety, health and non-contact human-machine interaction.

The development of self-powered, flexible, and multi-function sensors is highly anticipated in wearable electronics, however, it remains a daunting challenge to identify different signals based on a single device with singular sensing material without algorithmic support. Here, a smart adaptable hydrogel is developed by co-introducing two ions with vastly different hydrophilicity for the construction of an electrochemically self-powered, flexible, and reversibly switchable difunctional chemosensor with a metal-air battery structure. The prepared hydrogel can readily switch between water-rich and water-deficient states for crosstalk-free detection of oxygen and humidity respectively, since O2 gas and water molecules can directly participate in the oxygen reduction reaction in the device and act alone as limiting reactants and catalysts to affect the reaction rate under different hydrogel states. The resulting sensor demonstrates breakthrough O2 and humidity sensing performance with sensitivities as high as 4170.5%/% and 380.2%/% RH in water-rich and water-deficient states, respectively, and ultrawide detection ranges. Thanks to these, the devices can be applied for real-time and remote monitoring of ambient oxygen, transcutaneous oxygen pressure changes, respiration, and skin moisture by combining with wireless communication technology, and therefore have important application prospects in the fields of safety, health management, and non-contact human-machine interaction.

An ionic liquid 1-methyl-3-propylimidazolium triiodide (MPII3) based electrochromic battery is developed, achieving a high areal capacity of 56 396 mAh m−2, which is substantially higher than those of previously reported electrochromic batteries.

Electrochromic batteries are multifunctional devices that integrate optical modulation with energy storage capabilities through electrochemical reactions. Traditional electrochromic batteries rely on solid-state thin films, but their limited material loading constrains capacity to ≈100–300 mAh m−2, failing to meet practical demands. Herein, an electrochromic battery based on ionic liquid 1-methyl-3-propylimidazolium triiodide (MPII3) is proposed, where the color-changing mechanism is based on the reversible redox reaction of I−/I3 − in solution, with 1-methyl-3-propylimidazolium cation (MPI+) forming a complex with I3 − to suppress its shuttle effect. More importantly, the resulting ionic liquid MPII3 demonstrates exceptional reaction kinetics, enabling rapid and extensive charge transfer, thereby significantly enhancing the energy storage potential of electrochromic batteries. The fabricated devices achieve a high capacity of 56396 mAh m−2 at a current density of 0.5 mA cm−2. Additionally, these MPII3 electrochromic batteries exhibit an optical modulation as high as 68.1% and excellent cycling stability, with 92.3% capacity retention after 20 000 cycles. These findings represent a significant advancement and are expected to promote the practical application of electrochromic batteries in smart windows, energy-efficient buildings, and other fields.

High-purity graphite serves as a fundamental material for scientific research and technological applications. Here, an effective solid refining process is developed utilizing the nickel (Ni) atomic lattice to eliminate both intrinsic and extrinsic impurities, producing ultrapure graphite. The resultant graphite exhibits the highest elemental, structural, and doping purity among all the known natural and artificial graphite, enabling its excellent transport properties.

Graphite has sparked extensive quantum physical discoveries and demonstrated numerous cutting-edge applications. However, existing graphite typically contains considerable impurities, and effective purification is still lacking. Here, a solid refining purification method is reported for obtaining ultrapure graphite. Through this design, impurities are filtered by the atomic lattice of a solid-state nickel (Ni). Suitable absorption, diffusion, and precipitation energy barriers are utilized in this method, allowing only carbon (C) atoms to effectively migrate through the Ni lattice to form high-quality graphite. The obtained ultrapure graphite shows the lowest elemental impurity density (<10 parts per million (ppm), which is one order of magnitude lower than that of the best available graphite), the highest structural purity (<0.2 parts per billion (ppb) of in-plane structural defect density and >99% Bernal stacking), and the highest doping purity (carrier doping density <2.0 × 1010 cm−2). Such superior purity of graphite facilitates the all-integer visible Landau levels and the ultralow quantum transition magnetic field in the fabricated graphene device. This solid refinement technique should inspire the purification of various layered crystals, leading to the discovery of new phenomena and the development of advanced applications.

By employing the body thickness scaling and channel length scaling strategies, polymer monolayer transistors with a channel length of 18 nm are demonstrated, which exhibit good operational stability and reliability with the on-state current density of 2.4 × 10−4 A mm−1 and the intrinsic gate delay of 0.79 ps. Moreover, the short channel effect is investigated by varying the dielectric thickness.

The scaling strategy is widely used to achieve much improved performance and reduced cost in a single chip with more devices for field-effect transistors (FETs) based on Si and state-of-the-art 2D materials. However, the downscaling of polymer FETs with high performance has not been achieved. Here both the body thickness scaling and channel length scaling strategies are employed, and demonstrate a 2.4-nm-thick polymer monolayer FET, where the shortest channel length (L) of 18 nm is achieved that is comparable to the smallest technology node (≈20 nm) for planar Si FETs. Such short-channel FETs, with good operational stability and reliability, exhibit only slightly lower field-effect mobility than the device with micrometer-long channel, but the on-state current density reaches 2.4 × 10−4 A µm−1. More importantly, a high intrinsic gate delay of 0.79 ps is achieved, while maintaining the on/off current ratio up to 109. Additionally, by increasing the thickness of gate dielectric a remarkable short channel effect is observed, which is in excellent agreement with natural scale length evaluated by the Scale Length Theory.

Nanoporous (Cu0.25Ni0.25Fe0.25Co0.25)6Sn5 high entropy intermetallic compound achieves excellent performance for ammonia electrosynthesis, allowing electrocatalytic nitrate reduction in a wide concentration range, excellent stability, and direct production of ammonium product. The high intrinsic catalytic activity is attributed to improved H* generation, inhibited hydrogen evolution reaction, and low reaction free energy of the hydrogenation process.

Electrocatalytic nitrate reduction reaction (NO3RR) provides a feasible strategy for green ammonia production and the treatment of nitrate pollution in wastewater. The generation of active hydrogen (H*) plays an important role in improving the selectivity, yield rate, and Faradaic efficiency of ammonia products. Here, structurally ordered nanoporous Cu6Sn5-type high entropy intermetallics (HEI) with extremely superior performance toward NO3RR is demonstrated. The optimal nanoporous (Cu0.25Ni0.25Fe0.25Co0.25)6Sn5 HEI delivers a high NH3 Faradaic efficiency of 97.09 ± 1.15% and excellent stability of 120 h at the industrial level current density of 1 A cm−2, accordingly directly converting NO3 ‒ to high-purity (NH4)2HPO4 with near-unity efficiency. Theoretical calculations combined with experimental results reveal that the ordered multi-site nature of the nanoporous HEI can simultaneously promote water dissociation, reduce the reaction-free energy of the hydrogenation process, and suppress hydrogen evolution. This work provides the design of the precious-metal-free HEI for sustainable NH3 synthesis and paves insights into the H* enrichment mechanism.

In this work, a non-intrusive electrolyte presodiation strategy is reported. Active organic salt sodium thiocyanate (NaSCN) as an electrolyte additive, which is dissolved in the electrolyte and subsequently injected into dry cells. During cell charging, the salt undergoes anodic oxidation, releasing active Na ions to compensate for capacity loss. Meanwhile, the organic ligand (-SCN) dimerizes to form the electrolyte cosolvent NCS-SCN.

Na-ion batteries show great promise, but their practical utilization is hindered by irreversible Na-ion loss during cell formation, resulting in initial coulombic efficiencies typically below 80%. Conventional presodiation methods, which involve solid additives in the cathode, can compromise electrode integrity and leave deteriorated residues, especially with high Na ion compensation (20%). An electrolyte presodiation approach is introduced that utilizes sodium thiocyanate (NaSCN) as an electrolyte additive, discovered through cheminformatics and machine learning. This organic salt decomposes at 3.3–4.0 V, releasing active Na ions and forming a cosolvent without damaging the electrode and the cell, as confirmed by spectroscopic and microscopic analyses. The method improves the initial coulombic efficiency of a hard carbon|P2-Na2/3Ni1/3Mn1/3Ti1/3O2 pouch cell from 80.8% to 95.2%, with a capacity retention of 84.5% over 400 cycles. These findings present a practical and non-intrusive way to address Na-ion deficiency challenges in Na-ion batteries.

O, S, and N atoms are adopted to bridge the 2D conjugated central cores, yielding three acceptors of CH─O, CH─S, and CH─N. CH─N-based device affords the highest fill factor of 83.13% in organic photovoltaics and the first-class binary device efficiency of 20.23%.

Almost all of central cores in high-performance acceptors are limited to the electron-withdrawing diimide structure currently, which constrains further acceptor structural innovation greatly. Herein, oxygen (O), sulfur (S), and nitrogen (N) atoms are adopted to bridge the 2D conjugated central cores, yielding three acceptor platforms of CH─O, CH─S, and CH─N that differ in structure by only two atoms. Because of the characteristic atomic outer electron configuration and hybrid orbital orientation, O-, S-, and N-bridged central cores display quite different conformations and electronic properties, namely, dibenzodioxin (planar, non-aromatic), thianthrene (puckered, non-aromatic) and phenazine (planar, aromatic), respectively. A systematic investigation discloses how the central core, especially its p-π orbital overlap between lone pair on O/S/N and coterminous benzene planes, affect the intrinsic photoelectronic properties of acceptors for the first time. Finally, CH─N-based binary device affords the highest fill factor of 83.13% in organic photovoltaics along with a first-class efficiency of 20.23%. By evaluating the strictly controlled O-, S-, and N-bridged molecular platforms comprehensively, the work reveals the potential uniqueness of diimide in determining the excellent photovoltaic outcomes of acceptors.

Micromotion activates a “mechano-electro-pharmaceutical” system, converting mechanical energy to electrical cues that trigger Met release. These cues suppress inflammation via M1-M2 macrophage polarization and osteogenesis enhancement, while Met blocks NF-κB (reducing cytokines) and activates AMPK (promoting bone/vessel growth). In diabetic fractures, Met-PF@PPy cut inflammation, boosted vasculature, and elevated bone metrics.

The use of piezoelectric materials to convert micromechanical energy at the fracture site into electrical signals, thereby modulating stress-concentrated inflammation, has emerged as a promising treatment strategy for diabetic fractures. However, traditional bone-guiding membranes often face challenges in diabetic fracture repair due to their passive and imprecise drug release profiles. Herein, a piezoelectric polyvinylidene fluoride (PVDF) fibrous membrane is fabricated through electrospinning and oxidative polymerization to load metformin (Met) into a polypyrrole (PPy) coating (Met-PF@PPy), creating a “mechanical-electrical-pharmaceutical coupling” system. In a micromotion mechanical environment, Met-PF@PPy converts mechanical energy into electrical signals, activating the electrochemical reduction of PPy and triggering stress-responsive Met release. The generated electrical signals suppress inflammation through M1-to-M2 macrophage polarization and simultaneously enhance osteogenesis. Simultaneously, Met inhibits the NF-κB pathway to reduce pro-inflammatory cytokines while activating the AMPK pathway to promote osteogenesis and angiogenesis. In a diabetic mouse femoral fracture model, Met-PF@PPy significantly reduces inflammatory markers, enhances vascularization, and increases bone mineral density and bone volume fraction by over 30%. This “force-electric-drug coupling” strategy provides an innovative approach for active regulation in diabetic fracture repair and offers a versatile platform for advancing piezoelectric materials in regenerative medicine.

Disordered rocksalts with lithium excess (DRX) offer a new direction in Li-ion cathode design beyond conventional Ni- and Co-based materials. This review highlights the design principles, synthesis strategies, and performance optimization of DRX oxides and oxyfluorides for energy-dense, sustainable batteries using Earth-abundant transition metals and tailored cation disorder.

To address the growing demand for energy and support the shift toward transportation electrification and intermittent renewable energy, there is an urgent need for low-cost, energy-dense electrical storage. Research on Li-ion electrode materials has predominantly focused on ordered materials with well-defined lithium diffusion channels, limiting cathode design to resource-constrained Ni- and Co-based oxides and lower-energy polyanion compounds. Recently, disordered rocksalts with lithium excess (DRX) have demonstrated high capacity and energy density when lithium excess and/or local ordering allow statistical percolation of lithium sites through the structure. This cation disorder can be induced by high temperature synthesis or mechanochemical synthesis methods for a broad range of compositions. DRX oxides and oxyfluorides containing Earth-abundant transition metals have been prepared using various synthesis routes, including solid-state, molten-salt, and sol-gel reactions. This review outlines DRX design principles and explains the effect of synthesis conditions on cation disorder and short-range cation ordering (SRO), which determines the cycling stability and rate capability. In addition, strategies to enhance Li transport and capacity retention with Mn-rich DRX possessing partial spinel-like ordering are discussed. Finally, the review considers the optimization of carbon and electrolyte in DRX materials and addresses key challenges and opportunities for commercializing DRX cathodes.

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.