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

Robust and antioxidative quasi-solid-state polymer electrolytes are successfully fabricated with diblock polymer brushes as multifunctional supporting films. On this basis, practical long-cycling lithium metal batteries are achieved under high areal capacities and high-voltage conditions.

Quasi-solid-state polymer electrolytes (QSPEs) have been considered as one of the most promising electrolytes for high-safety high-energy-density lithium metal batteries (LMBs). However, their inadequate mechanical properties and instability under high voltages pose significant challenges for practical applications. Herein, robust and antioxidative QSPEs are developed based on a polymer-brush-based rigid supporting film (BC-g-PLiMTFSI-b-PPFEMA, BC: bacterial cellulose, PLiMTFSI: poly(lithium (3-methacryloyloxypropylsulfonyl) (trifluoromethylsulfonyl)imide), PPFEMA: poly(2-(perfluorohexyl)ethyl methacrylate)). The robust BC nanofibril backbone can produce a highly porous supporting structure with outstanding mechanical strength. More importantly, the PLiMTFSI-b-PPFEMA side-chains can not only obviously increase the conversion ratio of easily oxidized monomers in QSPEs, but also possess strong interaction with unstable electrolyte components. With such QSPEs as solid-state electrolytes, the Li/LiNi0.8Mn0.1Co0.1O2 full cell with a high cathode loading (20.3 mg cm−2) exhibits a specific discharge capacity of 200.7 mAh g−1 at 0.5 C and demonstrates a long lifespan of 137 cycles with a highly retained capacity of 170.7 mAh g−1 under a cut-off voltage of 4.5 V. More importantly, under a high cut-off voltage of 4.6 V, a high specific capacity of 147.0 mAh g−1 after 187 cycles can be retained for solid-state Li/LiCoO2 cells. This work provides a feasible development strategy of QSPEs for practical long-cycling high-voltage LMBs.

This work presents a breakthrough in overcoming the limitation of slow heat transfer by producing a novel Ni─Mn─In/In composite. The heat transfer property is significantly enhanced due to not only the high thermal conductivity of In metal but also the dense structure reducing phonon scattering. This innovation leads to a substantial increase in thermal conductivity and thermomagnetic generation performance, positioning our composite as a promising candidate for efficient waste heat harvesting.

Thermomagnetic generation (TMG) is a potential technology for harvesting low-grade waste heat. However, the limited heat transfer of TMG materials constrains their practical performance. In this study, low-melting point metal indium (In) with high thermal conductivity is introduced into a Ni─Mn─In Heusler alloy to fabricate Ni─Mn─In/In TMG composites. The thermal conductivity increased significantly from 14.86 W m−1 K−1 for the Ni─Mn─In alloy to 65.2 W m−1 K−1 for the Ni─Mn─In/In composite. The composite containing 40 wt.% In (In40) exhibits superior TMG performance, with an average voltage of 2.38 mV g−1, a maximum power density of 0.433 µW g−1, and a cost index of 0.116 µW per CNY, which are 3.8, 2.4, and 1.1 times higher than those of the Ni─Mn─In alloy. By further changing the geometry, a 2 mm thick In40 with 7 holes achieves a thermal conductivity 15 times higher and a power generation index 8 orders of magnitude greater than those of other reported TMG materials. The combination of enhanced TMG performance and improved heat transfer, along with zero thermal hysteresis, good machinability, high corrosion resistance, and long-term cycle stability, makes this composite a strong candidate for low-grade waste heat recovery applications.

An AI-guided design platform (AMP-hydrogel-Designer) is developed to design antibacterial biomaterials by integrating thiol-modified AMPs, hydrogels, and Cu-BTO. The AI-designed hydrogel exhibits potent bactericidal efficacy against MRSA and E. coli, promotes angiogenesis via mechano-electrical signals, and accelerates healing in infected wounds.

Traditional biomaterial development lacks systematicity and predictability, posing significant challenges in addressing the intricate engineering issues related to infections with drug-resistant bacteria. The unprecedented ability of artificial intelligence (AI) to manage complex systems offers a novel paradigm for materials development. However, no AI model currently guides the development of antibacterial biomaterials based on an in-depth understanding of the interplay between biomaterials and bacteria. In this study, an AI-guided design platform (AMP-hydrogel-Designer) is developed to generate antibacterial biomaterials. This platform utilizes generative design and multi-objective constrained optimization to generate a novel thiol-containing high-efficiency antimicrobial peptide (AMP), that is functionally coupled with hydrogel to form a complex network structure. Additionally, Cu-modified barium titanate (Cu-BTO) is incorporated to facilitate further complex cross–linking via Cu2+/SH coordination to produce an AI-AMP-hydrogel. In vitro, the AI-AMP-hydrogel exhibits > 99.99% bactericidal efficacy against Methicillin-resistant Staphylococcus aureus (MRSA) and Escherichia coli (E. coli). Furthermore, Cu-BTO converts mechanical stimulation into electrical signals, thereby promoting the expression of growth factors and angiogenesis. In a rat model with dynamic wounds, the AI-AMP hydrogel significantly reduces the MRSA load and markedly accelerates wound healing. Therefore, the AI-guided biomaterial development strategy offers an innovative solution to precisely treat drug-resistant bacterial infections.

High-entropy doped P'2-Na0.59Mn0.90Ti0.02Cu0.02Ni0.02Co0.02Fe0.02O1.95F0.05 layered oxide cathode material associated with P'2-OP4 bi-phase transition yields superior cyclability (97.8% over 100 cycles) in sodium-ion batteries. The high-entropy doping can effectively regulate the energy level splitting of the eg* orbital and crystal fields, thus mitigating the Jahn-Teller distortion while maintaining the TMO6 octahedra anisotropy.

P'2-Na x MnO2 (NMO) features an ultra-high specific capacity in sodium-ion batteries, which, however, suffers from a fast capacity decay. To improve the stability, a high-entropy doped P'2-Na0.59Mn0.90Ti0.02Cu0.02Ni0.02Co0.02Fe0.02O1.95F0.05 (NMHE0.1OF) is developed to lessen the Jahn-Teller distortion and address the multiple phase transition issue. Physicochemical characterizations reveal that the NMHE0.1OF yields a lower anisotropy in the Mn─O bond than does the undoped NMO. Theoretical calculations indicate that the cation doping enhances the coordination ability of oxygen and the F doping breaks the electronic symmetry of Mn. The in situ X-ray diffraction result reveals that the NMO experiences a more abrupt and irreversible OP4-P'2-P″2 tri-phase transition; and the NMHE0.1OF features a mild and reversible OP4-P'2 bi-phase transition, which originates from the alleviation in the contraction/expansion of the transition metal slabs evidenced by ex situ extended X-ray absorption fine structure. The bi-phase transition favors the compatibility between the NMHE0.1OF and the ether-based electrolyte at high voltages. As a result, the NMHE0.1OF yields a superior cyclability (97.8% capacity retention after 100 cycles at 100 mA g−1) with a notable specific capacity of 224 mAh g−1 at 10 mA g−1. This work provides an effective strategy for the rational design of cathode materials with high capacity and superior stability.

This study develops a synthetic membrane with sodium ionophores integrated into a covalent organic framework, mimicking the permselectivity and cation discrimination of biological ion channels. The membrane exhibits high Na+ selectivity, achieving Na+/K+ and Na+/Li+ selectivities of 3.6 and 103, respectively, and improves power density by a 4.6-fold in the presence of high-valent cation salts, enhancing energy conversion efficiency.

Biological ion channels achieve remarkable permselectivity and cation discrimination through the synergy of their intricate architectures and specialized ionophores within confined nanospaces, enabling efficient energy conversion. Emulating such selectivity in synthetic nanochannels, however, remains a persistent challenge. To address this, a novel host-guest assembly membrane is developed by incorporating sodium-selective ionophores into a β-ketoenamine-linked covalent organic framework (COF). This design confers exceptional permselectivity and Na+ selectivity, achieving Na+/K+ and Na+/Li+ selectivity ratios of 3.6 and 103, respectively, along with near-perfect Na+/Cl− selectivity under a 0.5 M || 0.01 M salinity gradient. Notably, the membrane dynamically switches its permselectivity to favor anion transport in the presence of high-valent cations (e.g., Ca2+), overcoming limitations such as uphill cation diffusion and back currents observed in conventional cation-selective membranes. This adaptive behavior yields a 4.6-fold increase in output power density in Ca2+-rich environments. These findings advance the design of biomimetic nanochannels with unparalleled ion selectivity and enhanced energy conversion efficiency.

This work presents a new metalgel that immobilizes liquid metal continuum within waterborne polyurethane networks through electrostatic interactions. The polymer network, enriched with dynamic reversible structures, provides a durable structure for repeated stretching. Simultaneously, the electrostatic interactions enable synchronous deformations of both polymer networks and liquid metal. Benefiting from this design, this durable metalgel exhibits a high and stable conductivity of 3 × 106 S∙m−1 even after 1 000 000 stretching cycles. This work overcomes the performance limitations of current conductive elastomers and unlocks new opportunities for cutting-edge applications.

Conductive elastomers are in high demand for emerging fields such as wearable electronics and soft robotics. However, it remains unavailable to realize the desired metal-level conductivity after extensive stretching cycles, which is a necessity for the above promising application. Here, a new material is presented that employs an elastic, homogeneous, and dense waterborne polyurethane network to immobilize the liquid metal continuum via electrostatic interactions. This new design enables the liquid metal continuum to deform synchronously and reversibly with the polymer network, preserving its conductive structure and significantly enhancing durability. The resulting durable metalgel exhibits conductivity of 3 × 106 S∙m−1, which remains stable after 1 000 000 stretching cycles. This work overcomes the performance limitations of current conductive elastomers and unlocks new opportunities for cutting-edge applications in wearable technology and robotics.

An effective strategy is presented to fabricate the chiral superstructure elastomers (CSEs) that display selective reflection colors, dynamically tunable CP-OURTP with robust glum values, full-color afterglow emissions, and superior processability within a single system.

Developing full-color circularly polarized organic ultralong room-temperature phosphorescence (CP-OURTP) materials with high dissymmetry factor (g lum) holds significant promise for diverse optoelectronic applications. Controlling g lum values is crucial for enhancing the performance and functionality of these materials, as it directly influences their chiroptical properties and potential utilities in advanced technologies. However, achieving reversible and dynamic manipulation of g lum in CP-OURTP materials remains a formidable challenge. Herein, an effective strategy is presented to fabricate the chiral superstructure elastomers (CSEs) that display selective reflection colors, dynamically tunable CP-OURTP with robust glum values, full-color afterglow emissions, and superior processability within a single system. By integrating room temperature phosphorescence (RTP) polymers into the CSEs, CSEs are produced demonstrating tunable CP-OURTP with g lum values switching between 0.8 and 0.15 by mechanical deformation. More importantly, these mechanochromic, programmable, and full-color CP-OURTP films enable the development of flexible and dynamic information encryption and decryption. The work provides new insights into the development of novel RTP materials and advances in their potential applications.

The research introduces a novel “visual engineering” strategy using electronegative CDs for dual-functional separator modification. The CDs enable real-time UV monitoring of coating uniformity and regulate Li-ion flux, enhancing battery performance by suppressing dendrite growth and polysulfide shuttling in both lithium-metal and lithium–sulfur batteries. This innovative approach bridges optics and electrochemistry, offering a versatile solution for advanced energy storage systems.

Various modification methods for lithium-metal battery separators have been well explored in the past decades, among which the most common process is to coat modified slurries onto the separators by blade-coating method. However, the distribution of the slurries is often non-uniform in this process, while the uniformity usually needs to be detected by electron microscope, which is time and cost-consuming. To solve this long-standing technical issue, it focuses on the “visualization” of modification effect with negatively charged carbon dots under UV light, and deeply investigates the ion transport problem caused by the non-uniform material modification. With this unique “visual engineering” strategy, uniform separator can be easily detected, which further allows for the construction of a uniform negative shielding layer and cation channels. It accelerates the ion transport process, realizes a stable Li stripping and deposition process, and avoids dendrite growth. To this end, in symmetric batteries with different electrolyte compositions, stable operation of 1200 h can be achieved. In addition, negatively charged polysulfide shuttles can be greatly suppressed, thus avoiding the infamous “shuttle effect” in lithium–sulfur batteries. This work provides a new avenue for screening well-modified separators through “visual engineering”, further accelerating the practical application of series of rechargeable batteries.

Organic photodiodes (OPDs) with low dark current and stable detectivity under light irradiation, air exposure, and heating are realized using a nanoparticle-based Zn-chelated PEIE (PEI-Zn NP) electron transport layer. This formulation effectively suppresses photocurrent degradation and dark current increase, ensuring enhanced environmental stability and maintained performance after 5000 cycles of device bending.

Flexible organic photodiodes (OPDs) are used to detect light in system-scale demonstrations of skin-conformable devices. However, the detectivity of OPDs deteriorates under various environmental conditions, such as light irradiation, air exposure, and heating. This decrease in detectivity is observed in OPDs with a widely used sol–gel ZnO (ZnO SG) electron transport layer (ETL), where the dark current at the reverse bias increased by several orders of magnitude. In this study, a low dark current and stable detectivity with respect to the aforementioned external changes are achieved. The enhanced stability stems from the suppression of the increase in dark current realized by using a mixture of an organic polymer, polyethyleneimine (PEIE), and inorganic crystals (ZnO nanoparticles) to create a nanoparticle-based, Zn-chelated PEIE (PEI-Zn NP) as the ETL of the OPDs. The detectivities of OPDs with PEI-Zn NP are 89%, 84%, and 93% of their original values after light irradiation, air storage, and thermal heating, respectively. In contrast, their ZnO SG counterparts exhibited stabilities of only 9.9%, 55%, and 2.6%, respectively, in the same tests. Furthermore, the use of PEI-Zn NP ETL in ultraflexible OPDs is demonstrated by the maintained detectivity after 5000 cycles of device bending.

A vanadium-cobalt (VCo) diatomic catalyst with strong electronic interactions is successfully integrated into vacancy-rich nitrogen-doped MXene for room temperature sodium–sulfur (RT/Na─S) batteries. This catalyst exhibits a unique electron spillover effect during sodium polysulfide redox reaction, enhancing polysulfide conversion kinetics and significantly improving cycling stability.

Room-temperature sodium─sulfur (RT/Na─S) batteries, with a theoretical capacity of 1672 mAh g⁻1, face challenges such as the insulating nature of sulfur and slow redox kinetics, particularly during complex liquid–solid (Na2S4→Na2S2) and solid–solid (Na2S2→Na2S) conversions. Herein, vanadium-cobalt (VCo) diatomic sites implanted in vacancy-rich N-doped MXene (VCo DACs/N-MXene) are introduced to address these issues. The N-bridged VCo diatomic pairs are demonstrated and their strong electronic interactions are also validated through experimental and theoretical analyses. The RT/Na─S battery with optimized VCo DACs/N-MXene delivers an average capacity of 1255.3 mAh g⁻1 at 0.1 C and remarkable cycling stability, with only ≈0.001% capacity decay per cycle over 1500 cycles at 1 C. DFT calculations reveal that VCo diatomic sites enhance reaction kinetics by reducing the Gibbs free energy for polysulfide conversions, notably reducing the solid–solid conversion energy barriers from 1.17/0.96 eV for V/Co SACs/N-MXene to 0.53 eV for VCo DACs/N-MXene. XANES and DFT analyses attribute this improvement to a unique electron spillover effect, facilitating efficient electron transport during charge and discharge. This work highlights the potential of optimizing electronic configurations and coordinating environments to activate bidirectional kinetics with improved capacity and longevity of RT/Na─S batteries.

Intrinsic, deep defective and surface states are proved in CDs. Hydrogen bonding (HB) is found to be detrimental to surface state emission of CDs through non-radiative decay pathway, while polarization promoted the surface state emission in a single decay pathway. By eliminating HB and promoting polarization-induced charge transfer, engineered CDs with fluorescence QY up to 98.1% are synthesized and applied for various applications.

Improving the fluorescence quantum yield (QY) of carbon dots (CDs) is essential for expanding their applications. Understanding the photoluminescence mechanism of CDs can provide valuable insights for QY improvement. In this study, it is demonstrated that polarization facilitated the surface state emission of CDs through a single decay pathway, while hydrogen bonding (HB) is identified as a factor that hindered the surface state emission of CDs through non-radiative decay. Following an in-depth evaluation of these mechanisms, the QY of CDs is markedly enhanced by engineering molecules onto their surfaces. This strategy not only eliminated HB but also promoted polarization-induced charge transfer. Notably, the QY of the yellow-emitting CD is elevated to 98.1%. Capitalizing on their long-term stability, excellent water solubility, two-photon excitation capacity, and non-toxicity, the engineered CDs are successfully applied in dual-color super-resolution fluorescence imaging in living cells, two-photon imaging of zebrafish, and optogenetic regulation in the deep brain of freely-moving animals.

A unique metal–organic framework (Cr-TBA), featuring chromium metal sites coordinated with tetrabromoterephthalic acid with a distinctive paper-clip-like shape, is successfully synthesized. The enhanced Lewis acidity of Cr-TBA promotes the accumulation of OH− ions on the catalyst surface. By effectively regulating the local reaction microenvironment, the H2O2 electrosynthesis performances of Cr-TBA in neutral electrolytes are significantly improved, achieving remarkable Faradaic efficiencies and an excellent H₂O₂ production rate.

The electrochemical synthesis of hydrogen peroxide represents a promising alternative to the traditional anthraquinone process, aiming for zero pollution. However, achieving efficient electrochemical synthesis of hydrogen peroxide in neutral electrolytes is challenging due to the sluggish kinetics of the two-electron oxygen reduction reaction. To address this issue, a unique metal–organic framework (MOF) featuring Cr metal sites coordinated with tetrabromoterephthalic acid (Cr-TBA) is synthesized. This specially designed MOF exhibits a distinctive paper-clip-like structure and remarkably enhanced Lewis acidity. Experimental results demonstrate that the obtained structure can facilitate the attraction of OH− ions in solution, promoting their accumulation on the catalyst surface. This enhancement leads to excellent performances of Cr-TBA in neutral electrolytes, achieving Faradaic efficiencies of 96–98% and a production rate of 13.4 mol gcat −1 h−1 at the current density of 150 mA cm−2. Operando spectroscopy and density functional theory calculations indicate that this modified microenvironment effectively facilitates the conversion of the *OOH intermediates to H2O2 on the catalyst surface.

This study investigates the high-field breakdown and energy dissipation of multilayer PdSe2 FETs, with a focus on the interfacial thermal transport at the PdSe2/SiO2 interface. The research proposes optimization strategies to enhance device performance and improve the thermal management, paving the way for the more efficient next-generation electronic and optoelectronic devices.

The continuous miniaturization of 2D electronic circuits results in increased power density during device operation, leading to heat localization and placing higher demands on their performance thresholds. The risk to thermal breakdown and subsequent damage, due to the energy dissipation in the 2D semiconductor field-effect transistors (FETs) supported on the bulk substrates, represents a significant challenge in maintaining their optimal performance. Herein, this study investigates energy dissipation behavior in multilayer PdSe2 FETs for the first time. The high-field breakdown behavior is firstly studied in multilayer PdSe2 FETs on SiO2/Si substrates, where a maximum current density of ≈2.74 MA cm−2 is observed, which is comparable to that of multilayer black phosphorus FET and significantly higher—by about five times—than that of multilayer MoS2 FET. Additionally, the thermal boundary conductance (TBC) of PdSe2/SiO2 interface is measured at room temperature using Raman thermometry. The TBC is found to be ≈12–13 MW m−2 K−1, which is relatively low compared to the other known solid–solid interfaces, indicating that enhancing the performance of PdSe2 FETs can be possible by optimizing the TBC at the PdSe2/SiO2 interface. These findings provide valuable insights for design of high-quality and high-performance PdSe2 electronic and optoelectronic devices.

An in situ multifunctional polymer interface layer with high-efficiency Zn2+ transport is prepared through the pre-established ion transport pathways of an innovative electrolyte initiator. This layer promotes rapid Zn2+ desolvation and uniform Zn2+ deposition, effectively suppressing interfacial side reactions and dendrite growths, thereby significantly extending the cycle life of aqueous zinc-metal batteries.

Achieving stable zinc-metal anodes is pivotal to realizing high-performance aqueous zinc-metal batteries (AZMBs). The construction of a functional polymer interface layer on the zinc-metal anode surface is confirmed as an effective strategy for mitigating dendrite growth and side reactions, thereby significantly enhancing the stability of zinc-metal anode. However, polymers capable of withstanding electrolyte environments over the long term typically suffer from elevated interfacial impedance, which hinders Zn2+ transport. Here, a pioneering zinc-metal anode enabled by a functional polymer interface layer with high-efficiency ion transport is introduced. This polymer layer is polymerized in situ on the zinc-metal anode surface through an innovative redox initiation system, where zinc trifluoromethanesulfonate (Zn(OTf)2) salts function as both reductant and ion transport pre-pathways, ensuring high-efficiency ion transport. The resultant interface layer achieves an ideal balance of ionic conductivity, water resistance, adhesion, and mechanical properties, effectively suppressing dendrite growth and side reactions. Symmetric cells assembled with this interface layer deliver an impressive lifespan of 8800 and 1600 h under 1 and 5 mA cm−2, respectively. This interface layer further demonstrates exceptional feasibility and versatility in Zn-NVO and Zn-PANI batteries. This work provides groundbreaking insights into the strategic design of high-performance polymer interface layers for AZMBs.

Multiple resonances thermally activated delayed fluorescence emitter is developed by synergizing multiple charge-transfer excited states, exhibiting excellent photoluminescence properties with a narrowband emission of 21 nm, rapid reverse intersystem crossing rate of 7.8 × 105 s−1 and suppressed concentration quenching, and electroluminescence performances with high maximum external quantum efficiencies and low-efficiency roll-offs in wide doping concentrations ranges of 3–50 wt.%.

The development of multiple resonances thermally activated delayed fluorescence (MR-TADF) emitters exhibiting high efficiency, narrowband emission, rapid reverse intersystem crossing rate (k RISC), and suppressed concentration quenching simultaneously is of great significance yet a formidable challenge. Herein, an effective strategy is presented to realize the above target by synergizing multiple charge-transfer excited states, including short-range charge transfer (SRCT), through-bond charge transfer (TBCT), and through-space charge transfer (TSCT). The proof-of-concept emitter 4tCz2B exhibits a bright green emission with a narrow full width at half maximum (FWHM) of 21 nm (0.10 eV) in solution, high photoluminescence quantum yield of 97%, fast k RISC of 7.8 × 105 s−1 and significantly suppressed concentration quenching in film state. As a result, the sensitizer-free organic light-emitting diodes (OLEDs) achieve maximum external quantum efficiencies (EQEmaxS) of over 34.5% together with an unaltered emission peak at 508 nm and FWHM of 26 nm at doping concentrations ranging from 3 to 20 wt.%. Even at a doping ratio of 50 wt.%, EQEmax is still as high as 25.5%. More importantly, the non-sensitized devices exhibit significantly reduced efficiency roll-offs, with a minimum value of 13.4% at a brightness of 1000 cd m−2.

An alcogel-based vertical thermal diode smart wall with interfacial evaporation for ambient thermal energy harvesting and spontaneous cooling/heating supply to the built environment. Owing to the vertical thermal diode structure design, the evaporation-condensation-based smart wall (ECSW) features flexible climate-adaptative heat transfer characteristics with a heat transfer coefficient from 3.33 to ≈30 W m−2 K−1 and building energy savings at 66.47% in Kunming.

Traditional building envelopes with constant thermophysical properties constrain their capabilities in temperature regulation. Whether it is possible to achieve single-direction heat transfer along building envelopes with climate-adaptative thermophysical properties to enhance passive heat gain in winter and thermal dissipation in summer? In this work, through the capillary effect in interfacial evaporation and thermal diode structure, single-direction heat transfer with passively adjustable thermal properties in a vertical building envelope is practically achieved. An evaporation-condensation-based smart wall (ECSW) is manufactured for spontaneous and continuous cooling/heating supply to the built environment. The ECSW features climate-adaptative heat transfer characteristics with heat transfer coefficient transiting from 3.33 to ≈30 W m−2 K−1. Additionally, coupling with radiant cooling and photothermal capabilities, ECSW shows excellent thermal performances, i.e., a heat transfer at 5.44 W m−2 by radiant cooling with a 5 °C cooler surface, and a heat transfer at 387.68 W m−2 under solar illumination at 1000 W m−2. Simulation results show that the ECSW enables building energy savings at 66.47% in Kunming. This study first reports vertical thermal diode building envelopes utilizing natural heating/cooling sources through interfacial evaporation for passive temperature regulation with low costs, performance stability and energy-saving potentials for smart and sustainable buildings.

A mixed ionic-electronic conducting 3D host is employed in solid-state batteries to modulate lithium plating and stripping behaviors, which can occur away from the interface to tackle dendrite and void formation issues. In situ electron microscopies and molecular dynamics simulations reveal the Li transport pathways in carbon-based Li metal anodes, which enable faster Li diffusion and high stripping capacity.

Solid-state lithium metal batteries (SSLMBs) are now under intensive research for their high energy density and excellent safety. However, the Li transport limitation in Li metal anode (LMA) leads to mass/stress accumulation, dendrite initiation and void formation at the interface, which seriously hinders the development of SSLMBs. Herein, it is demonstrated through in situ electron microscopies that a mixed ionic-electronic conducting (MIEC) 3D host can promote the Li transport in LMA by increasing the diffusion pathways along the carbonaceous framework, carbon/Li interface and Li metal surface, enabling a fast and long-distance (nearly 100 µm) diffusion of Li atoms in LMA. Consequently, the spatio-temporal sequence of Li plating/stripping can be fundamentally changed. Specifically, both deposition and dissolution can occur far away from the interface, thereby mitigating the dendrite and void issues. Impressively, the resulting cells with carbonaceous hosts can achieve excellent cyclability and the highest capacity (28.8 mAh cm−2) so far. This work provides valuable insight for understanding Li transport and deposition/dissolution mechanisms in MIEC host-based LMAs, and a feasible solution for tackling the interface issues without involving stack pressure in SSLMBs.

Biological processes rely on the concerted action of channels with different functionalities embedded in the same membrane. Inspired by nature, heterogeneous nanopore arrays are prepared where two nanopores are connected in parallel and function as two different elements of an ionic circuit: a diode and a resistor. The results provide the basis to design ionic circuits that mimic physiological processes and communication.

Much effort in the field of nanopore research has been directed toward reproducing the efficient transport phenomena of biological ion channels. For synthetic nanopores to replicate channel function on the scale of a cellular membrane, it is necessary to consider the modes of crosstalk between channels as well as to develop approaches to prepare nanopore arrays consisting of pores with different transport properties, akin to a membrane in an axon. In this manuscript, first ion concentration polarization (ICP) is identified as the primary means of the crosstalk, and subsequently, the extent and degree of ICP is tuned via targeted chemical modification of the pore walls’ functional groups. Next, two fabrication methods of a model two-nanopore array are presented in a silicon nitride membrane in which one nanopore contains a bipolar ionic junction and functions as an ionic diode, while the other one is a homogeneously charged ionic resistor. The targeted chemical modification of a thin gold layer at the opening of one pore in an array that leaves the other pore located a few tens of nm away, unmodified, is utilized. These results provide an important framework for designing abiotic ionic circuits that can mimic physiological multichannel ion transport and communication.

2D PtSe2 has been demonstrated as high-performance catalyst for electrocatalytic ethanol oxidation. Plasma treatment engineers the surface of single-crystalline PtSe2 by removing Se atoms, resulting in the exposure of PtSe2 (101) facet. Excellent EOR activity and poison-resistance are demonstrated, which is rationalized by in situ electrical transport measurement and theoretical calculations.

The development of efficient electrocatalysts for ethanol oxidation reaction (EOR) is crucial for the potential commercialization of direct ethanol fuel cells, yet it faces significant challenges between catalytic performance and cost-effectiveness. 2D materials have recently emerged as a promising group of electrocatalysts due to their large surface area, efficient charge transport, tunable band structures, and excellent catalytic activity. In this study, the novel 2D layered noble-metal dichalcogenide, PtSe2, is explored for efficient ethanol oxidation electrocatalysis from a microscopic perspective based on an on-chip microelectrochemical platform. While pristine PtSe2 demonstrates similar EOR activities to Pt, argon plasma treatment significantly enhances the performance on EOR activity, If/Ib ratio, onset and peak potentials, and durability. Detail investigations reveal that plasma treatment results in the exposure of PtSe2 surface, which is responsible for significantly enhanced EOR activity and poison-resistance as also confirmed by theoretical calculations. In situ electrical transport measurements for monitoring the catalyst surface intermediates, elucidate that both optimized OHads coverage and appropriate ethanol molecular adsorption on PtSe2 are the key for the high performance. This work demonstrates noble-metal dichalcogenides as promising EOR electrocatalysts, and establishes on-chip electrocatalytic microdevice as a promising probing platform for diverse electrocatalytic measurements.

The catalytic cage with carboxyl groups in PEH-COF stabilized the [K(H2O)n]+ ions, which enhanced the PCET kinetics of the conversion for intermediates to methanol, and ultimately allows the PEH-COF to exhibit stable operation at a jCH3OH$\mathrm{j}_{{CH}_3OH}$ of ≈100 mA cm−2.

Developing catalysts for electrocatalytic CO2 to CH3OH still faces great challenge due to the involvement of multiple proton-coupled electron transfer (PCET) processes. Molecular phthalocyanine electrocatalysts on carbon nanotubes have achieved production of methanol as the sole liquid-phase product but with the activity and stability far from meeting industrial demands. Herein, phthalocyaninato cobalt is fabricated into covalent organic frameworks PE-COF via polymerization with ellagic acid. Subsequent hydrolyzation of the ester groups in this framework affords COOH/OH-containing PEH-COF, resulting in the successful modulation over the local microenvironment of Co as electrochemical active center and in turn rendering the production of CH3OH with high yield and durability. Experimental and theoretical investigations reveal that construction of the COOH group and H2O participated catalytic cages in PEH-COF can effectively fix hydrated potassium ions, which efficiently enhances the PCET kinetics and lowers the energy barriers for the conversion of CO2 to CH3OH. The partial current density (j) and Faraday efficiency of methanol for PEH-COF could reach 100.9 mA cm−2 and 38.5%, respectively. Moreover, the jCH3OH$\mathrm{j}_{{CH}_3OH}$ of PEH-COF can be maintained at 100.4 mA cm−2 after 9 h of electrocatalysis, superior to the thus far reported catalysts.