With the increasing progress in the emerging field of phase engineering of nanomaterials, transition metal dichalcogenides (TMDs) with metastable phases have attracted extensive research interest owing to their unique physicochemical properties and promising potential for various applications. Unlike their semiconducting counterparts, metastable 1T'-phase group VIB TMDs exhibit distinctive metallic behavior, making them highly promising for clean energy electrocatalysis (for example, hydrogen evolution), high-performance electronics and superconducting devices. However, conventional synthetic strategies usually suffer from low yields, poor phase purity, small crystal size and harsh experimental conditions, hindering their fundamental research and practical applications. Here we describe a salt-assisted method for the controlled preparation of various metastable 1T'-phase group VIB TMDs with high crystalline quality and high phase purity. In this context, 'salt-assisted' refers to the co-annealing of commercially available 2H-phase TMDs, chalcogen powders (for example, S or Se) and alkali metal salts (for example, K2C2O4·H2O or K2CO3). When heated in a tube furnace under an H2/Ar atmosphere, these alkali metal salts trigger a phase transformation of TMDs from the thermodynamically stable 2H phase to the metastable 1T' phase. This Protocol describes the details of experimental procedures to prepare a series of 1T'-TMDs, that is, MoS2, MoSe2, WS2, WSe2, MoS2xSe2(1-x) and WS2xSe2(1-x). It takes ~37 h 20 min and yields robust 1T'-TMD crystals with their size of up to hundreds of micrometers at a gram scale (up to ~2 g per batch), overcoming the longstanding synthetic bottlenecks and paving the way for advanced fundamental studies and the exploration of practical applications.

The sustainable management of postconsumer rubber waste remains a significant global challenge, owing to the chemical resilience of sulfur-crosslinked networks, complicated components, and high filler content. Herein, we report a molecular-level upcycling strategy that converts sulfur-vulcanized rubber waste into structurally versatile hydroxyl-functionalized liquid rubbers (HLPRs). Central to this approach is a second-generation synergistic catalytic platform (Cp2ZrCl2/Al( i Bu)2H) capable of simultaneously cleaving polydiene backbones and polysulfide crosslinks and, more importantly, operating efficiently in a hydrocarbon solvent, thus enabling direct aerobic oxidation of metal-carbon intermediates to introduce hydroxyl groups. In the obtained HLPRs, the hydroxyl content, molecular weight, and compositional profiles can be tailored through catalyst loading, reaction time, and oxygen exposure, providing a facile regulation manner of chain parameters. Furthermore, the formed HLPRs serve as reactive building blocks for constructing polythiourethane networks, yielding high-performance elastomers that exhibit enhanced extensibility and toughness and excellent reprocessability stemming from reversible thiourethane exchange. Overall, this work establishes a circular materials strategy that both chemically deconstructs waste elastomers and reincorporates the flexible nature of the main chain into new functional polymer architectures, offering a compelling alternative pathway for the sustainable upcycling of postconsumer rubber.

High-entropy alloy (HEA) nanomaterials are promising catalysts for proton exchange membrane water electrolysers (PEMWE), yet their crystalline structures have typically been restricted to thermodynamically stable phases. Here, using Au nanomaterials with distinct crystal phases as templates, we synthesize and stabilize Au@HEA core-shell nanostructures through a general and robust wet-chemical method in which the HEA is composed of up to ten metallic elements (Ir, Pt, Ni, Fe, Co, Rh, Pd, Ru, Cu and Mn). Phase-dependent water electrolysis is demonstrated as a proof-of-concept application. The hexagonal close-packed 4H-Au@4H-IrPtNiFeCo catalyst exhibits superior activity and stability for the acidic hydrogen evolution reaction, oxygen evolution reaction and overall water electrolysis compared with the conventional face-centred cubic IrPtNiFeCo catalyst. In a PEMWE at 60 °C, the 4H-Au@4H-IrPtNiFeCo catalyst achieves 3,000 mA cm-2 at only 1.90 V and maintains stable operation for over 1,200 h at 1,000 and 2,000 mA cm-2, with degradation rates of ~6.3 and ~15.7 µV h-1, respectively. This work offers a strategy for designing highly efficient and stable HEA catalysts with tailored phases for future practical water electrolysis.

Artificial neural network-based machine learning provides foundations for artificial intelligence (AI), yet requires high energy costs for training. Beyond software-level simulation of neural networks, hardware-level implementation via neuromorphic devices becomes the next milestone in nanoscience towards energy-sustainable AI. Single-molecule devices have the potential for ultimate scale and energy efficiency, but challenges remain in achieving programmable multi-conductance states amidst room-temperature thermal fluctuations. Here we fabricated a bio-inspired single-molecule neuromorphic device consuming ~6.34 aJ/operation by electrochemically gating molecule-ion electrostatic interactions. This device realizes biomimetic emulation of neural plasticity from short-term to long-term memory featuring over 10 distinct conductance states, demonstrating the applications in Pavlovian conditioning for associative learning and pattern recognition in Morse code processing. Our approach enables multi-state synaptic emulation using an individual molecule toward energy-sustainable AI.

Recently, 2D materials have emerged as a focal point in materials science research. Conventional 2D systems predominantly derive from layered van der Waals (vdW) crystals, where individual atomic planes are held together by weak interlayer interactions. However, groundbreaking developments have challenged this paradigm through the successful isolation of 2D materials from non‐van der Waals (non‐vdW) bulk crystals. Non‐vdW 2D materials resemble their vdW counterparts in atomically thin sheets with strong in‐plane covalent/ionic bonding but manifest distinguished structural characteristics, including large lattice distortions, abundant dangling bonds, and coordinatively unsaturated surface atoms. These intrinsic features endow them with enhanced surface reactivity and dynamic electronic states, which promote chemisorption of reactive species and accelerate interfacial charge transfer kinetics‐properties that are highly advantageous for energy applications. Nevertheless, the absence of weak interlayer vdW forces poses significant challenges in exfoliation processes, with fundamental mechanisms remaining poorly understood. This review systematically examines state‐of‐the‐art liquid‐phase exfoliation (LPE) methodologies for non‐vdW nanoflakes synthesis, critically analyzing their mechanistic foundations, process‐structure‐property relationships, and performance benchmarks in energy‐related technologies. Furthermore, key challenges are identified in improving nanoflakes quality, precise kinetic control, and advancing next‐generation artificial intelligence (AI) and smart energy systems, while proposing interdisciplinary strategies to advance this burgeoning field.

Phase engineering of nanomaterials (PEN) has emerged as a new research field by enabling precise control of crystallographic phases at the nanometer scale. The capability of stabilizing unconventional phases unlocks a vast library of physiochemical properties inaccessible to the conventional, thermodynamically stable crystals. This review provides a comprehensive framework to map the past, present, and future of PEN. We first briefly introduce the concept of PEN. Then, we summarize synthetic methodologies, including direct phase-controlled synthesis and phase transition. The discussion also underscores the pivotal role of advanced characterization, particularly the transition from ex situ to in situ and operando techniques, in probing dynamic phase behaviors under realistic conditions. We present key applications in (electro)catalysis, energy conversion and storage, functional devices, and biomedicine to illustrate the PEN's broad impact. Looking ahead, we identify key challenges and future directions, emphasizing robust phase stabilization, architecture control, and artificial intelligence-integrated phase design. The field is ultimately advancing toward the artificial atomically-assembled structures (AAASs), enabling the deterministic assembly of atoms with precisely controlled phase and architecture to achieve targeted functions and applications.

This study introduces a novel multifunctional composite material composed of polyvinylidene difluoride (PVDF) fiber mats, MXene nanosheets, and superabsorbent polymer (SAP) particles, aimed at addressing limitations in traditional piezoelectric materials such as low strength and poor multifunctionality. The PVDF fiber mats were fabricated via electrospinning, with MXene nanosheets uniformly deposited on their surface through a filtration process. SAP particles were subsequently incorporated to enhance moisture absorption, functional diversity, and mechanical performance. Comprehensive characterization revealed the successful integration of MXene and SAP, achieving uniform distribution and synergy at the microstructural level. The composite exhibited excellent piezoelectric properties (4-6V) and mechanical stability (The sample can withstand thousands of cyclic compressions with good stability within a few hundred kPa), maintaining a linear response to pressure under both dry and water-absorbed conditions. Finite element analysis (FEA) and various application tests demonstrated the material’s ability to detect a wide range of external pressures, from subtle touches to high-pressure impacts, highlighting its potential for use in flexible sensors, electronic skin, and dynamic monitoring systems. The study underscores the importance of structural optimization in enhancing piezoelectric performance and environmental adaptability. Future research could explore long-term stability and further optimization of material composition to support broader applications in wearable devices, energy harvesting, and intelligent sensing technologies.

Acting as a pivotal cytokine of innate immunity, the signal transduction of interleukin 6 (IL-6) is always elevated in relation to the occurrence of injury, bacteria and chemical invasion. IL-6 as a critical care biomarker can be used for the clinical diagnosis of diseases ranging from bacterial infections to most inflammatory reactions. Then, a simple, cost-effective and sensitive colorimetric aptasensor was designed for the specific detection of IL-6. The IL-6 aptamer anchored on gold nanoparticles (AuNPs) by polyadenine accurately recognized IL-6, and then, the folded IL-6 aptamer enhanced the stability of AuNPs against salt-induced aggregation. The degree of AuNP aggregation increased inversely with the concentration of IL-6. A higher IL-6 content resulted in lower aggregation of AuNPs, which can be measured by spectrophotometry. The results showed that the proposed aptasensor exhibited a linear detectable range of 7-500 pg mL-1 with a limit of detection of 4.652 pg m-1. Furthermore, this proposed colorimetric aptasensor achieved the discrimination of IL-6 from other analogues and could detect IL-6 in human serum samples, which demonstrated its potential application for the detection of IL-6 in complex matrices.

Tuning the morphology and structure of Cu nanomaterials could effectively regulate their property, functions, and applications. However, it still remains challenging to directly synthesize Cu nanomaterials with an unconventional phase. Here, we report a one-pot wet-chemical synthesis of Cu nanocrystals (NCs) with a hexagonal close-packed (hcp, 2H type) phase, which is different from their thermodynamically stable face-centered cubic (fcc) phase. Compared to the conventional fcc-Cu NCs, the obtained 2H-Cu NCs exhibit enhanced catalytic activity and selectivity in the electrochemical carbon dioxide reduction reaction (CO2RR), achieving a high Faradaic efficiency (FE) of 73.1% toward multicarbon (C2+) products at 600 mA cm-2 under alkaline conditions in a flow cell. Moreover, in situ characterizations and density functional theory (DFT) calculations reveal that the 2H-Cu NCs can optimize the adsorption of the *CO intermediate, leading to a low energy barrier for the formation of C2+ products. This work not only demonstrates an improvement in CO2RR performance of Cu NCs by using the strategy of phase engineering of nanomaterials (PEN) but also opens up an avenue to explore the intrinsic properties and applications of unconventional-phase nanomaterials.

ABSTRACT Synergy between metallic nanoparticles and single‐atom sites offers considerable potential for developing advanced electrocatalysts. However, the synergistic mechanism in such complex architectures under operating conditions remains elusive. Herein, a two‐step approach involving selective etching and co‐confined adsorption was developed to precisely construct CoRu/Ru NPs catalyst, featuring Ru–Co diatomic sites coupled with Ru sub‐nanoparticles, which demonstrates excellent oxygen reduction reaction (ORR) performance with a half‐wave potential of 0.91 V and a peak power density of 369 mW cm −2 in zinc‐air batteries, along with outstanding cycling stability over 1350 h. Beyond modulating the electronic structure to weaken OH* adsorption on Ru–Co diatomic sites, the Ru sub‐nanoparticles also induce an alternative thermodynamic pathway for enhanced ORR kinetics, in which interfacial water dissociate on oxyphilic Ru sub‐nanoparticles and facilely supply protons to oxygen‐containing intermediates on neighboring Ru–Co diatomic sites. This work not only advances the construction of synergistic active sites but also opens a new paradigm for designing advanced electrocatalysts by harnessing the interfacial environment beyond electronic structure modulation.

Direct alcohol fuel cells (DAFCs) represent a highly promising sustainable energy technology, whose performance strongly depends on the efficiency of electrocatalysts. The surface morphology of these catalysts plays a critical role in determining their catalytic activity. Although core-shell nanostructures with abundant surface protrusions have attracted extensive attention, the impact of an internal gap within such morphologies has not been systematically investigated. In this study, we designed a unique quad-metallic AuAg@PdPt core-gap-shell (CGS) nanostructures featuring numerous surface protrusions for alcohol oxidation reactions. To evaluate the effect of the internal gap on catalytic performance, a corresponding solid AuAg@PdPt core-shell (CS) nanostructures without a gap was also synthesized for comparison. Toward alcohol oxidation reaction including methanol, ethanol, ethylene glycol, and glycerol, the mass activities of AuAg@PdPt CGS nanostructures for several alcohols are 1.89, 2.45, 2.11 and 1.58 A mg(-1)Pd+Pt, which are 1.67, 1.70, 1.95 and 1.97 times higher than that of the solid AuAg@PdPt CS nanostructures (1.14, 1.44, 1.08 and 0.80 A mg(-1)Pd+Pt), respectively. The results clearly demonstrate that the introduction of an internal gap in the core-shell structure significantly enhances the electrocatalytic performance. This work provides valuable insights and references for the design of highperformance catalysts through rational surface and interfacial engineering.

Zero-gap water electrolysers have shown their potential in large scale green hydrogen production, but their cost effectiveness and long-term durability remain limited by an incomplete understanding of electrocatalysts and electrode materials behaviour during full-cell electrolysis. Here, a gasket-free anion exchange membrane water electrolyser (AEMWE) has been designed with an integrated reference electrode (RE) next to the membrane electrode assembly (MEA). A zero-gap design between the electrode and the membrane is achieved without the limitations of a gasket, ensuring close contact and minimising the system resistance and allowing precise monitoring of anode and cathode potentials individually during electrolysis. With NiFe(OH)2 as the anode catalyst and NixSy as the cathode catalyst, electrolysis at a current density of 500 mA cm-2 was achieved at 1.86 V cell voltage with 1 M KOH electrolyte at 333 K. Electrochemical impedance spectroscopy (EIS) measurement with a Hg/HgO reference electrode during the electrolysis at the same conditions further reveal the potential loss distribution: 0.10 V from IR drop, 0.35 V from anode and 0.27 V from cathode. These results demonstrate a simple but useful platform for decoupling performance-limiting processes in AEMWE systems and guiding the design of more durable and efficient electrolysers.

Hydrogen is a promising clean energy carrier to address global energy and environmental challenges. Although platinum (Pt)-based catalysts are the benchmark for the hydrogen evolution reaction (HER), their high cost and scarcity limit their widespread application. Two-dimensional transition metal dichalcogenides (TMDs), particularly with the unconventional 1T' phase, have emerged as promising alternatives, yet synthesizing them with high phase purity and stability remains challenging. Here, by using amorphous phosphorus (P)-doped Pd nanoparticles (a-PdP NPs) as templates, we develop a facile and general wet-chemical method to synthesize high-phase-purity and stable 1T'-TMD monolayers (MLs), including MoS2, WS2, and MoWS2, to construct a-PdP@1T'-TMD core-shell NPs. Experimental and theoretical analyses reveal that the formation and stabilization of 1T'-MoS2 MLs are attributed to the strong Pd-S interaction, electron donation from oleylamine, and amorphous nature of the template. The resulting a-PdP@1T'-MoS2 catalyst exhibits superior HER performance, requiring an overpotential of only -182.3 mV to achieve 1,000 mA·cm-2 and maintaining high stability for over 500 h at 500 mA·cm-2, outperforming the commercial Pt/C and placing it among the best reported MoS2-based catalysts. Impressively, the synthesized a-PdP@1T'-MoS2 can also be used as an efficient and stable support to grow single-atomically dispersed Pt with further enhanced HER activity, indicating its promise as a versatile platform for the design and preparation of advanced electrocatalysts.

The recycling of widely used plastic wastes into high-valued carbon materials for electrochemical energy storage is promising but still challenging. In this study, we demonstrate a sustainable strategy for recycling polyolefin wastes into hierarchical nitrogen-doped porous carbon by utilizing the synergistic interaction between melamine and zinc chloride. The synergistic interaction not only facilitates the formation of thermally stable structure, achieving a high carbon yield (similar to 34.3 %) and a high nitrogen doping level (11.2 at.%), but also generates abundant meso-/micropores with a high specific surface area (1031.7 m(2)g(-1)). These merits endow the nitrogen-doped porous carbon electrode with an ultrahigh capacitance of 224.8 F g(-1) at 1 A g(-1) and 91.2 % retention after 50,000 cycles. Consequently, the assembled symmetrical supercapacitor exhibits a high energy density of 43.8 Wh kg(-1) at a power density of 750 W kg(-1) and outstanding electrochemical stability of similar to 87 % after 10,000 cycles in a TEABF(4)/AN electrolyte. In addition, the applicability of our strategy to other polyolefin-based plastic wastes such as polypropylene and polystyrene proves its versatility. Our study provides a promising approach for recycling polyolefin wastes into high-value products to alleviate environmental problems and opens a new horizon for the production of high-performance electrode materials for electrochemical energy storage.

. Synthesis and full characterization of a new coordination compound, which was synthesized by mixed ligands under hydrothermal condition, namely [Cu(L)2(phen)2(H2O)2]center dot 4H2O (1) (phen = 1,10-phenanthroline, H2L = 3-carboxy-1-carboxymethyl-2-oxidopyridinium). Cu(II) is six-coordinated in a slightly twisted [CuN2O4] octahedral geometry. 1 displays 2D supramolecular layer, which is further extended into a 3D network by the pi-pi stacking and hydrogen bonds. 3D Hirshfeld surface analysis is combined with 2D fingerprint plots to investigate the contribution of different intermolecular interactions within the crystal. DFT calculations are also performed.

Pressure has been considered as a versatile and promising means in the discovery of metal superhydrides. However, although a series of metastable metal hydrides with excellent superconducting properties have been predicted through theoretical calculations, it is still challenging to obtain metal hydrides with metastable phases via a high-pressure synthetic route. Herein, we have successfully fabricated a metastable PdH3 superhydride using amorphous Pd nanoparticles (NPs) as a starting material at ∼32.2 GPa and ∼2000 K. Intriguingly, after unloading the pressure and decreasing the temperature to ambient conditions, another metal hydride, i.e., PdH1.3, is obtained, which possesses the highest hydrogen ratio compared to the previously reported ambient-stable Pd hydrides. In contrast, Pd3H5 is obtained using crystalline Pd NPs with a conventional face-centered cubic (fcc) phase as the starting material under ∼2000 K and ∼33.5 GPa, which transforms to PdH0.706 after quenching to ambient conditions. The experimental results and theoretical calculations reveal that the disordered atomic arrangement and high entropy of amorphous Pd NPs play a critical role in the generation of metastable PdH3. This work provides insights into the preparation of metastable metal hydrides with a high hydrogen ratio for promising applications, such as superconductivity.

In contrast to metal ions that have been routinely used to construct metal-organic frameworks (MOFs), anions have rarely been used as essential coordination centers in supramolecular organic frameworks (SOFs). In this work, we present a SOF, chloride-SOF, based on the coordination of chloride anions and a flexible oligopyrrole. Owing to the multiple interactions between individual oligopyrrole molecules and an A-B-C-style stacking of the 2D honeycomb layers, crystalline chloride-SOF exhibits reasonable thermal stability and retains its structure upon desolvation. Treating contaminated water containing 100 mg L-1 picric acid (PA) with the desolvated form of chloride-SOF reduced the PA concentration to the low ng L-1 (ppt) level. Supporting studies provide evidence for the conclusion that the material captures PA through anion exchange and adaptive structural transformation, rather than pore-selectivity. Chloride-SOF thus showcases the potential of SOFs as structurally transformable materials useful for hazardous waste removal.

The rational construction of heterogeneous interfacial engineering presents a critical strategy for advancing efficient electrochemical water-splitting development. Here, a bimetallic sulfide-coupled MoNi alloy heterostructure catalyst (VMoS/MoNi) is synthesized via hydrothermal and sulfidation methods for high-performance alkaline water electrolysis. Benefiting from interfacial coupling within the VMoS/MoNi catalyst, the active sites are enriched, and electron transfer is promoted, leading to enhanced synergy and collaboration in electrocatalytic reactions. As a result, at 10 mA·cm−2, the VMoS/MoNi catalyst demonstrates excellent HER (26 mV) and OER (223 mV) performance. VMoS/MoNi catalysts used as double electrode in an alkaline electrolytic assembly are noteworthy for achieving a cell voltage of 1.56 V at 10 mA·cm−2, a significant improvement above most previously reported bifunctional electrocatalysts. This result provides further momentum for the design of heterostructure electrocatalysts, advancing the study of renewable energy conversion and storage.

Inspired by the initial proposal of σ-bridged donor-acceptor (D-σ-A) single-molecule diodes in 1974, extensive studies over the past 50 years have explored various designs for π-conjugated D-π-A single-molecule diodes due to their feasible chemical synthesis and effective charge transfer. However, the rectification ratio of π-conjugated single-molecule diodes has been long-term limited by the challenge of asymmetric electronic coupling to induce the rectification effect. Here, we present a supramolecular diode constructed through an intramolecular π-π interaction-driven assembly strategy. The asymmetric transmission in this system is tunable via subangström mechanical control, resulting in a rectification ratio of up to 16. Electron transport studies reveal that this through-space D-π-π-A system constructed by the π-π stacking between pyrene (Py) and naphthalenediimide (NDI) is crucial for achieving asymmetric currents under different bias polarization. Theoretical calculations suggest that the intermolecular destructive quantum interference not only enables a sharp variation in electron transmission but also facilitates asymmetric electronic energy shifts through mechanical stretching, significantly improving the rectification ratio. Our work provides a general approach to fabricating and modulating asymmetric molecular architectures through noncovalent supramolecular interactions, showcasing the potential of high-performance single-molecule rectifiers.