ZSM-5 zeolite is widely utilized in catalytic cracking reactions for high-efficiency propylene synthesis, whereas severe carbon deposition inevitably leads to rapid catalyst deactivation, greatly limiting its long-term industrial application. Currently, the intrinsic correlation between the Si/Al ratio of ZSM-5, coke evolution pathway, and the deactivation as well as regeneration mechanism still lacks systematic and in-depth clarification. Herein, multiple characterization techniques were combined to comprehensively reveal the coke formation and transformation behaviors during 1-hexene catalytic conversion over ZSM-5 catalysts with tailored Si/Al ratios, and the effects of Si/Al ratio on catalytic deactivation and regeneration property were further elucidated. Structural texture and acidic properties were analyzed by XRD, SEM, N2 adsorption–desorption, NH3-TPD and Py-IR. In-situ FT-IR results reveal that coke deposition proceeds synchronously with the reaction. As the Si/Al ratio increases, deposited coke evolves gradually from polycyclic aromatics to monocyclic aromatic species. Density functional theory calculations further demonstrate that ZSM-5 with a Si/Al ratio of 90–100 achieves a balanced adsorption–desorption energy, promoting reactant activation, accelerating the desorption of coke precursors, and inhibiting severe coking. Benefiting from the suppressed coke accumulation and well-retained recoverable Brønsted acid sites (Si–OH–Al), this optimal catalyst presents excellent regenerability. This work clarifies the acid-dependent coking behavior of ZSM-5, deepens the understanding of deactivation-regeneration principles, and provides reliable guidance for the rational design of high-stability ZSM-5 catalysts toward efficient olefin conversion.

Employing low-salt concentration electrolytes has been regarded as a cost-effective strategy to promote the industrialization of aqueous zinc ion batteries (AZIBs). However, excessive free H2O molecules and localized Zn2+ concentration gradients exacerbate dendrite formation and the hydrogen evolution reaction (HER), which affect the cycling stability and inherent safety of AZIBs. Herein, isoleucine (Ile) is introduced as a multifunctional additive into a dilute 0.5 M Zn(OTf)2 electrolyte to regulate the local pH and construct a fluorine-free hybrid solid electrolyte interphase (SEI), improving the interfacial stability of the Zn anode. First, Ile molecules participate in the Zn2+ solvation shell and substitute for coordinated H2O molecules, which minimizes H2O-triggered side reactions. Second, the preferential adsorption and electrochemical reduction of Ile molecules on the Zn anode surface induce the formation of a fluorine-free organic/inorganic hybrid SEI, enabling Zn deposition along the (002) orientation and suppressing dendrite growth. Furthermore, the Ile additive with zwitterionic nature maintains pH stability through dynamically regulating proton equilibria, mitigating the HER and Zn corrosion. Consequently, in the Ile/0.5 M Zn(OTf)2 electrolyte, the Zn parallel to Zn symmetric cell achieves impressive longevity of over 3000 h, and the Zn parallel to Cu asymmetric cell demonstrates a high coulombic efficiency of 99.36% after 1400 cycles.

Mitochondria, as the primary energy-producing organelles, maintain pH levels that are intimately associated with cellular viability and disease states. Therefore, precisely tracking subtle pH changes within mitochondria is crucial for understanding numerous cellular physiological processes. Herein, a hemicyanine based ratiometric fluorescent probe ID-MpH is reported, constructed by integrating an indole fluorophore with a pH-responsive phenol moiety. ID-MpH showed excellent water solubility and biocompatibility due to the introduction of a sulfobutyl group. Additionally, a key feature of ID-MpH is its dual-emission upon single excitation wavelength, which enables self-calibrating ratiometric pH measurements. The amphipathic cation nature of ID-MpH enables its selective enrichment in the mitochondrial inner membrane, thereby conferring the capacity to monitor mitochondrial pH fluctuations in living cells in real time and to further successfully monitor the mitophagy process induced by starvation and drugs. Meanwhile, ID-MpH-based test strips can be used as a portable detection tool to monitor pH values in fresh fruit juices as well as pH changes during shrimp spoilage. In summary, ID-MpH not only enables precise tracking of mitochondrial pH changes in living cells but also allows visual monitoring of food freshness, demonstrating its application potential in the fields of cell biology and food quality control.

Standardisation of data collection and analysis is essential to enable commercialisation of 2D materials in a wide range of technologies. Selected area electron diffraction (SAED) in the transmission electron microscope (TEM) is one of the key methods for distinguishing monolayer from bilayer and few-layer graphene by comparing the 1st and 2nd order diffraction spot intensities. Yet there are many factors that can affect the reliability of data collection and interpretation, causing the measurement of monolayer samples to deviate from the literature boundary condition of I-{2 & strns;110}/I-{11 & strns;00}< 1 for monolayer graphene (1LG). Here we present the results of a large interlaboratory SAED comparison study, where 15 international laboratories measured and analysed nominally identical samples of chemical vapour deposited graphene. Large variations were observed in the measured ratios of diffraction spot intensities, with the largest variance associated with poor quality SAED data resulting from inadequate specimen handling and storage. To inform the reliable determination of monolayer thickness from SAED patterns we provide a description of best practice for specimen handling, TEM operation, data collection and analysis. This work was undertaken within VAMAS Technical Working Area 41: Graphene and related 2D materials-Project 9, the results of which have been directly incorporated into ISO/TS 21356-2 for the characterisation of graphene sheets. We find that when this methodology is followed, 1LG can be distinguished from bilayer or thicker material with high confidence where analysis of a single SAED pattern gives I-{2 & strns;110}/I-{11 & strns;00}< 1.2, even in the absence of precise specimen tilting.

Architectural design of lithium metal anodes (LMAs) is crucial for smooth Li plating/stripping with suppressed dendrites, which is paramount for high-performance lithium metal batteries (LMBs). In this study, to leverage the carbonaceous host with low gravimetric density for enhanced Li accommodation and reversible Li deposition, mesoporous carbon nanocages comprising dendritic nanochannels embedded with lithophilic Ni nanoparticles are fabricated and exploited to mitigate superficial Li deposition and promote fast and reversible Li plating/stripping within the three-dimensional (3D) host of LMA. Through guided Li+ infiltration, enhanced Li+diffusivity, lowered nucleation barrier, and expedited redox kinetics, the optimal Li host exhibits a high Coulombic efficiency of Li plating/stripping in Li-Cu half cells with significantly reduced dendrite formation and superb cycling stability of symmetric cells over 2000 h at 1 mAcm-2. When paired with the LiFePO4 cathode, the LMB full cell demonstrates a prolonged cycle life, retaining 82.2% of its initial capacity after 600 cycles. This work highlights the crafting of 3D Li hosts with desired structure and functionality for guiding and accommodating smooth Li deposition.

Compared with single-layer two-dimensional (2D) materials, bilayer, trilayer, and few-layer 2D materials exhibit enhanced band structure tunability, improved electrical and thermal properties, and superior mechanical strength and barrier performance. However, the layer-controlled synthesis of 2D films with high layer number uniformity remains challenging, due to the difficulty in the additional layer nucleation and the effective realization of layer-by-layer growth. Herein, we report an edge-feeding synchronous epitaxial growth mode breaking the limit of traditional epitaxy theories. An efficient heterogeneous Cu-Cu2O catalyst is demonstrated, where graphene edge-surrounding Cu2O is crucial in precursor dissociation, atomic carbon diffusion, and edge energy reduction. The synchronous growth method can be generalized to the layer-controlled synthesis of 2-7-layer graphene films. Relying on this growth strategy, we successfully achieved the industrial-scale production of homogeneous A3-sized ABA-trilayer graphene films (42 × 30 square centimeters) with good mechanical properties and peeling-transferring intactness. Our method offers a robust strategy for the layer-controlled synthesis of 2D material films.

Exploring high-performance electrode materials are indispensable for the commercialization of potassium-ion batteries (PIBs). Nickel thiophosphate (NPS), a representative ternary metal thiophosphate, holds great promise as an anode due to its high theoretical capacity and distinctive layered structure, yet still facing critical challenges such as rapid capacity decay and sluggish rate performance. Herein, we developed a flexible, self-supporting composite film anode by integrating high-purity NPS nanosheets within a three-dimensional (3D) conductive scaffold composed of nitrogen-doped graphene (NG) and single-wall carbon nanotube (SWNT) via simple vacuum filtration method. The resulting hybrid film features abundant heterointerfaces, which enhance electron/ion transport, accommodate volume changes, and stabilize the electrode structure. As a result, the anode delivers high potassium storage capacity of 643.5 mAh g−1 at 0.1 A g−1 and maintains 163.9 mAh g−1 at 10 A g−1, showcasing excellent rate performance. Full cell assemblies exhibit stable cycling performance with a reversible capacity of 207.8 mAh g−1 after 100 cycles. Combined crystallography and valence state analyses reveal a disordered phase transition in crystalline NPS during potassiation, indicating a dual mechanism involving both conversion and alloying reactions. This study offers valuable insights into the rational design of advanced anode materials for next-generation PIBs.

Low-dimensional metallic nanomaterials feature inherent quantum confinement effects, which are regarded as promising building blocks for functional materials with versatile tunable properties. However, manipulating the dimensionality of nano-building blocks (referred to as microdimension) for metal aerogels (MAs), a class of emerging porous materials, remains a great challenge. Here, a universal freezing-mediated assembly strategy based on ice chemistry is demonstrated, yielding a wealth of MAs with customizable microdimensions (0D, 1D, and 2D) and compositions by one-pot synthesis. The mechanism of microdimension control is comprehensively deciphered, which relies on the leveraged engulfment and extrusion of metal nanoparticles by regulating the ice chemistry. The microdimension-dictated applications of MAs are unveiled accordingly exemplified by electrocatalysis and shining luxuries. This study not only provides a new dimension for material design but also opens up exciting possibilities for unlocking untouched application fields of aerogels.

Despite the promise of self-assembled organic hole-transport layers (HTLs) in inverted perovskite solar cells, critical concerns persist about their structural stability under external fields such as bias and illumination, which have been regarded as a potential threat to the device's longevity. To address this issue, instead of using self-assembled organic molecules, the intrinsically stable p-type, wide bandgap CuCrO2 colloidal nanocrystals with high monodispersity are synthesized and self-assembled them into HTL via a simple dip-coating method. By further HCl-mediated ligands exchange, the self-assembled CuCrO2-HTL creates a thermally stable chlorinated surface that can not only enhance the electronic coupling of inter nanocrystals but also provide contact passivation on the perovskite surface defects. These merits eventually endow the constructed buried interface with favorable contact, thus facilitating efficient and stable hole transfer. Consequently, an impressive power conversion efficiency of 25.35% is achieved, accompanied by greatly improved longevity under different accelerated-aging tests.

As a well‐known coin metal, silver (Ag) stands out for its unique plasmonic properties and the lowest cost among all noble metals. However, the sol–gel chemistry of the Ag system remains undeciphered, challenging the rational design of Ag aerogels. Additionally, the chemical reactivity of Ag is often neglected in designing noble metal aerogels (NMAs), leaving significant potential untapped for advanced applications. Here, versatile engineering of Ag aerogels is realized by precisely tuning metal‐ion, metal‐ligand, and metal‐metal interactions, achieving a ligament size modulation across 3 orders of magnitude and downsizing the ligament size to <10 nm. The redox potential difference (Δ E )‐driven gel‐level conversion methodology is further established by utilizing the chemical activity of Ag and the self‐healing properties of noble metal hydrogels, stepwise yielding various self‐standing and hollow‐structured Ag‐M aerogels with record‐high performance for (photo)electrocatalysis. This study not only offers guidelines for manipulating multiscale structures of broad metal aerogels but also unveils their unprecedented potential for energy‐related applications.

Benefiting from the attractive high carrier mobility, large absorption coefficient, and ambient stability, group IV-VI compounds show excellent potential applications for optoelectronic devices. Herein, a germanium telluride (GeTe) film with a nanosphere structure has been controllably grown by facile physical vapor deposition and utilized into a photoelectrochemical (PEC)-type photodetector. The GeTe-based PEC-type photodetector possesses an excellent photoresponse and high responsivity in the visible region. Meanwhile, density functional theory calculations were employed to investigate the electronic characteristics of GeTe, supplying evidence of the broadband absorption. The improvement of photoelectric response can be attributed to the thicker films due to the larger light harvesting and higher carrier concentration, which is also verified by the visible-near-infrared absorption spectra and electrochemical impedance spectroscopy. The photocurrent density (I-ph) and photoresponsivity (R-ph) values of the GeTe-based photodetector can reach 22.8 mu A/cm(2) and 228.9 mu A/W. Generally, our work provides an effective way to extend semiconductor materials in applications of PEC-type photodetectors.

The improvement of optical absorption behavior of the second near‐infrared region (NIR‐II, 1000–1350 nm) based on new function materials is significant for the development of biomedicine and optical imaging. Therefore, the electronic structures and optical absorption of 2H phase MoS2 doped by F, Cl, Br, and I atoms with various doping concentrations are calculated, results show that halogen elements introduced extra transition allowed bands which is about 1.0 eV wide to 2H‐MoS2, and the increasing of impurity concentration can trigger strong spin splits. The transformation of electronic structures leads to 2H‐MoS2 metallic behaviors, improves transition efficiency, and lowers photon energy loss. More importantly, strong light–mass interaction is verified and breaks the energy level degeneracy, makes absorption peaks at 0.6–1.0 eV photon energy region, successfully extends the work region of 2H‐MoS2 to NIR‐II window, greatly improves the optical response and application potential in the photoelectric field. These results not only prove the potential of halogen elements as dopants in bandgap engineering of 2H‐MoS2 but also may indicate a direction for seeking new generation function materials that own excellent performance in the NIR‐II window, which is of great significance to promote the development of optoelectronics and bioimaging applications.

High entropy alloys (HEAs) have attracted substantial interest in recent years. Thus far, most investigations have focused on their applications as structural materials rather than functional materials. In this paper, we show that FeMnNiAlCr HEAs can potentially be applied as both a structural and functional material for high-efficiency concentrated solar thermal power (CSP) systems working at >700 degrees C. The HEA itself would be used in high-temperature tubing to carry working fluids, while its surface oxide would act as a high-efficiency solar thermal absorber. These HEAs have demonstrated yield strengths 2-3x greater than that of stainless steel at 700 degrees C and a creep lifetime >800 h at 700 degrees C under a typical CSP tubing mechanical load of 35 MPa. Their Mn-rich surface oxides maintain a high optical-to-thermal conversion efficiency of ~87% under 1000x solar concentration for 20 simulated day-night thermal cycles between 750 degrees C and environmental temperature. These HEAs have also sustained immersion in unpurified bromide molten salts for 14 days at 750{\deg}C with <2% weight loss, in contrast to 70% weight loss from a 316 stainless steel reference. The simultaneous achievement of promising mechanical, optical, and thermochemical properties in this FeMnNiAlCr system opens the door to new applications of HEAs in solar energy harvesting.

Nanoconfined water plays an important role in broad fields of science and engineering. Classical molecular dynamics (MD) simulations have been widely used to investigate water phases under nanoconfinement. The key ingredient of MD is the force field. In this study, we systematically investigated the performance of a recently introduced family of globally optimal water models, OPC and OPC3, and TIP4P/2005 in describing nanoconfined two-dimensional (2D) water ice. Our studies show that the melting points of the monolayer square ice (MSI) of all three water models are higher than the melting points of the corresponding bulk ice Ih. Under the same conditions, the melting points of MSI of OPC and TIP4P/2005 are the same and are ∼90 K lower than that of the OPC3 water model. In addition, we show that OPC and TIP4P/2005 water models are able to form a bilayer AA-stacked structure and a trilayer AAA-stacked structure, which are not the cases for the OPC3 model. Considering the available experimental data and first-principles simulations, we consider the OPC water model as a potential water model for 2D water ice MD studies.

The radiochemical reaction products of T2/DT-CO system with different tritium pressures were studied in this work. The results show that the pressure of tritium and reactant was the key factor affecting the reaction rate of T2/DT-CO system, and the reaction products were closely related to the initial tritium concentration. Gradual evolution of reaction products including multi-carbon and multi-oxygen organic compounds were jointly affected by tritium decay in reactant molecules and bond breaking of reactant molecules by β-rays released from tritium decay. In addition, the tritium concentration in the deuterium-tritium mixture also affected the reaction products. High tritium concentration was conducive to the formation of multi-oxygen organics, while low tritium concentration was helpful to produce multi-carbon organics.

The coupling effects of surface plasmon resonance (SPR) from metamaterials induce variation in both the frequency and intensity of plasmonic modes. Here, we report an angular-dependent THz modulator with hybrid metal–graphene metastructures. The metastructures composed of the period gold split-rod arrays on top of a monolayer graphene, which show redshift modulation in the THz region with an increasing incident angle due to the strong out-of-plane magnetic flux introduced by the clockwise circular current at the oblique incidence. By utilizing graphene-based actively tunable conductor with ion-gel electrical gating, the THz transmission can be significantly modified. The modulation depth of the hybrid metal–graphene metastructure modulator can reach ~37.6% at 0.62 THz with a gate voltage of −3 V. The theoretical modeling of transmitted dependency on frequency and incident angle is demonstrated at different Fermi energies, which fits well with the experimental results. This hybrid device can offer a useful method for THz applications (such as angle sensors or angular-resolved spectroscopy), where angle-dependent modulation is needed.

Room-temperature sodium-sulfur batteries have attracted extensive attention as a cost-effective and high theoretical energy density next-generation energy storage systems. However, the insulating nature of sulfur, the sluggish reactivity of sulfur with sodium, and severe dissolution of polysulfide are the main challenges of this technology. Here, we propose a covalent sulfur bond breakage mechanism by bonding of sulfur chain onto the inner cavity of the sulfydryl-functionalized mesoporous hollow carbon spheres (MHCS) to efficiently promote the generation of short-chain sodium polysulfide and accelerate polysulfide redox kinetics. The covalent sulfur confined MHCS (S@MHCS) cathode delivers an unprecedented rate capability (250 mAh g-1 at 5 C) and exhibits excellent long-term cycling stability over 1000 cycles at 1 C with a high cathode loading of 5 mg cm-2. Moreover, the associated electrochemical reaction mechanism is also revealed by ex-situ X-ray photoelectron spectroscopy and theoretical calculation. This work introduces a novel sulfur cathode design to enhance the performance of room-temperature sodium-sulfur batteries.

Structural symmetry-breaking plays a crucial role in determining the second harmonic generation (SHG) intensity and pattern for two-dimensional (2D) materials. Herein, we report that the giant optical SHG can be achieved by designing a Janus structure for ReS2 and ReSe2. The designing of a Janus ReSSe monolayer structure can break both the in-plane and out-of-plane symmetry of monolayer ReS2 and ReSe2, resulting in the occurrence of larger second-order nonlinear coefficients in the in-plane (d11, d16, d21, and d22) and out-of-plane (d15 and d31) components. The second-order nonlinear coefficient dispersion properties for the asymmetric Janus ReSSe monolayer give rise to a multifaceted dependence of the SHG on the azimuthal and polarization angles at different incident wavelengths including double and quadruple symmetries, rotation of polar axis, and variations in intensity. These results highlight the potential to deterministically engineer novel nonlinear optical properties in the designing of the Janus structure based on layered materials.

Sodium (Na) metal batteries are promising as next-generation energy storage systems due to the high specific capacity of the Na metal anode as well as rich natural abundance and low cost of Na resources. Nevertheless, uncontrolled growth of dendritic/mossy Na arising from the unstable solid-electrolyte interphase (SEI) leads to rapid electrode degradation and severe safety issues. In this work, we introduce cetyltrimethylammonium bromide (CTAB) as an electrolyte additive that enables a synergistic effect from both the CTA+ cation and Br- anion in stabilizing the Na metal anode. Notably, cryogenic transmission electron microscopy is utilized to investigate the effect of the additive, revealing the critical morphology and structure of the SEIs and Na electrodes at the nano/atomic scale. Benefiting fromthe additive, a stable Na anode can be realized at an ultrahigh capacity of 30 mAh cm-2 at 10 mA cm-2 over 400 h.