A novel Zn-based luminescent coordination polymer [Zn(phen)(H2O)]2[L]·2H2O (1), [H4L=(E)-5,5′-(diazene-1,2-diyl) diisophthalic acid] was synthesized via a solvothermal reaction, which has a three-dimensional supramolecular structure. Compound 1 exhibits good chemical and thermal stability, and can effectively detect nitroaromatic explosives (NACs) via a fluorescence quenching effect. Especially for 2,4,6-trinitrophenol, compound 1 has demonstrated very high sensitivity (KSV=1.9×104 L/mol), low detection limit (LOD=9.6×10−6 mol/L) and good anti-interference ability. Additionally, Compound 1 also exhibits good selective recognition of Fe3+ with excellent anti-interference performance and reusability. Through UV-visible spectroscopy and density functional theory calculations, the fluorescence quenching mechanisms of compound 1 for various analytes are discussed in detail. Based on the above excellent properties of compound 1, it has great application potential in water quality monitoring.

Machine learning technologies have been employed to explore enormous chemical space of high-entropy alloys (HEAs) for electrocatalytic applications. However, their performance awaits further improvement due to the limited datasets and complex interaction between adsorbates and HEAs. In this study, we present a chemistry-wise transfer active learning framework designed to address these challenges by systematically capturing chemical interaction across increasing levels of compositional complexity. Specifically, we employ a sequential transfer learning strategy that progressively learns adsorption process from unary and binary intermetallic systems, through ternary compounds, and ultimately combined with active learning to HEAs. This hierarchical approach significantly enhances the prediction accuracy of adsorption energy for the intermediates involved in CO2 reduction, outperforming the models trained directly on the limited HEA dataset. Further analysis using t-distributed stochastic neighbor embedding (t-SNE) reveals that the improved performance arises from the effective transfer of chemically relevant features across domains. Our results demonstrate that chemistry-wise transfer active learning not only improves predictive capability in data-scarce regimes but also holds promise for accelerating the investigation of a broad range of functional materials with reduced cost and energy consumption.

Lithium metal batteries (LMBs) have shown great promise as the next-generation energy storage devices. However, the growth of lithium dendrites on the lithium metal anode and the volume expansion of lithium severely hindered their performance. Herein, we report a simple approach to address the challenges of volume expansion and dendritic growth in lithium plating/stripping by utilizing a nanostructured lithium host based on commercial copper foam (CuF). By growing copper nanowires in situ on the CuF and subsequently modifying them with nitrogen-doped carbon (N-C), we develop a nanostructured surface with abundant electrochemical activity sites and enhanced lithiophilic properties. These unique features enable the nanostructured CuF to effectively reduce the local current density and overpotential during lithium plating. Consequently, the nanostructured CuF exhibits remarkable improvements in the reversibility of lithium plating and stripping, maintaining a high coulombic efficiency of 98.6 % even after 430 cycles of continuous operation. Additionally, the assembled Li-S batteries also demonstrate improved capacity, rate capability and capacity retention. This simple and controllable method offers an effective strategy for constructing high-performance lithium anode for LMBs.

Electrochemical reduction of CO(2)into value-added chemicals is a promising way for carbon neutrality while hindered by the low activity and selectivity of electrocatalysts. Herein, a ZIF-8 modified silver nanowire (AgNW) was contracted and used as an efficient electrocatalyst for CO(2)reduction. The optimized ZIF-8/AgNW catalyst exhibited high CO selectivity with a faradic efficiency of CO (FECO) > 93 % within the -1.0 to -1.3 V versus the reversible hydrogen electrode (RHE). It also achieved a high CO partial current density of 13.3 mA center dot cm-2 and demonstrated good stability over 10 h in KCl electrolyte. Electrochemical results suggested that the synergistic effect between AgNWs and ZIF-8 enhanced the catalytic performance. Moreover, KCl as an electrolyte was found to be superior to KHCO3 for the ZIF-8/AgNW catalyst.

Splash, one of the most visually apparent droplet dynamics, can manifest on any surface above a certain impact velocity, regardless of surface wettability. Previous studies demonstrate that elevating the substrate temperature can suppress droplet splash, which is unfavorable for many practical applications, such as spray cooling and combustion. Here, we report that the suppression effect of substrate temperature on splash is nullified by utilizing surfaces with nanostructures. By manipulating air evacuation time through surface nanostructures, we have identified a pathway for precise control over the splash threshold and the ability to tailor the dependence of the splash onset on surface temperature. We further propose a theoretical criterion to determine different splash regimes by considering the competition between air evacuation and the development of flow instabilities. Our findings underscore the crucial role of nanostructures in splash dynamics, offering valuable insights for the control of splash in various industrial scenarios.

Commercial Ni foam (NF) as substrate is widely used in lithium metal anode for uniform Li deposition and dendrite-free condition by reduced local current density. However, it’s high mass density of 8.902 g cm-3 and bulky skeleton tend to the heavy weight, which remarkedly decreases the energy density of lithium metal batteries. Herein, three-dimensions carbon foam completely coated by Ni metal (Ni@CMF) is fabricated as an alternative to NF through commercial electroless Ni plating. The noneffective inner Ni metal, occupying most of mass and volume of NF, is masterly replaced by light carbon foam, which is carbonized from cost-effective melamine foam (MF), resulting in sharply reduced areal density from ~24.8 mg cm-2 to ~2.2 mg cm-2 and improved electrochemical performance compared with commercial NF. As a result, the superior Coulombic efficiency stability of 240 cycles for Ni@CMF substrate is achieved companying reduced Li nucleation overpotential of ~11 mV compared with that of NF (~53 mV). Moreover, the pouch Li metal full cell enlightens the light-emitting diode (LED) lights in both flat and deformation states. The neotype Ni foam, proposed in this work, with huge commercial value can be produced in large scale in lighter weight, lower cost and enhanced property.

Sodium-ion hybrid capacitors (SIHCs) have received extensive attention and research due to their combined advantages of high power performance and high energy density. However, the lack of high-performance anode materials has been a challenge for sodium storage devices. Herein, a heteroatom co-doped hollow spherical TiO2@MoSe2/reduced graphene oxide (RGO) with pea pods structure is designed and synthesized. This unique composite is made of TiO2 as the stable framework, MoSe2 sheet as the main active materials, and RGO conductive network as the protective cover. The sandwich structure provides stable and ordered transport channels for electrons and Na+, and greatly increases the number of active sites. As a result, TiO2@MoSe2/RGO exhibits satisfactory electrochemical performance. At a high current density of 2 A g-1, TiO2@MoSe2/RGO still maintains a capacity of 106 mAh g-1 after 1000 cycles. The hybrid device possesses an energy density of 135 Wh kg- 1 at power density of 1667 W kg- 1, demonstrating the design concept of heterogeneous composite provides a new route for the development of electrode materials in sodium-ion storage devices.

It remains a great challenge to design and manufacture battery-type supercapacitors with satisfactory flexibility, appropriate mechanical property, and high energy density under high power density. Herein, a concept of porous engineering is proposed to simply prepare two-layered bimetallic heterojunction with porous structures. This concept is successfully applied in fabrication of flexible electrode based on CuO-Co(OH)2 lamella on Cu-plated carbon cloth (named as CPCC@CuO@Co(OH)2 ). The unique structure brings the electrode a high specific capacity of 3620 mF cm-2 at 2 mA cm-2 and appropriate mechanical properties with Young's modulus of 302.0 MPa. Density functional theory calculations show that porous heterojunction provides a higher intensity of electron state density near the Fermi level (E-Ef  = 0 eV), leading to a highly conductive CPCC@CuO@Co(OH)2 electrode with both efficient charge transport and rapid ion diffusion. Notably, the supercapacitor assembled from CPCC@CuO@Co(OH)2 //CC@AC shows high energy density of 127.7 W h kg-1 at 750.0 W kg-1 , remarkable cycling performance (95.53% capacity maintaining after 10 000 cycles), and desired mechanical flexibility. The methodology and results in this work will accelerate the transformative developments of flexible energy storage devices in practical applications.

It remains a great challenge to design and manufacture battery-type supercapacitors with satisfactory flexibility, appropriate mechanical property, and high energy density under high power density. Herein, a concept of porous engineering is proposed to simply prepare two-layered bimetallic heterojunction with distinct layers of porous structures. This concept is successfully applied in the fabrication of flexible electrodes based on CuO-Co(OH) 2 lamella on Cu-plated carbon cloth (named as CPCC@CuO@Co(OH) 2 ). The unique structure brings the electrode a high specific capacity of 3620 mF cm -2 at 2 mA cm -2 and appropriate mechanical properties with Young's modulus of 302.0 Mpa. Density functional theory calculations show that porous heterojunction provides a higher intensity of electron state density near the Fermi level (E–E f =0 eV), leading to a highly conductive CPCC@CuO@Co(OH) 2 electrode with both efficient charge transport and rapid ion diffusion. Notably, the supercapacitor assembled from CPCC@CuO@Co(OH) 2 //CC@AC shows a high energy density of 127.7 W h kg -1 at 750.0 W kg -1 , and remarkable cycling performance (95.53% capacity maintaining after 10,000 cycles), and desired mechanical flexibility. The methodology and results in this work will accelerate the transformative developments of flexible energy storage devices in practical applications.

Flexible asymmetric supercapacitor (FASC) systems are expected to exhibit not only excellent energy storage properties and safety but also satisfactory flexibility and robust integration. However, tremendous issues such as low capacitance, narrow voltage window, and poor mechanical properties still exist. In this paper, a novel kind of 3D lamellar Mn(OH)(2) nanosheets on Cu-plated carbon cloth with a core-shell integrated framework (CPCC@CuO@Mn(OH)(2)) is fabricated to obtain the flexible material in the FASC. In this unique CPCC@CuO@Mn(OH)(2) electrode material, the high theoretical specific capacity of CuO and Mn(OH)(2) brings superior energy storage properties. Meanwhile, as the shell part, the deposited Mn(OH)(2) layer and coated CuO layer work as both capacity contributors and substrate protectors, simultaneously maintaining the high capacitance and satisfactory flexibility of the electrodes. Therefore, the capacitance successfully achieves around 8140 mF cm(-2) under 0.5 mA cm(-2). Significantly, the assembled FASC (named as CPCC@CuO@Mn(OH)(2)//CC@AC) achieves a working voltage of up to 2.4 V. In the case of a high-power density close to 34.31 mW cm(-3), its energy density reaches around 6.29 mW h cm(-3). Moreover, the capacity holds 88.9% even after 10,000 cycles, showing its great application potential in the field of wearable electronics.

Metastable 1T′-phase transition metal dichalcogenides (1T′-TMDs) with semi-metallic natures have attracted increasing interest owing to their uniquely distorted structures and fascinating phase-dependent physicochemical properties. However, the synthesis of high-quality metastable 1T′-TMD crystals, especially for the group VIB TMDs, remains a challenge. Here, we report a general synthetic method for the large-scale preparation of metastable 1T′-phase group VIB TMDs, including WS2, WSe2, MoS2, MoSe2, WS2xSe2(1−x) and MoS2xSe2(1−x). We solve the crystal structures of 1T′-WS2, -WSe2, -MoS2 and -MoSe2 with single-crystal X-ray diffraction. The as-prepared 1T′-WS2 exhibits thickness-dependent intrinsic superconductivity, showing critical transition temperatures of 8.6 K for the thickness of 90.1 nm and 5.7 K for the single layer, which we attribute to the high intrinsic carrier concentration and the semi-metallic nature of 1T′-WS2. This synthesis method will allow a more systematic investigation of the intrinsic properties of metastable TMDs. A general method for the synthesis of high-purity crystals of metastable 1T′-phase transition metal dichalcogenides is reported, providing a source of phase-engineered materials that can be used to systematically explore their intrinsic properties.

Metallic nanostructures are commonly densely packed into a few packing variants with slightly different atomic packing factors. The structural aspects and physicochemical properties related with the vacancies in such nanostructures are rarely explored because of lack of an effective way to control the introduction of vacancy sites. Highly voided metallic nanostructures with ordered vacancies are however energetically high lying and very difficult to synthesize. Here, we report a chemical method for synthesis of hierarchical Rh nanostructures (Rh NSs) composed of ultrathin nanosheets, composed of hexagonal close-packed structure embedded with nanodomains that adopt a vacated Barlow packing with ordered vacancies. The obtained Rh NSs exhibit remarkably enhanced electrocatalytic activity and stability toward the hydrogen evolution reaction (HER) in alkaline media. Theoretical calculations reveal that the exceptional electrocatalytic performance of Rh NSs originates from their unique vacancy structures, which facilitate the adsorption and dissociation of H 2 O in the HER.

Electrochemical water splitting into hydrogen is a promising strategy for hydrogen production powered by solar energy. However, the cell voltage of an electrolyzer is still too high for practical application, which is mainly limited by the sluggish oxygen evolution reaction process. To this end, hybrid water electrolyzers have drawn tremendous attention. Herein, coaxial Ni/Ni3S2@N-doped nanofibers are directly grown on nickel foam (NF), which is highly active for hydrogen evolution reaction. Meanwhile, the Ni3S2@N-doped nanofibers on NF prepared in an Ar atmosphere display superior urea oxidation reaction performance to previously reported catalysts. The cell voltage is about 1.50 V in urea electrolysis to deliver a current density of 20 mA cm-2, lower than that of a traditional water electrolyzer (1.82 V). The current density is around 77% relative to its initial value of 20 mA cm-2 after 20 h, superior to Pt/C|Ir/C-based urea electrolysis (14%). It is found that the synergistic effect between metallic Ni and Ni3S2, as well as the interfacial effect between metal centers and N-doped carbon, favors the initial dissociation of H2O and the adsorption/desorption of H* with thermal neutral Gibbs free energy. Meanwhile, the in-situ generated NiOOH on the outer surface of Ni3S2 possessed lower electrochemical activation energy for urea decomposition. Meanwhile, the abundant oxygen vacancies in electrodes could expose more active sites for the adsorption of intermediates, including H* and OOH*. It is also found that the hierarchical nanostructure of densely packed nanowires provides ideal electronic and ionic transport paths for fast electrocatalytic kinetics. The present work indicated that the modulation of compositions and hierarchical nanostructure is effective to prepare efficient catalysts for H2 production via urea electrolysis.

We designed and controllably prepared ZnO/ZnFe2O4 with a novel Janus hollow nanofiber (ZnO/ZFO JHNF) structure as an efficient photocatalyst. First, Fe(NO3)(3)/Zn(NO3)(2)/PVP composite nanofibers were prepared by an electrospinning technique. Next, ZnO layers were layer by layer deposited on the above nanofibers via the atomic layer deposition (ALD) method, forming Fe(NO3)(3)/Zn(NO3)(2)/PVP@ZnO nanofibers. Then, ZnO/ZFO JHNFs with uniform heterostructural distributions were obtained after calcination. The ratio of ZnO to ZnFe2O4 in the Janus structure, which affected the internal electric field, could be controlled by adjusting the ALD cycle numbers of the ZnO layers. The Janus hollow structure could efficiently separate the photogenerated carriers, as well as the surface reduction and oxidation processes. For the degradation of methylene blue under visible light, the apparent first-order rate constant (k(app)) of the ZnO/ZFO JHNFs was about 2 and 17 times greater than those of electrospun ZnO/ZnFe2O4 nanofibers with randomly distributed heterojunctions and pure ZnFe2O4 hollow nanofibers (ZFO HNFs). The effect of the Janus heterojunctions was also experimentally studied by using Al2O3 as a barrier layer between ZnFe2O4 and ZnO, forming ZnO/Al2O3/ZnFe2O4 hollow nanofibers with a sandwich structure (ZnO/Al2O3/ZFO SHNFs). The k(app) of ZnO/Al2O3/ZFO SHNFs was only 1/12 that of ZnO/ZFO JHNFs and only slightly higher than that of ZFO HNFs, suggesting that the electron transfer process in the Janus heterojunction was the key for promoting the photocatalytic performance. Moreover, the ZnO/ZFO JHNFs could be easily separated under magnetic field after the photocatalytic tests due to the ferromagnetic property of ZnFe2O4. The ZnO/ZFO JHNFs with good solar light utilization and magnetically separable ability may be suitable for application prospects in the environmental restoration and energy conversion fields. Moreover, the oxide-based Janus heterojunctions may provide new ideas for designing novel photocatalysts with high efficiencies.

Hierarchically porous In2O3/In2S3 heterostructures with micro-meso-macropores were prepared via a novel polymer-assisted sol–gel freeze-drying route, combined with self-sacrificial sulfidation processing. The three-dimensional hierarchical porous structure (3DHPS) In2O3/In2S3 showed outstanding photocatalytic activity, and the photocatalytic rate constant (k) of the 3DHPS In2O3/In2S3 was 3.7 times larger than that of In2O3/In2S3 nanoparticles. Such efficient photocatalytic ability could be mainly ascribed to the following aspects: first, the formation of In2O3/In2S3 heterostructures inhibited the recombination of the photogenerated carriers; second, the hierarchically porous structure, acting as micronano reactors, could offer high surface area and numerous reactive sites; third, the 3D open scaffolds could increase the light-harvesting and facilitate mass transport of reactants. Moreover, due to their self-supported structures, the 3DHPS In2O3/In2S3 did not need to be separated for reuse. The micronano r...

The methodology employed here utilizes the sodium super ion conductor type sodium iron phosphate wrapped with conducting carbon network to generate a stable Fe3+ /Fe4+ redox   couple, thereby exhibiting higher operating voltage and energy density of sodium-ion batteries. This new class of sodium iron phosphate wrapped by carbon also displays a cycling stability with >96% capacity retention after 200 cycles.

Inspired by the multiple functions of natural multienzyme systems, a new kind of hybrid nanosheet is designed and synthesized, i.e., ultrasmall Au nanoparticles (NPs) grown on 2D metalloporphyrinic metal-organic framework (MOF) nanosheets. Since 2D metalloporphyrinic MOF nanosheets can act as the peroxidase mimics and Au NPs can serve as artificial glucose oxidase, the hybrid nanosheets are used to mimic the natural enzymes and catalyze the cascade reactions. Furthermore, the synthesized hybrid nanosheets are used to detect biomolecules, such as glucose. This study paves a new avenue to design nanomaterial-based biomimetic catalysts with multiple complex functions.

Inspired by the unique properties of ultrathin 2D nanomaterials and excellent catalytic activities of noble metal nanostructures for renewable fuel cells, a facile method is reported for the high‐yield synthesis of ultrathin 2D PdCu alloy nanosheets under mild conditions. Impressively, the obtained PdCu alloy nanosheet after being treated with ethylenediamine can be used as a highly efficient electrocatalyst for formic acid oxidation. The study implicates that the rational design and controlled synthesis of an ultrathin 2D noble metal alloy may open up new opportunities for enhancing catalytic activities of noble metal nanostructures.

Noble multimetallic nanomaterials, if only consisting of Au, Ag, Pt, and Pd, typically adopt the high-symmetry face-centered cubic (fcc) structure. Here for the first time, by using the 4H/fcc Au@Ag nanoribbons (NRBs) as seeds, we report the synthesis of 4H/fcc trimetallic Au@PdAg core-shell NRBs via the galvanic reaction method under ambient conditions. Moreover, this strategy can also be used to synthesize 4H/fcc trimetallic Au@PtAg and quatermetallic Au@PtPdAg core-shell NRBs. Impressively, for the first time, these alloy shells, i.e., PdAg, PtAg, and PtPdAg, epitaxially grown on the 4H/fcc Au core with novel 4H hexagonal phase were successfully synthesized. Remarkably, the obtained 4H/fcc Au@PdAg NRBs exhibit excellent electrocatalytic activity toward the hydrogen evolution reaction, which is even quite close to that of the commercial Pt black. We believe that our findings here may provide a novel strategy for the crystal-structure-controlled synthesis of advanced functional noble multimetallic nanomaterials with various promising applications.

Ultrathin Pd nanosheets (NSs) coated with submonolayered Ru, referred to as Pd@Ru NSs, are synthesized via a seed-mediated growth method. The underpotential deposition can be the driving force for the formation of Pd@Ru NSs. The Pd@Ru NSs exhibit superior catalytic properties in the reduction of 4-nitrophenol and the semihydrogenation of 1-octyne, compared to the pure Pd NSs and Ru NSs.