An Ultra-Flexible Sodium-Ion Full Cell with High Energy/Power Density and Unprecedented Structural Stability.

Futuristic wearable electronics desperately need power sources with similar flexibility and durability. In this regard, the authors, therefore, propose a scalable PAN-PMMA blend-derived electrospinning protocol to fabricate free-standing electrodes comprised of cobalt hexacyanoferrate nanocube cathode and tin metal organic framework-derived nanosphere anode, respectively, for flexible sodium-ion batteries. The resulting unique inter-networked nanofiber mesh offers several advantages such as robust structural stability towards repeated bending and twisting stresses along with appreciable electronic/ionic conductivity retention without any additional post-synthesis processing. The fabricated flexible sodium ion full cells deliver a high working voltage of 3.0 V, an energy density of 273 Wh·kg-1 , and a power density of 2.36 kW·kg-1 . The full cells retain up to 86.73% of the initial capacity after 1000 cycles at a 1.0 C rate. After intensive flexibility tests, the full cells also retain 78.26% and 90.78% of the initial capacity after 1000 bending and twisting cycles (5 mm radius bending and 40o axial twisting), respectively. This work proves that the proposed approach can also be employed to construct similar robust, free-standing nanofiber mesh-based electrodes for mass-producible, ultra-flexible, and durable sodium ion full cells with commercial viability.

Triphasic Ni2P-Ni12P5-Ru with Amorphous Interface Engineering Promoted by Co Nano-Surface for Efficient Water Splitting.

This research designs a triphasic Ni2P-Ni12P5-Ru heterostructure with amorphous interface engineering strongly coupled by a cobalt nano-surface (Co@NimPn-Ru) to form a hierarchical 3D interconnected architecture. The Co@NimPn-Ru material promotes unique reactivities toward hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in alkaline media. The material delivers an overpotential of 30 mV for HER at 10 mA cm-2 and 320 mV for OER at 50 mA cm-2 in freshwater. The electrolyzer cell derived from Co@NimPn-Ru(+,-) requires a small cell voltage of only 1.43 V in alkaline freshwater or 1.44 V in natural seawater to produce 10 mA cm-2 at a working temperature of 80 °C, along with high performance retention after 76 h. The solar energy-powered electrolyzer system also shows a prospective solar-to-hydrogen conversion efficiency and sufficient durability, confirming its good potential for economic and sustainable hydrogen production. The results are ascribed to the synergistic effects by an exclusive combination of multi-phasic crystalline Ni2P, Ni12P5, and Ru clusters in presence of amorphous phosphate interface attached onto cobalt nano-surface, thereby producing rich exposed active sites with optimized free energy and multi open channels for rapid charge transfer and ion diffusion to promote the reaction kinetics.

Ru Single Atom Dispersed on MoS2/MXene for Enhanced Sulfur Reduction Reaction in Lithium-Sulfur Batteries.

The high theoretical energy density (2600 Wh kg-1) and low cost of lithium-sulfur batteries (LSBs) make them an ideal alternative for the next-generation energy storage system. Nevertheless, severe capacity degradation and low sulfur utilization resulting from shuttle effect hinder their commercialization. Herein, Single-atom Ru-doped 1T/2H MoS2 with enriched defects decorates V2C MXene (Ru-MoS2/MXene) produced by a new phase-engineering strategy employed as sulfur host to promote polysulfide adsorption and conversion reaction kinetics. The Ru single atom-doped adjusts the chemical environment of the MoS2/MXene to anchor polysulfide and acts as an efficient center to motivate the redox reaction. In addition, the rich defects of the MoS2 and ternary boundary among 1T/2H MoS2 and V2C accelerate the charge transfer and ion movements for the reaction. As expected, the Ru-MoS2/MXene/S cathode-based cell exhibits a high-rate capability of 684.3 mAh g-1 at 6 C. After 1000 cycles, the Ru-MoS2/MXene/S cell maintains an excellent cycling stability of 696 mAh g-1 at 2 C with a capacity degradation as low as 0.02% per cycle. Despite a high sulfur loading of 9.5 mg cm-2 and a lean electrolyte-to-sulfur ratio of 4.3, the cell achieves a high discharge capacity of 726 mAh g-1.

A Flexible and Transparent Zinc-Nanofiber Network Electrode for Wearable Electrochromic, Rechargeable Zn-Ion Battery.

The flexible electrochromic Zn-ion battery (FE-ZiB), a newly born energy-storage technology having both electrochromic characteristics and energy-storage capability in a single device, will be a promising technology for the future transparent wearable electronics. However, the current technology limits the fabrication of FE-ZIB because the zinc (Zn) anode material is opaque and rigid. The development of a flexible and transparent Zn anode is the key factor to overcoming the current limitation. Here, for the first time, a flexible, transparent zinc-nanofiber network anode electrode (Zn@Ni@AgNFs) is reported for an FE-ZiB device that yields a remarkable electrochemical performance of a high areal capacity of 174.82 mA h m2 at 0.013 mA cm-2 applied current density, high optical contrast (50%), and excellent mechanical flexibility. The fabricated FE-ZiB device also exhibits a high volumetric energy density of 378.8 W h m-3 at a power density of 562.7 W m-3 . Besides, the FE-ZiB demonstrates excellent electrochromic capability with a reversible color transition from a transparent in a discharged state (0.3 V) to a dark bluish-violet in a charged state (1.6 V). These results highlight a new pathway for the development of transparent batteries for smart wearable electronic devices.

Highly Effective Freshwater and Seawater Electrolysis Enabled by Atomic Rh-Modulated Co-CoO Lateral Heterostructures.

Atomic metal-modulated heterostructures have been evidenced as an exciting solution to develop high-performance multifunctional electrocatalyst toward water splitting. In this research, a catalyst of continuous cobalt-cobalt oxide (Co-CoO) lateral heterostructures implanted with well-dispersed rhodium (Rh) atoms and shelled over conductive porous 1D copper (Cu) nano-supports for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in both freshwater and seawater under alkaline condition is proposed. It is found that synergistic effects coming from uniform Rh atoms at doping level and Co-CoO heterostructures afford rich multi-integrated active sites and excellent charge transfer, thereby effectively promoting both HER and OER activities. The material requires overpotentials of 107.3 and 137.7 mV for HER and 277.7 and 260 mV for OER to reach an output of 10 mA cm-1 in freshwater and mimic seawater, respectively, surpassing earlier reported catalysts. Compared to a benchmark a Pt/C//RuO2 -based two-electrode electrolyzer, a device derived from the 1D-Cu@Co-CoO/Rh on copper foam delivers comparable cell voltages of 1.62, 1.60, and 1.70 V at 10 mA cm-2 in freshwater, mimic seawater, and natural seawater, respectively, together with robust stability. These results evidence that 1D-Cu@Co-CoO/Rh is a promising catalyst for green hydrogen generation via freshwater and seawater electrolysis applications.

Realizing the Tailored Catalytic Performances on Atomic Pt-Promoted Transition Metal Moieties Implanted Layered Double Hydroxides for Water Electrolysis.

High-performance production of green hydrogen gas is necessary to develop renewable energy generation technology and to safeguard the living environment. This study reports a controllable engineering approach to tailor the structure of nickel-layered double hydroxides via doped and absorbed platinum single atoms (PtSA) promoted by low electronegative transition metal (Mn, Fe) moieties (PtSA-Mn,Fe-Ni LDHs). We explore that the electron donation from neighboring transition metal moieties results in the well-adjusted d-band center with the low valence states of PtSA(doped) and PtSA(ads.), thus optimizing adsorption energy to effectively accelerate the H2 release. Meanwhile, a tailored local chemical environment on transition metal centers with unique charge redistribution and high valence states functions as the main center for H2O catalytic dissociation into oxygen. Therefore, the PtSA-Mn,Fe-Ni LDH material possesses a small overpotential of 42 and 288 mV to reach 10 mA·cm-2 for hydrogen and oxygen evolution, respectively, superior to most reported LDH-based catalysts. Additionally, the mass activity of PtSA-Mn,Fe-Ni LDHs proves to be 15.45 times higher than that of commercial Pt-C. The anion exchange membrane electrolyzer stack of PtSA-Mn,Fe-Ni LDHs(+,-) delivers a cell voltage of 1.79 V at 0.5 A·cm-2 and excellent durability over 600 h. This study presents a promising electrocatalyst for a practical water splitting process.

Encryptable Electrochromic Smart Windows: Uniaxially Oriented and Polymerized Hierarchical Nanostructures Constructed by Self-Assembly of Tetrathiafulvalene-Based Reactive Mesogens.

Tetrathiafulvalene (TTF)-based reactive mesogens (TTF-E and TTF-T) are synthesized, self-assembled, uniaxially oriented, and polymerized for the development of encryptable electrochromic smart windows. Electrochemical and spectroscopic experiments prove that the self-assembled TTF mixture (TTFM, TTF-E:TTF-T = 1:1) can reversibly switch the absorption wavelength of the TTF chromophore according to the redox reactions. Based on the identification of the phase transition and crystallographic structure, uniaxially oriented hierarchical nanostructures are easily constructed on the macroscopic area by simple coating and a self-assembly process. Subsequent polymerization of hierarchical nanostructures of TTFM significantly enhances thermal and mechanical stabilities and makes it possible for them to be fabricated as an electrochromic device. The angularly dependent correlation between the anisotropy of mesogens and the linearly polarized light allow us to demonstrate TTFM as smart windows capable of various optical security applications, including privacy protection and information encryption.

Mismatch Repair Deficiency and Lynch Syndrome Among Adult Patients With Glioma.

PURPOSE: The Lynch syndrome (LS)-glioma association is poorly documented. As for mismatch repair deficiency (MMRd) in glioma, a hallmark of LS-associated tumors, there are only limited data available. We determined MMRd and LS prevalence in a large series of unselected gliomas, and explored the associated characteristics. Both have major implications in terms of treatment, screening, and prevention. METHODS: Somatic next-generation sequencing was performed on 1,225 treatment-naive adult gliomas referred between 2017 and June 2022. For gliomas with ≥1 MMR pathogenic variant (PV), MMR immunohistochemistry (IHC) was done. Gliomas with ≥1 PV and protein expression loss were considered MMRd. Eligible patients had germline testing. To further explore MMRd specifically in glioblastomas, isocitrate dehydrogenase (IDH)-wild type (wt), we performed IHC, and complementary sequencing when indicated, in a series of tumors diagnosed over the 2007-2021 period. RESULTS: Nine gliomas were MMRd (9/1,225; 0.73%). Age at glioma diagnosis was <50 years for all but one case. Eight were glioblastomas, IDH-wt, and one was an astrocytoma, IDH-mutant. ATRX (n = 5) and TP53 (n = 8) PV were common. There was no TERT promoter PV or EGFR amplification. LS prevalence was 5/1,225 (0.41%). One 77-year-old patient was a known LS case. Four cases had a novel LS diagnosis, with germline PV in MSH2 (n = 3) and MLH1 (n = 1). One additional patient had PMS2-associated constitutional mismatch repair deficiency. Germline testing was negative in three MSH6-deficient tumors. In the second series of glioblastomas, IDH-wt, MMRd prevalence was 12.5% in the <40-year age group, 2.6% in the 40-49 year age group, and 1.6% the ≥50 year age group. CONCLUSION: Screening for MMRd and LS should be systematic in glioblastomas, IDH-wt, diagnosed under age 50 years.

Efficient synergism of NiO-NiSe2 nanosheet-based heterostructures shelled titanium nitride array for robust overall water splitting.

Water splitting via the use of an efficient catalyst is a clean and cost-effective approach to produce green hydrogen. In this study, we successfully developed a novel hybrid coming from thin NiO-NiSe2 nanosheet-based heterostructure shelled high-conductive titanium nitride nanoarrays (TiN@NiO-NiSe2) supported on carbon cloth (CC) via an optimized in-situ synthesis strategy. The hybrid possesses unique physicochemical properties due to the combination of merits from individual components and their synergistic effects, thereby boosting number and type of electroactive sites, reasonably adjusting Gibbs free adsorption energy, and promoting charge/mass transfers. As a potential bifunctional electrocatalyst, the hybrid requires low overpotentials of 115 and 240 mV to reach a current response of 10 mA cm-2 towards hydrogen evolution reaction and oxygen evolution reaction in 1.0 M KOH, respectively. Therefore, an electrolyzer of the TiN@NiO-NiSe2 on CC exhibits a low operation voltage of 1.57 V at 10 mA cm-2 together with a prospective durability, which exceed behaviors of Pt/C//RuO2 as well as recently reported bifunctional electrocatalysts. The results suggest a promising approach for developing cost-effective catalyst towards green hydrogen production via water splitting.

Cobalt-doped cerium oxide nanocrystals shelled 1D SnO2 structures for highly sensitive and selective xanthine detection in biofluids.

In this study, we prepared a three-dimensional self-supported electrocatalyst based on a thin layer of cerium oxide nanocrystals doped with cobalt heteroatoms (CeO2-Co) and then uniformly shelled over one-dimensional tin oxide (SnO2) nanorods supported by carbon cloth substrate. The material was used as a binder-free sensor that could nonenzymatically detect xanthine (XA) with an excellent sensitivity of 3.56 µA µM-1, wide linear range of 25 nM to 55 µM, low detection limit of 58 nM, and good selectivity. A screen-printed electrode based on the material accurately detected XA in food samples as well. The achievements were resulted from synergistic effects coming from the unique core@shell formation and Co-doping strategy, which efficiently modified electronic structure of the material to expose more electroactive site numbers/types and fast charge transfer, thereby producing intrinsic catalytic properties for XA oxidation. These results suggested that the SnO2@CeO2-Co is potential for developing efficient sensor to detect XA with good sensitivity and accuracy in food-quality monitoring.

Worm-like gold nanowires assembled carbon nanofibers-CVD graphene hybrid as sensitive and selective sensor for nitrite detection.

The development of a rapid, selective, and sensitive sensor to precisely monitor nitrite oxidation is of growing importance, given the strong interest in the protection of drinking water quality, treatment of wastewater, food production, and control of remediation processes. In this research, we successfully fabricated a hybrid originated from worm-like gold nanowires (Au WNWs) assembled on a high-quality carbon nanofibers-graphene (CNFs-Gr) hybrid network through a facile synthesis method. The hybrid as a binder-free sensor exhibited excellent activity towards nitrite detection in phosphate buffer solution (pH of 7.4) with a wide linear detection range of (1.98 µM - 3.77 mM), excellent sensitivity of 836 µA cm-2 mM-1, low detection limit of 1.24 µM, and long-term durability. The results were attributed to a special synergistic effect originating from unique hybridization of Au WNWs with large-area CNFs-Gr network to produce more electroactive sites and excellent conductivity, favorably boosting catalytic performance of the sensor. The successful fabrication of Au WNWs/CNFs-Gr suggested an interesting candidate for practically determining low-level nitrite in analytical applications.

Thermal Energy Harvest and Reutilization by the Combination of Thermal Conducting Reactive Mesogens and Heat-Storage Mesogens.

Utilizing a newly programmed and synthesized heat storage mesogen (HSM) and reactive mesogen (RM), advanced heat managing polymer alloys that exhibit high thermal conductivity, high latent heat, and phase transition at high temperatures were developed for use as smart thermal energy harvesting and reutilization materials. The RM in the heat-managing RM-HSM polymer alloy was polymerized to form a robust polymeric network with high thermal conductivity. The phase-separated HSM domains between RM polymeric networks absorbed and released a lot of thermal energy in response to changes in the surrounding temperature. For the fabrication of smart heat-managing RM-HSM polymer alloys, the composition and polymerization temperature were optimized based on the constructed phase diagram and thermal energy managing properties of the RM-HSM mixture. From morphological investigation and thermal analysis, it was realized that the heat storage capacity of polymer alloys depends on the size of the phase-separated HSM domain. The structure-morphology-property relationship of the heat managing polymer alloys was built based on the combined techniques of thermal, scattering, and morphological analysis. The newly developed mesogen-based polymer alloys can be used as smart thermal energy-harvesting and reutilization materials.

Development of Diketopyrrolopyrrole-Based Smart Inks by Substituting Ionic Pendants and Engineering Molecular Packing Structures.

A series of diketopyrrolopyrrole (DPP) luminogen amphiphiles were newly designed and synthesized by a single-step anionic exchange reaction for controlling the photoluminescence properties in both solution and solid states. Multicolor emission in response to thermal, mechanical, and chemical stimuli was successfully demonstrated by engineering well-defined supramolecular assemblies. Phase transformation from the metastable amorphous solid to the stable orthorhombic crystal of [DP-Im][Br] provided the reversibly patternable light emission. Self-organization into the smectic crystalline phase of [DP-Im][TFSI] allowed us to show the linearly polarized light emission. By simultaneously applying [DP-Im][Br] and [DP-Im][TFSI], we demonstrated the fabrication of smart sensors for packaging of food or vaccines that can detect thermal attacks.

Bifunctional Catalyst Derived from Sulfur-Doped VMoOx Nanolayer Shelled Co Nanosheets for Efficient Water Splitting.

A novel sulfur-doped vanadium-molybdenum oxide nanolayer shelling over two-dimensional cobalt nanosheets (2D Co@S-VMoOx NSs) was synthesized via a facile approach. The formation of such a unique 2D core@shell structure together with unusual sulfur doping effect increased the electrochemically active surface area and provided excellent electric conductivity, thereby boosting the activities for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). As a result, only low overpotentials of 73 and 274 mV were required to achieve a current response of 10 mA cm-2 toward HER and OER, respectively. Using the 2D Co@S-VMoOx NSs on nickel foam as both cathode and anode electrode, the fabricated electrolyzer showed superior performance with a small cell voltage of 1.55 V at 10 mA cm-2 and excellent stability. These results suggested that the 2D Co@S-VMoOx NSs material might be a potential bifunctional catalyst for green hydrogen production via electrochemical water splitting.

Transfer and Amplification of Iodine-Based Diacetylene Amphiphiles to Anisotropic Optical Properties by Uniaxial Orientation in Thin Films.

For flexible displays, there is a desperate need for a broadband coatable polarizer that can absorb light in a specific direction. Conventional polarizers fabricated by the polymer stretching process are too thick (50-200 µm) to be used as polarizers that can be applied to antireflective films in flexible displays. For the development of the broadband coatable thin film polarizer, diacetylene (DA) amphiphiles containing I- or I3- are newly designed and synthesized, and the content of DA amphiphiles in the 4,6-decadiyne solvent is optimized to form a lyotropic liquid crystal (LLC) phase. Topochemical polymerization of uniaxially oriented iodine-based DA not only stabilizes the film but also broadens the polarization light region from 350 to 700 nm. The transfer and amplification of iodine and DA functions in uniaxially oriented thin films enable the fabrication of broadband coatable thin film polarizers.

Mesoporous layered spinel zinc manganese oxide nanocrystals stabilized nitrogen-doped graphene as an effective catalyst for oxygen reduction reaction.

The design of low-cost, highly efficient, and the durable catalyst is essential to replace commercial platinum metal-based catalysts for the oxygen reduction reaction (ORR) in fuel cell applications. Herein, a novel mesoporous hybrid based on nitrogen-doped graphene nanosheets-stabilized layered spinel zinc manganese oxide (Zn2Mn3O8-NG) is successfully engineered and applied as an effective catalyst to accelerate the ORR process in alkaline medium. Electrochemical performance analysis of this catalyst shows excellent catalytic activity with high current density, positive onset potential (-0.013 V), and positive half-wave potential (-0.12 V), which are relative to the commercial Pt/C in 0.1 M KOH electrolyte. The kinetic study of the synthesized catalyst towards ORR demonstrates a direct 4e- transfer pathway. The methanol tolerance and long-term stability test suggest its superior behavior to Pt/C. The excellent performance of the Zn2Mn3O8-NG is attributed to the synergistic effects of nanosized Zn2Mn3O8 nanocrystals and NG nanosheets, which effectively improve the electroactive surface area, conductivity, diffusion channels, and mass transfer ability. This result suggests that the resulting catalyst could be used as a potential alternative of Pt-based catalysts towards ORR application.

Hierarchical Cu@CuxO nanowires arrays-coated gold nanodots as a highly sensitive self-supported electrocatalyst for L-cysteine oxidation.

The sensitivity, selectivity, and stability of an electrochemical sensor for detecting small biomolecules can be significantly upgraded through properly controlling the morphology and chemical structure of electrocatalyst. Herein, we fabricated a unique hierarchical nanostructure based on Cu@CuxO nanowires (NWs) array uniformly depositing with a layer of gold nanoparticles (2-3 nm) through a simple electroless deposition process. The Au-Cu@CuxO NWs hybrid was successfully applied as a novel binder-free self-supported biosensor towards L-cysteine detection with low limit of detection (1.25 µM), wide linear detection range (1.25 µM-1.94 mM), long-term stability (four weeks), and excellent selectivity. In addition, the hybrid-based sensor accurately detected L-cysteine in real samples. It was found that the obtained nanostructure with the formation of strong interaction between Au and Cu phase produces synergistic effects, which improve exposed electroactive site number, accelerate charge transfer rate, and increase surface area, thereby boosting the sensing performance. The results open a potential way to develop electrochemical sensor for efficiently detecting not only L-cysteine but also other small molecules with high sensitivity, accuracy, stability, and cost-effectiveness in health care and disease diagnosis.

Cu-Au nanocrystals functionalized carbon nanotube arrays vertically grown on carbon spheres for highly sensitive detecting cancer biomarker.

A three-dimensional hierarchical nanohybrid based on Cu-Au bimetallic nanocrystals integrated carbon nanotube arrays vertically grown on carbon spheres was successfully developed as an active platform for sensing application. Such nanohybrid can provide abundant active sites and act as an exceptional platform for immobilizing highly dense and well-dispersed carcinoembryonic antibody (anti-CEA) to sensitively detect CEA, an emerging biomarker of various cancer diseases. Due to the unique nanoarchitecture with altered electronic structure of Cu-Au bimetallic catalyst and enhanced interactions between components, such nanohybrid based biosensor demonstrated excellent electrochemical performance towards CEA detection with great sensitivity, wide linear detection range (0.025-25 ng/mL), very low limit of detection (0.5 pg/mL), and good selectivity. The results imply that this sensor has great potential to offer essential information for cancer diagnosis and management with great clinical importance.

Nitrogen-Doped Graphene-Encapsulated Nickel Cobalt Nitride as a Highly Sensitive and Selective Electrode for Glucose and Hydrogen Peroxide Sensing Applications.

To explore a natural nonenzymatic electrode catalyst for highly sensitive and selective molecular detection for targeting biomolecules is a very challenging task. Metal nitrides have attracted huge interest as promising electrodes for glucose and hydrogen peroxide (H2O2) sensing applications due to their exceptional redox properties, superior electrical conductivity, and superb mechanical strength. However, the deprived electrochemical stability extremely limits the commercialization opportunities. Herein, novel nitrogen-doped graphene-encapsulated nickel cobalt nitride (Ni xCo3- xN/NG) core-shell nanostructures with a controllable molar ratio of Ni/Co are successfully fabricated and employed as highly sensitive and selective electrodes for glucose and H2O2 sensing applications. The highly sensitive and selective properties of the optimized core-shell NiCo2N/NG electrode are because of the high synergistic effect of the NiCo2N core and the NG shell, as evidenced by a superior glucose sensing performance with a short response time of <3 s, a wide linear range from 2.008 µM to 7.15 mM, an excellent sensitivity of 1803 µA mM-1 cm-2, and a low detection limit of 50 nM (S/N = 3). Furthermore, the core-shell NiCo2N/NG electrode shows excellent H2O2 sensing performances with a short response time of ∼3 s, a wide detection range of 200 nM to 3.4985 mM, a high sensitivity of 2848.73 µA mM-1 cm-2, and ultra-low limit detection of 200 nM (S/N = 3). The NiCo2N/NG sensor can also be employed for glucose and H2O2 detection in human blood serum, promising its application toward the determination of glucose and H2O2 in real samples.