Ultrahigh Stability Research Articles

Engineering potassium-ion battery anodes with ultra-high structural stability and their potassium storage mechanism

Engineering potassium-ion battery anodes with ultra-high structural stability and their potassium storage mechanism

Improving the near-infrared luminescence of Ca3MgSnGe3O12:Cr3+ using cation modulation and energy transfer for night-vision and nondestructive testing.

A series of Ca3Mg1-x Sr x SnGe3O12:0.05Cr3+ (x = 0.005-0.3) phosphors were synthesized in this study; varying the Cr3+-ion crystal-field strength through Sr2+-concentration variation resulted in a luminescence-center redshift. Nd3+-ion co-doping resulted in a broad-spectrum emissive material with a 468 nm excitation wavelength, expanded full width at half maximum (FWHM) (195 nm), Cr-Nd energy transfer, and an ultra-high temperature stability (99.59% at 423 K). Combining Ca3Mg0.7Sr0.3SnGe3O12:0.05Cr3+, 0.05Nd3+ with blue LED chips resulted in near-infrared (NIR) phosphor-converted light-emitting diodes (pc-LEDs) for night-vision and nondestructive testing applications. This study reports what we believe is a novel method for designing NIR light-emitting materials with excellent luminescence properties that could guide future research on NIR phosphors with widespread applicability.

Thiol-Ene Click Chemistry: A General Strategy for Tuning the Properties of Vinylene-Linked Covalent Organic Frameworks.

Vinylene-linked Covalent Organic Frameworks (V-2D-COFs) are a class of promising porous organic materials that feature fully π-conjugated structures, high crystallinity, ultrahigh chemical stability, and extraordinary optoelectronic properties. However, the types of reactions and the availability of monomers for synthesizing sp2-c linked COFs are considerably limited by the irreversibility of the C═C bond, and the complete π-conjugated structure restricts their in-depth research in hydrophilicity, membrane materials, and proton conductivity. Postsynthetic modification (PSM), which can avoid these problems by incorporating functional moieties into the predetermined framework, provides an alternative way to construct diverse V-2D-COFs. Herein, we report a general strategy to introduce C-C, C-S-C, and functional groups into sp2-c-COFs via the thiol-ene click reaction. To demonstrate the universality of this approach, we synthesized two sp2-c COFs (COF-CN and COF-1), and subsequently introduced six different types of thiol compounds at their skeletal C═C sites. The quantitative yield was confirmed by X-ray Photoelectron Spectroscopy (XPS) and cross-polarization magic angle spinning 13C NMR spectroscopy. This thiol-ene click modification of vinylene-linked COFs at skeletal C═C sites allows for flexible structural design, providing these COFs with new linkages (C-C and C-S-C) that are otherwise difficult to produce directly. Thus, it facilitates precise modulation of their properties, such as photophysical properties, hydrophilicity, and proton conductivity, promising a diverse range of compelling applications for the future.

Construction of core-shell NiFe LDH/Co(OH)F amorphous/crystalline heterostructure for synergistically enhanced electrocatalytic water oxidation

The development of high performance non-precious transition metal electrocatalysts for the oxygen evolution reaction (OER) is essential for the practical application of electrocatalytic water splitting. A promising strategy to prepare highly efficient and stable electrocatalysts for the OER can be achieved by constructing heterointerfaces between the amorphous and crystalline phases. Herein, a novel three-dimensional (3D) core-shell structured NiFe-LDH/Co(OH)F electrocatalyst on nickel foam (NF) with an amorphous/crystalline interface was achieved by growing 2D amorphous NiFe LDH nanosheets onto 1D crystalline Co(OH)F nanorod arrays using a simple two-step hydrothermal method. The resulting NiFe LDH/Co(OH)F/NF electrode exhibits outstanding electrochemical OER performance with an overpotential of 202 and 260mV at the current density of 10 and 100mAcm-2, a Tafel slope of 44.06mV dec-1, and an ultra-high stability over 100h at 300mAcm-2 without obvious degradation in 1M KOH. This research affords a new way to construct high-performance 3D hierarchical non-noble metal electrocatalysts for OER.

Modulating the electron spin states of Na2FePO4F cathode via high entropy strategy for enhanced sodium storage and ultra-high cycling stability

Modulating the electron spin states of Na2FePO4F cathode via high entropy strategy for enhanced sodium storage and ultra-high cycling stability

Dually encapsulated LiMn0.6Fe0.4PO4 architecture with MXenes and amorphous carbon to achieve high-performance and ultra-stable lithium batteries

An LMFP@MXene@C cathode material was fabricated by electrostatic adsorption and in situ graphitization, providing optimized Li+ transmission and a stable structure featuring ultrahigh average capacity and cycle stability.

Transformation of vulnerable imine bond into aromatic in 3D COF for ultrastable lithium-ion batteries

About half of the thus far reported covalent organic frameworks (COFs) are of imine-linked 2D and 3D structures, which usually suffer from relatively low working stability due to the vulnerable easily nucleophile-attacked C=N bond nature. Herein, an imine-linked 3D COF, TAM-DMPZD-COF, was constructed by reaction between 4-connected Td 4,4′,4′',4′''-methanetetrayltetraaniline and 2-connected 5,10-methyl-5,10-dihydrophenazine-2,7-dicarbaldehyde. Addition of S8 into the above mentioned reaction leads to the transformation of imine bond into an aromatic thiazole moiety in the framework, affording the thiazole-linked 3D COF, TAM-DMPZD-COF-S. This result in significant enhancement over the ultrahigh cycling stability of the TAM-DMPZD-COF-S-based LIBs cathode, with the thus far reported highest 50000 cycles and 0.00016% capacity decay per cycle at 10 A g-1, in good contrast to only 55% capacity retention after 5000 cycles at 10 A g-1 for TAM-DMPZD-COF-based LIBs cathode. Nevertheless, transformation of imine bond into an aromatic thiazole moiety in the 3D framework also induces an increase in the redox active sites for both Li+ and PF6- ions, resulting in enhanced ion storage capacity and energy density of TAM-DMPZD-COF-S (325 mA h g-1 and 736 W h kg−1 at 0.1 A g-1), surpassing those for traditional inorganic cathodes and all the thus far reported COFs-based electrodes.

Designing homochiral metal-organic frameworks with ultrahigh surface areas and stability for practical applications.

Designing homochiral metal-organic frameworks with ultrahigh surface areas and stability for practical applications.

Crafting the architecture of biomass-derived activated carbon via electrochemical insights for supercapacitors: a review.

Escalating energy demands have often ignited ground-breaking innovations in the current era of electrochemical energy storage systems. Supercapacitors (SCs) have emerged as frontrunners in this regard owing to their exclusive features such ultra-high cyclic stability, power density, and ability to be derived from sustainable sources. Despite their promising attributes, they typically fail in terms of energy density, which poses a significant hindrance to their widespread commercialization. Hence, researchers have been exploring different cutting-edge technologies to address these challenges. This review focuses on biomass-derived activated carbon (BDAC) as a promising material for SCs. Initially, the methodology and key factors involved in synthesising BDAC, including crafting the building blocks of SCs, is detailed. Further, various conventional and novel material characterization techniques are examined, highlighting important insights from different biomass sources. This comprehensive investigation seeks to deepen our understanding of the properties of materials and their significance in various applications. Next, the architectural concepts of SCs, including their construction and energy storage mechanisms, are highlighted. Finally, the translation of the unravelled BDAC metrics into promising SCs is reviewed with comprehensive device-level visualisations and quantifications of the electrochemical performance of SCs using various techniques, including cyclic voltammetry (CV), galvanostatic charge-discharge test (GCD), electrochemical impedance spectroscopy (EIS), cyclic tests (CT), voltage holding tests (VHT) and self-discharge tests (SDT). The review is concluded with a discussion that overviews peanut-shell-derived activated carbon as it is a common and promising source in our geographical setting. Overall, the review explores the current and futuristic pivotal roles of BDAC in the broad field of energy storage, especially in SC construction and commercialisation.

Synergistic enhancement of Ag/ZIF-67 cage@Mxene 3D heterogeneous structure for ultrahigh SERS sensitivity and stability

There is an urgent need in the field of in situ for rapid extraction and analysis of target molecules from irregular surfaces. The application of SERS technology is often limited...

DNA Origami-Templated Individual Gold Nanocluster: Probing The Photophysical Dynamics Using Single Molecule Fluorescence Spectroscopy

Single-molecule fluorescence microscopy demands ultrahigh stability of single fluorophore with less photobleaching and essentially no intensity fluctuations on experimentally relevant time scales. In this respect, there is a need to...

Electrochemical biosensor for detection of ampicillin in milk based on Au5Pt and DNA cycle dual-signal amplification strategy.

A biosensor is reportedfor electrochemical detection of ampicillin based on Au5Pt and DNA cycle dual-signal amplification strategy. Firstly, Au5Pt is prepared by reduction of chloroauric acid and chloroplatinic acid with serine-functionalized graphene quantum dot (SGQD). The resulting Au5Pt shows an excellent catalytic activity because of the synergy of Au and Pt. Then, Au5Pt is covalently combined with hairpin DNA and thionine molecule to form aredox probe. The probe was used for construction of theampicillin biosensor coupling with DNA cycling. In the presence of ampicillin, the DNA cycle was triggered and leads to many redox probes being carried to the biosensor. This produces a significant signal amplification by oxidation and reduction of thionine molecules in these probes. The combination of Au5Pt catalysis with DNA cycle achieve ultrahigh sensitivity, selectivity, and stability for the electrochemical detection of ampicillin. Differential pulse voltammetry current linearly increases with the increase of ampicillin concentration in the range 1 × 10-18-1 × 10-12M with a detection limit of 3.2 × 10-19M (S/N = 3). The proposed analytical method has been satisfactorily used for electrochemical detection of ampicillin in milk.

Iron complex with multiple negative charges ligand for ultrahigh stability and high energy density alkaline all-iron flow battery

Alkaline all-iron flow batteries (AIFBs) are highly attractive for large-scale and long-term energy storage due to the abundant availability of raw materials, low cost, inherent safety, and decoupling of capacity and power. However, a stable iron anolyte is still being explored to address complex decomposition, ligand crossover, and energy density to improve battery performance. Herein, a promising metal-organic complex, Fe(NTHPS), consisting of FeCl3 and 3,3',3''-nitrilotris(2-hydroxypropane-1-sulfonate) (NTHPS), is specifically designed for alkaline all-iron flow battery. The NTHPS exhibits strong binding strength with iron ions, resulting in ultrahigh stability during the charge-discharge process. AIFB based on the [Fe(CN)6]4- catholyte and Fe(NTHPS) showcases an exceptionally high capacity retention of 97.8% after 2000 cycles (0.0011% per cycle), maintaining high coulombic efficiency near 100%. Furthermore, with a solubility as high as 1.82 mol L-1, the Fe(NTHPS) anolyte demonstrates an ultra-high theoretical capacity of 47.23 Ah L-1. This multiple negative charges ligand not only resolves existing barrier associated with AIFBs, but also provides valuable insight for their commercial application.

Structural characterization of cage clusters assembled borophene and implication for cathode electrocatalysts in Li–O2 batteries

The successful fabrication of quasi-freestanding bilayer borophene in experiments, combined with its superior metallic character, has propelled it to a rising star among two-dimensional materials, making it highly promising for applications in micro-electronic devices. Using first-principles calculations, we comprehensively explore and characterize cage cluster assembled borophenes through various methods for experimental references. The simulated scanning tunneling microscope (STM) images under diverse bias voltages exhibit distinct morphologies and closely associated with the partial densities of states (PDOS) of the surface boron atoms. High-resolution and large-scale simulated transmission electron microscope (TEM) images are investigated to detect the internal crystal structures, facilitating better identification of non-monolayer borophenes. The partial densities of states, electronic localization functions and Mulliken bond populations have been calculated to analyze the differences of morphology in STM and TEM images. Furthermore, simulated X-ray diffraction (XRD), Raman, and infrared (IR) spectra are characterized to further assist in distinguishing the phases of borophene. In light of ultrahigh stability and excellent metallic character, cluster assembled borophene of P3¯m1 symmetry act as cathode materials of Li-O2 battery with lower overpotential in oxygen evolution reaction (OER) than oxygen reduction reaction (ORR) processes. The overpotential is closely related to the adsorption strength of LiO2 and Li2O2 intermediates on surface of boron sheets. These theoretical results offer crucial guidance for the experimental identification of borophenes and suggest that the new type of cluster assembled systems might be suitable for the cathode materials of future Li-O2 batteries.

Ingeniously controlling interface diffusion endows the Skutterudite thermoelectric device with ultra-high service stability

Building a barrier layer/thermoelectric material interface with high-bonding strength, low-contact resistivity, and high-thermal stability is a prerequisite for reliable applications of thermoelectric devices and is currently a bottleneck problem. Herein, we designed a unique Ni-Cr barrier layer with a narrow-channel structure for thermoelectric skutterudite (SKD) to ingeniously control the diffusion/reaction process of Sb and Ni (Co, Fe) at the interface, affecting the interfacial phase structure and then preventing the interface structural damage caused by thermal mismatch during thermal aging while ensuring strong metallurgical bonding. After enduring at 823 K for 70 days, the contact resistivities of Ni45Cr55/n-SKD and Ni75Cr25/p-SKD joints increase slowly and their bonding strengths remain stable, based on which the calculated annual attenuation rates of conversion efficiency and output power are both less than 2 %, reaching a leading level. The assembled 8-pair SKD module shows no performance degradation after 168-hour continuous service test with hot-side temperature of 823 K. This work not only strongly elevated the service stability of SKD device, but also opens the new horizon of designing barrier layers for other TE materials.

Machine Intelligence-Accelerated Optimization of All-Temperature Aqueous Electrolyte for Stable Zn-Ion Batteries

Rechargeable aqueous batteries are the leading candidate to meet the surging demand for safe and low-cost energy storage systems. To achieve their development, the optimization of aqueous electrolyte for wide electrochemical stability window (ESW) and stable electrolyte/electrode interfaces is crucial. However, the selection of salts and solvents is critical to dictate the ultimate performance of Zn-ion batteries. Conventional approach requires trial-and-error optimization experiments, which is time-consuming and laborious. Herein, we show an integrated workflow that combines robotics and machine learning to accelerate the optimization of all temperature stable aqueous electrolyte with programmable ESW, ionic conductivity, and electrolyte/electrode interface stability. First, an automated pipetting robot is commanded to prepare 557 electrolyte mixtures using 2 salts (ZnCl2 and Zn(OTf)2) and 2 solvents (water and methanol). After equilibration/stabilization at 30 °C, the solubility of the electrolyte mixtures is evaluated to train a support-vector machine classifier. Next, through active learning loops with data augmentation, 60 electrolyte solutions are prepared/evaluated, establishing an artificial neural network prediction model. The achieved model is capable of two main functions: (1) predicting the electrochemical performance of an electrolyte solution based on its formulation, and (2) conducting multi-objective optimization on electrolytes to identify stable electrolytes with high Coulombic efficiency, rate performance, and interfacial stability. The model-suggested electrolyte with wide ESW, high conductivity, and stable electrolyte/electrode interfaces deliver ultrahigh cyclic stability in Zn||Zn symmetric cells, as well as outstanding capacity retention, fast charge/discharge capability, and excellent efficiency in full cells. The fusion of robotics-accelerated experimentation, machine intelligence, and simulation tools facility the discovery of electrolytes that involve time-intensive experiments and multi-dimensional design spaces.

High Performance and Durable Electrochromic Device of Fe(II)-Based Metallo-Supramolecular Polymer for Smart Electrochromic Window Application

A durable semi-solid-state electrochromic device (ECD) of Fe(II)-based metallo-supramolecular polymer (polyFe) was fabricated by incorporating Nickel hexacyanoferrate (NiHCF) as a charge-balancing layer. The ECD exhibited reversible blue-violet to bleached optical transition in a very low potential window of +1.2V to +0.2V. The low operating potential window enabled ultra-high cycle stability and improved optical memory of the ECD. For the further improvement of the EC properties, it was revealed that the optimization of the film thickness of the polyFe and NiHCF is critical to maintaining the charge balance between the working and counter electrodes. At last, the cyclic stability for the repeated color changes over 100,000 cycles were achieved. This finding will help engineers and scientists to fabricate a low-voltage-driven, long-lasting ECD for real-life application in smart electrochromic window technology.

Utilizing a High-Efficiency and Durable Electrocatalyst on GaAs for PEC Water Oxidation

Gallium arsenide (GaAs) semiconductor photoanode has been the subject of extensive research due to its promising potential for photoelectrochemical water splitting. However, GaAs photoanodes have been severely limited by stability issues, including photocorrosion, light-induced degradation, and oxidation. The oxidation of GaAs can lead to the formation of surface defects, which reduce the photocurrent generation. Herein, we investigate the effects of surface modification of GaAs photoanodes with electrocatalysts consisting small amount of Pt@NiOOH and their mixture, on the PEC oxygen evolution reaction (OER) performance. Among the pristine samples, Pt@NiOOH-modified GaAs photoanodes showed the lowest onset potential for PEC water oxidation. Here, we demonstrate Pt@NiOOH/GaAs photoanodes can exhibit an ultrahigh stability of 200 h at a large photocurrent density (>25 mA cm-2) in 3-electrode configuration under AM 1.5G one-sun illumination and further provide extremely robust protection for the GaAs surface for over time without any performance degradation, i.e., without any loss of photocurrent, onset potential, or efficiency.

Ultrahigh temperature stability in heterovalent-ion doped PZT ceramics

We achieved ultrahigh temperature stability of the piezoelectric coefficient d33 by doping heterovalent ions in the PbZr0.54Ti0.46O3 ceramics at the A/B sites in the ABO3 lattice. The Sm3+-ion amount at the A-site remains constant, while the Ta5+-ion amount at the B-site changes. We utilized electron paramagnetic resonance (EPR) and X-ray photoelectron spectroscopy (XPS) to investigate the reduction of oxygen vacancies, which are closely associated with the defect dipoles formed by heterovalent doping. We utilized piezoresponse force microscopy (PFM), temperature-dependent X-ray diffraction (XRD) combined with Rietveld refinement, and temperature-dependent Raman spectroscopy to understand the mechanism of the temperature stability of the piezoelectric coefficient d33. When x = 0.01, the performance of xTa-0.01Sm-PbZr0.54Ti0.46O3 ceramic is optimal: d33 = 530 pC/N, electromechanical coupling factor kp = 0.72, Curie temperature TC = 343 °C, where the temperature stability of the piezoelectric coefficient is ultrahigh, and the d33 changes only 2.2 % over the 25–200 °C temperature range.

Efficient CO2 capture by ZIF-8-derived in-situ nitrogen-doped nanoporous carbon with ultra-high selectivity and stability

Global warming and the increasing frequency of extreme weather caused by the gradual increase in CO2 concentration in the atmosphere are urgent issues that must be addressed. In this study, ZIF-8-derived in-situ nitrogen-doped porous carbon materials were prepared through one-step pyrolysis of ZIF-8. The synthesis was gradually optimized by exploring different pyrolysis temperatures to determine the optimal ZIF-8-derived porous carbon for CO2 adsorption. The CO2-adsorption capacity of ZIF-8–800 reached 5.22 and 6.19 mmol g−1 at 25 ℃ and 0 ℃ (1 bar), respectively. After five cycles, its CO2-adsorption capacity decreased by only about 1.7 %. Moreover, the CO2/N2 selectivity at 1 bar was as high as 21.2 (48.9 at 0.05 bar), and the isothermal adsorption heat was also within a moderate range (31 kJ mol−1). The superior CO2 adsorption performance was found to originate from the comprehensive effect of the three-dimensional pore structure that combined reasonably coordinated micropores, mesopores, and macropores, as well as some specific favorable N/O groups. The results indicate the broad application prospects of ZIF-8-Ts in CO2 capture and separation and provide new ideas for the sustainable application of novel MOF-derived porous carbon materials.