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At least 1,621 records · Page 90

Single-atom materials boosting wearable orthogonal uric acid detection

Abstract Uric acid (UA) is a vital biomarker for the diagnosis and management of various health conditions, including cardiovascular diseases, gout, kidney disorders, metabolic syndrome, and wound healing. Despite significant advances in wearable sensor technology, challenges persist in developing wearable sensors that are capable of maintaining high sensitivity, selectivity, and stability. In this study, we present an epidermal sensing platform enhanced with single-atom materials (SAMs) designed for flexible and orthogonal electrochemical detection of UA. We designed and synthesized an SAM with Fe-N 5 active sites to boost the electrochemical sensing signals, integrating it with laser-engraved graphene (LEG) to fabricate a wearable SAM-based UA patch sensor. This design provides superior UA detection performance compared to sensors based on conventional nanomaterials. In addition, we enhanced the detection accuracy and range by using an orthogonal approach that combines direct oxidation through differential pulse voltammetry (DPV) along with parallel biocatalytic amperometric detection. The resulting SAM-based UA orthogonal sensor patch demonstrated exceptional performance in wearable applications through tests measuring sweat UA levels in subjects before and after consuming a purine-rich diet. Graphical Abstract

Ding, Shichao↗

High temperature stabilization of ultrafine grain tungsten alloys through synergistic compositional complexities

Thermally-stabilized fine-grained microstructures in tungsten provide a pathway to harnessing enhanced properties such as a reduced ductile-to-brittle transition temperature and improved strength while mitigating the adverse effects of grain growth and recrystallization. Here, in this study, we employ a material design strategy that relies on grain boundary segregation in the nanocrystalline state driven by alloy thermodynamics balanced with impurity scavenging through in situ formation of kinetically-stabilizing metal carbides. A W-Ti-Cr alloy is designed through lattice Monte Carlo methods and subsequently synthesized in a single-phase nanocrystalline state, which upon annealing, evolves into an ultrafine grained microstructure containing chromium grain boundary segregation collectively with a dispersed TiX (X=C,O) phase through the reaction of titanium with carbon and oxygen impurities. In situ synchrotron X-ray diffraction experiments demonstrate that increased Ti promotes stabilization across a larger temperature range but with diminishing returns above 10 at.% Ti. Long-term stability was confirmed through the retention of the ultrafine grained microstructure for a total of 8 days (192 h) at 1300 °C without grain/carbide growth and/or recrystallization. Our results demonstrate that, through strategic tailoring of composition and microstructure, one can harness the benefits of both thermodynamic and kinetic stabilization mechanisms, opening pathways for future alloy formulations that expand the window of stability.

36 MATERIALS SCIENCE↗

A high-performance and durable direct NH 3 tubular protonic ceramic fuel cell integrated with an internal catalyst layer

Nickel-based cermet anode-supported protonic ceramic fuel cells (PCFCs) show great potential for direct utilization of ammonia. However, the insufficient activity of anode and the deterioration of anode activity/durability caused by the undesired interaction between nickel and ammonia greatly limit the application. Here, we report tubular PCFCs embedded with a catalytic iron layer. Such cells show peak power densities of 1.507 W cm -2 and 1.078 W cm -2 at 700 °C when using H 2 and NH 3 as fuel, respectively, which are the highest tubular PCFC performance so far ever reported. In addition, the stability of cells with the catalyst layer has been dramatically enhanced when compared with that of cells without the catalyst layer. As a result, the enhancement of activity and durability is attributed to the catalytic activity of iron for ammonia decomposition, through which the direct contact between nickel and ammonia has been minimized and the anode structure has therefore been protected.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Hybrid geothermal-wind integration in the US energy grid

Here, we combine US wind generation—a cheap yet intermittent source of electricity—with the latest geothermal resource estimates to understand the technoeconomic possibilities of pairing enhanced geothermal systems (EGSs) with existing wind farms to develop a hybrid energy system. Using observed generation data from 583 wind farms, generation gaps are quantified and geographically paired with the latest EGS estimates. Results demonstrate that EGS potential within a 1 km 2 footprint can supplement wind generation at 56% of onshore wind farms. Each wind farm can be supplemented by EGSs when 10% of its surface-occupying footprint is available. The cost of EGSs at wind farms is lowest in the western US and southern Texas border and highest in the central US. While further experiments are warranted, a wind + EGS hybrid system offers an opportunity to increase power output from the same land footprint while maximizing the use of existing electrical infrastructure.

EGS↗

GRIM-19 inhibits proliferation and induces apoptosis in a p53-dependent manner in colorectal cancer cells through the SIRT7/PCAF/MDM2 axis

Colorectal cancer (CRC) is the leading deadly cancer worldwide. Gene associated with retinoid-IFN-induced mortality-19 (GRIM-19), a novel tumor suppressor, has been reported to be expressed at low levels in human CRC. However, the role of GRIM-19 in CRC progression and the corresponding detailed mechanisms are unclear. The results of this study indicated that GRIM-19 expression is related to CRC progression. Overexpression of GRIM-19 was found to inhibit CRC cell proliferation and induce apoptosis in vitro and in vivo. Our results demonstrated that GRIM-19 suppresses CRC through posttranslational regulation of p53, in which SIRT7 is activated by GRIM-19 and triggers PCAF-mediated MDM2 ubiquitination, eventually stabilizing the p53 protein. We also observed that GRIM-19 enhances the effect of oxaliplatin against CRC. In conclusion, GRIM-19 plays an important role in CRC development and is a potential biomarker and therapeutic target for clinical treatment of CRC.

60 APPLIED LIFE SCIENCES↗

Element-Specific Study of Magnetic Anisotropy and Hardening in SmCo 5– x Cu x Thin Films

This work investigates the effect of copper substitution on the magnetic properties of SmCo 5 thin films synthesized by molecular beam epitaxy. A series of thin films with varying concentrations of Cu were grown under otherwise identical conditions to disentangle structural and compositional effects on the magnetic behavior. The combined experimental and theoretical studies show that Cu substitution at the Co 3g sites not only stabilizes the formation of the SmCo 5 structure but also enhances magnetic anisotropy and coercivity. Density functional theory calculations indicate that Sm(Co 4 Cu 3g ) 5 possesses a higher single-ion anisotropy as compared to pure SmCo 5 . In addition, X-ray magnetic circular dichroism reveals that Cu substitution causes an increasing decoupling of the Sm 4f and Co 3d moments. Scanning transmission electron microscopy confirms predominantly SmCo 5 phase formation and reveals nanoscale inhomogeneities in the Cu and Co distribution. Our study based on thin film model systems and advanced characterization as well as modeling reveals novel aspects of the complex interplay of intrinsic and extrinsic contributions to magnetic hysteresis in rare-earth-based magnets, i.e., the combination of increased intrinsic anisotropy due to Cu substitution and the extrinsic effect of inhomogeneous elemental distribution of Cu and Co.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Role of Curvature in Stabilizing Boron-Doped Nanocorrugated Graphene

Boron-doped carbon nanostructures have attracted great interest recently because of their remarkable electrocatalytic performance comparable to or better than that of conventional metal catalysts. In a previous work (Carbon 123, 605 (2017)), we reported that along with significant performance improvement, B doping enhances the oxidation resistance of few-layer graphene (FLG) that provides increased structural stability for intermediate-temperature fuel-cell electrodes. In general, detailed characterization of the atomic and electronic structure transformations that occur in B-doped carbon nanostructures during fuel-cell operation is lacking. In this work, we use aberration-corrected scanning transmission electron microscopy, nanobeam electron diffraction, and electron energy-loss spectroscopy (EELS) to characterize the atomic and electronic structures of B-doped FLG before and after fuel-cell operation. These data point to the nanoscale corrugation of B-doped FLGs as the key factor responsible for increased stability and high corrosion resistance. In conclusion, the similarity of the 1s to π* and σ* transition features in the B K-edge EELS to those in B-doped carbon nanotubes provides an estimate for the curvature of nanocorrugation in B-FLG.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Enabling Ethanol Dehydrogenation Catalysis by Postsynthetic Anion Exchange of Triazolate-Based Metal–Organic Frameworks

Materials containing soft, polarizable elements are expanding the boundaries of catalytic properties, offering unique electronic communication and stability characteristics compared with their harder counterparts due to the enhanced covalent nature of metal–ligand interactions. However, integrating soft components like sulfur into metal–organic frameworks (MOFs) for catalytic applications remains a largely underexplored challenge. Here, we report the synthesis of a family of triazole-based MOFs and expand upon established postsynthetic anion exchange methods to incorporate sterically encumbered polarizable elements, such as alkyl thiolates. Single-crystal X-ray diffraction, coupled with elemental analysis, confirms the successful anion exchange within M 2 X 2 BBTA (M = Co, Ni; X = μ-Cl, μ-OH, μ-SH, μ-SMe, μ-SEt; H 2 BBTA = 1H,5H-benzo(1,2-d:4,5-d′)bistriazole). We found that the anion identity significantly impacts the catalytic activity and selectivity of the MOFs, especially in nonoxidative ethanol dehydrogenation. Temperature-programmed experiments indicated that the metal single sites act as catalytically active sites below 250 °C. This work not only expands the synthetic toolbox for incorporating polarizable components into MOFs but also provides critical insights into their catalytic potential.

Anions↗

Strong Coupling of Iridium and Boron–Carbon-Nitride Support for Enhanced Acidic Water Oxidation

Supporting iridium (Ir)-based materials on stable and suitable substrates is an efficient strategy to improve their catalytic performance for the oxygen evolution reaction (OER) in harsh acidic environments. Herein, we report a series of Ir catalysts supported on boron–carbon-nitride (BCN), denoted as Ir/BCN. Detailed experiments combined with density functional theory calculations demonstrate strong interactions between Ir nanoparticles (NPs) and the BCN support, significantly contributing to the improved OER performance. Among the synthesized catalysts, the Ir/BCN-75 catalyst outperforms commercial Ir black and IrO 2 in both half-cell and proton exchange membrane water electrolysis (PEMWE) tests. Specially, the Ir/BCN-75 catalyst achieves a high current density of 2.94 A cm –2 at 1.9 V with a low Ir loading of 0.26 mg cm –2 in PEMWE measurements, exceeding most Ir-based catalysts reported to date. The BCN support interacts strongly with Ir, wherein Ir–N bonding directs the Ir NP growth and enhances electrocatalytic activity, while Ir–B bonding contributes to the stability of the Ir/BCN catalyst.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Modulation of the Eastern Equatorial Pacific Seasonal Cycle by Tropical Instability Waves

Feedbacks from tropical instability waves (TIWs) on the seasonal cycle of the eastern Pacific Ocean are studied using two eddy-rich ocean simulations, with and without TIWs. By warming the equatorial waters by up to 0.4°C through nonlinear advection in boreal summer and fall, TIWs reduce the amplitude of the seasonal cycle in upper ocean temperatures. In addition, TIWs stabilize the upper part of the Equatorial Undercurrent (EUC) through enhanced barotropic energy conversion, leading to a year-round weakening by -0.15 m s -1 and preventing an unrealistic re-intensification in boreal fall usually found in non-eddy resolving models. A coarser simulation at 1-degree horizontal resolution fails to reproduce the TIW-induced nonlinear warming of equatorial waters, but succeeds in inhibiting the EUC re-intensification. This suggests a threshold effect in TIW strength, associated with the model's ability to simulate eddies, which may be responsible for long-standing biases displayed by global climate models in this region.

58 GEOSCIENCES↗

Crystal structure of silver pentazolates AgN 5 and AgN 6

Silver pentazolate, a high energy density compound containing the cyclo-N 5 – anion, has recently been synthesized under ambient conditions. However, due to high sensitivity to irradiation, its crystal structure has not been determined. In this work, silver–nitrogen crystalline compounds under ambient conditions and at high pressures, up to 100 GPa, are predicted and characterized by performing first-principles evolutionary crystal structure searching with variable stoichiometry. It is found that newly discovered AgN 5 and AgN 6 are the only thermodynamically stable silver–nitrogen compounds at pressures between 42 and 80 GPa. In contrast to AgN 5 , the pentazolate AgN 6 compound contains N 2 diatomic molecules in addition to cyclo-N 5 – . These AgN 5 and AgN 6 crystals are metastable under ambient conditions with positive formation enthalpies of 54.95 kJ mol –1 and 46.24 kJ mol –1 , respectively. Here, the underlying cause of the stability of cyclo-N 5 – silver pentazolates is the enhanced aromaticity enabled by the charge transfer from silver atoms to nitrogen rings. To aid in the experimental identification of these materials, calculated Raman spectra are reported at ambient pressure: the frequencies of N 5 – vibrational modes of AgN 5 are in good agreement with those measured in the experiment.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Synergizing superwetting and architected electrodes for high-rate water splitting

Water splitting is one of the most promising technologies for generating green hydrogen. To meet industrial demand, it is essential to boost the operation current density to industrial levels, typically in the hundreds of mA cm -2 . However, operating at these high current densities presents significant challenges, with bubble formation being one of the most critical issues. Efficient bubble management is crucial as it directly impacts the performance and stability of the water splitting process. Superwetting electrodes, which can enhance aerophobicity, are particularly favorable for facilitating bubble detachment and transport. By reducing bubble contact time and minimizing the size of detached bubbles, these electrodes help prevent blockage and maintain high catalytic efficiency. Here, in this review, we aim to provide an overview of recent advancements in tackling bubble-related issues through the design and implementation of superwetting electrodes, including surface modification techniques and structural optimizations. We will also share our insights into the principles and mechanisms behind the design of superwetting electrodes, highlighting the key factors that influence their performance. Our review aims to guide future research directions and provides a solid foundation for developing more efficient and durable superwetting electrodes for high-rate water splitting.

36 MATERIALS SCIENCE↗

Advanced thermal/environmental barrier coatings of high-entropy rare earth disilicates tuned by strong anharmonicity of Eu 2 Si 2 O 7

Advancing thermal/environmental barrier coating (TEBC) materials with integrated thermal-mechanical functions is paramount for safeguarding SiC-based ceramic matrix composites (CMCs) in high-efficiency gas turbines. Herein, we employ a synergistic approach, combining density functional theory (DFT) methods and combinatorial chemistry techniques, to design high-performance and low-cost RE 2 Si 2 O 7 (RE = rare earth elements) TEBC materials tailored for enhanced compatibility with SiC-based CMCs. Expanding on phase stability of alloying pure RE 2 Si 2 O 7 , the investigation extends to the mechanical and thermal properties of solid solution systems, including Er 1/2 Y 3/4 Yb 3/4 Si 2 O 7 , Gd 1/4 Er 1/4 Y 3/4 Yb 3/4 Si 2 O 7 , and Eu 1/4 Er 1/4 Y 3/4 Yb 3/4 Si 2 O 7 . The solid solution systems exhibit a major reduction in lattice thermal conductivity relative to their pure counterparts, achieving ultralow values of 0.25 to 0.39 W m −1 K −1 at 1500 K. Furthermore, the coefficients of thermal expansion (CTE) of these solid solutions are precisely tuned within the desired range for SiC (4.4 to 5.5 × 10 −6 K −1 ), while maintaining good mechanical properties. Here, in particular, the addition of Eu 2 Si 2 O 7 demonstrates to be an important variable to the tuning of CTE and lattice thermal conductivity by leveraging its strong anharmonicity, presenting a pioneering avenue for fine-tuning material properties. In summary, this research not only identifies promising TEBC materials with superior thermal properties, but also introduces a valuable computational material design methodology for the rapid discovery of complex materials for harsh environments.

36 MATERIALS SCIENCE↗

Information integrated glass module fabricated by integrated additive and subtractive manufacturing

In this Letter, we report a novel integrated additive and subtractive manufacturing (IASM) method to fabricate an information integrated glass module. After a certain number of glass layers are 3D printed and sintered by direct C O 2 laser irradiation, a microchannel will be fabricated on top of the printed glass by integrated picosecond laser, for intrinsic Fabry–Perot interferometer (IFPI) optical fiber sensor embedment. Then, the glass 3D printing process continues for the realization of bonding between optical fiber and printed glass. Temperature sensing up to 1000°C was demonstrated using the fabricated information integrated module. In addition, the long-term stability of the glass module at 1000°C was conducted. Enhanced sensor structure robustness and harsh temperature sensing capability make this glass module attractive for harsh environment structural health monitoring.

Zhang, Qi (ORCID:0000000268655981)↗

Interdiffusion in the Ni/TD-NiCr and Cr/TD-NiCr systems

The diffusion of Ni and Cr into TD-NiCr has been studied over the 900 to 1100 C temperature range. The diffusion couples were prepared by electroplating Cr and Ni on polished TD-NiCr wafers. Concentration profiles produced as a result of isothermal diffusion at 905, 1000, and 1100 C were determined by electron microprobe analysis. The Boltzmann-Matano analysis was used to determine concentration-dependent diffusion coefficients which were found to compare favorably with previously reported values. These data suggest that 2 vol % ThO2 distribution has no appreciable effect on the rates of diffusion in TD-NiCr with a large grain size. This supports the view that an inert dispersoid in an alloy matrix will not in itself lead to enhanced diffusion unless a short-circuit diffusion structure is stabilized.

Pawar, A. V.↗

Iridium Film For Charge-Coupled Device

Usability extended to different environments. Application of thin film of iridium to back surface of back-surface-illuminated charge-coupled device expected to increase and stabilize quantum efficiency at wavelengths less than 4,500 Angstrom. Enhances quantum efficiency according to principle discussed in "Metal Film Increases CCD Output" (NPO-16815). Does not react with hydrogen, so device need not be kept in oxygen: Advantage where high absorption of ultraviolet light by oxygen undesirable; for example, when device used to make astronomical observations from high altitudes.

Hecht, Michael H.↗

Thermal state of an ice shell on Europa

The thickness of the ice shell presently hypothesized for Europa, which is decoupled from a silicate core by a liquid water layer, is calculated as a function of colatitude and longitude under suitable assumptions for two plausible ice rheology behaviors: that of Maxwell type, and that of generalized flow-law rheology. Due to the dissipation rate's pronounced temperature dependence, virtually all tidal dissipation is found to concentrate in the lowest few kilometers of the shell. While for some parameter choices an insulating regolith that raises the near-surface temperature by more than a few tens of degrees C may stabilize the shell against polar wander, a modest regolith may enhance the probability of such wander's occurrence through the reduction of the shell's retarding friction.

Ojakangas, Gregory W.↗