The most recent advances in high-entropy materials provide impetus for the development of high-performance materials, simultaneously providing high-temperature robustness and excellent functional ...properties owing to the high configurational entropy and distorted lattices. Thus, in this work, double-layer high-entropy alloy nitride HfNbTaTiZrN with a well-designed metal content gradient is employed to fabricate a solar selective absorber coating (SSAC). We extensively investigated whether the coating meets the definition of a high-entropy material from the points of elemental analysis and phase structure, combined with thermodynamic calculation. Remarkably, the new, tailored SSAC exhibits an exceptionally high solar absorptance (
α
= 96%) and a suppressed thermal emittance (
= 8.2%) at 82 °C and omnidirectional absorption. Investigations of the long-term thermal stability indicate that the HfNbTaTiZrN-based SSAC due to the entropy-driven structural stabilization could endure heat treatment at 600 °C for 168 h, retaining a performance criterion (PC) value less than 0.05, which implies the feasibility of practical applications. More importantly, the photothermal conversion efficiency (
η
), which is utilized to quantitatively evaluate the performance at elevated temperatures, reaches 90.1% at a working temperature of 550 °C under 100 suns, and even after annealing at 600 °C for 168 h, the efficiency drop is still less than 5%. Overall, the combination of thermal robustness and photothermal conversion efficiency at working temperatures less than 600 °C provides significant potential to maximize solar energy harvesting and pioneers an opportunity to explore simultaneous multifunctional applications of high-entropy alloys.
The most recent advances in high-entropy materials provide impetus for the development of high-performance materials, simultaneously providing high-temperature robustness and excellent functional properties owing to the high configurational entropy and distorted lattices.
Highlights
The cationic waterborne polyurethanes microspheres with Diels-Alder bonds were synthesized for the first time.
The electrostatic attraction not only endows the composite with segregated ...structure to gain high electromagnetic-interference shielding effectiveness, but also greatly enhances mechanical properties.
Efficient healing property was realized under heating environment.
It is still challenging for conductive polymer composite-based electromagnetic interference (EMI) shielding materials to achieve long-term stability while maintaining high EMI shielding effectiveness (EMI SE), especially undergoing external mechanical stimuli, such as scratches or large deformations. Herein, an electrostatic assembly strategy is adopted to design a healable and segregated carbon nanotube (CNT)/graphene oxide (GO)/polyurethane (PU) composite with excellent and reliable EMI SE, even bearing complex mechanical condition. The negatively charged CNT/GO hybrid is facilely adsorbed on the surface of positively charged PU microsphere to motivate formation of segregated conductive networks in CNT/GO/PU composite, establishing a high EMI SE of 52.7 dB at only 10 wt% CNT/GO loading. The Diels–Alder bonds in PU microsphere endow the CNT/GO/PU composite suffering three cutting/healing cycles with EMI SE retention up to 90%. Additionally, the electrostatic attraction between CNT/GO hybrid and PU microsphere helps to strong interfacial bonding in the composite, resulting in high tensile strength of 43.1 MPa and elongation at break of 626%. The healing efficiency of elongation at break achieves 95% when the composite endured three cutting/healing cycles. This work demonstrates a novel strategy for developing segregated EMI shielding composite with healable features and excellent mechanical performance and shows great potential in the durable and high precision electrical instruments.
The further development of high-performance fluorescent biosensors to image intracellular microRNAs is beneficial to cancer medicine. By virtue of the need for enzymes and hairpin DNA probes, the ...entropy-driven reaction-assisted signal amplification strategy has shown an enormous potential to accomplish this task. Nevertheless, this good option still meets with poor biostability, low cell uptake efficiency, and unsatisfactory accuracy. On the basis of these challenges, we put forward here a battery of solving pathways. First, the straight DNA probes are anchored onto the vertexes of dual DNA tetrahedrons, and thus the enzyme resistance of the whole sensing system is observably enhanced. A metal–organic framework (ZIF-8 nanoparticle), which can be effectively dissociated into a weakly acidic environment, then is employed as an additional delivery vehicle to encapsulate such a DNA tetrahedron sustained biosensor and finally bring about a more efficient endocytosis. Last, a kind of photocleavage-linker triggered photoresponsive manner is incorporated to achieve an exceptional precise target identification, by which the biosensor can only be initiated under the irradiation of an externally mild 365 nm ultraviolet light source. In accordance with the above efforts, worthy assay performance toward microRNA-196a has given rise to this newly constructed biosensor, whose sensitivity is down to 2.7 pM and also able to distinguish single-base variation. Beyond that, the amplifier can work as a powerful imaging toolbox to accurately determine the targets in living cells, providing a promising intracellular sensing platform.
Due to the robust oxidation conditions in strong acid oxygen evolution reaction (OER), developing an OER electrocatalyst with high efficiency remains challenging in polymer electrolyte membrane (PEM) ...water electrolyzer. Recent theoretical research suggested that reducing the coordination number of Ir−O is feasible to reduce the energy barrier of the rate‐determination step, potentially accelerating the OER. Inspired by this, we experimentally verified the Ir−O coordination number's role at model catalysts, then synthesized low‐coordinated IrOx nanoparticles toward a durable PEM water electrolyzer. We first conducted model studies on commercial rutile‐IrO2 using plasma‐based defect engineering. The combined in situ X‐ray absorption spectroscopy (XAS) analysis and computational studies clarify why the decreased coordination numbers increase catalytic activity. Next, under the model studies’ guidelines, we explored a low‐coordinated Ir‐based catalyst with a lower overpotential of 231 mV@10 mA cm−2 accompanied by long durability (100 h) in an acidic OER. Finally, the assembled PEM water electrolyzer delivers a low voltage (1.72 V@1 A cm−2) as well as excellent stability exceeding 1200 h (@1 A cm−2) without obvious decay. This work provides a unique insight into the role of coordination numbers, paving the way for designing Ir‐based catalysts for PEM water electrolyzers.
Reducing the coordination number is feasible to lower the rate‐determination‐step energy barrier, thus accelerating the electrocatalytic reaction process. Our designed low‐coordination IrOx delivers superior activity as well as excellent stability in water electrolyzers.
Passive daytime radiative cooling (PDRC) is an emerging energy-free cooling technology, which can weaken our dependence on energy-consuming air-conditioning requirements. Though the advance in ...micro/nanostructure PDRC materials achieves excellent sub-ambient cooling performance, the majority of them are facing a huge challenge in terms of practical large-scale applications owing to complicated preparation methods and high costs. Herein, combining a low-cost polymer matrix with inorganic dielectric particles, a hierarchically porous composite (HPC) film with a micro/nanostructure and adjustable spectral properties is developed through a flexible phase-inversion-based method. The HPC-film exhibits a strong solar reflectivity (∼98.26%) and infrared emissivity (∼97.56%), thus realizing a sub-ambient average cooling temperature of ∼9.1 °C and effective radiative cooling power of ∼87.2 W m
−2
under a solar irradiance of ∼890 W m
−2
. As a proof of concept, we demonstrate that the proposed cooler is capable of delaying ice melting by four times compared with the pristine case due to the remarkable radiative cooling performance, which provides inspiration for developing a scalable and sustainable pathway of ice protection and preservation. Overall, the multiple advantages of the facile and flexible manufacturing technique, excellent stability and repeatability in this study promise potentially valuable applications in passive radiative cooling.
The polymer-dielectric composite film is reported to obtain a hierarchical micro-nano structure. Composites exhibit excellent optical properties and their actual radiative cooling effect was tested in an outdoor environment.
DNA modifications vary in form and function but generally do not alter Watson-Crick base pairing. Diaminopurine (Z) is an exception because it completely replaces adenine and forms three hydrogen ...bonds with thymine in cyanophage S-2L genomic DNA. However, the biosynthesis, prevalence, and importance of Z genomes remain unexplored. Here, we report a multienzyme system that supports Z-genome synthesis. We identified dozens of globally widespread phages harboring such enzymes, and we further verified the Z genome in one of these phages,
phage SH-Ab 15497, by using liquid chromatography with ultraviolet and mass spectrometry. The Z genome endows phages with evolutionary advantages for evading the attack of host restriction enzymes, and the characterization of its biosynthetic pathway enables Z-DNA production on a large scale for a diverse range of applications.
Abstract
The high cost of noble metals is one of the key factors hindering the large‐scale application of proton exchange membrane (PEM) water electrolyzer for hydrogen production. Recently, ...single‐atom catalysts (SACs) with a potential of maximum atom utilization efficiency enable lowering the metal amount as much as possible; unfortunately, their durability remains a challenge under PEM water electrolyzer working conditions. Herein, a highly‐stable alloyed Pt SAC is demonstrated through a plasma‐assisted alloying strategy and applies to a PEM water electrolyzer. In this catalyst, single Pt atoms are firmly anchored onto a Ru support via a robust metal–metal bonding strength, as evidenced by these complementary characterizations. This SAC is used in a PEM water electrolyzer system to achieve a cell voltage as low as 1.8 V at 1000 mA cm
−2
. Impressively, it can operate over 1000 h without obvious decay, and the catalyst is present in the form of individual Pt atoms. To the knowledge, this will be the first SAC attempt at a cell level toward long‐term PEM. This work paves the way for designing durable SACs employed in the actual working condition in the PEM water electrolyzer.
Early diagnosis and treatment of patients with sepsis reduce mortality significantly. In terms of exploring new diagnostic tools of sepsis, monocyte distribution width (MDW), as part of the white ...blood cell (WBC) differential count, was first reported in 2017. MDW greater than 20 and abnormal WBC count together provided a satisfactory accuracy and was proposed as a novel diagnostic tool of sepsis. This study aimed to compare MDW and procalcitonin (PCT)'s diagnostic accuracy on sepsis in the emergency department.
This was a single-center prospective cohort study. Laboratory examinations including complete blood cell and differentiation count (CBC/DC), MDW, PCT were obtained while arriving at the ED. We divided patients into non-infection, infection without systemic inflammatory response syndrome (SIRS), infection with SIRS, and sepsis-3 groups. This study's primary outcome is the sensitivity and specificity of MDW, PCT, and MDW + WBC in differentiating septic and non-septic patients. In addition, the cut-off value for MDW was established to maximize sensitivity at an optimal level of specificity.
From May 2019 to September 2020, 402 patients were enrolled for data analysis. Patient number in each group was: non-infection 64 (15.9%), infection without SIRS 82 (20.4%), infection with SIRS 202 (50.2%), sepsis-3 15 (7.6%). The AUC of MDW, PCT, and MDW + WBC to predict infection with SIRS was 0.753, 0.704, and 0.784, respectively (p < 0.01). The sensitivity, specificity, PPV, and NPV of MDW using 20 as the cutoff were 86.4%, 54.2%, 76.4%, and 70%, compared to 32.9%, 88%, 82.5%, and 43.4% using 0.5 ng/mL as the PCT cutoff value. On combing MDW and WBC count, the sensitivity and NPV further increased to 93.4% and 80.3%, respectively. In terms of predicting sepsis-3, the AUC of MDW, PCT, and MDW + WBC was 0.72, 0.73, and 0.70, respectively. MDW, using 20 as cutoff, exhibited sensitivity, specificity, PPV, and NPV of 90.6%, 37.1%, 18.7%, and 96.1%, respectively, compared to 49.1%, 78.6%, 26.8%, and 90.6% when 0.5 ng/mL PCT was used as cutoff.
In conclusion, MDW is a more sensitive biomarker than PCT in predicting infection-related SIRS and sepsis-3 in the ED. MDW < 20 shows a higher NPV to exclude sepsis-3. Combining MDW and WBC count further improves the accuracy in predicting infection with SIRS but not sepsis-3. Trial registration The study was retrospectively registered to the ClinicalTrial.gov (NCT04322942) on March 26th, 2020.
Celotno besedilo
Dostopno za:
DOBA, IZUM, KILJ, NUK, PILJ, PNG, SAZU, SIK, UILJ, UKNU, UL, UM, UPUK