Dynamical Janus-Like Behavior Excited by Passive Cold-Heat Modulation in the Earth-Sun/Universe System: Opportunities and Challenges.

The utilization of solar-thermal energy and universal cold energy has led to many innovative designs that achieve effective temperature regulation in different application scenarios. Numerous studies on passive solar heating and radiation cooling often operate independently (or actively control the conversion) and lack a cohesive framework for deep connections. This work provides a concise overview of the recent breakthroughs in solar heating and radiation cooling by employing a mechanism material in the application model. Furthermore, the utilization of dynamic Janus-like behavior serves as a novel nexus to elucidate the relationship between solar heating and radiation cooling, allowing for the analysis of dynamic conversion strategies across various applications. Additionally, special discussions are provided to address specific requirements in diverse applications, such as optimizing light transmission for clothing or window glass. Finally, the challenges and opportunities associated with the development of solar heating and radiation cooling applications are underscored, which hold immense potential for substantial carbon emission reduction and environmental preservation. This work aims to ignite interest and lay a solid foundation for researchers to conduct in-depth studies on effective and self-adaptive regulation of cooling and heating.

High-Entropy Photothermal Materials.

High-entropy (HE) materials, celebrated for their extraordinary chemical and physical properties, have garnered increasing attention for their broad applications across diverse disciplines. The expansive compositional range of these materials allows for nuanced tuning of their properties and innovative structural designs. Recent advances have been centered on their versatile photothermal conversion capabilities, effective across the full solar spectrum (300-2500 nm). The HE effect, coupled with hysteresis diffusion, imparts these materials with desirable thermal and chemical stability. These attributes position HE materials as a revolutionary alternative to traditional photothermal materials, signifying a transformative shift in photothermal technology. This review delivers a comprehensive summary of the current state of knowledge regarding HE photothermal materials, emphasizing the intricate relationship between their compositions, structures, light-absorbing mechanisms, and optical properties. Furthermore, the review outlines the notable advances in HE photothermal materials, emphasizing their contributions to areas, such as solar water evaporation, personal thermal management, solar thermoelectric generation, catalysis, and biomedical applications. The review culminates in presenting a roadmap that outlines prospective directions for future research in this burgeoning field, and also outlines fruitful ways to develop advanced HE photothermal materials and to expand their promising applications.

Effect of RSN1 gene knockout on the adsorption of strontium ions by irradiated Saccharomyces cerevisiae.

The irradiated Saccharomyces cerevisiae (Y-7) has good biosorption ability for strontium ions. To investigate the mechanism of strontium ion bioaccumulation in Y-7, we employed CRISPR/Cas9 gene editing technology to engineer Saccharomyces cerevisiae Y-7 and knock out the RSN1 gene, successfully constructing a RSN1 gene knockout strain (Y-7-rsn1Δ). When tested for strontium ion adsorption, the Y-7-rsn1Δ strain exhibited decreased capacity for adsorbing strontium ions and increased resistance to strontium ions. The results showed that RSN1 is involved in the transport of Sr2+, and observed significant decreases in intracellular Ca2+ of Y-7-rsn1Δ, indicating a strong correlation between bioaccumulation of Sr2+ and Ca2+. This demonstrated that the adsorption of strontium ions by Y-7 is regulated by the RSN1 gene. The knockout of the RSN1 gene resulted in the shift of the peak positions of carboxyl, amino, amide, hydroxyl, and phosphate groups on the cell surface.

Copper-Catalyzed Asymmetric Allylation of N-Aryl Aldimines.

The copper-catalyzed enantioselective allylation reaction of N-aryl aldimines has been developed using a combination of Cu(OAc)2 and SPINOL-based phosphonamidite. This protocol significantly broadens the substrate scope, such that imines bearing various ortho-substituents on the N-aryl were converted smoothly into homoallylic amines in up to 99% yield and 98% ee. Taking advantage of the diversity of the N-aryl motif, three kinds of N-heterocyclic compounds were constructed, respectively, from the corresponding homoallylic amines in merely one step.

Modeling Indirect Greenhouse Gas Emissions Sources from Urban Wastewater Treatment Plants: Integrating Machine Learning Models to Compensate for Sparse Parameters with Abundant Observations.

Electricity consumption and sludge yield (SY) are important indirect greenhouse gas (GHG) emission sources in wastewater treatment plants (WWTPs). Predicting these byproducts is crucial for tailoring technology-related policy decisions. However, it challenges balancing mass balance models and mechanistic models that respectively have limited intervariable nexus representation and excessive requirements on operational parameters. Herein, we propose integrating two machine learning models, namely, gradient boosting tree (GBT) and deep learning (DL), to precisely pointwise model electricity consumption intensity (ECI) and SY for WWTPs in China. Results indicate that GBT and DL are capable of mining massive data to compensate for the lack of available parameters, providing a comprehensive modeling focusing on operation conditions and designed parameters, respectively. The proposed model reveals that lower ECI and SY were associated with higher treated wastewater volumes, more lenient effluent standards, and newer equipment. Moreover, ECI and SY showed different patterns when influent biochemical oxygen demand is above or below 100 mg/L in the anaerobic-anoxic-oxic process. Therefore, managing ECI and SY requires quantifying the coupling relationships between biochemical reactions instead of isolating each variable. Furthermore, the proposed models demonstrate potential economic-related inequalities resulting from synergizing water pollution and GHG emissions management.

Wettability of Ionic Liquids in High Magnetic Fields.

Here, we demonstrate that high magnetic fields alter the wettability of water and ionic solutions on the single-crystal α-Al2O3. We investigated the relationship between the substrate crystal orientation, material magnetism, liquid conductivity, and the surface contact angle. Applying high magnetic fields decreased the water contact angles on all of the surface orientations studied, and the reduction was larger for more magnetic substrates. For ionic solutions, high magnetic fields increased the contact angle on the (0001) α-Al2O3 surface but decreased the contact angles on the (112̅0), (101̅0), and (011̅2) surfaces. We attribute these orientation-dependent ionic solution responses to competition between the field-induced sample magnetization energy and the Lorentz force acting on the ionic solution. Overall, this work provides new magnetic-field-based strategies for changing the wettability and provides guidelines for fabricating novel microfluidic systems or biointerfaces with in situ magnetic control.

Synthesis of Cyclopenta[b]indoles via Sc(III)-Catalyzed Annulation of Vinyl Diazoacetates with Indole-Derived Unsaturated Imines.

A Lewis acid Sc(OTf)3-catalyzed annulation reaction of vinyl diazoacetates with in situ formed α,ß-unsaturated imines for the preparation of indole-fused tricyclic rings has been reported. This strategy involves a sequential addition/rebound addition process of vinyl diazoacetates and an in situ dedinitrogenation. This annulation protocol features low-cost catalysts, mild reaction conditions, and facilely prepared substrates.

Cyclization of Vinyl Diazo Compounds with Benzofuran-Derived Azadienes Enabled by NaBArF4.

An unprecedented cycloaddition of vinyl diazo compounds with benzofuran-derived azadienes catalyzed by rarely independently used NaBArF4 has been established. Benzofuran-fused hydropyridines were constructed with excellent yields and high diastereoselectivity via a Na+-catalyzed inverse-electron-demand aza-Diels-Alder reaction. Notably, this transformation also features good compatibility with a one-pot protocol to deliver the spiro[benzofuran-cyclopentene] skeleton, as well as perfect atom economy and simple reaction conditions.

Accurate Classification of Chunmee Tea Grade Using NIR Spectroscopy and Fuzzy Maximum Uncertainty Linear Discriminant Analysis.

The grade of tea is closely related to tea quality, so the identification of tea grade is an important task. In order to improve the identification capability of the tea grade system, a fuzzy maximum uncertainty linear discriminant analysis (FMLDA) methodology was proposed based on maximum uncertainty linear discriminant analysis (MLDA). Based on FMLDA, a tea grade recognition system was established for the grade recognition of Chunmee tea. The process of this system is as follows: firstly, the near-infrared (NIR) spectra of Chunmee tea were collected using a Fourier transform NIR spectrometer. Next, the spectra were preprocessed using standard normal variables (SNV). Then, direct linear discriminant analysis (DLDA), maximum uncertainty linear discriminant analysis (MLDA), and FMLDA were used for feature extraction of the spectra, respectively. Finally, the k-nearest neighbor (KNN) classifier was applied to classify the spectra. The k in KNN and the fuzzy coefficient, m, were discussed in the experiment. The experimental results showed that when k = 1 and m = 2.7 or 2.8, the accuracy of the FMLDA could reach 98.15%, which was better than the other two feature extraction methods. Therefore, FMLDA combined with NIR technology is an effective method in the identification of tea grade.

Efficient Warming Textile Enhanced by a High-Entropy Spectrally Selective Nanofilm with High Solar Absorption.

Solar and radiative warming are smart approaches to maintaining the human body at a metabolically comfortable temperature in both indoor and outdoor scenarios. Nevertheless, existing warming textiles are ineffective in frigid climates because the solar absorption of selective absorbing coating is significantly reduced when coated on rough textile surface. Herein, for the first time, high-entropy nitrides based spectrally selective film (SSF) is introduced on common cotton through a one-step magnetron sputtering method. The well-designed refractive index gradient enables destructive interference effects, offering a roughness-insensitive high solar absorptance (92.8%) and low thermal emittance (39.2%). Impressively, the solar absorptance is 9.1% higher than the reported best-performing selective nanofilm-based textile. As a result, such a textile achieves a record-high photothermal conversion efficiency (82.2% under 0.6 suns, at 0 °C). This textile yields a 3.5 °C drop in the set-point of indoor air-conditioner temperature. Besides, in a winter morning with an air temperature of 7.5 °C, it warms up the human skin by as large as 12 °C under weak sunlight (350 W m-2 ). More importantly, such a superior radiative warming performance is achieved by engineering the widely used cotton without compromising its breathability and durability, showing great potential for practical applications.

Enabling Highly Enhanced Solar Thermoelectric Generator Efficiency by a CuCrMnCoAlN-Based Spectrally Selective Absorber.

Harvesting solar energy to enhance thermoelectric generator efficiency is a highly effective strategy. However, it is a grand challenge but essential to increase solar-thermal conversion efficiency. A spectrally selective absorber, which is capable of boosting solar absorptance (α) while suppressing thermal emittance (ε), shows great potential to elevate the solar-thermal conversion efficiency. Herein, we fabricate a multilayer spectrally selective absorber with the assistance of high-entropy nitrides, which shows outstanding spectral selectivity (α/ε = 95.2/10.9%). Benefitting from the high-entropy nitrides, it is experimentally demonstrated that the as-deposited absorber exhibits superior thermal stability, which is crucial to ensure service life. Under 1000 W·m-2 simulated solar illumination, it achieves a very high surface temperature of 109.6 °C, making it suitable to enhance the efficiency of solar thermoelectric generators. Impressively, the integration of the proposed absorber with a commercial thermoelectric generator efficiently reinforces thermoelectric performance, offering a high output power of 1.99 mW. More importantly, by taking advantage of a thermal concentration strategy, it enables a further increase of the output power by 2.98 mW. This work provides a promising solar-thermal material to boost high thermoelectric performance and extends the application category of high-entropy nitrides.

Is the virus-laden standing water change the transmission intensity of SARS-CoV-2 after precipitation? A framework for empirical studies.

Understanding the relationship between precipitation and SARS-CoV-2 is significant for combating COVID-19 in the wet season. However, the causes for the variation of SARS-CoV-2 transmission intensity after precipitation is unclear. Starting from "the Zhengzhou event," we found that the virus-laden standing water formed after precipitation might trigger some additional routes for SARS-CoV-2 transmission and thus change the transmission intensity of SARS-CoV-2. Then, we developed an interdisciplinary framework to examine whether the health risk related to the virus-laden standing water needs to be a concern. The framework enables the comparison of the instant and lag effects of precipitation on the transmission intensity of SARS-CoV-2 between city clusters with different formation risks of the virus-laden standing water. Based on the city-level data of China between January 01, 2020, and December 31, 2021, we conducted an empirical study. The result showed that in the cities with a high formation risk of the virus-laden standing water, heavy rain increased the instant transmission intensity of SARS-CoV-2 by 6.2% (95%CI: 4.85-10.2%), while in the other cities, precipitation was uninfluential to SARS-CoV-2 transmission, revealing that the health risk of the virus-laden standing water should not be underestimated during the COVID-19 pandemic. To reduce the relevant risk, virus-laden water control and proper disinfection are feasible response strategies.

Robust Heterostructures in Two-Dimensional Perovskites by Threshold-Dominating Anion Exchange.

Heterostructures play an irreplaceable role in high-performance optoelectronic devices. However, the preparation of robust perovskite heterostructures is challenging due to spontaneous interdiffusion of halogen anions. Herein, a vapor-phase anion exchange method universally suitable for the preparation of robust 2D Ruddlesden-Popper perovskite (RPP) heterostructures is developed. A variety of heterostructures are fabricated based on exfoliated RPP microplates (MPs). Depending on the specific organic cations, the heterostructures can be either sharp and uniform, or broad and gradient, suggesting a new anion diffusion behavior different from that in 3D perovskites. Further experimental studies reveal that the lateral transport of anions follows a threshold-dominating mechanism, while the vertical transport can be partially or completely suppressed by organic cations. Subsequently, quantitative investigation of anion diffusion in 2D perovskites is conducted. The lateral diffusion coefficient of halogen anions is calculated to be 6 to 7 orders of magnitude larger than the vertical coefficient, consistent with the observed highly anisotropic anion diffusion. In addition, it is shown that the anion exchange threshold can also enhance the thermodynamic stability of the heterostructures at elevated temperature. These results provide a general method to fabricate robust lateral RPP heterostructures, and offer important insights into anion behavior in low-dimensional perovskites.

Palladium-Catalyzed Intermolecular Asymmetric Dearomative Annulation of Phenols with Vinyl Cyclopropanes.

Herein, we report the Pd(0)-catalyzed intermolecular asymmetric dearomative [3 + 2] annulation of phenols with vinyl cyclopropanes via in situ generated ortho-quinone methide intermediates. A series of highly functionalized spiro-[5,6] bicycles which bear three contiguous stereogenic centers including one all-carbon quaternary were obtained with excellent stereoselectivities. Density functional theory (DFT) calculations indicate that the reactions were controlled by thermodynamics.

CuH-Catalyzed Enantioselective Reductive Coupling of 1,3-Dienes and Trifluoromethyl Ketoimines or α-Iminoacetates.

The intermolecular addition of allylic copper species generated from diene and copper hydride remains elusive. Herein copper hydride catalyzed asymmetric cross reductive coupling of conjugated dienes and ketoimines including trifluoromethyl ketoimines and α-iminoacetates was first achieved using chiral Ph-BPE as the ligand, providing rapid access to structurally and optically enriched homoallylic amines containing two vicinal stereogenic centers with up to 95% yield, 99% ee, and 11:1 diastereoselectivities.

Enantioselective [3 + 2] Cycloaddition of Vinylcyclopropanes with Alkenyl N-Heteroarenes Enabled by Palladium Catalysis.

The first catalytic enantioselective [3 + 2] cycloaddition reaction between vinylcyclopropanes and alkenyl N-heteroarenes in the presence of LiBr and a Pd(0)/SEGPHOS complex was developed. LiBr plays a key role in improving the reactivity of alkenyl N-heteroarenes as a mild Lewis acid.

Anion-Exchange Driven Phase Transition in CsPbI3 Nanowires for Fabricating Epitaxial Perovskite Heterojunctions.

Anion-exchange in halide perovskites provides a unique pathway of bandgap engineering for fabricating heterojunctions in low-cost photovoltaics and optoelectronics. However, it remains challenging to achieve robust and sharp perovskite heterojunctions, due to the spontaneous anion interdiffusion across the heterojunction in 3D perovskites. Here, it is shown that the anionic behavior in 1D perovskites is fundamentally different, that the anion exchange can readily drive an indirect-to-direct bandgap phase transition in CsPbI3 nanowires (NWs) and greatly lower the phase transition temperature. In addition, the heterojunction created by phase transition is epitaxial in nature, and its chemical composition can be precisely controlled upon postannealing. Further study of the phase transition dynamics reveals a threshold-dominating anion exchange mechanism in these 1D NWs rather than the gradient-dominating mechanism in 3D systems. The results provide important insights into the ionic behavior in halide perovskites, which is beneficial for applications in solar cells, light-emitting diodes (LEDs), and other semiconductor devices.

Entropy-Assisted High-Entropy Oxide with a Spinel Structure toward High-Temperature Infrared Radiation Materials.

Developing advanced materials with a high-entropy concept is one of the hot trends in materials science. The configurational entropy of high-entropy materials can be tuned by introducing different atomic species, which can also impart a result in excellent physical and chemical properties. In this work, we synthesized a solid-solution oxide (Cu, Mn, Fe, Cr)3O4 by a simple and scalable solid-phase synthesis method. We extensively investigated the microstructure and chemical composition, indicating that (Cu, Mn, Fe, Cr)3O4 has a single-phase spinel structure. Simultaneously, we reasonably evaluated the position occupied by the elements of (Cu, Mn, Fe, Cr)3O4 in a spinel structure as (Cu0.75Fe0.25)(Fe0.25Cr0.375Mn0.375)2O4. Here, we first evaluated the infrared radiation performance of (Cu, Mn, Fe, Cr)3O4. The new, high-entropy oxide (HEO) (Cu, Mn, Fe, Cr)3O4 powder exhibits high infrared emissivity values of 0.879 and 0.848 in the wavelengths of 0.78-2.5 and 2.5-16 µm, respectively, and has excellent thermal stability. More importantly, the infrared emissivity values of as-prepared HEO coating reach 0.955 (0.78-2.5 µm) at room temperature and 0.936 (3-16 µm) at 800 °C. This work provides a viable strategy toward the laboratory mass production of this HEO for infrared radiation materials, which shows great potential in the energy-related applications.

Asymmetric Synthesis of 3-Methyleneindolines via Rhodium(I)-Catalyzed Alkynylative Cyclization of N-(o-Alkynylaryl)imines.

The first asymmetric synthesis of 3-methyleneindolines from alkynyl imines has been developed via a rhodium-catalyzed tandem process: regioselective alkynylation of the internal alkynes and subsequent intramolecular addition to the imines. The reaction proceeded with unconventional chemoselectivity and provided 3-methyleneindolines with good yields (up to 82% yield) and high enantioselectivities (up to 97% ee). Moreover, this transformation also features mild reaction conditions, perfect atom economy, and a broad substrate scope.

Highly Enhanced Thermal Robustness and Photothermal Conversion Efficiency of Solar-Selective Absorbers Enabled by High-Entropy Alloy Nitride MoTaTiCrN Nanofilms.

Recent advances in high-entropy alloys have spurred many breakthroughs in the fields of high-temperature materials and optical materials and they provide incredible application potentialities for photothermal conversion systems. Solar-selective absorbers (SSAs), as key components, play a vital role in photothermal conversion efficiency and service life. The most pressing problem with SSAs is their inconsistent optical performance, an instability constraint induced by thermal stress. A feasible method of improving performance stability is the introduction of high-entropy materials, such as high-entropy alloy nitrides. In this study, enabled by an intrinsic MoTaTiCrN absorption layer, the solar configuration achieves greatly enhanced, exceptional thermotolerance and optical properties, leading to the formation of a scalable, highly efficient, and cost-effective structure. Computational and experimental approaches are employed to achieve optimum preparation parameters for thicknesses and constituents. The crystal structure of high-entropy ceramic MoTaTiCrN is fully investigated, including thickness-dependent crystal nucleation. High-temperature and long-term thermal stability tests demonstrate that our proposed SSA is mechanically robust and chemically stable. Moreover, a low thermal emittance (15.86%) at 500 °C promotes the photothermal conversion efficiency. In addition, due to the exceptional spectral selectivity (α/ε = 92.3/6.5%), thermal robustness (550 °C for 168 h), and photothermal conversion efficiency (86.9% at 550 °C under 100 sun), it is possible for our proposed SSA to enhance the practical realization of large-area photothermal conversion applications, especially for concentrated solar power systems.