Browse Articles

Multiple Strong Ion–Dipole Interactions in Hierarchical Porous Polymer/Covalent Organic Framework Electrolytes Accelerating Stable and Efficient Ion Transport

ABSTRACT The development of solid‐state lithium metal batteries (SSLMBs) is severely restricted by the inherent drawbacks of conventional solid electrolytes, including sluggish ionic conduction and unstable solid electrolyte interphase (SEI). Herein, we propose a strategy for constructing vinylene‐linked covalent organic framework (COF)‐based porous composite polymer electrolytes (TFP‐COF@PNFs CPEs). The strongly polar –C≡N and –F moieties in TFP‐COF form prominent ion‐dipole interactions with Li + , which reduce the dissociation energy barrier of Li salts, guide the oriented transport of Li + , and induce the formation of stable SEI. Therefore, the optimized 2‐TFP‐COF@PNFs CPEs exhibit a high room‐temperature ionic conductivity of 1.68 × 10 − 3 S cm − 1 along with ultra‐stable Li||Li symmetric cell cycling exceeding 8500 h. Interestingly, the well‐designed CPEs are highly compatible with layered oxides and polyanion compounds; especially, the Li|2‐TFP‐COF@PNFs|LiFePO 4 full cells deliver a higher initial discharge capacity of 106 mAh g − 1 at 10 C with long‐term cycling stability after 4000 cycles as well as excellent wide‐temperature adaptability (−40°C to 60°C) and compatibility with high mass loadings. Impressively, the assembled pouch cells realize stable cycling for 100 cycles. This work efficiently addresses the core issues of unstable SEI layers and low ionic transport efficiency, offering a highly promising strategy for designing high‐performance SSLMBs.

Eco sustainable IoT based roof garden monitoring and planting recommendation system with machine learning

Unbiased Structure Prediction of Sophisticated Cage Structures

ABSTRACT Cage structure prediction has made significant strides by generating structures based on what the community has seen before. However, to computationally design and discover novel structures, the community must be able to evaluate and model all structural candidates. Here, we introduce unbiased structure prediction workflows in our software, cgx , facilitated by exploration algorithms and our low‐cost minimal models. By comparing to experiments, we show that our approach predicts cage structures starting only from the experimental inputs (building block types, features and their stoichiometry). We demonstrate the use of this method prior to any costly experimental commitment, providing an efficient automated approach that is open source and applicable to multiple model resolutions. By providing recipes with copyable code in the documentation, we make uptake of this new method as facile as possible for chemists with a wide‐range of expertise.

Spatial statistics and point pattern analysis reveal lifespan trajectories of microglial density and clustering in the primate hippocampus

Electronic‐Structure‐Directed Pore Engineering in Metal–Organic Frameworks for Molecular Sieving of C ₃ F ₆ /C ₃ F ₈

ABSTRACT Trace removal of hexafluoropropylene (C 3 F 6 ) from octafluoropropane (C 3 F 8 ) is crucial for producing high‐purity fluorinated electronic gases, yet it remains highly challenging because of their similar molecular dimensions. Here, we report an electronically driven pore‐engineering strategy for C 3 F 6 /C 3 F 8 separation, in which Jahn–Teller‐active Cu 2+ directs framework reconstruction from the large‐aperture channels of ZnTPO (H 3 TPO = tris(4‐carboxyphenyl) phosphine oxide) to the narrow cage‐like pore network of CuHTPO, thereby switching the separation behavior from co‐adsorption to molecular sieving. Consequently, CuHTPO delivers > 99.999% pure C 3 F 8 with productivities of 314.9 and 2819 L kg −1 from 1/9 and 1/99 C 3 F 6 /C 3 F 8 mixtures, respectively. Optical imaging at the single‐particle level directly visualizes the rapid transport of C 3 F 6 through the channels, while single‐crystal X‐ray diffraction, FTIR spectroscopy, and molecular simulations collectively elucidate the structural origin of the electronically regulated sieving behavior. Taken together, this work positions electronic‐structure‐directed pore reconstruction as a powerful material‐design strategy for programming confined pore spaces, enabling robust and recyclable molecular sieving of closely related gases.

Frontal alpha asymmetry and NoGo N2 amplitude interact to explain non-supportive parenting practices

Cross‐Interface Quasi‐Tandem Catalysis Over Amorphous Oxide‐Metal Junctions Steers CO ₂ Electroreduction Toward C ₃ Products

ABSTRACT The selective electroreduction of CO 2 to n ‐propanol is fundamentally constrained by sluggish C 1 ─C 2 coupling and the instability of key oxygenated intermediates. Here, we propose a quasi‐tandem catalytic strategy enabled by defect‐rich amorphous ZrO 2 , where the amorphous oxide‐metal interfacial environment promotes *CO generation, stabilization of oxygenated C 2 intermediates (*OCCOH), and subsequent C─C coupling toward n ‐propanol formation. The resulting catalyst, composed of amorphous ZrO 2 , Cu, and Ag, delivers a Faradaic efficiency of 23.2% ± 1.6% and a partial current density of 50.6 mA cm −2 for n ‐propanol, representing more than 2.5‐ and 3.5‐fold enhancements, respectively, compared to its crystalline ZrO 2 analogue. Density functional theory (DFT) calculations reveal that the amorphous ZrO 2 ─Cu interface, not only enhances the formation of *COH, but also significantly lowers the energy barriers for *CO‐COH coupling and *CO‐*OCCOH coupling toward n ‐propanol generation. These findings establish amorphous oxide‐metal interfacial engineering as an effective strategy for quasi‐tandem catalysis, enabling cooperative multistep C─C coupling pathways toward selective C 3 electrosynthesis from CO 2 .

Evaluating the impact of different green infrastructure strategies on particulate pollutant concentrations in street canyons: a numerical simulation study in Qingdao

The Role of Zn–Hf Site Proximity and Oxygen Vacancies for Methanol Formation Over ZnHfO <i> _x </i> Catalysts Under CO ₂ Hydrogenation Conditions

ABSTRACT Mixed metal oxides, such as ZnZrO x , have attracted considerable interest as CO 2 hydrogenation to methanol catalysts due to their high methanol selectivity (&gt; 70%) and catalytic stability at elevated reaction temperatures (&gt; 300°C). In this work, we introduce a novel ZnHfO x catalyst that exceeds the intrinsic methanol formation rate of the reference ZnZrO x at a Zn content of 20 mol% ( r MeOH,20ZnZrOx = 0.59 mol MeOH (mol cat h) −1 , r MeOH,20ZnHfOx = 0.68 mol MeOH (mol cat h) −1 ). Remarkably and in contrast to ZnZrO x , the ZnHfO x ‐based catalysts exhibit a high methanol selectivity (&gt; 70%) up to Zn contents of 99.5 mol% despite the segregation of ZnO. Operando spectroscopy, in combination with computational analysis, identifies the Zn–V O –Hf motif as the active site for methanol formation that proceeds via the formate‐methoxy pathway. Such active sites are not only present in solid solution‐type ZnHfO x catalysts (≤ 35 mol% Zn), but also in the form of isolated HfO x clusters on segregated ZnO surfaces (for high Zn contents of &gt; 35 mol%), explaining the high selectivity (and activity) over a wide range of Zn contents.

Transformer-based temporal models for probabilistic load and photovoltaic power forecasting in commercial microgrids

A Novel Class of “Super‐Strained” Spiro Heterocycles: Gateway to 1‐Azaspiro[3.3]heptane Derivatives, and Biological Validation

ABSTRACT Strained spiro heterocycles have gained popularity in medicinal chemistry due to their potential to act as conformationally rigid non‐classical three‐dimensional bioisosteres. Recently, 1‐azaspiro[3.3]heptane has been validated as a piperidine bioisostere, although synthetic methods available for functionalized or heteroatom‐containing derivatives are scarce. We address this shortcoming by accessing spirocyclic 1‐azabicyclo[1.1.0]butanes—a novel class of “super‐strained” spirocycles—through a Johnson‐Corey‐Chaykovsky reaction between cyclobutane‐, oxetane‐, and azetidine‐substituted sulfonium salts, and azirines. We demonstrate that such spirocycles are suitable precursors for highly functionalized 1‐azaspiro[3.3]heptane derivatives. In addition, such super‐strained spirocycles have been validated in vitro as potential sigma‐1 receptor agonists, a target identified through an artificial intelligence‐supported target fishing approach.

Oak aging mitigates the sensory impact of smoke taint in Cabernet Sauvignon wine

Abstract The wildfires that swept through Napa Valley in 2020 caused an estimated USD$3.7 billion economic loss to the grape and wine industry. The wines made from smoke-impacted grapes are often described as medicinal, smoky, and possessing a retronasal ashtray character. However, matrix differences among varieties and winemaking styles can impact smoke taint expression as well as the synergistic effects among the volatile phenols responsible for these off-flavors. Serial dilutions of non-impacted and impacted (intentionally smoked post-harvest) wines were used to create wines with differing levels of smoke impact for two wine regions (Napa and Lodi) and styles of Cabernet Sauvignon that were fermented and finished in stainless steel (SS) or subsequently aged in new oak barrels for 12 months. Gas chromatography–mass spectrometry (GC–MS) and liquid chromatography-triple quadrupole mass spectrometry (LC-QqQ-MS) were used to quantify free and total volatile phenols (VPs), and individual bound glycosides, respectively. Descriptive analysis using trained judges and Wine Cuality™ evaluations with wine experts were used to evaluate the sensory characteristics and overall quality of the wines, respectively. Generally, barrel-aged wines saw a decrease in the level of “ashy aftertaste” and smoke-related attributes for both Cabernet Sauvignon wines as compared to their stainless-steel counterparts. Wines with high levels of smoke impact received significantly lower quality ratings ( p  &lt; 0.05). Interestingly, wines with low levels of smoke-impact consistently received a slightly higher quality rating though not statistically significant when compared to their non-impacted counterparts. These findings contribute to our understanding of grape smoke exposure at different levels of taint and demonstrate the potential value of barrel aging to mitigate overall smoke perception in wine across these taint levels.

Adsorption‐Mediated Sodium Compensation for Hard Carbon Anodes Enabled by Soft‐Contact Presodiation

ABSTRACT Hard carbon (HC) anode in sodium‐ion batteries suffer from low initial Coulombic efficiency and irreversible capacity loss, limiting practical energy density and cycle life of SIBs. While direct‐contact presodiation of HC has been proposed to increase the initial Coulombic efficiency of SIBs, but its low utilization efficiency can cause residual Na on the HC surface, resulting in rapid degradation and even safety concerns. Herein, we proposed a soft‐contact presodiation (SCP) method, which can remove and recycle Na source and therefore greatly improve the utilization of the Na source and safety of SIBs. The SCP‐treated HC anode achieves a ≈30.0% increase in ICE when paired with a NaNi 1/3 Fe 1/3 Mn 1/3 O 2 cathode, while maintaining minimal temperature rise (Δ T ≈1.3°C) during treatment. The resulting SCP‐HC exhibits exceptional thermal stability with negligible exothermic activity at 125.0°C and remains chemically stable for over 3.0 days. Through multimodal analysis, we reveal an adsorption‐dominated compensation mechanism where replenished Na participates in solid electrolyte interphase formation while simultaneously occupying adsorption sites as metallic clusters. The pouch cell incorporating SCP‐HC anode delivers 90.6% ICE and retains 80.0% capacity after 150 cycles. This work establishes a safe, efficient, and economically viable presodiation platform that paves the way for practical high‐energy sodium‐ion batteries.

Multi-feature fusion monthly runoff prediction under different climate conditions using APO-optimized CNN-BiGRU-Self-Attention

An Adaptive Ionic Sieve: Flexible Hydrogen‐Bonded Organic Frameworks Decouple the Trade‐Off Between Zn Ions Desolvation and Mass Transfer

ABSTRACT Efficient ion desolvation and rapid mass transport are crucial yet often competing requirements for stabilizing Zn anodes in aqueous Zn‐ion batteries. This dilemma arises because ion desolvation introduces additional energy barriers that increase ion diffusion resistance. To reconcile this inherent trade‐off, a hydrogen‐bonded organic framework (HOF) based on C 3 ‑symmetric trigonal carboxyl ligands is engineered as an ion‐sieving interface. This design integrates precise pore size control with tailored chemical environment to regulate Zn 2+ desolvation behavior. As expected, the flexible HOF incorporating an electron‐deficient triazine core (HOF‐TAT) dynamically strips solvated water molecules while maintaining continuous ion flux. This process fosters a gradient solid electrolyte interphase that synergizes with the self‐adaptive porous framework to guide dense (101)‐oriented Zn deposition. The HOF‐TAT@Zn symmetric cells stably cycle exceeding 3400 h at 5 mA cm −2 . Furthermore, the iodophilic porous framework immobilizes shuttling polyiodides through strong physicochemical interactions. When integrated with an ultrathin Zn anode (10 µm), the Zn‐iodine batteries deliver a high‐rate capacity (142.2 mAh g −1 at 5 A g −1 ) and long‐term lifetime (50 000 cycles). This work offers an intelligent strategy to concurrently overcome the high energy barriers of ion desolvation and the kinetic limitations of ion transport for building advanced electrochemical devices.

Distinct motivational factors shape news-seeking in young adults

Sustainable Electrochemical Valorization of Sulfite in Industrial Wastewater Into Sulfonate‐Based Molecules

ABSTRACT Sulfite (SO 3 2− ), abundant in industrial wastewater, poses environmental challenges due to its instability, oxygen scavenging, and microbial toxicity. However, current sulfite treatment methods primarily focus on oxidation to inert sulfate or biological reduction, both of which suffer from low efficiency, secondary emissions, or loss of sulfur value. In this study, we present a sustainable electrocatalytic strategy for upgrading sulfite‐laden wastewater by directly converting SO 3 2− into value‐added sulfonates under ambient conditions. Using commercial Ni catalysts and methanol as a representative feedstock, the system achieves a sulfite‐to‐sulfonate conversion ratio exceeding 90% after 3 h of continuous electrolysis, with a maximum sulfonate production rate of 7870 µmol cm −2  h −1 at 1000 mA cm −2 , highlighting efficient upgrading of sulfite‐laden wastewater into organosulfur products. To enable continuous system operation, Ni nanoparticles were incorporated into a carbon nanotube (CNT)‐based electrochemical membrane, which shows a sulfite removal ratio above 93% and a sulfite‐to‐sulfonate conversion ratio above 90%, demonstrating suitability for scalable wastewater treatment and sulfur valorization. Moreover, techno‐economic analysis reveals a minimum levelized production cost of $300.84 per ton at 400 mA, corresponding to an 79.85% reduction compared with conventional routes. This integrated electrocatalytic membrane system offers a promising route for coupling sulfite removal with organosulfur synthesis.

Historical biogeography and environmental filtering jointly shape ant diversity in Huanglianshan National Nature Reserve, China

Metal–Organic Framework‐Gated Biocatalysis Enables Triggered Depolymerization of Melt‐Processed Polyesters

ABSTRACT Controlling biocatalytic activity in melt‐processed polymers is a central challenge for triggered depolymerization, because enzymes deactivate at melt‐extrusion temperatures. Here, metal–organic framework‐gated biocatalysis, achieved by encapsulating enzymes within zeolitic imidazolate framework‐8 (ZIF‐8), preserves &gt; 85% activity after 2 min at 180°C while regulating substrate access. Enzyme@ZIF‐8 biocomposite production scales to ∼50 kg day − 1 and is compounded by twin‐screw extrusion into poly(ε‐caprolactone) (PCL), poly(butylene adipate‐co‐terephthalate) (PBAT), and polylactide (PLA) at a tonne‐per‐day scale; pellets are compatible with standard thermoforming. The enzyme@ZIF/plastic composites retain mechanical performance comparable to the neat polymers during processing and use. At the end‐of‐life, chemical triggers dissolve the ZIF‐8 gate, releasing the enzyme, Zn 2 + and imidazolate to cooperatively accelerate depolymerization. Degradation increases 13.3–62.8‐fold for PCL and PLA in water and 1.7‐fold under industrial composting for PBAT and enables anaerobic PBAT digestion, whereas pristine polyesters show negligible conversion. This melt‐processable platform establishes gated, on‐demand depolymerization compatible with industrial polymer manufacturing.

Fabrication and DFT assisted investigation of novel Ru (III) imine complex for nickel corrosion inhibition and energy storage applications