bluuebunny/crossref_metadata_2025_split huggingface dataset:
In Situ Regulating Cobalt/Iron Oxide‐Oxyhydroxide Exchange by Dynamic Iron Incorporation for Robust Oxygen Evolution at Large Current Density
Authors: Li Dongyang , Xiang Rong , Yu Fang , Zeng Jinsong , Zhang Yong , Zhou Weichang , Liao Liling , Zhang Yan , Tang Dongsheng , Zhou Haiqing 
Published: September 2023

AbstractThe key dilemma for green hydrogen production via electrocatalytic water splitting is the high overpotential required for anodic oxygen evolution reaction (OER). Co/Fe‐based materials show superior catalytic OER activity to noble metal‐based catalysts, but still lag far behind the state‐of‐the‐art Ni/Fe‐based catalysts probably due to undesirable side segregation of FeOOH with poor conductivity and unsatisfied structural durability under large current density. Here, a robust and durable OER catalyst affording current densities of 500 and 1000 mA cm−2 at extremely low overpotentials of 290 and 304 mV in base is reported. This catalyst evolves from amorphous bimetallic FeOOH/Co(OH)2 heterostructure microsheet arrays fabricated by a facile mechanical stirring strategy. Especially, in situ X‐ray photoelectron spectroscopy (XPS) and Raman analysis decipher the rapid reconstruction of FeOOH/Co(OH)2 into dynamically stable Co1‐xFexOOH active phase through in situ iron incorporation into CoOOH, which perform as the real active sites accelerating the rate‐determining step supported by density functional theory calculations. By coupling with MoNi4/MoO2 cathode, the self‐assembled alkaline electrolyzer can deliver 500 mA cm−2 at a low cell voltage of 1.613 V, better than commercial IrO2(+)||Pt/C(‐) and most of reported transition metal‐based electrolyzers. This work provides a feasible strategy for the exploration and design of industrial water‐splitting catalysts for large‐scale green hydrogen production.
Regulating Intramolecular Electron Transfer of Nickel‐Based Coordinations through Ligand Engineering for Aqueous Batteries
Authors: Su Yichun , Hu Jinliang , Yuan Guoqiang , Zhang Guangxun , Wei Wenxian , Sun Yangyang , Zhang Xiaoxing , Liu Zheng , Suen Nian‐Tzu , Chen Hsiao‐Chien , Pang Huan 
Published: September 2023

AbstractThe integration of electronic effects into complexes for the construction of novel materials has not yet attracted significant attention in the field of energy storage. In the current study, eight one‐dimensional (1D) nickel‐based salicylic acid complexes (Ni‐XSAs, X = pH, pMe, pMeO, mMe, pBr, pCl, pF, and pCF3), are prepared by ligand engineering. The coordination environments in the Ni–XSAs are explored using X‐ray absorption fine structure spectroscopy. The charge transfer of the complexes is modulated according to the difference in the electron‐donating ability of the substituents, in combination with frontier orbital theory. Furthermore, density functional theory is used to investigate the effect of the substituent position on the electronic properties of the complexes. Ni‐mMeSA exhibits better electrical conductivity than Ni‐pMeSA. The electrochemical performance of Ni‐mMeSA as an aqueous battery cathode is remarkably improved with a maximum energy density of 0.30 mWh cm−2 (125 Wh kg−1) and a peak power density of 33.72 mW cm−2 (14.03 kW kg−1). This study provides ideas for the application of new coordination chemistry in the field of energy materials science.
Electrochemical and Biocatalytic Signal‐Controlled Payload Release from a Metal–Organic Framework
Authors: Sterin Ilya , Hadynski John , Tverdokhlebova Anna , Masi Madeline , Katz Evgeny , Wriedt Mario , Smutok Oleh 
Published: September 2023

AbstractA metal–organic framework (MOF), ZIF‐8, which is stable at neutral and slightly basic pH values in aqueous solutions and destabilized/dissolved under acidic conditions, is loaded with a pH‐insensitive fluorescent dye, rhodamine‐B isothiocyanate, as a model payload species. Then, the MOF species are immobilized at an electrode surface. The local (interfacial) pH value is rapidly decreased by means of an electrochemically stimulated ascorbate oxidation at +0.4 V (Ag/AgCl/KCl). Oxygen reduction upon switching the applied potential to −0.8 V allows to return the local pH to the neutral/basic pH, then stopping rapidly the release process. The developed method allows electrochemical control over stimulated or inhibited payload release processes from the MOF. The pH variation proceeds in a thin film of the solution near the electrode surface. The switchable release process is realized in a buffer solution and undiluted human serum. As the second option, the pH decrease stimulating the release process is achieved upon an enzymatic reaction using esterase and ester substrate. This approach potentially allows the release activation controlled by numerous enzymes assembled in complex biocatalytic cascades. It is expected that related electrochemical or biocatalytic systems can represent novel signal‐responding materials with switchable features for delivering (bio)molecules within biomedical applications.
Probing Enhanced Electrochemical Performance of Poly (3,4‐ethylenedioxy Thiophene) Encapsulated 5.3 V Spinel LiCoMnO4 Cathode for Li‐ion Batteries
Authors: Sreedeep Sreekumar , Lee Yun‐Sung , Aravindan Vanchiappan 
Published: September 2023

AbstractHerein, the effect of poly(3,4‐ethylenedioxythiophene) polystyrene sulfonate (PEDOT) coating is reported on the electrochemical properties of high voltage, 5.3 V lithium cobalt manganese oxide (LiCoMnO4, LCMO) cathodes. Scalable precipitation followed by a wet coating method is employed for the synthesis of LCMO@PEDOT. Various analytical studies are performed to validate the performance of the cathode. The cycling profile exhibits an enhanced electrochemical performance among the LCMO@PEDOT compared to that of pristine LCMO in a half‐cell configuration. Also, the LCMO@PEDOT: 0.5–3 wt.% is optimized to show better electrochemical performance. The diffusion coefficient calculated from both cyclic voltammetry and electrochemical impedance spectroscopy (EIS) exhibits an increase in the magnitude from PEDOT coating of 0.5 to 3 wt.% in the order of ≈10−12 cm2 s−1. An in‐operando X‐ray diffraction and in‐situ EIS are performed to validate the electrochemical activity. The full‐cell assembly is also fabricated with spinel Li4Ti5O12 (LTO) anode under balanced loading conditions. The LCMO@PEDOT (1–3 wt.%)/LTO exhibits better electrochemical performance compared to pristine LCMO/LTO. In addition, a temperature study of full‐cell is carried out within the range of −10 to 20 °C and compared.
Wood Derived Flexible and Spongy Architectures for Advanced Electrochemical Energy Storage and Conversion
Authors: Patil Rahul , Mishra Meemansha , Liu Shude , Jun Seong Chan , Dutta Saikat 
Published: September 2023

AbstractWood‐based flexible and porous architectures are currently receiving extensive attention in the development of flexible devices. The unique water adsorption properties of natural wood enable rapid and spontaneous water uptake, leading to concentration differences that facilitate the diffusion of ions with opposite charges. This article gives a summary of the differences between flexible and porous architectures made from natural wood. It also gives a detailed look at the porous architecture, which is made up of nanochannels, low‐tortuosity channels, and single‐atom sites to improve the electrochemical performance of supercapacitors, metal‐air batteries, lithium‐sulfur batteries, and lithium‐oxide batteries. Moreover, the processing approaches that utilize cell wall engineering to transform flat wood sheets into adaptable 3D structures such as flexible films and foams are described. Finally, some existing challenges and future perspectives faced by wood‐based flexible and spongy architectures for electrochemical energy conversion and storage are described.
Deep Learning‐Based Classification of Image Data Sets Containing 111 Different Seeds
Authors: Tugrul Bulent , Eryigit Recep , Ar Yilmaz 
Published: September 2023

AbstractImage analysis plays a crucial role in understanding and protecting biodiversity. A wide variety of images are used in research on identifying and classifying plants, including stems, leaves, flowers, and fruits. In order to increase crop production, more research needs to be done on the image analysis of seeds. This study aims to fill the gap in this field by creating an image data set of 111 different species in 42 families. An improved Convolutional Neural Networks (CNNs) model is developed by adding new layers to the last layers of the well‐known CNNs in the literature. A well‐balanced image data set is used to train the proposed model and calculate its performance. The accuracy of the custom CNNs model for seed classification is between 91% and 94%. The custom model's top‐2 and top‐3 accuracy values are 98.56% and 98.92%, respectively. The proposed CNNs model shows encouraging results in terms of accuracy and computation time for seed classification and recognition.
Dually Sulphophilic Chromium Boride Nanocatalyst Boosting Sulfur Conversion Kinetics Toward High‐Performance Lithium–Sulfur Batteries
Authors: Li Hongyang , Chen Guxian , Zhang Kailong , Wang Liangbiao , Li Gaoran 
Published: September 2023

AbstractThe sluggish kinetics of sulfur conversions have long been hindering the implementation of fast and efficient sulfur electrochemistry in lithium–sulfur (Li–S) batteries. In this regard, herein the unique chromium boride (CrB) is developed via a well‐confined mild‐temperature thermal reaction to serve as an advanced sulfur electrocatalyst. Its interstitial‐alloy nature features excellent conductivity, while the nano‐lamination architecture affords abundant active sites for host‐guest interactions. More importantly, the CrB nanocatalyst demonstrates a dual sulphophilicity with simultaneous Cr─S and B─S bondage for establishing strong interactions with the intermediate polysulfides. As a result, significant stabilization and promotion of sulfur redox behavior can be achieved, enabling an excellent Li–S cell cyclability with a minimum capacity fading rate of 0.0176% per cycle over 2000 cycles and a favorable rate capability up to 7 C. Additionally, a high areal capacity of 5.2 mAh cm−2, and decent cycling and rate performances are still attainable under high sulfur loading and low electrolyte dosage. This work offers a facile approach and instructive insights into metal boride sulfur electrocatalyst, holding a good promise for pursuing high‐efficiency sulfur electrochemistry and high‐performance Li–S batteries.
Capturing Nano‐Scale Inhomogeneity of the Electrode Electrolyte Interface in Sodium‐Ion Batteries Through Tip‐Enhanced Raman Spectroscopy
Authors: Dinda Sirshendu , Trivedi Shivam , Roy Ananyo , Pammer Frank D. , Fichtner Maximilian 
Published: September 2023

AbstractA prime challenge in the development of new battery chemistries is the fundamental understanding of the generation of the electrode–electrolyte interface (EEI) and its evolution upon cycling. Tip‐enhanced Raman spectroscopy (TERS) under an inert gas atmosphere is employed to study the chemical components of the anode/cathode electrolyte interface in a sodium‐ion battery. After the first cycle, TERS reveals that the EEI mostly consists of organic carbonate/dicarbonate, oligoethylene oxides, α,β‐unsaturated vinyl ketones/acetates, and inorganic species ClO4−, ClO3−, and Na2CO3. Whereas after 5× cycling, the EEI composition has evolved to contain long chain monodentate or bridging/bidentate carboxylates and alkoxides. The TERS map reveals the nano‐scale heterogeneity present in the EEI layers and elucidates a multilayered nano‐mosaic coating structure. The sheer volume of Raman signature present in the TERS signal can completely unravel the mysteries regarding the chemical composition and may shed light to the physicochemical behavior of the EEI.
Interface Coating Design for Dynamic Voltage Stability of Solid‐State Batteries
Authors: Wang Yichao , Ye Luhan , Fitzhugh William , Chen Xi , Li Xin 
Published: September 2023

AbstractIntrinsic or interface thermodynamic voltage windows of solid electrolytes are often narrower than the operational voltage range needed by a full battery, thus various interface decomposition reactions can happen in a practical solid‐state battery. Experimentally, it is found that a proper battery design utilizing the reactions can lead to a dynamic evolution from interface instability to stability, giving the so‐called dynamic voltage stability for advanced battery performance. Here, first the state‐of‐the‐art understanding is articulated about how the dynamic voltage stability should be interpreted in physical picture and treated in computation, emphasizing the potential importance of nonequilibrium reaction pathways. The constrained ensemble computational approach is further applied across most types of solid‐state electrolytes to systematically evaluate and compare their dynamic stability voltage windows in response to the mechanical constriction effect. High‐throughput calculations are used to search for coating materials for different interfaces between sulfide, halide, and oxide electrolytes and typical cathode materials with enhanced dynamic voltage stability. A comparison with experiment is given to highlight the value of these computational predictions.
Healthy transition: Roadmap for young adults with Down syndrome to adulthood
Authors: Weaver Maya , McCormick Andrew 
Published: September 2023

AbstractHealthcare transition is the purposeful and planned process for preparing young adults with Down syndrome for an adult oriented healthcare system. Significant gaps of a delayed, incomplete, siloed and decentered transition can be avoided when transition is approached in a longitudinal and holistic manner. Young adults with Down syndrome are specifically vulnerable to these gaps as the combination of intellectual differences and healthcare complexity leads to the need for a process that allows for appropriate preparation to develop the skills and process for an appropriate. To establish a successful transition care plan, the six core elements of policy, tracking, readiness, planning, transfer of care, and complete transition will compose the scaffolding of the transition process and address these gaps in care. A comprehensive tool kit including policy statements, healthcare transition tracking forms, the TRAQ tool, and template portable medical summaries will operationalize those elements and counteract any gaps in the transition process.
Effects of cardiopulmonary resuscitation instructions on the outcomes of out‐of‐hospital cardiac arrest: An analysis of the JAAM‐OHCA registry
Authors: Inoue Tomoaki , Kaneda Kotaro , Ise Natsu , Koga Yasutaka , Yagi Takeshi , Todani Masaki , Nakahara Takashi , Fujita Motoki , Tsuruta Ryosuke 
Published: September 2023

AbstractAimTo determine whether dispatcher‐provided cardiopulmonary resuscitation (CPR) instructions improve the outcomes of out‐of‐hospital cardiac arrest (OHCA).MethodsCases registered in the Japanese Association for Acute Medicine Out‐of‐Hospital Cardiac Arrest (JAAM‐OHCA) Registry between June 2014 and December 2019 were included. Cases in which the dispatcher provided CPR instructions to the bystander were included in the “Instructions” group”, and cases without CPR instructions were included in the “No Instructions” group. The primary outcome was the proportion of patients with a favorable neurological outcome, defined as a Glasgow–Pittsburgh cerebral performance category scale of 1 to 2 at 1 month after OHCA.ResultsOverall, 51,199 patients with OHCA were registered in the JAAM‐OHCA Registry during the study period. Of these, 33,745 were eligible for the study, with 16,509 in the Instructions group and 17,236 in the No Instructions group. The proportion of patients with a favorable neurological outcome at 1 month after OHCA was inferior in the Instructions group than in the No Instructions group (2.3% versus 3.0%, p < 0.001). After adjustment for patient background characteristics, no association was found between CPR instructions provided by a dispatcher and favorable neurological outcomes at 1 month after OHCA (adjusted odds ratio, 1.000; 95% confidence interval, 0.869–1.151, p = 0.996).ConclusionThe present study found no clear clinical benefit of dispatcher‐provided CPR instructions on the neurological outcomes of cases with OHCA.
Forcing Twisted 1,7‐Dibromoperylene Diimides to Flatten in the Solid State: What a Difference an Atom Makes
Authors: Konidaris Konstantis F. , Zambra Marco , Giannici Francesco , Guagliardi Antonietta , Masciocchi Norberto 
Published: September 2023

AbstractPerylene diimides (PDI) are workhorses in the field of organic electronics, owing to their appealing n‐semiconducting properties. Optimization of their performances is widely pursued by bay‐atom substitution and diverse imide functionalization. Bulk solids and thin‐films of these species crystallize in a variety of stacking configurations, depending on the geometry of the stable conformation of the polyaromatic core. We here demonstrate that 1,7‐dibromo‐substituted perylene diimides, PDI(H2Br2), possessing a heavily twisted conformation in the gas phase, in solution and in the solids, can be easily flattened in the solid state into centrosymmetric molecules if the polyaromatic cores form π–π stabilized chains. This is achieved by using axial residues with low stereochemical hindrance, as guaranteed by a single CH2/NH spacer directly linked to the imide function. Structural powder diffraction and DFT calculations on four newly designed species of the PDI(H2Br2) class coherently show that, thanks to the flexibility of the N−X−Ar link (X=CH2/NH), flat cores are indeed obtained by overcoming the interconversion barrier between twisted atropoisomers, of only 26.5 kJ mol−1. This strategy may then be useful to induce “anomalously flat” polyaromatic cores of different kinds (substituted acenes/rylenes) in the solid state, towards suitable crystal packing and orbital interactions for improved electronic performances.
Fluorine‐Boosted Kinetic and Selective Molecular Sieving of C6 Derivatives
Authors: Moosa Basem , Alimi Lukman O. , Lin Weibin , Fakim Aliyah , Bhatt Prashant M. , Eddaoudi Mohamed , Khashab Niveen M. 
Published: September 2023

AbstractPorous molecular sorbents have excellent selectivity towards hydrocarbon separation with energy saving techniques. However, to realize commercialization, molecular sieving processes should be faster and more efficient compared to extended frameworks. In this work, we show that utilizing fluorine to improve the hydrophobic profile of leaning pillararenes affords a substantial kinetic selective adsorption of benzene over cyclohexane (20 : 1 for benzene). The crystal structure shows a porous macrocycle that acts as a perfect match for benzene in both the intrinsic and extrinsic cavities with strong interactions in the solid state. The fluorinated leaning pillararene surpasses all reported organic molecular sieves and is comparable to the extended metal–organic frameworks that were previously employed for this separation such as UIO‐66. Most importantly, this sieving system outperformed the well‐known zeolitic imidazolate frameworks under low pressure, which opens the door to new generations of molecular sieves that can compete with extended frameworks for more sustainable hydrocarbon separation.
Tuning Binding Strength of Multiple Intermediates towards Efficient pH‐universal Electrocatalytic Hydrogen Evolution by Mo8O26‐NbNxOy Heterocatalysts
Authors: Yang Yang , Liu Lijia , Chen Shuai , Yan Wenjun , Zhou Haiqing , Zhang Xian‐Ming , Fan Xiujun 
Published: September 2023

AbstractDeveloping efficient and robust hydrogen evolution reaction (HER) catalysts for scalable and sustainable hydrogen production through electrochemical water splitting is strategic and challenging. Herein, heterogeneous Mo8O26‐NbNxOy supported on N‐doped graphene (defined as Mo8O26‐NbNxOy/NG) is synthesized by controllable hydrothermal reaction and nitridation process. The O‐exposed Mo8O26 clusters covalently confined on NbNxOy nanodomains provide a distinctive interface configuration and appropriate electronic structure, where fully exposed multiple active sites give excellent HER performance beyond commercial Pt/C catalyst in pH‐universal electrolytes. Theoretical studies reveal that the Mo8O26‐NbNxOy interface with electronic reconstruction affords near‐optimal hydrogen adsorption energy and enhanced initial H2O adsorption. Furthermore, the terminal O atoms in Mo8O26 clusters cooperate with Nb atoms to promote the initial H2O adsorption, and subsequently reduce the H2O dissociation energy, accelerating the entire HER kinetics.
Visible‐Light Initiated Dispersion Photopolymerization of Styrene
Authors: Canterel Rémi , Lalevée Jacques , Bourgeat‐Lami Elodie , Lacôte Emmanuel , Lansalot Muriel 
Published: September 2023

AbstractPolystyrene (PS) particles were synthesized in ethanol/water mixture by dispersion polymerization using visible light irradiation, with either a N‐heterocyclic carbene borane‐based photoinitiating system (PIS) or a disulfide. With the full PIS and poly(ethylene glycol) methyl ether methacrylate (PEGMA) as stabilizer, the size distributions were broad and the amount of PEGMA had a strong impact on the experiment reproducibility. The addition of a base solved the problem, leading to faster polymerizations, narrower size distributions and larger particles. With the disulfide as sole PIS, bigger and narrowly distributed PS particles were again formed. Quantitative conversion was achieved in each system, with particle size ranging between 100 and 350 nm. The use of poly(N‐vinylpyrrolidone) as stabilizer led to significantly larger particles, up to 1.2 μm, with narrow size distributions. The production of such large latex particles by photoinitiated polymerizations is unprecedented.
Solar‐driven seawater production H2O2 catalyzed by hydroxyl functionalized crystalline K‐doped g‐C3N4 under ambient conditions
Authors: Luo Pan‐Pan , Li Xin‐Zhong , Qu Bei‐Bei , Xue Han‐Yu , Yang Yan‐Hui 
Published: September 2023

Three hydroxyl functionalized crystalline K‐doped g‐C3N4 were synthesized from dicyandiamide, melamine, ammonium chloride, ammonium oxalate, and ammonium citrate via ionothermal polycondensation using KCl as molten salt under N2 atmosphere, which served as efficient recyclable photocatalysis realized that generating H2O2 directly from seawater with air by 2e− ORR pathway under stimulated solar irradiation in ambient conditions. Under optimized conditions, the highest H2O2 production rate of 1622 μmol g−1 h−1 for duration of 10 h was obtained. The cycling performances of HPCN‐2 displayed reusable for five times without noticeably loss of its catalytic activity. This work presents a real safer, sustainable, and economical approach for production of H2O2 directly from abundant natural seawater.