bluuebunny/crossref_metadata_2025_split huggingface dataset:
Autogenetic Carbon Oxyanions Enable Interfacial OH− Deconfinement for Reinforced Biomass Electrooxidation over Wide Potential Window
Authors: Wang Keping , Wu Mei , Zhang Yan , Jiang Binbin , Su Yaqiong , Yang Song , Lu Xihong , Li Hu 
Published: December 2024

AbstractThe preferential adsorption toward OH− on the anode most likely blocks the accessibility of organic molecules and triggers competitive oxygen evolution reaction (OER), typically precipitating a narrow potential window. Here, an OH− deconfinement strategy enabled by CO32− self‐transformed from C2O42− on metallic nickel oxalate (NiC2O4) for efficient synthesis of bioplastic monomer 2,5‐furanedicarboxylic acid (FDCA) with faradaic efficiency of >95% via electrocatalytic 5‐hydroxymethylfurfural (HMF) oxidation reaction (e‐HMFOR) at a wider potential window of 1.38–1.56 VRHE, outperforming state‐of‐the‐art Ni‐based electrocatalysts is presented. In situ, tests corroborate that the construction of NiOOH with surface‐adsorbed CO32− (NiOOH‐CO32−) from NiC2O4 can be facilitated by self‐liberating CO32−. The CO32− ions serving as an electric field engine can effectively weaken OH− coverage through electrostatic repulsion and enhance HMF adsorption at the NiOOH‐CO32− surface, thereby heightening e‐HMFOR while inhibiting OER. Computational results further indicate that the CO32− on NiOOH hoists the energy barrier of oxygen intermediate conversion (O* → OOH*) to suppress OER but promotes the e‐HMFOR kinetics. The precise modulation of OH− adsorption behavior on the electrocatalyst offers a powerful kit for boosting the oxidative upgrading process while circumventing the competing reaction OER.
Ultrasensitive Detection of FEN1 Activity for Cancer Diagnosis Using a CRISPR/Cas13a‐Based Triple Cascade Amplification System
Authors: Cheng Xia , Zhao Wenchen , Chen Daixi , Ren Dandan , Qian Tianwei , Xia Xinyi , Wang Xiaohong , Li Qijun , Yang Jianjun , Gu Yan , Zhang Peng , Yin Kun , Yu Ping , Dong Wenpei 
Published: December 2024

AbstractFlap endonuclease 1 (FEN1) is closely associated with tumor progression and proliferation, making it a promising biomarker for cancer diagnosis. However, developing a sensitive, reliable, and user‐friendly method for quantitative FEN1 detection remains technically challenging. In this study, an ultrasensitive FEN1 biosensor is established using a target‐induced cleavage‐ligation‐transcription‐activation cascade strategy (LTACas13a) to enhance the cleavage ability of CRISPR/Cas13a. The LTACas13a method has shown excellent performance in screening FEN1 inhibitors and detecting endogenous FEN1 activity in living cells, as well as in clinical biological samples such as human serum and tissue samples. Additionally, using a universal dumbbell probe derived from FEN1, a multiplex LTACas13a strategy is developed for detecting various DNA glycosylases, including formamidopyrimidine DNA glycosylase, uracil DNA glycosylase, and human alkyl adenine DNA glycosylase. This straightforward approach provides a reliable and effective diagnostic tool for early‐stage cancer detection and offers significant opportunities for FEN1 biosensing and related drug discovery.
Reticulating Crystalline Porous Materials for Asymmetric Heterogeneous Catalysis
Authors: Han Xing , Li Weiwei , Yang Bolinyishi , Jiang Chao , Qu Zan , Xu Haomiao , Liu Yan , Cui Yong 
Published: December 2024

AbstractAsymmetric catalysis is essential for addressing the increasing demand for enantiopure compounds. Recent advances in reticular chemistry have demonstrated that metal–organic frameworks (MOFs) and covalent organic frameworks (COFs) possess highly regular porous architectures, exceptional tunability, and the ability to incorporate chiral functionalities through their open channels or cavities. These characteristics make them highly effective and enantioselective catalysts for a wide range of asymmetric transformations. The chiral microenvironments within these frameworks facilitate precise control over reactant orientation and transition states, enhancing both catalytic activity and enantioselectivity, thereby offering significant advantages over traditional systems. This review overviews recent developments in chiral MOFs (CMOFs) and chiral COFs (CCOFs), focusing on their design strategies, and synthetic methods, and highlights the structure–property relationships that connect key structural features to asymmetric catalytic performance. Additionally, the current challenges and future prospects in this field are addressed, highlighting the pivotal role of reticular chemistry in the creation of chiral porous materials. It is anticipated that this review will inspire further research into the application of crystalline porous materials in asymmetric catalysis and promote the rational design of novel chiral heterogeneous catalysts for industrial use.
Nanoliter Hydrogel Array for Cell Screening and Cell Spheroid Sorting
Authors: Salarian Maryam , Levkin Pavel A. , Popova Anna A. 
Published: December 2024

AbstractThe transition from two‐dimensional (2D) to physiologically relevant three‐dimensional (3D) cell models has revolutionized biomedical research. Hydrogels are frequently used to produce 3D models for tissue engineering, disease modeling, and high‐throughput screenings (HTS). However, integrating 3D cultures into HTS workflows presents challenges, including automation compatibility and cost constraints. Addressing these challenges requires innovative approaches that enable miniaturization, automation, and cost reduction while maintaining experimental fidelity. The Droplet Microarray platform, based on hydrophilic‐superhydrophobic surface patterning, facilitates the formation of nanoliter‐hydrogel arrays containing cells or spheroids. This method allows dispensing of hundreds of nanoliter‐hydrogel droplets with precise control over volume and cell density, reducing reagent consumption and offering high‐throughput applications. Here, we demonstrate stable nanoliter‐hydrogel arrays on a chip, enabling experimental procedures such as washing and medium immersion. Our approach demonstrates that spheroid‐containing droplets can be gelled at any point of the experiment, allowing for the fixation of cell structures on the surface. The selective gelation of individual droplets enables spheroid sorting by stabilizing desired droplets while pooling the others. This method holds the potential for HTS and miniaturized workflows in 3D microenvironments, thereby advancing research in different fields such as cell, cell spheroid, or organoid screenings, drug screenings, and precision medicine.
Spectro‐Spatial Unmixing in Optical Microspectroscopy for Thickness Determination of Layered Materials
Authors: Schwarz Julian , Niebauer Michael , Römling Lukas , Pham Adrian , Koleśnik‐Gray Maria , Evanschitzky Peter , Vogel Nicolas , Krstić Vojislav , Rommel Mathias , Hutzler Andreas 
Published: December 2024

AbstractVan der Waals materials and devices incorporating them exhibit highly thickness‐dependent properties. The small lateral dimensions of mechanically exfoliated 2D‐layered flakes, however, remarkably complicate their precise thickness determination. Quantitative analysis of reflectance measurements using optical microspectroscopy is proven to be as precise as spectroscopic ellipsometry while providing an easily adaptable and non‐destructive method for thickness determination. The use of magnifying objective lenses allows obtaining the reflectance within a measurement spot of only a few microns in diameter. When the dimensions of exfoliated flakes are even smaller, however, the acquired reflectance is a superposition of those of the material of interest and the subjacent materials. To overcome this limitation, a facile approach to reduce the resolvable structure size by combining the evaluation of the reflectance measurement via transfer matrix method with spatial information extracted from optical micrographs is introduced. The efficacy when characterizing micrometer‐sized flakes is exemplarily demonstrated for thickness determination of highly oriented pyrolytic graphite and a thin film of silicon dioxide. It is shown that a maximum error of less than 10% is achieved even when the flake only covers 20% of the measurement spot.
High‐Efficiency and Stable Green InP‐QLED Enabled by Lowering Electron Injection Barrier
Authors: Chen Mengyuan , Li Qian , Bian Yangyang , Wang Shuaibing , Hu Binbin , Tang Aiwei , Chen Fei , Lv Yanbing , Shen Huaibin 
Published: December 2024

AbstractThe external quantum efficiencies (EQE) and luminances of red InP‐based and blue ZnTeSe‐based quantum dot light‐emitting diodes (QLEDs) have exceeded 20% and 80 000 cd m−2, respectively, and the T50@100 cd m−2 (time for the luminance decreasing by 50%) operational lifetime of red InP‐based QLEDs also have exceeded 1 000 000 h, nearing industrial application standards. However, the low EQE, luminance, and inferior lifetime of green InP‐based QLEDs restrict the application for their full‐color Cd‐free display and lighting applications. The large electron injection barrier and severe exciton quenching caused by defect states of ZnMgO (ZMO) nanoparticles (NPs) lead to lower electron concentration in the emitting layer, which results in reduced radiative recombination. Here, with the surface passivation of MgCl2, the exciton quenching sites are significantly suppressed, and the electron injection barrier is reduced owing to the conduction band minimum (CBM) levels upshift of ZMO. As a result, a high EQE of 21.43%, maximum luminance of 25 5985 cd m−2, along with a long T50@1000 cd m−2 (over 4 600 h) and T50@100 cd m−2 (over 290 000 h) operational lifetime is achieved for green InP‐based QLEDs. These values have all exceeded the previous best values of green InP‐based QLEDs.
(C6H5N2)HgCl3: Discovery of a Polar Hg‐Based Hybrid Halide as Preeminent Nonlinear Optical and Birefringent Material Activated by π‐Conjugated Organic Cation Substitution
Authors: Tang Ru‐Ling , Yang Die‐Xue , Ma Liang , Lv Yi‐Lei , Liu Wenlong , Guo Sheng‐Ping 
Published: December 2024

AbstractHybrid organic–inorganic halides have attracted widespread attention due to their multiple optical performances. The combination of distorted metal cation polyhedra and π‐conjugated organic ions is an effective strategy to derive hybrid nonlinear optical (NLO) and birefringent crystals. Here, a new acentric 4‐cyanopyridine mercury halide, (C6H5N2)HgCl3, have been obtained via replacing an inorganic cation with an organic cation based on parent compound CsHgCl3. (C6H5N2)HgCl3 shows the strongest second harmonic generation (SHG) effect among mercury‐pyridine hybrid metal halides, with an intensity of 3.04 times of KH2PO4 (KDP) at 1.064 µm laser radiation. The crystal structure of (C6H5N2)HgCl3 is composed of specially [HgCl3]∞ chains and [(C6H5N2)+] cations. Additionally, (C6H5N2)HgCl3 shows an outstanding experimental birefringence (Δn = 0.360@0.546 µm), which is the largest value among mercury‐based hybrid halides, and its birefringence is greater than those of all inorganic metal halide birefringent crystals. The discovery of (C6H5N2)HgCl3 indicates the potential advantage of mercury‐based hybrid halides in optical materials.
Metasurface‐Enabled Cascaded Multispectral Polarization Structures Along the Longitudinal Direction
Authors: Li Yan , Yu Qunxing , Zhao Shuaifu , Yuan Quan , Zhong Facheng , Chen Xianzhong , Wang Shuming 
Published: December 2024

AbstractGeneration and manipulation of polarization structures have attracted significant interest due to their unusual optical features and extensive applications. Multispectral information can further increase the information capacity of polarization structures. However, generating multiple cascaded multispectral polarization numbers (letters) at multiple planes arranged along light propagation has not been reported. A geometric metasurface is used to experimentally realize eight cascaded multispectral polarization numbers (letters) at predesigned observation planes along the longitudinal direction. The efficacy of this approach is demonstrated by encoding a single polarization number (letter) with two wavelengths and cascading two polarization numbers with orthogonal polarization rotation angles. Different two‐color polarization numbers (letters) are generated by controlling the incident wavelength, while their polarization distributions are modulated by controlling the incident linear polarization. This approach integrates two‐dimentional (2D) polarization generation, multiple colors, longitudinal control, and cascading design, providing extra degrees of freedom for customized polarization design and enabling small‐volume polarization systems for color display, image steganography, and optical encryption.
Supporting Effect and Influence Law of Energy‐Absorbing Rockbolts in Soft Rock Roadway with Large Deformation
Authors: Yang Ning , Su Li‐yang , Li Wei‐teng , Li Xiu‐ming , Wang Li‐yuan , Mei Yu‐chun , Sun Bing‐jun 
Published: December 2024

AbstractTo clarify the supporting effect and influencing factors of energy‐absorbing rockbolts in soft rock roadways with large deformation, by considering four factors including rock deformation, plastic zone, rockbolt force, and stress of the surrounding rock, comparative analysis of no‐rockbolt, conventional rockbolt, and energy‐absorbing rockbolt schemes is conducted. The effect of the energy‐absorbing rockbolt is analyzed based on a self‐developed numerical simulation program, and a study is conducted on the influence of five factors such as the energy‐absorption starting axial force, ultimate yielding distance on the supporting effect. The results show that: 1) Compared to conventional rockbolts, the energy‐absorbing rockbolts maintain a intact support system and continuously providing support resistance within 75 d of calculation. 2) Energy‐absorbing rockbolts significantly increase the maximum and minimum principal stresses of the roadway. The increase in maximum principal stress significantly enhances the range of the bearing arch in the surrounding rock. Energy‐absorbing rockbolts have a high capacity to compensate for radial stresses unloaded. 3) The greater the energy‐absorption starting axial force, the more significant the compensation effect of the rockbolts on the radial stress. Appropriately increasing the ultimate yielding distance and rockbolt length can effectively prevent rockbolt failure and control the area of plastic zone.
Comparing Large Language Models and Human Programmers for Generating Programming Code
Authors: Hou Wenpin , Ji Zhicheng 
Published: December 2024

AbstractThe performance of seven large language models (LLMs) in generating programming code using various prompt strategies, programming languages, and task difficulties is systematically evaluated. GPT‐4 substantially outperforms other LLMs, including Gemini Ultra and Claude 2. The coding performance of GPT‐4 varies considerably with different prompt strategies. In most LeetCode and GeeksforGeeks coding contests evaluated in this study, GPT‐4, employing the optimal prompt strategy, outperforms 85 percent of human participants in a competitive environment, many of whom are students and professionals with moderate programming experience. GPT‐4 demonstrates strong capabilities in translating code between different programming languages and in learning from past errors. The computational efficiency of the code generated by GPT‐4 is comparable to that of human programmers. GPT‐4 is also capable of handling broader programming tasks, including front‐end design and database operations. These results suggest that GPT‐4 has the potential to serve as a reliable assistant in programming code generation and software development. A programming assistant is designed based on an optimal prompt strategy to facilitate the practical use of LLMs for programming.
The Gut Microbiota Affects Anti‐TNF Responsiveness by Activating the NAD+ Salvage Pathway in Ulcerative Colitis
Authors: Lei Jing , Lv Lin , Zhong Li , Xu Feng , Su Wenhao , Chen Yan , Wu Zhixuan , He Song , Chen Yongyu 
Published: December 2024

AbstractApproximately 50% of the patients with ulcerative colitis (UC) are primarily nonresponsive to anti‐tumor necrosis factor (TNF) therapy or lose their responsiveness over time. The gut microbiota plays an important role in the resistance of UC to anti‐TNF therapy; however, the underlying mechanism remains unknown. Here, it is found that the transplantation of gut fecal microbiota from patients with UC alters the diversity of the gut microbiota in dextran sulfate sodium‐induced colitis mice and may affect the therapeutic responsiveness of mice to infliximab. Furthermore, the abundances of Romboutsia and Fusobacterium increase in the tissues of patients with UC who do not respond to anti‐TNF therapy. Differentially abundant metabolites are mainly enriched in nicotinate and nicotinamide metabolism in NCM460 cells after Fusobacterium nucleatum infection. Mechanistically, F. nucleatum promotes the nicotinamide adenine dinucleotide (NAD+) salvage pathway by upregulating NAMPT expression, which subsequently leads to the activation of the p38 mitogen‐activated protein kinase (MAPK) signaling pathway and promotes the secretion of inflammatory factors, ultimately inhibiting the therapeutic response to anti‐TNF drugs. These findings demonstrate that the gut microbiota can influence the response to anti‐TNF therapy in patients with UC and highlight the therapeutic potential of targeting F. nucleatum and its associated pathways for preventing and treating drug resistance in UC.
Polyethyleneimine‐Based Cryogels Enabling the Selective and Reversible Adsorption of Chlorine
Authors: Lorente Alejandro , Sturm Johanna S. , Kleoff Merlin , Lorenz Fabio , Voßnacker Patrick , Wagner Olaf , Haag Rainer , Riedel Sebastian 
Published: December 2024

AbstractHerein hyperbranched polyethyleneimine (hPEI) cryogels are reported for the selective and reversible adsorption of elemental chlorine. The cryogels are prepared in an aqueous solution by crosslinking with glutaraldehyde at subzero temperatures. The final macroporous composites bearing ammonium chloride groups are obtained after freeze‐drying. The cryogels CG1[Cl]–CG3[Cl] adsorb chlorine with capacities of 0.22–0.26 g Cl2/g cryogel as an average over three adsorption‐desorption cycles. The adsorption process is based on the reversible and selective halogen bonding of chlorides (Cl−) with chlorine (Cl2) forming the corresponding trichloride ([Cl3]−) species, indicated by Raman spectroscopy. The reversibility of chlorine adsorption is shown by applying heat and vacuum to the loaded cryogel CG1[Cl3] releasing 63% of the adsorbed chlorine within 3 h and 72% within 16 h. The unique ability to selectively adsorb chlorine in the presence of other gases is successfully employed for the selective adsorption of chlorine from a gas mixture, potentially enabling the recycling of chlorine from tail gas streams.
A Stage‐Gate Framework for Upscaling of Single‐Junction Perovskite Photovoltaics
Authors: Forberich Karen , Albrecht Steve , Castriotta Luigi Angelo , Distler Andreas , Hauch Jens , Kirchartz Thomas , Paetzold Ulrich W. , Schorr Susan , Sprau Christian , Stannowski Bernd , Ternes Simon , Unger Eva , Unold Thomas , Brabec Christoph J. 
Published: December 2024

AbstractTo address the challenge of upscaling single‐junction perovskite photovoltaics (PV) toward market‐relevant performance in a structured and efficient manner, a stage‐gate approach that divides the process into stages according to technology readiness levels (TRLs) is proposed. Whereas the first stage contains only material research, the later stages are concerned with the development from lab‐scale devices to large‐area modules, and properties such as device size as well as processing methods are adapted step‐by‐step toward commercializable techniques. The stages are connected by gates that specify the criteria that must be met for a material or process to be transferred to the next stage. In addition, a literature survey for the keywords “perovskite” and “module” is performed. This analysis shows that most of the reported modules have an area between 10 cm2 and 20 cm2, corresponding to stage 3 or TRL 5 in the scheme, and operational stability is often incompletely reported. These findings analysis indicate a significant gap in the research focus on large‐area modules and elevated stress and field tests, which are essential for transitioning to commercial applications. It is suggested to use the proposed stage‐gate process as an efficient and structured guideline toward commercializing perovskite PV.
Molecular Insights into the Interfacial Phenomena at the Li Metal | Polymer Solid‐State Electrolyte in Anode‐Free Configuration During Li Plating‐Stripping via Advanced Operando ATR‐FTIR Spectroscopy
Authors: Wang Jian‐Fen , Weiling Matthias , Pfeiffer Felix , Liu Kun‐Ling , Baghernejad Masoud 
Published: December 2024

AbstractSolid‐state batteries are regarded as safe and high‐energy‐density candidates for next‐generation energy storage. However, gaining a mechanistic understanding of the interfacial phenomena under real electrochemically working conditions remains a major challenge for cells containing solid‐state electrolytes. This work presents an in‐house built attenuated total reflection fourier‐transform infrared (ATR‐FTIR) spectroscopy cell equipped with an internal temperature‐control unit. This cell is used for operando characterization of interfacial processes between plated Li and polymer during Li plating/stripping. As a proof of concept, a polymer electrolyte (cr‐PEO10LiTFSI) containing poly(ethylene oxide), Li bis‐(trifluoromethanesulfonyl)imide and crosslink‐initiator benzophenone (BP) is introduced on a copper mesh as current collector at 60 °C. The developed ATR‐FTIR spectroscopy setup provides detailed insights into the electrolyte degradation and reveals the crystallinity transformation of PEO at the interface during plating. Moreover, for the first time, the degradation of BP is observed. This compound, often overlooked in electrolyte systems due to its low concentration, is found to play a significant role in the interfacial electrochemistry process. Overall, this study provides a comprehensive overview of the characterization on the PEO electrolyte‐lithium metal interface and introduces a novel perspective on the reaction of BP as a crosslinking initiator in the solid‐state batteries.
PtRu Intra‐Cluster Electron Modulation Accelerates Multi‐Scenario Hydrogen Evolution Reaction
Authors: Zhao Xue , Jiang Yaling , Wang Dan , Zhang Yicheng , Chen Mengshan , Hu Guangzhi , Zhang Haibo , Jin Zhong , Zhou Yingtang 
Published: December 2024

AbstractThe development of advanced nanomaterial manufacturing technology and the in‐depth analysis of the structure‐activity relationship are conducive to the sustainable development of platinum‐based catalysts in terms of low cost and high performance. The in situ conversion of Pt4+ and Ru3+ is creatively achieved into highly dispersed, small‐sized heterojunction clusters in the confined space by reductant preset framework materials, and these clusters benefited from the hollow carbon spheres gap supramolecular self‐assembly strategy to achieve high exposure. The intra‐cluster Ru→Pt electron transfer and induced electronic structure modulation enhance the adsorption and activation of H2O molecules at the interface, accelerating the desorption coupling of [H] at the Pt or Ru site. As a catalyst, PtRu/BNHCSs have achieved significant hydrogen production from electrolyzed water in multiple scenarios, exceeding the performance of the commercial Pt/C catalyst. These scenarios include high‐current water splitting to hydrogen in both pH‐neutral and simulated seawater, direct seawater hydrogen production, and anion‐exchange membrane integrated continuous and efficient electrolytic hydrogen production. In situ Fourier transform infrared and in situ Raman interface monitoring techniques reveal the interfacial adsorption behavior of H2O, providing important experimental and theoretical insights for understanding and revealing the synergistic effect and the interfacial reaction behavior of intra‐cluster atoms of PtRu heterojunction.