bluuebunny/crossref_metadata_2025_split huggingface dataset:
Enhanced Thermoelectric Performance in GeTe by Synergy of Midgap state and Band Convergence
Authors: Guo Zhe , Wu Gang , Tan Xiaojian , Wang Ruoyu , Zhang Zongwei , Wu Guangjie , Zhang Qiang , Wu Jiehua , Liu Guo‐Qiang , Jiang Jun 
Published: December 2022

AbstractThe good co‐existence of midgap state and valence band degeneracy is realized in Bi‐alloyed GeTe through the In‐Cd codoping to play different but complementary roles in the valence band structure modification. In doping induces midgap state and results in a considerably improved Seebeck coefficient near room temperature, while Cd doping significantly increases the Seebeck coefficient in the mid‐high temperature region by promoting the valence band convergence. The synergistic effects obviously increase the density of state effective mass from 1.39 to 2.65 m0, and the corresponding carrier mobility still reaches 34.3 cm2 V−1 s−1 at room temperature. Moreover, the Bi‐In‐Cd co‐alloying introduces various phonon scattering centers including nanoprecipitates and strain field fluctuations and suppresses the lattice thermal conductivity to a rather low value of 0.56 W m−1 K−1 at 600 K. As a result, the Ge0.89Bi0.06In0.01Cd0.04Te sample obtains excellent thermoelectric properties of zTmax ≈2.12 at 650 K and zTavg ≈1.43 between 300 and 773 K. This study illustrates that the thermoelectric performance of GeTe can be optimized in a wide temperature range through the synergy of midgap state and valence band convergence.
Graphene Oxide‐Assisted Multiple Cross‐Linking of MXene for Large‐Area, High‐Strength, Oxidation‐Resistant, and Multifunctional Films
Authors: Li Bin , Wu Na , Yang Yunfei , Pan Fei , Wang Changxian , Wang Gang , Xiao Long , Liu Wei , Liu Jiurong , Zeng Zhihui 
Published: December 2022

AbstractTransition metal carbides/nitrides (MXenes) with metallic electrical conductivity and excellent processability attract increasing attention for assembling multifunctional macrostructures. However, the challenges, involving poor mechanical strength, inferior oxidation stability, and limited scalable manufacturing, impede their wide applications. Herein, the large‐area, high‐strength, ultra‐flexible hybrid films are developed through the multiple physical and chemical cross‐linking of MXene/cellulose films facilitated by graphene oxide. The MXene‐based films manifest significantly improved hydrophobicity, water/solvent resistance, and oxidation stability, and meanwhile, maintain excellent conductivity and electromagnetic interference shielding performance. The X‐band surface‐specific shielding effectiveness (SE) of 18,837.5 dB cm2 g−1 and an SE over 60 dB in an ultra‐broadband frequency range are achieved, comparable to the best shields ever reported. Furthermore, the wearable films demonstrate excellent photothermal antibacterial and electrothermal deicing applications. Thus, such high‐performance MXene‐based films developed through a facile and scalable manufacturing method have substantial application prospects in flexible electronics, thermotherapy, electromagnetic compatibility, and aerospace.
Photo‐Driven Hydrogen Production from Methanol and Water using Plasmonic Cu Nanoparticles Derived from Layered Double Hydroxides
Authors: Li Zhenhua , Liu Jinjia , Zhao Jiaqi , Shi Run , Waterhouse Geoffrey I. N. , Wen Xiao‐Dong , Zhang Tierui 
Published: December 2022

AbstractMethanol steam reforming (MSR) is viewed as an important technology in the growth of a future hydrogen economy, with methanol serving as an easily transportable and storable liquid hydrogen carrier. However, the thermocatalytic MSR reaction is energy intensive as it requires high temperatures. Herein, a novel L‐Cu catalyst is successfully fabricated for photo‐driven MSR through reduction of CuAl layered double hydroxide (CuAl‐LDH) nanosheets. L‐Cu offers outstanding activity for the photothermal conversion of methanol and water to hydrogen (160.5 µmol gcat−1 s−1) under ultraviolet‐visible irradiation, with this rate being much higher than that achieved for L‐Cu at the same temperature in the dark. Characterization studies using X‐ray diffraction, X‐ray photoelectron spectroscopy, X‐ray absorption spectroscopy, and high‐resolution transmission electron microscopy determine that L‐Cu catalyst comprise Cu nanoparticles on an amorphous alumina support. Computational calculations reveale that Cu localized surface plasmon resonance effects promote the activation of H2O, thereby underpinning the remarkable hydrogen production rates achieved during photo‐driven MSR. This study introduces a novel photothermal strategy for hydrogen generation from methanol, demonstrating the enormous potential of photothermal catalysis in the chemical and energy sectors.
A Highly Active, Long‐Lived Oxygen Evolution Electrocatalyst Derived from Open‐Framework Iridates
Authors: Yang Lan , Shi Lei , Chen Hui , Liang Xiao , Tian Boyuan , Zhang Kexin , Zou Yongcun , Zou Xiaoxin 
Published: December 2022

AbstractThe acidic oxygen evolution reaction underpins several important electrical‐to‐chemical energy conversions, and this energy‐intensive process relies industrially on iridium‐based electrocatalysts. Here, phase‐selective synthesis of metastable strontium iridates with open‐framework structure and their unexpected transformation into a highly active, ultrastable oxygen evolution nano‐electrocatalyst are presented. This transformation involves two major steps: Sr2+/H+ ion exchange in acid and in situ structural rearrangement under electrocatalysis conditions. Unlike its dense perovskite‐structured polymorphs, the open‐framework iridates have the ability to undergo rapid proton exchange in acid without framework amorphization. The resulting protonated iridates further reconstruct into ultrasmall, surface‐hydroxylated, (200) crystal plane‐oriented rutile nanocatalyst, instead of the common amorphous IrOxHy phase, during acidic oxygen evolution. Such microstructural characteristics are found to benefit both the oxidation of hydroxyls and the formation of OO bonds in electrocatalytic cycle. As a result, the open‐framework iridate derived nanocatalyst gives a comparable catalytic activity to the most active iridium‐based oxygen evolution electrocatalysts in acid, and retains its catalytic activity for more than 1000 h.
Self‐Assembly of Nanocrystalline Structures from Freestanding Oxide Membranes
Authors: Harbola Varun , Wu Yu‐Jung , Wang Hongguang , Smink Sander , Parks Sarah C. , van Aken Peter A. , Mannhart Jochen 
Published: December 2022

AbstractThe exploration of crystalline nanostructures enhances the understanding of quantum phenomena occurring in spatially confined quantum matter and may lead to functional materials with unforeseen applications. A novel route to fabricating nanocrystalline oxide structures of exceptional quality is presented. This is achieved by utilizing a self‐assembly process of ultrathin membranes composed of the desired oxide. The thermally induced self‐assembly of nanocrystalline structures is driven by dewetting the oxide membranes once they are lifted off and transferred onto sapphire surfaces. In three successive steps, the process provides nanovoids, nanowires, and nanocrystals. Regardless of substrate orientation, the nanostructures are highly anisotropic in shape due to material retraction favoring low‐index crystalline lattice directions of the membranes. The orientation of the nanostructures is provided precisely by the crystal lattice of the transferred membrane. The microstructure of the nanocrystals exhibits exceptional quality, characterized by a pristine crystal structure and uniform stoichiometry, both maintained all the way down to the well‐developed crystalline facets. The demonstrated self‐assembly process holds the potential to improve the understanding of surface diffusion phenomena at the interface of materials, which is important for advancing epitaxial growth technology and paves the way to fabricating crystalline nanostructures by the transfer and self‐assembly of membranes.
Synergetic Passivation of Metal‐Halide Perovskite with Fluorinated Phenmethylammonium toward Efficient Solar Cells and Modules
Authors: Zhu Yanqing , Lv Pin , Hu Min , Raga Sonia R. , Yin Huiyu , Zhang Yuxi , An Ziqi , Zhu Qinglong , Luo Gan , Li Wangnan , Huang Fuzhi , Lira‐Cantu Monica , Cheng Yi‐Bing , Lu Jianfeng 
Published: December 2022

AbstractSurface passivation with organic halide salts is a powerful strategy to enhance the performance of perovskite solar cells. However, the inevitable formed in‐plane favored two‐dimensional perovskite layers with low carrier mobility and high binding energy inhibit the interfacial charge transfer within the device. Herein, a bulky fluorinated phenmethylammonium salt is designed and synthesized to passivate the perovskite film without forming 2D perovskites. A strong interaction which is induced by an electron donation from passivation agent to perovskite not only reduces the defects at the top surface of the perovskite, but also suppresses the recombination reaction at the buried surface due to a permeation of the organic halide salt. Moreover, the results of time resolved photoluminescence and confocal microscopy images suggest that the interfacial charge transfer speed and uniformity are enhanced. As a result, the efficiency of a small‐area device increases from 20.7 ± 0.9% to 22.8 ± 0.4% (aperture: 0.16 cm2). Moreover, a stabilized efficiency of 18.0% (aperture: 10.0 cm2) is achieved for larger‐area modules with 6‐series connected sub‐cells. Equally important, the non‐encapsulated modules show significantly improved stability at ambient conditions (ISOS‐D‐1). These significant improvements provided by a simple and reproducible procedure can be readily adopted in other types of devices.
Double‐Dependence Correlations in Graphdiyne‐Supported Atomic Catalysts to Promote CO2RR toward the Generation of C2Products
Authors: Sun Mingzi , Wong Hon Ho , Wu Tong , Lu Qiuyang , Lu Lu , Chan Cheuk Hei , Chen Baian , Dougherty Alan William , Huang Bolong 
Published: December 2022

AbstractDeveloping efficient and stable atomic catalysts (ACs) to achieve high faradaic efficiency and selectivity of C2products is a significant challenge for research on the CO2reduction reaction (CO2RR). Although significant efforts have been devoted to this endeavor, the understanding of C2pathways and the influences of metal selection and active sites on the CO2RR still remain unclear. Herein, this work presents a comprehensive theoretical exploration of full C2reaction pathway mapping based on graphdiyne (GDY)‐supported ACs with considerations of different metals and active sites for the first time. This work demonstrates the integrated large‐small cycle mechanism to explain the challenges for C2product generation, where the double‐dependence correlation with metal and active sites is identified. A series of novel transition metal based GDY‐SACs, GDY‐Pr, and GDY‐Pm SACs are demonstrated as promising electrocatalysts to generate CH3CH2OH, CH3COOH, CH3CHO, and CH2OHCH2OH while the formation of C2H4is very difficult for all GDY‐ACs. First‐principle machine learning predicts the reaction energy for the first time, where the adsorptions of the intermediates are critical to achieving accurate predictions of multi‐carbon products. This work supplies an advanced understanding of the complicated CO2RR mechanisms, which is expected to aid the development of novel atomic catalysts for efficient C2product generation.
Longitudinal Synaptic Density PET with 11C‐UCB‐J 6 Months After Ischemic Stroke
Authors: Michiels Laura , Thijs Liselot , Mertens Nathalie , Coremans Marjan , Vandenbulcke Mathieu , Verheyden Geert , Koole Michel , Van Laere Koen , Lemmens Robin 
Published: December 2022

ObjectiveThe purpose of this study was to explore longitudinal changes in synaptic density after ischemic stroke in vivo with synaptic vesicle protein 2A (SV2A) positron emission tomography (PET).MethodsWe recruited patients with an ischemic stroke to undergo 11C‐UCB‐J PET/MR within the first month and 6 months after the stroke. We investigated longitudinal changes of partial volume corrected 11C‐UCB‐J standardized uptake value ratio (SUVR; relative to centrum semiovale) within the ischemic lesion, peri‐ischemic area and unaffected ipsilesional and contralesional grey matter. We also explored crossed cerebellar diaschisis at 6 months. Additionally, we defined brain regions potentially influencing upper limb motor recovery after stroke and studied 11C‐UCB‐J SUVR evolution in comparison to baseline.ResultsIn 13 patients (age = 67 ± 15 years) we observed decreasing 11C‐UCB‐J SUVR in the ischemic lesion (ΔSUVR = −1.0, p = 0.001) and peri‐ischemic area (ΔSUVR = −0.31, p = 0.02) at 6 months after stroke compared to baseline. Crossed cerebellar diaschisis as measured with 11C‐UCB‐J SUVR was present in 11 of 13 (85%) patients at 6 months. The 11C‐UCB‐J SUVR did not augment in ipsilesional or contralesional brain regions associated with motor recovery. On the contrary, there was an overall trend of declining 11C‐UCB‐J SUVR in these brain regions, reaching statistical significance only in the nonlesioned part of the ipsilesional supplementary motor area (ΔSUVR = −0.83, p = 0.046).InterpretationAt 6 months after stroke, synaptic density further declined in the ischemic lesion and peri‐ischemic area compared to baseline. Brain regions previously demonstrated to be associated with motor recovery after stroke did not show increases in synaptic density. ANN NEUROL 2023;93:911–921
Synthese, Biochemische Charakterisierung und Genetische Kodierung einer 1,2,4‐Triazol‐Aminosäure als Acetyllysin‐Mimetikum für Bromodomänen der BET‐Familie
Authors: Kirchgäßner Sören , Braun Michael B. , Bartlick Natascha , Koç Cengiz , Reinkemeier Christopher D. , Lemke Edward A. , Stehle Thilo , Schwarzer Dirk 
Published: December 2022

AbstractDie Acetylierung von Lysinen ist eine ladungsneutralisierende posttranslationale Modifikation von Proteinen, die Bromodomänen (Brds) als Bindungsmotiv dient. Eine 1,2,4‐Triazol‐Aminosäure (ApmTri) wurde als Acetyllysin (Kac)‐Mimetikum entwickelt, das Brds der BET‐Familie rekrutiert, im Gegensatz zu Glutamin, das üblicherweise zur Simulierung dieser Modifikation genutzt wird. Durch Optimierung der Triazol‐Substituenten und der Seitenkettenlänge konnten ähnliche Affinitäten von BET‐Brds zu ApmTri‐enthaltenden Peptiden wie zu nativen Substraten erreicht werden. Kristallstrukturen zweier BET‐Brds mit gebundenen ApmTri‐Peptiden zeigten einen Bindungsmechanismus, der den von gebundenen Kac‐Liganden widerspiegelte. ApmTri wurde genetisch kodiert und rekombinante ApmTri‐enthaltende Proteine konnten gemeinsam mit BRD3(2) aus Zelllysat angereichert werden. Diese Interaktion wurde durch den BET‐Inhibitor JQ1 blockiert. Die Biochemie wird durch ApmTri mit einem neuen, stabilen Kac‐Mimetikum ausgestattet, das sowohl die Ladung neutralisiert, als auch Brds rekrutiert. Dadurch werden neue Untersuchungen von BET‐Proteinen in vitro und in vivo ermöglicht.
A Molybdenum Disulfide Nanozyme with Charge‐Enhanced Activity for Ultrasound‐Mediated Cascade‐Catalytic Tumor Ferroptosis
Authors: Wang Longwei , Zhang Xiaodi , You Zhen , Yang Zhongwei , Guo Mengyu , Guo Jiawei , Liu He , Zhang Xiaoyu , Wang Zhuo , Wang Aizhu , Lv Yawei , Zhang Jian , Yu Xin , Liu Jing , Chen Chunying 
Published: December 2022

AbstractThe deficient catalytic activity of nanozymes and insufficient endogenous H2O2 in the tumor microenvironment (TME) are major obstacles for nanozyme‐mediated catalytic tumor therapy. Since electron transfer is the basic essence of catalysis‐mediated redox reactions, we explored the contributing factors of enzymatic activity based on positive and negative charges, which are experimentally and theoretically demonstrated to enhance the peroxidase (POD)‐like activity of a MoS2 nanozyme. Hence, an acidic tumor microenvironment‐responsive and ultrasound‐mediated cascade nanocatalyst (BTO/MoS2@CA) is presented that is made from few‐layer MoS2 nanosheets grown on the surface of piezoelectric tetragonal barium titanate (T‐BTO) and modified with pH‐responsive cinnamaldehyde (CA). The integration of pH‐responsive CA‐mediated H2O2 self‐supply, ultrasound‐mediated charge‐enhanced enzymatic activity, and glutathione (GSH) depletion enables out‐of‐balance redox homeostasis, leading to effective tumor ferroptosis with minimal side effects.
Host–Guest Doping in Flexible Organic Crystals for Room‐Temperature Phosphorescence
Authors: Xia Yang , Zhu Chenfei , Cao Feng , Shen Yunxia , Ouyang Mi , Zhang Yujian 
Published: December 2022

AbstractOrganic single crystals (OSCs) with excellent flexibility and unique optical properties are of great importance due to their broad applicability in optical/optoelectronic devices and sensors. Nevertheless, fabricating flexible OSCs with room‐temperature phosphorescence (RTP) remains a great challenge. Herein, we propose a host–guest doping strategy to achieve both RTP and flexibility of OSCs. The single‐stranded crystal is highly bendable upon external force application and can immediately return to its original straight shape after removal of the stress, impressively emitting bright deep‐red phosphorescence. The theoretical and experimental results demonstrate that the bright RTP arises from Förster resonance energy transfer (FRET) from the triphenylene molecules to the dopants. This strategy is both conceptually and synthetically simple and offers a universal approach for the preparation of flexible OSCs with RTP.
Highly Robust Microporous Metal‐Organic Frameworks for Efficient Ethylene Purification under Dry and Humid Conditions
Authors: Liu Wansheng , Geng Shubo , Li Ning , Wang Sa , Jia Shuping , Jin Fazheng , Wang Ting , Forrest Katherine A. , Pham Tony , Cheng Peng , Chen Yao , Ma Jian‐Gong , Zhang Zhenjie 
Published: December 2022

AbstractTwo C2H6‐selective metal‐organic framework (MOF) adsorbents with ultrahigh stability, high surface areas, and suitable pore size have been designed and synthesized for one‐step separation of ethane/ethylene (C2H6/C2H4) under humid conditions to produce polymer‐grade pure C2H4. Experimental results reveal that these two MOFs not only adsorb a high amount of C2H6but also display good C2H6/C2H4selectivity verified by fixed bed column breakthrough experiments. Most importantly, the good water stability and hydrophobic pore environments make these two MOFs capable of efficiently separating C2H6/C2H4under humid conditions, exhibiting the benchmark performance among all reported adsorbents for separation of C2H6/C2H4under humid conditions. Moreover, the affinity sites and their static adsorption energies were successfully revealed by single crystal data and computation studies. Adsorbents described in this work can be used to address major chemical industrial challenges.
Massless scalar scattering by a charged regular black hole
Authors: de Paula Marco Aurélio Abreu , dos Santos Leite Luiz Carlos , Crispino Luís Carlos Bassalo 
Published: December 2022

AbstractThe scattering cross section of massless scalar waves in the background of an Ayón–Beato–García electrically charged regular black hole is investigated. We obtain the scattering pattern by numerically solving the Klein–Gordon equation. We show that it is possible to find configurations for which the Ayón–Beato–García regular black hole can mimic the scattering properties of the Reissner–Nordström black hole, for arbitrary values of the scattering angle and of the wave frequency, considering low‐to‐moderate values of the normalized electric charge. Our results suggest that the scattering spectra of regular and standard black holes can be indistinguishable.
A review on biological synthesis of ZnO nanostructures and its application in photocatalysis mediated dye degradation: An overview
Authors: Areeshi Mohammed Y. 
Published: December 2022

AbstractZinc oxide (ZnO) has several industrial applications due to its versatile properties, which lead to its continuously increasing demand in different industrial sectors. Additionally, ZnO nanostructures possess unique photocatalytic activity, and because of this, they are being applied to degrade organic dyes through photocatalysis for wastewater treatment. Nevertheless, chemical synthesis methods to develop ZnO nanostructures have raised concerns related to environmental issues, furthermore, these methods are found to be costly and tedious. As a result, the synthesis of ZnO nanostructures using green methods is gaining popularity due to its low cost and eco‐friendly mode, while avoiding the use of toxic chemicals. Green synthesis of ZnO nanostructures using different biological approaches involving plants, algae, and different microorganism‐derived bioactive compounds has been well reported for diverse applications. Among different applications, ZnO nanostructures that enable photocatalysis to degrade dye have been found to be imperative for wastewater treatments. Therefore, the current review explores recent studies on green synthesis approaches to prepare ZnO nanostructures via adopting different biological methods that rely on plants, algae, and bacterial microorganisms. The properties of ZnO nanostructures, along with their green synthesis routes and feasible mechanisms, have also been discussed in this review. This review focuses on the use and efficiency of green route synthesized ZnO nanostructures as nanophotocatalysts for the degradation of organic dyes in wastewater treatment. Additionally, existing challenges in green synthesis methods and the efficiency of ZnO nanostructures to degrade organic dyes following photocatalysis has been discussed.
Linking Catalysis in Biochemical and Geochemical CO2 Fixation at the Emergence of Life
Authors: Belthle Kendra S. , Tüysüz Harun 
Published: December 2022

AbstractH2‐producing, submarine hydrothermal vents present a plausible environment for the prebiotic synthesis of the first organic compounds at the emergence of life. Geochemical CO2 reduction at these vent systems harbors similarity to the ancient, biochemical acetyl‐CoA pathway of CO2 fixation in modern autotrophs. Both pathways involve catalytic transformations with transition metals as active centers. This concept article provides some insight about origins of life, mineral‐catalyzed CO2 reduction, and its correlation to the enzymatic pathway by focusing on key studies.
Glycosyl Radical‐Based Synthesis of C‐Glycoamino Acids and C‐Glycopeptides
Authors: Wang Chao , Qi Rupeng , Xu Zhaoqing 
Published: December 2022

AbstractRadical‐based reactions usually exhibit excellent functional‐group compatibilities due to their mild initiation conditions. Glycosyl radical involved C‐glycosylation modifications are important strategies to achieve highly regio‐ and chemoselective constructions of C‐glycosidic bonds or C‐glycoside linkages of peptides and proteins. In this Concept, we cover recent developments in glycosyl radical‐based synthesis of unnatural amino acids and late‐stage modification of peptides and proteins, and provide a preliminary outlook on the possible development of this direction in the future.