bluuebunny/crossref_metadata_2025_split huggingface dataset:
Computational Screening of 2D All‐Inorganic Lead‐Free Halide Perovskites A3B2X9 for Photovoltaic and Photocatalytic Applications
Authors: Luo Qingyuan , Su Liqin , Lu Yanan , Fang Linghui , Shu Haibo , Cao Dan , Chen Xiaoshuang 
Published: December 2023

AbstractExploration of low‐dimensional Pb‐free halide perovskites with high stability and outstanding properties is still a pursuing target for developing integrated optoelectronic devices. Herein, comprehensive computational screening of a new class of two‐dimensional (2D) all‐inorganic Pb‐free A3B2X9 perovskites is performed based on the first‐principles calculations. The results indicate that the structural and electronic properties of 2D A3B2X9 structures strongly depend on the B‐X bonding interactions, which makes that their thermodynamic stability follows the trend of A3Bi2X9≈A3Sb2X9>A3In2X9>A3Ga2X9 and their interlayer interactions show a reversal trend. Owing to the lack of lone‐pair electron effect, A3In2X9 indicate direct bandgap characteristics and present the relatively smaller bandgaps and higher electron mobilities than A3Sb2X9 and A3Bi2X9. Benefit from optimal bandgaps (0.8–2.1 eV) and large absorption coefficients (104–105 cm−1) in the visible region, A3B2I9 (B = In, Sb, Bi) exhibit high power conversion efficiency up to 18.2%. Moreover, A3B2I9 (B = Sb, Bi) is verified as efficient photocatalysts for overall water splitting. The theoretical solar‐to‐hydrogen efficiency of Rb3Bi2I9 and Cs3Bi2I9 are >16%. This work suggests huge potential of 2D A3B2X9 perovskites for photovoltaic and photocatalytic applications.
Radical‐Dearomative Generation of Cyclohexadienyl Pd(II) toward the 3D Transformation of Nonactivated Phenyl Rings
Authors: Fan Qi , Jiang Kai , Liu Bo , Jiang Huanfeng , Cao Xiaohui , Yin Biaolin 
Published: December 2023

AbstractTraditional palladium‐catalyzed dearomatization of (hetero)arenes takes place via an ionic pathway and usually requires elevated temperatures to overcome the energy barrier of the dearomative insertion step. Herein, a combination of the radical and two‐electron pathways is disclosed, which enables room temperature dearomative 3D transformations of nonactivated phenyl rings with Pd(0) as the catalyst. Experimental results together with density functional theory (DFT) calculations indicate a versatile π‐allyl Pd(II) species, cyclohexadienyl Pd(II), possibly is involved in the dearomatization. This species is generated by combining the cyclohexadienyl radical and Pd(I). The cyclohexadienyl Pd(II) provides chemoselective (carboamination and trieneylation), regioselective (1,2‐carboamination), and diastereoselective (carbonyl‐group directed face selectivity) conversions.
Pressure‐Induced Remarkable Spectral Red‐Shift in Mn2+‐Activated NaY9(SiO4)6O2 Red‐Emitting Phosphors for High‐Sensitive Optical Manometry
Authors: Zeng Qifeng , Runowski Marcin , Xue Junpeng , Luo Laihui , Marciniak Lukasz , Lavín Víctor , Du Peng 
Published: December 2023

AbstractTo settle the low sensitivity of luminescent manometers, the Mn2+‐activated NaY9(SiO4)6O2 red‐emitting phosphors with splendid pressure sensing performances are developed. Excited by 408 nm, the resulting products emit bright red emission originating from 4T1(4G) → 6A1 transition of Mn2+, in which the optimal concentration of the activator ion is ≈1 mol%. Moreover, the admirable thermal stability of the developed phosphors is studied and confirmed by the temperature‐dependent emission spectra, based on which the activation energy is derived to be 0.275 eV. By analyzing the pressure‐dependent Raman spectra, the structural stability of the synthesized compounds at extreme conditions is verified. Furthermore, the designed phosphors exhibit remarkable spectral red‐shift at elevated pressure. Especially, as pressure increases from 0.75 to 7.16 GPa, the emission band centroid shifts from 617.2 to 663.4 nm, resulting in a high sensitivity (dλ/dP) of 7.00 nm GPa−1, whereas the full width at half maximum (FWHM) increases from 83.0 to 110.6 nm, leading to the ultra‐high sensitivity (dFWHM/dP) of 10.13 nm GPa−1. These achievements manifest that the designed red‐emitting phosphors are appropriate for ultrasensitive optical manometry. More importantly, the developed manometer is a current global leader in sensitivity, when operating in the band‐width mode, that is, FWHM.
High Gain Graphene Based Hot Electron Transistor with Record High Saturated Output Current Density
Authors: Strobel Carsten , Chavarin Carlos A. , Knaut Martin , Völkel Sandra , Albert Matthias , Hiess Andre , Max Benjamin , Wenger Christian , Kirchner Robert , Mikolajick Thomas 
Published: December 2023

AbstractHot electron transistors (HETs) represent an exciting new device for integration into semiconductor technology, holding the promise of high‐frequency electronics beyond the limits of SiGe bipolar hetero transistors. With the exploration of 2D materials such as graphene and new device architectures, hot electron transistors have the potential to revolutionize the landscape of modern electronics. This study highlights a novel hot electron transistor structure with a record output current density of 800 A cm−2 and a high current gain α, fabricated using a scalable fabrication approach. The hot electron transistor structure comprises 2D hexagonal boron nitride and graphene layers wet transferred to a germanium substrate. The combination of these materials results in exceptional performance, particularly in terms of the highly saturated output current density. The scalable fabrication scheme used to produce the hot electron transistor opens up opportunities for large‐scale manufacturing. This breakthrough in hot electron transistor technology holds promise for advanced electronic applications, offering high current capabilities in a practical and manufacturable device.
Construction of Stable Li2O‐Rich Solid Electrolyte Interphase for Practical PEO‐Based Li‐Metal Batteries
Authors: Zhang Jiahui , Li Siyuan , Wang Xinyang , Mao Shulan , Guo Junze , Shen Zeyu , Mao Jiale , Wu Qian , Shen Kang , Cheng Hao , Tan Yuanzhong , Lu Yingying 
Published: December 2023

AbstractPolyethylene oxide (PEO)‐based solid polymer electrolytes (SPE) have garnered recognition as highly promising candidates for advanced lithium‐metal batteries. However, the practical application of PEO‐based SPE is hindered by its low critical current density (CCD) resulting from undesired dendrite growth. In this study, a PEO‐based SPE that exhibits an ultra‐high CCD (4 mA cm−2) is presented and enhanced lithium ionic conductivity through the incorporation of small amounts of P2S5 (PS). The crystalline Li2O‐rich and P/S‐containing solid electrolyte interphase (SEI) is revealed by cryo‐electron microscope (cryo‐EM) and Time of flight secondary ion mass spectrometry (TOF‐SIMS), which inhibits dendrite growth and adverse reactions between SPE and reductive lithium, thus offering a spherical growth behavior for dendrite‐free lithium metal anode. Consequently, utilizing the PS‐integrated SPE, a Li‐Li symmetric cell demonstrates reduced resistance during operation, enabling stable cycles exceeding 200 hours at 0.5 mA cm−2 and 0.5 mAh cm−2, a stringent test condition for PEO‐based electrolytes. Moreover, a Li/SPE/LiFePO4 (LFP) pouch cell exhibits 80% capacity retention after 100 cycles with 50 µm Li and 30 µm PEO electrolyte, showcasing its potential for practical applications.
Bimetallic PdFe3 Nano‐Alloy with Tunable Electron Configuration for Boosting Electrochemical Nitrogen Fixation
Authors: Mu Jianjia , Zhao Zhiwei , Gao Xuan‐Wen , Liu Zhao‐Meng , Luo Wen‐Bin , Sun Zhenhua , Gu Qin‐Fen , Li Feng 
Published: December 2023

AbstractElectrocatalyst plays animportant role in electrochemical ammonia synthesis by determining the nitrogen reduction reaction pathway. Featuring the inherent half‐filled 3d orbitals, ion‐based alloy electrocatalysts have been attracting much more attention owing to the controllable driving force to adsorb and activate N≡N bonds. Besides supplying unoccupied d‐orbital to accommodate lone‐pair electrons to facilitate nitrogen adsorption, donating d‐orbital electrons to nitrogen antibonding orbitals to dissociate N≡N bond is demandedas well. By palladium (Pd) to synthesize PdFe3 nano‐alloy, numerous Fe 3d orbitals can be reconstructed via charge polarization between Fe and Pd, simultaneously lowering corresponding work functions. Meanwhile, the positively charged Fesites in PdFe3 can strengthen suppress the proton adsorption by electrostatic repulsion. A considerably optimized ammonia production rate of 29.07 µg h−1 mgcat.−1 and Faradic efficiency of 22.8% are accomplished at a low overpotential of −0.2 V vs. RHE. Density functional theory combined with in‐situ ATR‐FTIR results confirmthe electrocatalytic nitrogen reduction follows the associative distalmechanism and the electron‐deficient Fe induced through Pd facilitates significantly lowering the first‐step‐protonation energy barrier of only 0.07 eV (*N2 + *H →*NNH).
3D models guide the design of hollow fiber membrane contactors with complex internal structures for CO2 capture
Authors: Yin Yihan , Liu Qi , Gao Hongxia , Xiao Min , Sema Teerawat , Liang Zhiwu 
Published: December 2023

AbstractMembrane contactors have good prospects in the field of CO2 capture. In this study, the effects of operation conditions (gas velocity, liquid flow, CO2 pressure, amine concentration, and CO2 loading) on CO2 absorption flux (JCO2) for CO2 absorption into N‐methyl‐4‐piperidinol (MPDL) solution in membrane contactors were investigated through experiments and simulations. A three‐dimensional (3D) model was developed using COMSOL Multiphysics software to study the comprehensive CO2 mass transfer process in the multifiber membrane contactor and the effect of the number of fibers on the flow and CO2 concentration distribution without simplifying the geometry compared with those of traditional one‐dimensional (1D) and two‐dimensional (2D) models. Non‐ideal effects occurring in hollow fiber membrane contactors can be explained using a 3D modeling. By comparing the simulated with the experimental , the effectiveness of the model was determined. The simulation results emphasize that the spatial concentration distribution has a great correlation with the corresponding velocity distribution. Additionally, reducing the uneven velocity distribution of gas and liquid is a very important factor to improve the mass transfer performance of CO2. Increasing the number of fibers with a constant total volumetric flux can reduce the thickness of the boundary layer and promote the mass transfer.
Assessing the role of social determinants of health in health disparities: The need for data on work
Authors: Silver Sharon R. , Sweeney Marie H. , Sanderson Wayne T. , Pana‐Cryan Regina , Steege Andrea L. , Quay Brian , Carreón Tania , Flynn Michael A. 
Published: December 2023

AbstractBackgroundWork is a key social determinant of health. Without the collection of work‐related information in public health data systems, the role of social determinants in creating and reinforcing health disparities cannot be fully assessed.MethodsThe Centers for Disease Control and Prevention (CDC) maintains or supports a number of public health surveillance and health monitoring systems, including surveys, case‐based disease and exposure systems, vital status records, and administrative data systems. We evaluated a convenience sample of these systems for inclusion of information in three work‐related domains: employment status, industry and occupation, and working conditions.ResultsWhile 12 of 39 data systems were identified as collecting work‐related data, this information was often minimal (e.g., only employment status), restricted to a subset of respondents, or only gathered periodically. Information on working conditions was particularly sparse.ConclusionHistorically, the limited and inconsistent collection of work‐related information in public health data systems has hindered understanding of the role work plays in health disparities. Current CDC data modernization efforts present opportunities to enhance the identification and mitigation of health disparities by prioritizing inclusion of an expanded set of work‐related data elements.
Quantum Fourier Transform‐Based Arithmetic Logic Unit on a Quantum Processor
Authors: Çakmak Selçuk , Kurt Murat , Gençten Azmi 
Published: December 2023

AbstractThis study proposes and construct a primitive quantum arithmetic logic unit (qALU) based on the quantum Fourier transform (QFT). The qALU is capable of performing arithmetic ADD (addition) and logic NAND gate operations. It designs a scalable quantum circuit and presents the circuits for driving ADD and NAND operations on two‐input and four‐input quantum channels, respectively. By comparing the required number of quantum gates for serial and parallel architectures in executing arithmetic addition, it evaluates the performance. It also execute the proposed quantum Fourier transform‐based qALU design on real quantum processor hardware provided by IBM. The results demonstrate that the proposed circuit can perform arithmetic and logic operations with a high success rate. Furthermore, it discusses in detail the potential implementations of the qALU circuit in the field of computer science, highlighting the possibility of constructing a soft‐core processor on a quantum processing unit.
Iminothioindoxyl Donors with Exceptionally High Cross Section for Protein Vibrational Energy Transfer
Authors: Feid Carolin , Luma Larita , Fischer Tobias , Löffler Jan Gerrit , Grebenovsky Nikolai , Wachtveitl Josef , Heckel Alexander , Bredenbeck Jens 
Published: December 2023

AbstractVarious protein functions are related to vibrational energy transfer (VET) as an important mechanism. The underlying transfer pathways can be experimentally followed by ultrafast Vis‐pump/IR‐probe spectroscopy with a donor‐sensor pair of non‐canonical amino acids (ncAAs) incorporated in a protein. However, so far only one donor ncAA, azulenylalanine (AzAla), exists, which suffers from a comparably low Vis extinction coefficient. Here, we introduce two novel donor ncAAs based on an iminothioindoxyl (ITI) chromophore. The dimethylamino‐ITI (DMA‐ITI) and julolidine‐ITI (J‐ITI) moieties overcome the limitation of AzAla with a 50 times higher Vis extinction coefficient. While ITI moieties are known for ultrafast photoswitching, DMA‐ITI and J‐ITI exclusively form a hot ground state on the sub‐ps timescale instead, which is essential for their usage as vibrational energy donor. In VET measurements of donor‐sensor dipeptides we investigate the performance of the new donors. We observe 20 times larger signals compared to the established AzAla donor, which opens unprecedented possibilities for the study of VET in proteins.
Boosting Electrocatalytic Carbon Dioxide Reduction via Self‐Relaxation of Asymmetric Coordination in Fe‐Based Single Atom Catalyst
Authors: Jin Zhaoyong , Jiao Dongxu , Dong Yilong , Liu Lin , Fan Jinchang , Gong Ming , Ma Xingcheng , Wang Ying , Zhang Wei , Zhang Lei , Gen Yu Zhi , Voiry Damien , Zheng Weitao , Cui Xiaoqiang 
Published: December 2023

AbstractAddressing the limitations arising from the consistent catalytic behavior observed for various intermediates during the electrochemical carbon dioxide reduction reaction (CO2RR) poses a significant challenge in the optimization of catalytic activity. In this study, we aimed to address this challenge by constructing an asymmetric coordination Fe single atom catalyst (SCA) with a dynamically evolved structure. Our catalyst, consisting of a Fe atom coordinated with one S atom and three N atoms (Fe−S1N3), exhibited exceptional selectivity (CO Faradaic efficiency of 99.02 %) and demonstrated a high intrinsic activity (TOF of 7804.34 h−1), and remarkable stability. Using operando XAFS spectra and Density Functional Theory (DFT) calculations, we elucidated the self‐relaxation of geometric distortion and dynamic evolution of bond lengths within the catalyst. These structure changes enabled independent regulation of the *COOH and *CO intermediate adsorption energies, effectively breaking the linear scale relationship and enhancing the intrinsic activity of CO2RR. This study provides valuable insights into the dynamic evolution of SACs and paves the way for targeted catalyst designs aimed to disrupt the linear scaling relationships.
Facile fabrication of highly efficient bifunctional polydopamine–polyethyleneimine copolymerization‐modified magnetic material and its effective applications for both adsorption of gold ions and catalytic reduction of 4‐nitrophenol
Authors: Wu Xiaoqiong , Zhang Wansong , Yin Ping , Xu Qiang , Yang Zhenglong , Xu Yanbin , Liu Xiguang , Wang Feng , Wang Ying , Cai Honglan 
Published: December 2023

AbstractThe heavy metal ions and organic pollutants are major harmful substances in wastewater because of their toxicity on human health and environment. Nowadays, the adsorption–catalysis treatment to remove them simultaneously is still a challenge because of their different reaction mechanisms. Herein, a novel bifunctional polymer magnetic material Fe3O4@PDA‐PEI was successfully developed through a facile co‐deposition method by the copolymerization modification of polydopamine (PDA) and polyethyleneimine (PEI) on magnetic ferroferric oxide, which can both be utilized for both heavy metal ion removal from simulated industrial wastewater and further effective catalytic reduction of toxic 4‐nitrophenol (4‐NP) to useful 4‐aminophenol. The maximum adsorption capacity of Fe3O4@PDA‐PEI for gold ions was 465.12 mg/g at 35°C, and the adsorption thermodynamic parameters ΔG, ΔH, and ΔS of Fe3O4@PDA‐PEI (m(PDA):m(PEI) = 2:1) were −5.28 (35°C), 25.58, and 111.30 J K−1 mol−1, respectively. In addition, a sustainable strategy of converting gold ions to gold nanoparticles has been demonstrated for additional catalytic functionality of Fe3O4@PDA‐PEI, and Fe3O4@PDA‐PEI‐Au could effectively catalyze the reduction of 4‐NP at ambient temperature within 9 min. Fe3O4@PDA‐PEI with the advantages of facile fabrication, easy separation, excellent adsorption, and catalysis performance could be used as a promising polymer composite material in complicated wastewater environment. © 2023 Wiley Periodicals LLC.
Sustainable application study of disposable medical waste masks in cement based on green Fenton reaction
Authors: Chen Youchao , Luo Wenjie , Meng Fanyu , Zhou Tao , Lai Fang , Zhao Zhenxia , Liu Yu , Li Jing 
Published: December 2023

AbstractThis study addresses disposable medical mask (DMM) environmental issues through recycling polypropylene fibers. Polypropylene fibers were collected from DMMs, artificially crush them, and enhance fiber–cement interaction via advanced Fenton oxidation. Analysis (Fourier transform infrared spectrometer, x‐ray photoelectron spectrometer, field emission scanning electron microscope (FE‐SEM), energy‐dispersive x‐ray spectrometer, atomic force microscope, contact angle) confirms successful FeOOH grafting onto M‐DMM fibers, increasing roughness and wettability. Compared with DMM fibers, the surface free energy of M‐DMM fibers increased by 46.3%. Consequently, the grafting of FeOOH onto the fiber surface improves the physical friction and interlocking effects between the fibers and cement. FE‐SEM results after 28 days of curing reveal that M‐DMM fibers exhibit better bonding ability with cement compared with unmodified DMM fibers. Mechanical tests unequivocally demonstrated the enhanced impact resistance of the cement mortar incorporating M‐DMM fibers compared to the reference. Specifically, there was a significant 16.0% increase at 7 days of curing, followed by an additional 4.5% improvement after 28 days of curing. This study provides an eco‐friendly solution for addressing the post‐pandemic surge in DMM waste, reducing microplastic pollution, and lowering disposal costs. It also offers the construction industry an innovative material enhancing cement mortar's impact resistance, aligning with sustainable development principles.
Fabrication of alginate/sericin/cellulose nanocrystals interpenetrating network composite hydrogels with enhanced physicochemical properties and biological activity
Authors: Wu Ting , Liu Haiying , Wang Hongcai , Bu Yanan , Liu Jiayi , Chen Xiuqiong , Yan Huiqiong , Lin Qiang 
Published: December 2023

AbstractSodium alginate (SA) possesses good biocompatibility and can form hydrogel materials under certain conditions, which has been widely used in tissue engineering. However, the absence of cellular recognition sites and low mechanical strength for single‐component alginate (ALG) hydrogels limit their practical applications. Therefore, enhancing the shortcomings of ALG hydrogels and augmenting their characteristics hold immense importance for their medical uses. In this study, comprehensively considering the excellent properties of cellulose nanocrystals (CNCs) and sericin (SS), the alginate/sericin/cellulose nanocrystalline (ALG/SS/CNCS) composite hydrogels were constructed by interpenetrating network (IPN) technique using hydroxyapatite/D‐glucono‐δ‐lactone (HAP/GDL) as the endogenous ionic cross‐linking agent of SA, 1‐ethyl‐(3‐dimethylaminopropyl) carbodiimide hydrochloride/N‐hydroxysuccinimide (EDC/NHS) as the chemical covalent cross‐linking agent of SS and CNCS as the reinforcing agent. The effects of SS and CNCs additions on the comprehensive properties of ALG/SS/CNCs composite hydrogels, such as their morphologies, structure, mechanical properties, swelling, degradability, and cytocompatibility were investigated. The findings indicated that the ALG/SS/CNCS IPN composite hydrogels which were created through the physical blending of SA and SS, displayed a consistent three‐dimensional form and a porous configuration. The weak mechanical strength of pure ALG hydrogels can be effectively improved and the swelling stability and mechanical properties of the composite hydrogels can be enhanced through the construction of IPN network and the incorporation of CNCs, thanks to the presence of intermolecular hydrogen bonding. The biodegradability of ALG/SS/CNCS composite hydrogels increased as the SS content increased, indicating that SS facilitated their biomineralization due to its inherent susceptibility to degradation. The results of the cell compatibility test conducted in a laboratory setting showed that SS and CNCS had the ability to enhance the attachment, proliferation, and differentiation of MC3T3‐E1 cells on the ALG/SS/CNCS composite hydrogels. Hence, incorporating SS and CNCS into the alginate matrix to create IPN composite hydrogels could significantly enhance the physicochemical and biological characteristics of ALG hydrogels, thus rendering them appropriate for tissue engineering purposes.