bluuebunny/crossref_metadata_2025_split huggingface dataset:
Bifunctional Catalysts with Separated and Tunable Sites on Zeolites for Relay Catalysis of the Oxidative Dehydrogenation of Propane Using CO2
Authors: Li Wanting , Wang Tianchang , Cao Xinxin , Li Yuze , Miao Gai , Sun Nannan , Li Jiong , Han Wei , Wei Wei , Chen Xinqing 
Published: December 2024

AbstractThe oxidative dehydrogenation of propane using CO2 (CO2‐ODH) technology has broad application prospects in the production of propylene and the utilization of CO2, and the development of efficient CO2‐ODH catalysts is of great significance. However, it remains a challenge to develop a highly efficient catalyst that can activate both C─H and C═O. Herein, a PtZn/Co@S‐1 catalyst with a very low precious metal content of 0.2 wt.% is reported. Benefiting from the PtZn4 nanoclusters dispersed on the surface of Silicalite‐1 zeolite and tetrahedrally coordinated Co2+ in the Silicalite‐1 zeolite framework via relay catalysis, the independent dual sites structure (PtZn/Co@S‐1) greatly promotes CO2‐ODH reaction with a high conversion rate of both C3H8 (59.7%) and CO2 (44.3%), and propylene selectivity of 94.9%, thus upsetting the equilibrium for direct dehydrogenation of propane. Experimental measurements and density functional theory calculations suggest that the PtZn4 and Co2+ interfaces are likely propane dehydrogenation and carbon dioxide hydrogenation active sites respectively.
Embedded Bioprinting of Breast Cancer–Adipose Composite Tissue Model for Patient‐Specific Paracrine Interaction Analysis
Authors: Jeong Wonwoo , Han Jonghyeuk , Choi Jeonghan , Kang Hyun‐Wook 
Published: December 2024

AbstractThe interaction between breast cancer and stromal tissues varies significantly from patient to patient, greatly impacting cancer prognosis. However, conventional models struggle to accurately replicate these patient‐specific interactions. Herein, a novel breast cancer–adipose composite tissue model capable of precisely adjusting the inter‐tissue interaction is developed. The composite tissue model is produced through precise embedded bioprinting of breast‐cancer spheroids and live‐adipose‐tissue ink. This model possessed not only precisely patterned cancer spheroids but also well‐preserved intrinsic extracellular matrices (ECMs) and heterogeneous cell populations of adipose tissue (AT). Evaluation results successfully demonstrated that the bioprinted composite model can precisely regulate adipokine secretion, drug resistance, and cancer‐cell invasion characteristics by adjusting the distance between the cancer spheroids and adipose tissue. The utility of the model is validated using adipokine‐targeted therapies (C‐compound/SC600125 (SC), AG 490 (AG), and Metformin (MET)). Interestingly, the inhibition of cancer cell proliferation and invasion by these adipokine‐targeted drugs nearly doubled as the tissue distance decreased. This suggests that the efficacy of the drugs can be precisely evaluated using the new model. These findings underscore the potential of the developed composite model to replicate patient‐specific crosstalk, thereby offering a promising platform for the sophisticated evaluation of various breast‐cancer therapies.
Deep Learning‐Assisted Design of Novel Donor–Acceptor Combinations for Organic Photovoltaic Materials with Enhanced Efficiency
Authors: Zhang Shizhao , Li Shuixing , Song Siqin , Zhao Yang , Gao Liang , Chen Hongzheng , Li Hanying , Lin Jiaping 
Published: December 2024

AbstractDesigning donor (D) and acceptor (A) structures and discovering promising D‐A combinations can effectively improve organic photovoltaic (OPV) device performance. However, to obtain excellent power conversion efficiency (PCE), the trial‐and‐error structural design in the infinite chemical space is time‐consuming and costly. Herein, a deep learning (DL)‐assisted design framework for OPV materials is proposed. To effectively digitally represent the D and A structures, a structure representation method, polymer fingerprints, is developed, and a database of OPV materials is constructed. By applying an end‐to‐end graph neural network modeling method, high‐precision DL models for predicting OPV performance are established. After combining the existing structures, ≈0.6 million virtual D‐A combinations are generated. Then, the OPV performance of these candidate combinations is predicted by the well‐trained models, and numbers of novel D‐A combinations with high efficiency are identified. Experimental validations confirm that the prediction accuracy is greater than 93% and one of the screened combinations (i.e., D18:BTP‐S11) exhibits an efficiency above 19.3% in single‐junction organic solar cells. Finally, based on the structural gene analysis, the design rules to guide experimental explorations are suggested. The developed DL‐assisted approach can accelerate the design of D‐A combinations with ultrahigh efficiency and bring property breakthroughs for OPV devices.
Enhance Photo‐Stability of Up‐Scalable Organic Solar Cells: Suppressing Radical Generation in Polymer Donors
Authors: Xiao Mengfei , Wang Chen , Xu Yujie , Zhang Wenqing , Fu Zhen , Qiao Jiawei , Wang Hao , Xia Xinxin , Zhang Maojie , Qin Wei , Hao Xiaotao , Du Xiaoyan 
Published: December 2024

AbstractThe power conversion efficiency (PCE) of single‐junction organic solar cells (OSCs) has been promoted above 20%. Device up‐scaling draws more and more research attentions. Besides the high PCE for devices with up‐scalable fabrication methods and conditions, achieving high stability simultaneously is essential for pushing industrialization of this technology. Here, the stability of the state‐of‐the‐art OSCs blade‐coated in air with non‐halogenated solvents in a wide thickness range is thoroughly investigated. The losses in short‐circuit current density under photo‐thermal stress strongly depend on processing conditions. Devices with less crystalline phases in unit thickness show faster generation of trap states and hence strongly reduced charge collection efficiency. Through in‐depth photo‐chemical, photo‐physical, and morphological characterizations during ageing, faster generation of radicals in PM6 for active layers with more amorphous structures is identified as the cause for device degradation. Increasing the crystallinity of active layer films for suppressing radical generation in polymer donors is critical to enhance the photo‐thermal stability of devices processed in air with a wide thickness range.
Accelerating Tandem Electroreduction of Nitrate to Ammonia via Multi‐Site Synergy in Mesoporous Carbon‐Supported High‐Entropy Intermetallics
Authors: Zhu Guihua , Bao Weichao , Xie Meng , Qi Chunhong , Xu Fangfang , Jiang Ying , Chen Bingwei , Fan Yuchi , Liu Bin , Wang Lianjun , Jiang Wan , Qiu Pengpeng , Luo Wei 
Published: December 2024

AbstractThe electrochemical nitrate reduction reaction (NO3
−RR) for ammonia (NH3) synthesis represents a significant technological advancement, yet it involves a cascade of elementary reactions alongside various intermediates. Thus, the development of multi‐site catalysts for enhancing NO3
−RR and understanding the associated reaction mechanisms for NH3 synthesis is vital. Herein, a versatile approach is presented to construct platinum based high‐entropy intermetallic (HEI) library for NH3 synthesis. The HEI nanoparticles (NPs) are uniformly supported on a 2D nitrogen doped mesoporous carbon (N‐mC) framework, featured with adjustable compositions (up to eight elements) and a high degree of atomic order (over 90%). Guided by the density functional theory (DFT) calculations and atomic structural analysis, a quinary Pt0.8Fe0.2Co0.2Ni0.2Cu0.2 HEI NPs based N‐mC catalyst is designed, which demonstrates a large ammonia Faradaic efffciency (>97%) and a remarkable recyclability (>20 cycles) under both acidic and basic conditions. The combined in situ experimental analysis and further DFT calculation suggests that the well‐defined multi‐sites nature of the HEI NPs cooperate for a tandem reduction mechanism, in which the Pt‐X (X represents the other four transition elements) bridging sites offer optimal adsorption for key nitrogen–oxygen species while the Pt sites facilitate the generation and adsorption of *H species.
Clickable, Thermally Responsive Hydrogels Enabled by Recombinant Spider Silk Protein and Spy Chemistry for Sustained Neurotrophin Delivery
Authors: Li Yue , Yang Chao , Fang Shiyu , Zhou Yiren , Li Manjia , Liu Zhewei , Zhang Xin , Duan Liting , Liu Kai , Sun Fei 
Published: December 2024

AbstractThe ability to deliver protein therapeutics in a minimally invasive, safe, and sustained manner, without resorting to viral delivery systems, will be crucial for treating a wide range of chronic injuries and diseases. Among these challenges, achieving axon regeneration and functional recovery post‐injury or disease in the central nervous system remains elusive to most clinical interventions, constantly calling for innovative solutions. Here, a thermally responsive hydrogel system utilizing recombinant spider silk protein (spidroin) is developed. The protein solution undergoes rapid sol‐gel transition at an elevated temperature (37 °C) following brief sonication. This thermally triggered gelation confers injectability to the system. Leveraging SpyTag/SpyCatcher chemistry, the hydrogel, composed of SpyTag‐fusion spidroin, can be functionalized with diverse SpyCatcher‐fusion bioactive motifs, such as neurotrophic factors (e.g., ciliary neurotrophic factor) and cell‐binding ligands (e.g., laminin), rendering it well‐suited for neuronal culturing. More importantly, the intravitreous injection of the protein materials decorated with SpyCatcher‐fusion CNTF into the vitreous body after optic nerve injury leads to prolonged JAK/STAT3 signaling, increased neuronal survival, and enhanced axon regeneration. This study illustrates a generalizable material system for injectable and sustained delivery of protein therapeutics for neuroprotection and regeneration, with the potential for extension to other chronic diseases and injuries.
Manipulation of Unconventional Spin Polarization in Non‐Collinear Exchange‐Spring Magnetic Structures
Authors: Wu Chuangwen , Cui Shuting , Guo Yaqin , Zhang Zhaowei , Zhang Jing , Deng Xiao , Zeng Guang , Ren Chuantong , Li Peizhi , Zhou Xiangqing , Zhang Xu , Li Jingfeng , Zhu Tao , Han Xiufeng , Zhao Jinkui , Wang Hao , Zhang Yue , Liang Shiheng , Wu Hao 
Published: December 2024

AbstractManipulating the polarization of spin current is essential for understanding the mechanism of charge‐to‐spin conversion and achieving efficient electrically driven magnetization switching. Here, a novel exchange‐spring magnetic structure is introduced formed by the coupling of perpendicular magnetic anisotropy (PMA) CoTb and in‐plane magnetic anisotropy (IMA) Co films. When a spin current with the polarization along the y‐direction flows through this exchange‐spring (x‐z plane) structure, the interaction between the y‐spin and the local exchange field with a non‐collinear spatial distribution gives rise to substantial unconventional spin polarizations in the x‐ and z‐directions, enabling field‐free spin‐orbit torque driven perpendicular magnetization switching at room temperature. More importantly, the polarization directions of this unconventional spin current can be reversed depending on whether the interfacial exchange coupling is ferromagnetic or antiferromagnetic. This work establishes a platform to explore emergent mechanisms for manipulating unconventional spin polarization with rich non‐collinear magnetic exchange spin structures.
Hollow Mo/MoSVn Nanoreactors with Tunable Built‐in Electric Fields for Sustainable Hydrogen Production
Authors: Gong Feilong , Chen Zhilin , Chang Chaoqun , Song Min , Zhao Yang , Li Haitao , Gong Lihua , Zhang Yali , Zhang Jie , Zhang Yonghui , Wei Shizhong , Liu Jian 
Published: December 2024

AbstractConstructing built‐in electric field (BIEF) in heterojunction catalyst is an effective way to optimize adsorption/desorption of reaction intermediates, while its precise tailor to achieve efficient bifunctional electrocatalysis remains great challenge. Herein, the hollow Mo/MoSVn nanoreactors with tunable BIEFs are elaborately prepared to simultaneously promote hydrogen evolution reaction (HER) and urea oxidation reaction (UOR) for sustainable hydrogen production. The BIEF induced by sulfur vacancies can be modulated from 0.79 to 0.57 to 0.42 mV nm−1, and exhibits a parabola‐shaped relationship with HER and UOR activities, the Mo/MoSV1 nanoreactor with moderate BIEF presents the best bifunctional activity. Theoretical calculations reveal that the moderate BIEF can evidently facilitate the hydrogen adsorption/desorption in the HER and the breakage of N─H bond in the UOR. The electrolyzer assembled with Mo/MoSV1 delivers a cell voltage of 1.49 V at 100 mA cm−2, which is 437 mV lower than that of traditional water electrolysis, and also presents excellent durability at 200 mA cm−2 for 200 h. Life cycle assessment indicates the HER||UOR system possesses notable superiority across various environment impact and energy consumption. This work can provide theoretical and experimental direction on the rational design of advanced materials for energy‐saving and eco‐friendly hydrogen production.
Improved Efficiency and Stability in Pure‐Red CdSe Nanoplatelet LEDs Enabled by Gradient Alloyed CdSeS/CdZnS Crown/Shell
Authors: Zeng Yicheng , Yu Wenke , Liu Yuan , Chen Weiwei , Wang Qingya , Cao Fan , Wei Jing , Liu Fangze , Yang Xuyong , Li Hongbo 
Published: December 2024

AbstractAnisotropic nanoplatelets (NPLs) possess strong in‐plane transition dipole moments and out‐of‐plane emission, which enable a maximum photon out‐coupling efficiency of 40% and a high gain coefficient, making them ideal candidates for light‐emitting diodes (LEDs) and lasers. However, the unbalanced surface energy between the side and top facets of NPLs results in poor thermal stability and high susceptibility to ripening at elevated temperatures, which complicates the growth of the shell. To address this issue, a gradient crown (CdSeS) around the CdSe NPLs is designed to stabilize the high energy side facets. Consequently, the gradient alloyed shell (CdZnS) is successfully grown, and the CdSe/CdSeS/CdZnS core/crown/shell NPLs exhibited near‐unity photoluminescence quantum yield. The CdSeS/CdZnS crown/shell structure suppressed non‐radiative Auger recombinations, achieving a record‐low amplification spontaneous emission threshold of 2.11 µJ cm−2 under femtosecond laser excitation. In addition, by selecting the carrier transport layers with matched energy levels, the NPL‐LEDs demonstrate a record‐high external quantum efficiency of 30.1% in the pure‐red range, driven by the 94% in‐plane transition dipole moment distribution of NPL film. The NPL‐LEDs also exhibited a long operational lifetime of T95 > 600 h at a luminance of 1000 cd m−2.
Bias‐Switchable Photodetection and Photosynapse Dual‐Functional Devices Based on 2D Perovskite/Organic Heterojunction for Imaging‐to‐Recognition Conversion
Authors: Zhao Zijin , Hu Zijun , Deng Ming , Hong Enliu , Wang Peixi , Li Ziqing , Fang Xiaosheng 
Published: December 2024

AbstractOptoelectronic devices with imaging and recognition capabilities are crucial for developing artificial visual system (AVS). Bias‐switchable photodetection and photosynaptic devices have been developed using 2D perovskite oxide/organic heterojunctions. This unique structure allows for modulated carrier dynamics under varied bias conditions, enabling the devices to function as photodetectors without bias and as photosynapses with bias. At zero bias, the device achieves high responsivity (≈0.36 A W−1 at 320 nm) and rapid response speed (0.57 s). Under a −0.5 V bias, it exhibits persistent photoconductivity (PPC), resulting in neuromorphic synaptic behaviors with a paired‐pulse facilitation (PPF) index exceeding 300%. Moreover, an 8 × 8 sensor array demonstrates image sensing and memory capabilities, showing in situ enhanced imaging when switching the bias from 0 to −0.5 V, and over 200 s of image memory. The image processing and recognition abilities are further explored by constructing an AVS using a 28 × 28 device array combined with an artificial neural network (ANN). The adjustable synaptic weight under different reverse biases allowed for optimized simulated recognition, achieving an accuracy of 92% after 160 training epochs. This work presents a novel method for creating dual‐functional photodetection and photosynaptic devices, paving the way for a more integrated and efficient AVS.
Boron Trioxide‐Assisted Post‐Annealing Enables Vertical Oriented Recrystallization of Sb2Se3 Thin Film for High‐Efficiency Solar Cells
Authors: Sheng Shuwei , Che Bo , Cai Zhiyuan , Li Jianyu , Peng Xiaoqi , Xiao Peng , Zhao Qi , Yang Junjie , Tang Rongfeng , Chen Tao 
Published: December 2024

AbstractCrystallization process is critical for enhancing the crystallinity, regulating the crystal orientation of polycrystalline thin films, as well as repairing defects within the films. For quasi‐1D Sb2Se3 photovoltaic materials, the preparation of Sb2Se3 thin films still faces great challenges in adjusting orientation and defect properties, which limits the device performance. In this study, a novel post‐treatment strategy is developed that uses a low melting point B2O3 coating layer as a flux to drive the recrystallization of Sb2Se3, thereby regulating the micro‐orientation of thermal evaporation‐derived Sb2Se3 films and optimizing their electrical properties. Mechanistic investigations show that B2O3 exhibits stronger adsorption with (hk1) planes of Sb2Se3 to induce a vertical orientation growth of the film, while blocking the volatilization channels of Se and inhibiting Se vacancy defects by interacting with Sb2Se3. The Sb2Se3 film with [hk1] preferential orientation and suppressed deep‐level defects promotes the effective transport of charge carriers in solar cells. As a result, the B2O3‐treated device delivers a champion efficiency of 9.37% without MgF2 anti‐reflection coating, which is currently the highest efficiency in Sb2Se3 solar cells achieved by thermal evaporation method. This study provides a new method and mechanism for regulating optical and electrical properties of low‐dimensional inorganic thin films.
Stereoselective Synthesis of Aliphatic α‐Amino Acids by Chemo‐Enzymatic Hydroamination‐Hydrodesulfurisation
Authors: Nobbio Celeste , Birmingham William R. , Brenna Elisabetta , Turner Nicholas J. , Tessaro Davide , Parmeggiani Fabio 
Published: December 2024

AbstractPhenylalanine ammonia lyase (PAL) enzymes have been extensively exploited to produce differently substituted arylalanine analogues, but their use in the stereoselective synthesis of aliphatic fatty amino acids has never been addressed. In this work, a two‐step hydroamination‐hydrodesulfurisation process has been investigated for the production of aliphatic L‐α‐amino acids from thienylacrylic acids, easily accessible by condensation from the corresponding arylaldehydes. Wild‐type PALs from Planctomyces brasiliensis and Streptomyces rimosus were selected as the most promising candidates and improved by site‐directed mutagenesis, thus unlocking the hydroamination of a broad panel of 10 different thienylacrylic acids bearing aliphatic and aromatic substituents. The subsequent hydrodesulfurisation step, accomplished by means of inexpensive Raney nickel in mild conditions and aqueous medium, afforded the corresponding aliphatic α‐amino acids in 10–63% overall isolated yield and perfect enantiopurity. This chemo‐enzymatic process represents the first example of aliphatic amino acid production using PALs, circumventing a major limitation of those biocatalysts.
Green Nanoengineered Keratin Derived Bio‐Adsorbent for Heavy Metals Removal from Aqueous Media
Authors: Zubair Muhammad , Roopesh M. S. , Ullah Aman 
Published: December 2024

AbstractExploiting poultry chicken feathers, a keratin‐rich by‐product offers a sustainable raw material for bio‐adsorbents in water remediation. This study developed a bio‐adsorbent from chicken feathers keratin (CFK), functionalized with surface‐modified graphene oxide (SMGO). The bio‐adsorbent was tested for adsorbing metal cations (Pb, Cd, Ni, Zn, Co) and oxyanions (As, Se, Cr) from water contaminated with 600 µg/L of each metal at pH 5.5, 7.5, and 10.5. Results showed optimal removal efficiencies at pH 7.5, with anions achieving ≥91.10% for As (III), ≥89.55% for Cr (VI), and ≥74.33% for Se (IV). Cations removal reached 96.34% for Co (II), 97.36% for Ni (II), 99.03% for Cd (II), 99.21% for Pb (II), and 59.06% for Zn (II). Kinetic studies indicated rapid initial uptake within the first 6 hours, reaching equilibrium at 24 hours. The bio‐adsorbent maintained high adsorption capacities over four regeneration cycles with minimal efficiency loss, showing strong stability and reusability. Removal efficiency followed the order: Pb (II) 〉 Cd (II) 〉 Ni (II) 〉 Co (II) 〉 Zn (II), correlating with their ionic radii. Ni2+ adsorbed more effectively than Co2+ due to a smaller ionic radius and stronger electrostatic attraction. These findings highlight CFK‐SMGO's efficacy in wastewater treatment, promoting bio‐based sustainable adsorbents.
Field‐Induced Antiferromagnetic Correlations in a Nanopatterned Van der Waals Ferromagnet: A Potential Artificial Spin Ice
Authors: Noah Avia , Fridman Nofar , Zur Yishay , Markman Maya , King Yotam Katz , Klang Maya , Rama‐Eiroa Ricardo , Solanki Harshvardhan , Ashby Michael L. Reichenberg , Levin Tamar , Herrera Edwin , Huber Martin E. , Gazit Snir , Santos Elton J. G. , Suderow Hermann , Steinberg Hadar , Millo Oded , Anahory Yonathan 
Published: December 2024

AbstractNano‐patterned magnetic materials have opened new venues for the investigation of strongly correlated phenomena including artificial spin‐ice systems, geometric frustration, and magnetic monopoles, for technologically important applications such as reconfigurable ferromagnetism. With the advent of atomically thin 2D van der Waals (vdW) magnets, a pertinent question is whether such compounds could make their way into this realm where interactions can be tailored so that unconventional states of matter can be assessed. Here, it is shown that square islands of CrGeTe3 vdW ferromagnets distributed in a grid manifest antiferromagnetic correlations, essential to enable frustration resulting in an artificial spin‐ice. By using a combination of SQUID‐on‐tip microscopy, focused ion beam lithography, and atomistic spin dynamic simulations, it is shown that a square array of CGT island as small as 150 × 150 × 60 nm3 have tunable dipole–dipole interactions, which can be precisely controlled by their lateral spacing. There is a crossover between non‐interacting islands and significant inter‐island anticorrelation depending on how they are spatially distributed allowing the creation of complex magnetic patterns not observable at the isolated flakes. These findings suggest that the cross‐talk between the nano‐patterned magnets can be explored in the generation of even more complex spin configurations where exotic interactions may be manipulated in an unprecedented way.