bluuebunny/crossref_metadata_2025_split huggingface dataset:
High‐Throughput Screening of Dual‐Atom Catalysts for Methane Combustion: A Combined Density Functional Theory and Machine‐Learning Study
Authors: Ding Jiaqi , Gu Haonan , Shi Yao , He Yi , Su Yaqiong , Yan Mi , Xie Pengfei 
Published: November 2024

AbstractCeria‐supported precious metal catalysts have undergone extensive investigation for the catalytic methane combustion. However, it remains a significant challenge to achieve both highly synergistic oxidation activity and efficient atom utilization remains a challenge for commonly used supported nanoparticles and single‐atom catalysts. Dual‐atom catalysts (DACs) emerges as a frontier of advanced catalysts, presenting unique catalytic properties that benefit from the synergy of neighboring metal sites. In this study, 361 ceria‐supported DACs (M1M2/CeO2) encompassing combinations of 19 transition metals are systematically explored. Using high‐throughput density functional theory calculations, the structures, stability as well as activity of M1M2/CeO2 are assessed. Notably, Au1Ga1/CeO2 is identified as a promising DAC exhibiting high activity for methane total oxidation, substantiated by comprehensive DFT‐calculated reaction pathways. Furthermore, employing six machine‐learning algorithms, the structure‐properties relationship is explored within ceria‐based DACs and highlight the importance of oxidation states and atomic radii of doped metals as the descriptors. The trained model by computational dataset exhibits high accuracy and predict a more active Mn1Au1/CeO2 than those screened using only DFT datasets. The high‐throughput strategy demonstrated in this work not only provides insights into the rational design of methane oxidation catalysts, but also paves the way for exploring DACs for diverse applications.
Enhancing the Stability of Cu‐Based Electrocatalyst via Fe Alloy in Electrocatalytic Formaldehyde Oxidation with Long Durability
Authors: Gao Xiafei , Pan Yuping , Qiu Janghui , Peng Juan , Wang Shuangyin , Zou Yuqin 
Published: November 2024

AbstractElectrocatalytic formaldehyde oxidation with metal Cu electrocatalyst has attracted significant interest since it can produce H2 at the anode and make it possible to construct a bipolar hydrogen production cell with low voltage. However, the activity of the Cu electrocatalyst will be greatly weakened after oxidizing it to Cu+ or Cu2+. Here, a CuFe bimetallic catalyst is developed to efficiently catalyze the electro‐oxidation process of HCHO to produce H2 at a potential of 0.10 VRHE with a current density of 100 mA cm−2. It is confirmed that introducing Fe in a CuFe catalyst can regulate the electron configuration to prevent Cu0 oxidation and improve the stability of the catalysts. The introduction of Fe can reduce the energy barrier of the reaction process, and make the C─H bond more easily split on CuFe. A bipolar hydrogen production device is constructed by combining the anodic oxidation of HCHO with the cathodic hydrogen evolution. The current density of 500 mA cm−2 is achieved at a cell voltage of 0.6 V. The faradaic efficiency is ≈100% and the device is stable for ≈50 h. The research provides a promising path toward the secure, effective, and expandable generation of high‐purity H2 at both anodic and cathodic electrodes.
Organic Ink Multi‐Material 3D Printing of Sustainable Soft Systems
Authors: Heiden Andreas , Schardax Michael , Hüttenberger Michael , Preninger David , Mao Guoyong , Schiller David , Kaltenbrunner Martin 
Published: November 2024

AbstractDrawing inspiration from nature, soft materials are at the core of a transformation toward adaptive and responsive engineered systems, capable of conquering demanding terrain and safe when interacting with biological life. Despite recent advances in 3D printing of soft materials, researchers are still far from being able to print complex soft systems where a multitude of different components need to work together symbiotically. Closing this gap necessitates a platform that unites diverse materials into one synergetic process. Here, a multi‐material printing system is presented, combining gelatin‐based hydrogels with a new biodegradable support material. This organic ink maintains up to 60° overhang and is printable over gaps to structurally support the main biogel body, while triggered dissolution enables its selective removal and the formation of internal cavities. Therefore, the creation of vascular networks, tunable scaffolds, and embedded sensors within a single printing process becomes feasible. Furthermore, a perforation‐resistant, joint‐like vacuum actuator (VAc) is designed and 3D printed, capable of bending to angles up to 60° at fast response times down to 0.23 s. Combining these approaches in an efficient, streamlined fabrication process with biodegradable materials will unlock new sustainability dimensions for complex and durable soft systems.
Matrix Metalloproteinase‐Responsive Controlled Release of Self‐Assembly Nanoparticles Accelerates Heart Valve Regeneration In Situ by Orchestrating Immunomodulation
Authors: Chen Xing , Wu Yunlong , Song Peng , Feng Liandong , Zhou Ying , Shi Jiawei , Dong Nianguo , Qiao Weihua 
Published: November 2024

AbstractIn situ tissue engineering heart valves (TEHVs) are the most promising way to overcome the defects of existing valve prostheses. Despite their promising prospects, the clinical translation of TEHVs remains a formidable challenge, mainly due to unpredictable host interactions post‐implantation. An immunomodulatory idea based on hydrogel encapsulation of nanoparticle‐coated heart valve scaffolds is introduced. Specifically, galactose‐modified human serum albumin nanoparticles (miR‐93@HSA NPs) to deliver microRNA‐93 mimics are utilized, which target macrophages and induce their differentiation into the anti‐inflammatory M2 subtype, fostering a conducive immune microenvironment. Matrix metalloproteinase (MMP)‐responsive hydrogel is used to encapsulate the nanoparticles, enabling targeted and sustained release. Results show that the miR‐93@HSA NPs exhibit excellent ability to induce macrophage polarization toward the M2 phenotype. A decellularized valve modified with hydrogel reveals MMP‐response release of the miR‐93@HSA NPs. In vitro, the immunomodulatory heart valve possesses good endocytocompatibility and effectively reprograms macrophages when cocultured with HUVECs or RAW264.7 macrophages. In vivo, this valve scaffold promises to mitigate early inflammatory damage and provide a pro‐endothelialization niche for scaffolds' constructive remodeling. With the use of cell coculture systems and transcriptome sequencing, the mechanism of immune‐modulating scaffold accelerating endothelialization is being elucidated. The immunomodulatory heart valve scaffold holds promising potential for clinical translation.
A Self‐Constructed Mg2+/K+ Co‐Doped Prussian Blue with Superior Cycling Stability Enabled by Enhanced Coulombic Attraction
Authors: Xu Zheng , Chen Fengqin , Li Yinda , Lu Yunhao , Zhou Aijun , Jiang Jicheng , Xu Xiongwen , Tu Jian , Pan Bin , Chen Fang , Huang Yi , Zhao Xinbing , Xie Jian 
Published: November 2024

AbstractPrussian blue (PB) is regarded as a promising cathode for sodium‐ion batteries because of its sustainable precursor elements (e.g., Mn, Fe), easy preparation, and unique framework structure. However, the unstable structure and inherent crystal H2O restrain its practical application. For this purpose, a self‐constructed trace Mg2+/K+ co‐doped PB prepared via a sea‐water‐mediated method is proposed to address this problem. The Mg2+/K+ co‐doping in the Na sites of PB is permitted by both thermodynamics and kinetics factors when synthesized in sea water. The results reveal that the introduced Mg2+ and K+ are immovable in the PB lattices and can form stronger K‒N and Mg‒N Coulombic attraction to relieve phase transition and element dissolution. Besides, the Mg2+/K+ co‐doping can reduce defect and H2O contents. As a result, the PB prepared in sea water exhibits an extremely long cycle life (80.1% retention after 2400 cycles) and superior rate capability (90.4% capacity retention at 20 C relative to that at 0.1 C). To address its practical applications, a sodium salts recycling strategy is proposed to greatly reduce the PB production cost. This work provides a self‐constructed Mg2+/K+ co‐doped high‐performance PB at a low preparation cost for sustainable, large‐scale energy storage.
Low‐Temperature Processed CsPbI3 for Flexible Perovskite Solar Cells Through Cs─I bond Weakening
Authors: Guo Xuemin , Zhang Wenxiao , Yuan Haobo , Cui Zhengbo , Li Wen , Shu Ting , Li Yunfei , Feng Bo , Hu Yuyang , Li Xiaodong , Fang Junfeng 
Published: November 2024

AbstractAll‐inorganic triiodide cesium lead (CsPbI3) exhibits huge potential in perovskite solar cells (PSCs). However, the high‐temperature crystallization process (≈340 or 180 °C) limits their further development, especially in flexible PSCs. Here, a Cs─I bond weakening approach is proposed to realize the low‐temperature crystallization of CsPbI3 by introducing organic sulfonate of 1‐propylsulfonate‐3‐methylimidazolium chloride (SMCl). SMCl can strongly interact with CsI and weaken the Cs─I bond to dissociate free I− ions for the effective transition of initial PbI2 to [PbI6]4−, which greatly decreases the crystallization temperature of black CsPbI3 to 90 °C. As a result, flexible PSCs are realized with efficiency of 13.86%, which is the highest efficiency of flexible CsPbI3 devices. Besides, SMCl will also help to release the tensile strain and stabilize CsPbI3 phase, leading to good thermal and mechanical stability. Almost no efficiency loss is observed in flexible PSCs after 36000 bending cycles with a curvature radius of 5 mm.
Association between surgical difficulty and tumor location based on subsegments of the Glisson branches in laparoscopic liver resection
Authors: Imamura Taisuke , Yamamoto Yusuke , Morimura Ryo , Ikoma Hisashi , Arita Tomohiro , Konishi Hirotaka , Shiozaki Atsushi , Kubota Takeshi , Fujiwara Hitoshi , Otsuji Eigo 
Published: November 2024

AbstractBackgroundLaparoscopic liver resection has a steep learning curve, and multiple difficulty‐scoring systems have been proposed to support safe implementation. Though the IWATE scoring system is widely used, the rationale for its tumor location score is unclear. The objective of our study was to establish a more accurate definition of tumor location based on subsegments of the Glisson branches.MethodsWe included 176 patients who underwent laparoscopic liver resection between January 2017 and February 2024, excluding those who underwent multiple or concomitant resections of other organs. Tumor location was defined by the most proximal subsegment of the Glisson branches (1sp, Spiegel; 1pc, para‐caval; 1cp, caudate process; 3a, apical; 3b, basal; 4a; 4b; 5v, ventral; 5d, dorsal; 6v; 6d; 6 L, lateral; 7v; 7d; 8v; 8d).ResultsWithin each segment, comparing operative time between subsegments showed significant differences, except for S1 (3a vs. 3b, p = 0.011; 4a vs. 4b, p = 0.001; 5v vs. 5d, p = 0.012; 6v vs. 6d vs. 6 L, p = 0.007; 7v vs. 7d, p = 0.003; 8v vs. 8d, p = 0.030). Blood loss significantly differed except for S1 (3a vs. 3b, p = 0.018; 4a vs. 4b, p = 0.002; 5v vs. 5d, p = 0.016; 6v vs. 6d vs. 6 L, p = 0.011; 7v vs. 7d, p = 0.013; 8v vs. 8d, p < 0.001). The incidence of postoperative complications did not differ significantly; however, hospital stay was significantly different only in S4 (4a vs. 4b, p = 0.049).ConclusionsThere are significant differences in the difficulty of laparoscopic liver resection among subsegments. More detailed scoring based on subsegments may improve accuracy, and we propose a new scoring system.
Comprehensive Study on Cell Components in High‐Voltage Pouch Cells with Lithium Perchlorate: Decomposition, Transesterification, Chlorination, Deposition, and Self‐Discharge
Authors: Weiling Matthias , Pfeiffer Felix , Lechtenfeld Christian , Stuckenberg Silvan , Fehlings Nick , Frankenstein Lars , Küpers Verena , Wang Jian‐Fen , Nowak Sascha , Baghernejad Masoud 
Published: November 2024

AbstractBattery development has traditionally focused on high energy and long lifetime cells, but there is now a shift towards their sustainability and safety. One example of this trend is the search for fluorine‐free conductive salts. The overwhelming majority of lithium‐ion conductive salts contain fluorine, which is critical regarding their environmental impact, sustainability, and toxicology. In this study, we perform a comprehensive investigation of the performance and aging mechanisms of cell components with LiClO4 as conductive salt in high‐voltage NMC622‖Graphite pouch cells. The cells containing LiClO4 show poorer electrochemical performance compared to their LiPF6 equivalents. However, to the best of our knowledge, a mechanistic understanding of the effect of LiClO4 on the aging of electrode and electrolyte components for high‐voltage cells is largely missing. Developing such an understanding will pave the way toward designing alternative salts to LiPF6, ultimately leading to fluorine‐free and more sustainable battery cells. Our results show, that the chlorination of ethyl methyl carbonate at both methyl and ethyl groups and the formation of large (Liw)AlxOyClz composite deposits on the cathode surface result from perchlorate degradation at the cathode. This leads to increased cell resistance, reduced capacity retention, and accelerated degradation of the LiClO4‐containing electrolytes.
Genotype and grain pretreatment effects on digestibility of sorghum proteins in the Ethiopian fermented bread
Authors: Belaineh Yemane G. , Bean Scott R. , Aramouni Fadi M. , Wu Xiaorong , Liu Sanzhen , Tesso Tesfaye T. 
Published: November 2024

AbstractBackground and ObjectivesSorghum is the principal food source for smallholder farmers in Sub‐Saharan Africa. Animal proteins are beyond economic reach, and only few food legumes are well‐adapted in major sorghum‐growing regions. Hence, sorghum serves as the primary source of protein and calories. However, the low digestibility of its proteins renders the communities vulnerable to protein malnutrition. Several factors, including genotypes and processing methods, have been shown to affect the digestibility of proteins in sorghum food products. The objective of this study was to investigate the impact of grain pretreatment on the protein digestibility of Ethiopian fermented flatbread.FindingsThe effect of four grain pretreatment processes: decortication, sprouting, parching, and untreated control was compared using four diverse sorghum genotypes milled to medium (2 mm) and fine (0.5 mm) particle sizes. The in‐vitro protein digestibility (IVPD) was significantly lower in the parched samples compared to the unprocessed control, while sprouting significantly increased IVPD. Decortication appears to have no impact on IVPD. Finer particle size tended to enhance IVPD in all genotypes and for all pretreatement methods. The treatments had no significant effect on protein content except the sprouting consistently but marginally increased total protein.ConclusionsSprouting sorghum grains can significantly improve the protein digestibility of fermented breads. Given that it involves little cost, the process can be readily adopted by the local community, provided that they are educated about the impact of protein deficiency on the health and productivity of the community.Significance and NoveltyLow‐cost grain pretreatment procedures such as sprouting can have a significant impact on the availability of nutrients, especially protein, the most limiting nutrient in smallholder communities. Combining the procedure with genetically enhanced varieties and improved cropping systems that integrate food legumes can significantly enhnace protein nutrition for smallholder farmers.
Pd/S cooperativity: from stoichiometric activation of Si−H bonds to catalytic hydrosilylation
Authors: Clerc Arnaud , Humbert Marceline , Mallet‐Ladeira Sonia , Miqueu Karinne , Monot Julien , Martín‐Vaca Blanca , Bourissou Didier 
Published: November 2024

AbstractWith the aim to explore metal‐ligand cooperation across Pd−S linkages, we designed a quinoline‐based PNS tridentate ligand and prepared Pd(II) complexes thereof. Optimal solubility and stability of the dicationic complex [(PNS)Pd(II)]22+ IV2 were achieved with B(C6F5)4– as counter‐anion. It adopts a thiolate‐bridged dimeric structure with a (PdS)2 core, but readily activates hydrosilanes across the Pd−S linkage. The resulting mononuclear Pd(II) hydride [(PNSSiR3)Pd(II)H]+ VI was characterized by multi‐nuclear NMR spectroscopy and the Si−H bond coordination/activation was studied computationally. Complex IV2 was found to efficiently catalyze the hydrosilylation of alkynes, internal as well as terminal, with good stereo and regioselectivity.
A Nanosized {NiII18} Cluster with a ‘Flying Saucer’ Topology Exhibiting Slow Relaxation of Magnetisation Phenomena at Both 15 K and 1.3 K
Authors: Athanasopoulou Angeliki A. , Abbasi Parisa , Alexandropoulos Dimitris I. , Hayward John J. , Beavers Christine M. , Teat Simon J. , Wernsdorfer Wolfgang , Mayans Júlia , Escuer Albert , Pilkington Melanie , Stamatatos Theocharis C. 
Published: November 2024

AbstractA high‐nuclearity {Ni18} complex (1) with a unique ‘flying saucer’ motif has been prepared from the organic chelate, α‐methyl‐2‐pyridine‐methanol (mpmH), in conjunction with bridging azido (N3−) and peroxido (O22−) ligands. Magnetic susceptibility measurements revealed the presence of both ferro‐ and antiferromagnetic exchange interactions between the metal centres in 1, and the stabilization of spin states with appreciable S values at two different temperature regimes. The end‐on bridging azido and alkoxido groups are in all likelihood the ferromagnetic mediators, while the η3:η3:μ6‐bridging peroxides most likely promote the antiparallel alignment of the metals’ spin vectors, yielding an overall non‐zero spin ground state for the centrosymmetric compound 1. Furthermore, the {Ni18} nanosized cluster behaves as a single‐molecule magnet, exhibiting magnetic hysteresis at low temperatures and two relaxation processes at 15 K and 1.3 K, a very rare phenomenon in polynuclear magnetic 3d‐metal clusters.
Switch of Five Contiguous Chiral Centers in the Synthesis of Both Enantiomers of Hajos–Parrish Ketone Analogs via Diphenylprolinol Silyl Ether‐Mediated Domino Reaction
Authors: Hayashi Yujiro , Xu Qianqian , Koshino Seitaro 
Published: November 2024

AbstractBoth enantiomers of functionalized Hajos–Parrish ketone (HPK) analogs were prepared with excellent diastereoselectivities and enantioselectivities using the same chiral catalyst under two slightly different conditions. In condition A, dioxane was used as the solvent with 3 equivalents of water. In condition B, acetonitrile was used as the solvent with 30 equivalents of water, followed by epimerization with a base in a one‐pot. The reaction consisted of a domino reaction including a diphenylprolinol silyl ether–mediated asymmetric Michael reaction and an intramolecular Henry reaction. In the Michael reaction, depending on the solvent and water amounts, syn‐ and anti‐isomers were selectively synthesized with excellent enantioselectivity, in which the absolute configuration at C5 (indanone numbering) was opposite. The subsequent Henry reaction was diastereoselective, in which the C5 substituent controlled the three chiral centers in a highly diastereoselective manner. The final base treatment in condition B caused epimerization, changing the configuration at C6. Switching more than two chiral centers with high enantioselectivity is extremely difficult using the same chiral catalyst; the present reaction is a very rare enantiodivergent reaction that switches five continuous chiral centers with high enantioselectivity.
Pattern‐moving‐based dynamic description and optimal control for non‐Newtonian mechanical systems with generalized cell mapping
Authors: Li Ning , Xu Zheng Guang , Zhao Cheng Tao , Li Xiang Quan 
Published: November 2024

AbstractThis article focuses on the problem of modelling and control for a non‐Newtonian mechanical system that may be subject to the statistical law instead of the traditional Newtonian principles mechanics. A discrete method, synthesizing the generalized cell mapping (GCM) together with dynamic programming (DP), with inverse search strategy, using pattern moving theory (PMT) framework, was proposed. The basic idea is to describe and control the system's dynamic peculiarity utilizing pattern class variable in ‘pattern moving space’. First, a few prior concepts were reviewed, including PMT, cell mapping, and optimal control for this kind system. Then, we articulated a cross‐mapping method to analyze the system dynamic behaviour, which takes into account the computational and statistical properties of pattern class variable simultaneously. For system optimal control, the improved GCM and cost function were performed to determine the discrete optimal control table (DOCT) in accordance with dynamic programming and inverse search. Finally, simulation results of two cases demonstrate the efficiency and practicality of the proposed approach. The study has resulted in a solution of describing and controlling based on pattern class variable for non‐Newtonian mechanical systems, and its main objective was to give a different perspective in term of research into non mechanistic principles modelling and application of nonlinear systems.
An Encoding ASIC With Real‐Time Correction for Inductive Angular Sensing Systems
Authors: Zhao Yuchen , Wang Kai , Shen Tao , Hu Weimin , Li Jianzheng , Qin Yajie 
Published: November 2024

ABSTRACTThis article presents an application specific integrated circuit (ASIC) for inductive angular sensing systems, integrating analog‐to‐digital converters (ADCs), digital signal processing (DSP) circuits, and a RISC‐V core on‐chip. The chip, fabricated in a 0.11‐μm CMOS process, is capable of real‐time error correction and angle encoding in response to nonideal factors such as offset, nonlinearity, and noise in the system's sensing signals. This integrated encoding solution could effectively address the issues of large system volume, saving hardware resources while achieving high precision angular measurement. A rotary encoder was additionally developed, utilizing a compact printed circuit board (PCB), which integrates the proposed ASIC, sensing front‐end circuits, and inductive coils. When the on‐chip real‐time correction is enabled, the resolution of the encoder is improved from 0.3516° to 0.0054°, and the nonlinearity error in the 360° range is reduced from 0.5507° to 0.0320°. Besides, the nonlinear error has decreased by more than 90% at different rotation speeds.