bluuebunny/crossref_metadata_2025_split huggingface dataset:
Boosting Electrochemical Nitrogen Reduction via Axial Coordination Engineering on Single‐Iron‐Atom Catalysts
Authors: Yang Yang , Wang Hanlin , Tan Xuehai , Jiang Keren , Zhai Shengli , Li Yifan , Xie Xuesong , Chen Ning , Zhang Hao , Li Zhi 
Published: May 2024

AbstractElectrocatalytic nitrogen (N2) reduction reaction (NRR) presents a sustainable alternative to the Haber–Bosch process for ammonia (NH3) synthesis. Iron phthalocyanine (FePc) is demonstrated as a promising catalyst for the electrocatalytic NRR. However, FePc with planar symmetric Fe‐N4 sites exhibits poor N2 adsorption and activation capabilities, resulting in an unsatisfactory NRR performance. Herein, an axial oxygen coordination strategy is developed to optimize the local electron distribution on FePc for improving N2 adsorption and activation. The as‐obtained FePc‐O‐CP shows a superior NH3 yield rate (59.72 µg h−1 mg−1cat.) and a considerable Faradaic efficiency (13.76%) in 0.1 m HCl. Density functional theory (DFT) calculations verify that the axial oxygen ligand on FePc inhibits the adsorption of H+ and enhances the N2 adsorption and activation, thereby greatly promoting NH3 generation. This work reveals the significance of regulating the local coordination environment of single‐atom catalysts for improving electrocatalytic NRR performance and provides a feasible strategy for the rational design of atomic‐scale active sites.
Electron Transfer from Encapsulated Fe3C to the Outermost N‐Doped Carbon Layer for Superior ORR
Authors: Quílez‐Bermejo Javier , Daouli Ayoub , Dalí Sergio García , Cui Yingdan , Zitolo Andrea , Castro‐Gutiérrez Jimena , Emo Mélanie , Izquierdo Maria T. , Mustain William , Badawi Michael , Celzard Alain , Fierro Vanessa 
Published: May 2024

AbstractEncapsulating Fe3C in carbon layers has emerged as an innovative strategy for protecting Fe3C while preserving its high oxygen reduction activity. However, fundamental questions persist regarding the active sites of encapsulated Fe3C due to the restricted accessibility of oxygen molecules to the metal sites. Herein, the intrinsic electron transfer mechanisms of Fe3C nanoparticles encapsulated in N‐doped carbon materials are unveiled for oxygen reduction electrocatalysis. The precision‐structured C1N1 material is used to synthesize N‐doped carbons with encapsulated Fe3C, significantly enhancing catalytic activity (EONSET = 0.98 V) and achieving near‐100% operational stability. In anion‐exchange membrane fuel cells, an excellent peak power density of 830 mW cm−2 is reached at 60 °C. The experimental and computational results revealed that the presence of Fe3C cores dynamically triggers electron transfer to the outermost carbon layer. This phenomenon amplifies the oxygen reduction reaction performance at N sites, contributing significantly to the observed catalytic enhancement.
All‐in‐One: Photo‐Responsive Lanthanide‐Organic Framework for Simultaneous Sensing, Adsorption, and Photocatalytic Reduction of Uranium
Authors: Huang Zhi‐Wei , Li Xiao‐Bo , Mei Lei , Han Yi‐Zhi , Song Yu‐Ting , Fu Xuan , Zhang Zhi‐Hui , Guo Zhi‐Jun , Zeng Jian‐Rong , Bian Feng‐Gang , Wu Wang‐Suo , Hu Kong‐Qiu , Shi Wei‐Qun 
Published: May 2024

AbstractThe selective removal and immobilization of uranyl ions from aqueous solutions is essential for the sustainable development of nuclear energy. Herein, a robust lanthanide‐organic framework material (IHEP‐24) is developed for simultaneous fluorescence sensing, selective adsorption, and photocatalytic reduction of uranium, integrating three different functions in one material. The confined space formed by the coordination assembly of viologen derivative ligands and metal‐oxygen clusters can act as precise recognition sites for uranyl, allowing IHEP‐24 to efficiently detect and capture uranyl ions. In addition, the presence of a viologen‐based radical ligand enables IHEP‐24 to a further photocatalytic reduction of the adsorbed uranyl to amorphous UO2. The mechanisms of adsorption and photocatalysis are revealed by batch experiments, photoelectrochemical characterizations, and theoretical calculations. This study provides a reference for the construction of robust multi‐functional MOF materials and also provides support for the deep removal and immobilization of radionuclides from aqueous solution.
Wet Spun Composite Fiber with an Ordered Arrangement of PEDOT:PSS‐Coated Te Nanowires for High‐Performance Wearable Thermoelectric Generator
Authors: Li Jiajia , Wang Junhui , Yang Xiao , Dong Guoying , Liu Ying , Wang Zixing , Zhang Mingcheng , Zuo Xinru , Han Xiaowen , Wu Changxuan , Zhang Ting , Liu Ruiheng , Cai Kefeng , Chen Lidong 
Published: May 2024

AbstractThermoelectric (TE) fibers are more suitable than films for portable or wearable devices. Herein, 2–3 nm thick poly (3,4‐ethylenedioxythiophene): poly (styrenesulfonate) (PEDOT:PSS) layer‐coated tellurium nanowires (PC‐Te NWs) are in situ prepared by a hydrothermal method. Then a series of PEDOT: PSS/PC‐Te NWs composite fibers are prepared by wet spinning and post‐treatment. The nanolayer prevents the agglomeration of the Te NWs and makes the NWs and PEDOT:PSS matrix have good compatibility, which results in the PC‐Te NWs content to a high value of 70 wt% and the fibers still with flexibility. The high aspect ratio of the PC‐Te NWs and the stress from the inner wall of the needle during spinning make the NWs ordered align along the composite fiber. Due to the large content and orientational arrangement of the PC‐Te NWs, as well as effective post‐treatment, an optimized composite fiber shows a power factor of 385.4 µW m−1 K−2 at 300 K, which is ≈4.9 times as high as the highest value of previously reported PEDOT:PSS/Te NWs‐based composite fibers. In addition, the composite fiber has good flexibility. The flexible TE generators assembled have excellent output performance. This work provides an effective strategy for the preparation of high‐performance flexible TE composite fibers.
Porous Aromatic Frameworks Enabling Polyiodide Confinement toward High Capacity and Long Lifespan Zinc–Iodine Batteries
Authors: Hu Junfang , Zhang Zhaofu , Deng Ting , Cui Feng Chao , Shi Xiaoyuan , Tian Yuyang , Zhu Guangshan 
Published: May 2024

AbstractAqueous zinc–iodine batteries (AZIBs) are attracting increasing attention because of their high safety and abundance of resources. However, the performance of AZIBs is compromised by inadequate confinement of soluble polyiodides, the undesired shuttle effect, and slow reaction kinetics. In this study, a porous aromatic framework (PAF) with abundant benzene motifs and a well‐organized pore structure is adopted as the iodine host, which exhibits high iodine adsorption capacity and robust polyiodide confinement. Both experimental characterizations and theoretical simulations indicate that the interactions between iodine species and the PAF‐1 facilitate the redox reaction by coupling the electronic structures of the active species in the framework. A comparison of PAF‐1, PAF‐5, and PAF‐11 also emphasizes the structural advantages of the high surface area and interconnected three‐dimensional channels of PAF‐1. Consequently, the I2@PAF‐1 cathode can deliver a high capacity of 328 mAh g−1 at 0.5 C, outstanding rate performance, and a stable cycling life of 20 000 cycles (86 % retention at 10 C). The robust polyiodide confinement and superb electrochemical performance of Zn–I2@PAF‐1 provide insights into the practical application of PAFs as excellent electrode materials for AZIBs.
Enabling Low Pressure, Low Temperature, and Particle Control for Anisotropic Conductive Adhesives
Authors: Huynh Van Long , Aasmundtveit Knut E. , Nguyen Hoang‐Vu 
Published: May 2024

AbstractAnisotropic conductive adhesives (ACAs) are the preferred interconnection technology for applications that employ large dies, flexible substrates, and ultra fine‐pitch interconnects. Conventional ACAs require relatively high bonding pressures and temperatures, and ultra fine‐pitch applications challenge the trade‐off between low interconnect resistance and risk of short circuits. This study introduces an ACA‐like interconnection technology that addresses these limitations, allowing for low‐pressure, low‐temperature assembly processes with enhanced particle control at the interconnects. Conductive particles are deposited onto a patterned carrier and subsequently transferred to electrical pads using either non‐conductive film or Ag sintering. The Ag sintering process is performed at a low temperature (140 °C) and low bonding pressure (1 N for a 10 × 10 mm2 chip). The capability of controlling the position and number of conductive particles within individual interconnects is demonstrated. This presents possibilities for achieving ultra‐fine pitch interconnects with negligible risk of short circuits, without compromising electrical resistance. It is demonstrated that interconnect resistance can be tuned by varying the number of conductive particles (achieving a resistance as low as 33 mΩ with 25 particles per interconnect). This approach is applicable to scenarios where the bonding force and temperature must remain low due to the nature of substrate materials.
One‐Pot Synthesis of 2‐Aminothiophenes by Au(I)‐Catalyzed Cascade Reaction Including Hydrothiolation, Thio‐Claisen Rearrangement, and Cycloisomerization
Authors: Oonishi Yoshihiro , Ueda Yukiko , Sato Yoshihiro 
Published: May 2024

AbstractThe cascade reaction of ynamides with propargyl thiols by Au(I) catalysis involving regioselective hydrothiolation, thio‐Claisen rearrangement, and cycloisomerization to generate 2‐aminothiophenes in a one‐pot manner is described. In this reaction, the selection of reaction temperature is crucial, with the initial step, namely hydrothiolation, conducted at a low temperature (40 °C), followed by the subsequent reaction requiring an increase in temperature (>110 °C). Furthermore, it was revealed that multi‐substituted anilines could be synthesized from the resulting 2‐aminothiophenes.
Bromine‐Enhanced Organic Materials for X‐ray Sensors: Unveiling the Potential of Small Molecules and Polymers through Material Design and Film Fabrication
Authors: Dobužinskas Rokas , Poškus Andrius , Jankauskas Vygintas , Viliūnas Mindaugas , Kamarauskas Egidijus , Daškevičienė Marytė , Getautis Vytautas , Arlauskas Kęstutis , Abramavičius Darius 
Published: May 2024

AbstractOrganic X‐ray sensors are a promising new class of detectors with the potential to revolutionize medical imaging, security screening, and other applications. However, the development of high‐performance organic X‐ray sensors is challenged by low sensitivity. This paper reports on the development of nine X‐ray sensors based on new organic materials. It is demonstrated that the incorporation of bromine atoms into the sidechains of carbazolyl‐containing organic molecules significantly enhances their X‐ray sensitivity. This research suggests that incorporating a variety of high‐atomic‐number chemical elements into well‐established organic semiconductors is a promising strategy for designing efficient X‐ray sensor materials.
Antibiotic‐Induced Gut Microbiota Dysbiosis Modulates Host Transcriptome and m6A Epitranscriptome via Bile Acid Metabolism
Authors: Yang Meng , Zheng Xiaoqi , Fan Jiajun , Cheng Wei , Yan Tong‐Meng , Lai Yushan , Zhang Nianping , Lu Yi , Qi Jiali , Huo Zhengyi , Xu Zihe , Huang Jia , Jiao Yuting , Liu Biaodi , Pang Rui , Zhong Xiang , Huang Shi , Luo Guan‐Zheng , Lee Gina , Jobin Christian , Eren A. Murat , Chang Eugene B , Wei Hong , Pan Tao , Wang Xiaoyun 
Published: May 2024

AbstractGut microbiota can influence host gene expression and physiology through metabolites. Besides, the presence or absence of gut microbiome can reprogram host transcriptome and epitranscriptome as represented by N6‐methyladenosine (m6A), the most abundant mammalian mRNA modification. However, which and how gut microbiota‐derived metabolites reprogram host transcriptome and m6A epitranscriptome remain poorly understood. Here, investigation is conducted into how gut microbiota‐derived metabolites impact host transcriptome and m6A epitranscriptome using multiple mouse models and multi‐omics approaches. Various antibiotics‐induced dysbiotic mice are established, followed by fecal microbiota transplantation (FMT) into germ‐free mice, and the results show that bile acid metabolism is significantly altered along with the abundance change in bile acid‐producing microbiota. Unbalanced gut microbiota and bile acids drastically change the host transcriptome and the m6A epitranscriptome in multiple tissues. Mechanistically, the expression of m6A writer proteins is regulated in animals treated with antibiotics and in cultured cells treated with bile acids, indicating a direct link between bile acid metabolism and m6A biology. Collectively, these results demonstrate that antibiotic‐induced gut dysbiosis regulates the landscape of host transcriptome and m6A epitranscriptome via bile acid metabolism pathway. This work provides novel insights into the interplay between microbial metabolites and host gene expression.
A Composite Hydrogel Functionalized by Borosilicate Bioactive Glasses and VEGF for Critical‐Size Bone Regeneration
Authors: Huang Chao , Shi Shun , Qin Muyan , Rong Xiao , Ding Zichuan , Fu Xiaoxue , Zeng Weinan , Luo Lei , Wang Deping , Luo Zeyu , Li Yiwen , Zhou Zongke 
Published: May 2024

AbstractCritical‐size bone defects pose a formidable challenge in clinical treatment, prompting extensive research efforts to address this problem. In this study, an inorganic–organic multifunctional composite hydrogel denoted as PLG‐g‐TA/VEGF/Sr‐BGNPs is developed, engineered for the synergistic management of bone defects. The composite hydrogel demonstrated the capacity for mineralization, hydroxyapatite formation, and gradual release of essential functional ions and vascular endothelial growth factor (VEGF) and also maintained an alkaline microenvironment. The composite hydrogel promoted the proliferation and osteogenic differentiation of rat bone marrow mesenchymal stem cells (rBMSCs), as indicated by increased expression of osteogenesis‐related genes and proteins in vitro. Moreover, the composite hydrogel significantly enhanced the tube‐forming capability of human umbilical vein endothelial cells (HUVECs) and effectively inhibited the process of osteoblastic differentiation of nuclear factor kappa‐B ligand (RANKL)‐induced Raw264.7 cells and osteoclast bone resorption. After the implantation of the composite hydrogel into rat cranial bone defects, the expression of osteogenic and angiogenic biomarkers increased, substantiating its efficacy in promoting bone defect repair in vivo. The commendable attributes of the multifunctional composite hydrogel underscore its pivotal role in expediting hydrogel‐associated bone growth and repairing critical bone defects, positioning it as a promising adjuvant therapy candidate for large‐segment bone defects.
Lignin‐Derived Lightweight Carbon Aerogels for Tunable Epsilon‐Negative Response
Authors: Qu Yunpeng , Zhou Yunlei , Yang Qiuyun , Cao Jun , Liu Yao , Qi Xiaosi , Jiang Shan 
Published: May 2024

AbstractElectromagnetic (EM) metamaterials have garnered considerable attention due to their capacity to achieve negative parameters, significantly influencing the integration of natural materials with artificially structural media. The emergence of carbon aerogels (CAs) offers an opportunity to create lightweight EM metamaterials, notable for their promising EM shielding or absorption effects. This paper introduces an efficient, low‐cost method for fabricating CAs without requiring stringent drying conditions. By finely tuning the ZnCl2/lignin ratio, the porosity is controlled in CAs. This control leads to an epsilon‐negative response in the radio‐frequency region, driven by the intrinsic plasmonic state of the 3D carbon network, as opposed to traditional periodic building blocks. This approach yields a tunable and weakly epsilon‐negative response, reaching an order of magnitude of −103 under MHz frequencies. Equivalent circuit analysis highlights the inductive characteristics of CAs, correlating their significant dielectric loss at low frequencies. Additionally, EM simulations are performed to evaluate the distribution of the electric field vector in epsilon‐negative CAs, showcasing their potential for effective EM shielding. The lignin‐derived, lightweight CAs with their tunable epsilon‐negative response hold promise for pioneering new directions in EM metamaterials and broadening their application in diverse extreme conditions.
Single‐Cell Transcriptome Landscape and Cell Fate Decoding in Human Brain Organoids after Transplantation
Authors: Xu Shi‐Bo , Li Xin‐Rui , Fan Pan , Li Xiyang , Hong Yuan , Han Xiao , Wu Shanshan , Chu Chu , Chen Yuejun , Xu Min , Lin Mingyan , Guo Xing , Liu Yan 
Published: May 2024

AbstractHuman stem cells and derivatives transplantation are widely used to treat nervous system diseases, while the fate determination of transplanted cells is not well elucidated. To explore cell fate changes of human brain organoids before and after transplantation, human brain organoids are transplanted into prefrontal cortex (PFC) and hippocampus (HIP), respectively. Single‐cell sequencing is then performed. According to time‐series sample comparison, transplanted cells mainly undergo neural development at 2 months post‐transplantation (MPT) and then glial development at 4MPT, respectively. A different brain region sample comparison shows that organoids grafted to PFC have obtained cell fate close to those of host cells in PFC, other than HIP, which may be regulated by the abundant expression of dopamine (DA) and acetylcholine (Ach) in PFC. Meanwhile, morphological complexity of human astrocyte grafts is greater in PFC than in HIP. DA and Ach both activate the calcium activity and increase morphological complexity of astrocytes in vitro. This study demonstrates that human brain organoids receive host niche factor regulation after transplantation, resulting in the alignment of grafted cell fate with implanted brain regions, which may contribute to a better understanding of cell transplantation and regenerative medicine.
Plastic Crystal Fast Ion‐Conductor Electrolyte Enabled Ultra‐Low Temperature Rechargeable Organic Battery
Authors: Qin Jian , Liu Yutao , Li Gaofeng , Lan Qing , Song Zhiping , Ai Xinping , Zhan Hui 
Published: May 2024

AbstractBattery performance is much damaged by ultra‐low‐temperature (<−80 °C), due to the insufficient ionic conductivity and high desolvation energy barrier. The strong coupling between ion dissociation and ion‐desolvation much increases the difficulty in electrolyte‐design. Here, it is demonstrated that such issue can be fundamentally addressed by a salt‐led electrolyte engineering. The salt with poor interionic interaction can be easily dissociated under appropriate solvation force even at extremely low‐temperature. The new electrolyte‐design logic is validated by 1‐ethyl‐1‐methylpyrrolidinium bis(fluorosulfonyl)imide, an organic ionic plastic‐crystals (OIPCs)‐characteristic salt. With the mild solvation assistance from methyl acetate, the electrolyte supplies considerable conductivity of 0.36 mS cm−1 at −110 °C and enables the smooth charging/discharging of polyimide/polytriphenylamine all‐organic cell at ultra‐low‐temperature. Even with high material loading, the cell reserves 65% of theoretical capacity under 0.2 C‐rate at −110 °C. This work represents a significant advancement in the low‐temperature batteries, and provides new knowledge of the ionic dynamics of electrolyte.
Interfacial Design Strategy for Polymeric Lithium Metal Batteries with Superfast Charge‐Transfer Kinetics
Authors: Li Kai , Wang Jifeng , Shen Qingyun , Song Yuanyuan , Gao Rui , Wang Ying 
Published: May 2024

AbstractInterfacial instability including the high charge‐transfer resistance and the uncontrolled lithium dendrite growth have severely restricted the safety, fast‐charging, and high‐power capabilities of solid‐state polymeric lithium metal batteries (PLMBs). Here, the study demonstrates the ionic nanoclusters self‐assembled between the lithium ions and a rigid‐rod sulfonated aromatic polyamide Poly 2,2′‐disulfonyl‐4,4′‐benzidine terephthalamide (PBDT) can facilitate uniform lithium deposition; meanwhile, realizing 102–103 times lower interfacial charge‐transfer resistance than PEO‐based electrolytes and excellent lithium dendrite suppression at the interfaces. The cells assembled with this solid‐state polymer electrolyte at room temperature show a record high critical current density (6 mA cm−2/3 mAh cm−2), 80% capacity retention at 10 000 cycles (5 C) with the LiFePO4 cathode. With the temperature increased to 80 °C, the cells enable almost 100% of the theoretical capacity at 3 C and high specific power density (20 kW kg−1). According to the Cryo‐TEM imaging and computational simulation results, it is concluded that these nanoscale self‐assembled ionic nanoclusters play a critical role in realizing the superfast charge‐transfer kinetics by balancing the pre‐exponential factor and activation energy at the lithium‐polymer space‐charge interfaces. This interfacial design strategy based on thermodynamically favored ion‐association and self‐assembly between the metal ions and the polyanions guarantees superior charge‐transfer kinetics in PLMBs.
Patient with a heterozygous pathogenic variant in CSNK2A1 gene: A new case to update the Okur–Chung neurodevelopmental syndrome
Authors: Blanc Albin , Bonnet Céline , Wandzel Marion , Roth Virginie , Duffourd Yannis , Safraou Hanna , Leheup Bruno , Muller Florence , D Colne Julie , Feillet François , Schmitt Emmanuelle , Castro Matheus , Savatt Jullian , Burcheri Adriano , Nemos Christophe , Philippe Christophe , Lambert Laëtitia 
Published: May 2024

AbstractThe autosomal dominant Okur–Chung neurodevelopmental syndrome (OCNDS: OMIM #617062) is a rare neurodevelopmental disorder first described in 2016. Features include developmental delay (DD), intellectual disability (ID), behavioral problems, hypotonia, language deficits, congenital heart abnormalities, and non‐specific dysmorphic facial features. OCNDS is caused by heterozygous pathogenic variants in CSNK2A1 (OMIM *115440; NM_177559.3). To date, 160 patients have been diagnosed worldwide. The number will likely increase due to the growing use of exome sequencing (ES) and genome sequencing (GS). Here, we describe a novel OCNDS patient carrying a CSNK2A1 variant (NM_177559.3:c.140G>A; NP_808227.1:p.Arg47Gln). Phenotypically, he presented with DD, ID, generalized hypotonia, speech delay, short stature, microcephaly, and dysmorphic features such as low‐set ears, hypertelorism, thin upper lip, and a round face. The patient showed several signs not yet described that may extend the phenotypic spectrum of OCNDS. These include prenatal bilateral clubfeet, exotropia, and peg lateral incisors. However, unlike the majority of descriptions, he did not present sleep disturbance, seizures or gait difficulties. A literature review shows phenotypic heterogeneity for OCNDS, whether these patients have the same variant or not. This case report is an opportunity to refine the phenotype of this syndrome and raise the question of the genotype–phenotype correlation.