bluuebunny/crossref_metadata_2025_split huggingface dataset:
Confinement of Ultrasmall Bimetallic Nanoparticles in Conductive Metal–Organic Frameworks via Site‐Specific Nucleation
Authors: Park Chungseong , Koo Won‐Tae , Chong Sanggyu , Shin Hamin , Kim Yoon Hwa , Cho Hee‐Jin , Jang Ji‐Soo , Kim Dong‐Ha , Lee Jiyoung , Park Seyeon , Ko Jaehyun , Kim Jihan , Kim Il‐Doo 
Published: August 2021

AbstractConductive metal–organic frameworks (cMOFs) are emerging materials for various applications due to their high surface area, high porosity, and electrical conductivity. However, it is still challenging to develop cMOFs having high surface reactivity and durability. Here, highly active and stable cMOF are presented via the confinement of bimetallic nanoparticles (BNPs) in the pores of a 2D cMOF, where the confinement is guided by dipolar‐interaction‐induced site‐specific nucleation. Heterogeneous metal precursors are bound to the pores of 2D cMOFs by dipolar interactions, and the subsequent reduction produces ultrasmall (≈1.54 nm) and well‐dispersed PtRu NPs confined in the pores of the cMOF. PtRu‐NP‐decorated cMOFs exhibit significantly enhanced chemiresistive NO2 sensing performances, owing to the bimetallic synergies of PtRu NPs and the high surface area and porosity of cMOF. The approach paves the way for the synthesis of highly active and conductive porous materials via bimetallic and/or multimetallic NP loading.
Low‐Density Fluorinated Silane Solvent Enhancing Deep Cycle Lithium–Sulfur Batteries’ Lifetime
Authors: Liu Tao , Shi Zhe , Li Huajun , Xue Weijiang , Liu Shanshan , Yue Jinming , Mao Minglei , Hu Yong‐sheng , Li Hong , Huang Xuejie , Chen Liquan , Suo Liumin 
Published: August 2021

AbstractThe lithium metal anode (LMA) instability at deep cycle with high utilization is a crucial barrier for developing lithium (Li) metal batteries, resulting in excessive Li inventory and electrolyte demand. This issue becomes more severe in capacity‐type lithium–sulfur (Li–S) batteries. High‐concentration or localized high‐concentration electrolytes are noted as effective strategies to stabilize Li metal but usually lead to a high electrolyte density (>1.4 g mL−1). Here we propose a bifunctional fluorinated silane‐based electrolyte with a low density of 1.0 g mL−1 that not only is much lighter than conventional electrolytes (≈1.2 g mL−1) but also form a robust solid electrolyte interface to minimize Li depletion. Therefore, the Li loss rate is reduced over 4.5‐fold with the proposed electrolyte relative to its conventional counterpart. When paired with onefold excess LMA at the electrolyte weight/cell capacity (E/C) ratio of 4.5 g Ah−1, the Li–S pouch cell using our electrolyte can survive for 103 cycles, much longer than with the conventional electrolyte (38 cycles). This demonstrates that our electrolyte not only reduces the E/C ratio but also enhances the cyclic stability of Li–S batteries under limited Li amounts.
Rational Design of Highly Stable and Active MXene‐Based Bifunctional ORR/OER Double‐Atom Catalysts
Authors: Wei Bo , Fu Zhongheng , Legut Dominik , Germann Timothy C. , Du Shiyu , Zhang Haijun , Francisco Joseph S. , Zhang Ruifeng 
Published: August 2021

AbstractDesigning highly active and bifunctional oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) catalysts has attracted great interest toward metal–air batteries. Herein, an efficient solution to the search for MXene‐based bifunctional catalysts is proposed by introducing non‐noble metals such as Fe/Co/Ni at the surfaces. These results indicate that the ultrahigh activities in Ni1/Ni2‐ and Fe1/Ni2‐modified MXene‐based double‐atom catalysts (DACs) for bifunctional ORR/OER are better than those of well‐known unifunctional catalysts with low overpotentials, such as Pt(111) for the ORR and IrO2(110) for the OER. Strain can profoundly regulate the catalytic activities of MXene‐based DACs, providing a novel pathway for tunable catalytic behavior in flexible MXenes. An electrochemical model, based on density functional theory and theoretical polarization curves, is proposed to reveal the underlying mechanisms, in agreement with experimental results. Electronic structure analyses indicate that the excellent catalytic activities in the MXene‐based DACs are attributed to the electron‐capturing capability and synergistic interactions between Fe/Co/Ni adsorbents and MXene substrate. These findings not only reveal promising candidates for MXene‐based bifunctional ORR/OER catalysts but also provide new theoretical insights into rationally designing noble‐metal‐free bifunctional DACs.
An Anti‐Fatigue Design Strategy for 3D Ribbon‐Shaped Flexible Electronics
Authors: Cheng Xu , Zhang Fan , Bo Renheng , Shen Zhangming , Pang Wenbo , Jin Tianqi , Song Honglie , Xue Zhaoguo , Zhang Yihui 
Published: August 2021

AbstractThree‐dimensional (3D) flexible electronics represent an emerging area of intensive attention in recent years, owing to their broad‐ranging applications in wearable electronics, flexible robots, tissue/cell scaffolds, among others. The widely adopted 3D conductive mesostructures in the functional device systems would inevitably undergo repetitive out‐of‐plane compressions during practical operations, and thus, anti‐fatigue design strategies are of great significance to improve the reliability of 3D flexible electronics. Previous studies mainly focused on the fatigue failure behavior of planar ribbon‐shaped geometries, while anti‐fatigue design strategies and predictive failure criteria addressing 3D ribbon‐shaped mesostructures are still lacking. This work demonstrates an anti‐fatigue strategy to significantly prolong the fatigue life of 3D ribbon‐shaped flexible electronics by switching the metal‐dominated failure to desired polymer‐dominated failure. Combined in situ measurements and computational studies allow the establishment of a failure criterion capable of accurately predicting fatigue lives under out‐of‐plane compressions, thereby providing useful guidelines for the design of anti‐fatigue mesostructures with diverse 3D geometries. Two mechanically reliable 3D devices, including a resistance‐type vibration sensor and a janus sensor capable of decoupled temperature measurements, serve as two demonstrative examples to highlight potential applications in long‐term health monitoring and human‐like robotic perception, respectively.
SnO2‐SiO2 1D Core‐Shell Nanowires Heterostructures for Selective Hydrogen Sensing
Authors: Raza Muhammad Hamid , Kaur Navpreet , Comini Elisabetta , Pinna Nicola 
Published: August 2021

AbstractSnO2 is one of the most employed n‐type semiconducting metal oxide in chemo‐resistive gas‐sensing although it presents serious limitations due to a low selectivity. Herein, the authors introduce 1D SnO2‐SiO2 core‐shell nanowires (CSNWs). The amorphous SiO2‐shell layer with varying thicknesses (1.8–10.5 nm) is grown onto the SnO2 nanowires (NWs) by atomic layer deposition (ALD). SiO2‐coated SnO2 CSNWs show a dramatic improvement of the selectivity towards hydrogen. Moreover, the sensing‐response is strongly correlated to the thickness of the SiO2‐shell and the working temperature. The SnO2‐SiO2 CSNWs sensor with a 4.8‐nm SiO2 shell thickness exhibits the best selectivity and sensitivity, having ca. 7‐fold higher response toward hydrogen compared to bare‐SnO2 NWs. The selectivity and enhanced sensing‐response are related to the masking effect of the SiO2 shell and an increase in the width of the electron‐depletion‐layer due to a strong electronic coupling between the SnO2 core and SiO2 coating, respectively.
Insights into Optical Probes Based on Aggregation‐Induced Emission: from Restriction of Intramolecular Motions to Dark State
Authors: Huang Shuai , Ding Jipeng , Bi Anyao , Yu Kunqian , Zeng Wenbin 
Published: August 2021

AbstractSince the exposure of the concept of aggregation‐induced emission (AIE) to the scientific community in 2001, AIE fluorophores attract much attention for biological imaging, detection, and advanced material fabrications. Some efforts have been devoted to the mechanism studies on the luminescence nature of AIE fluorophores. Restriction of intramolecular motions (RIM) can explain the luminescence mechanism at a relatively large level and has been recognized as the general working mechanism of AIE. To disclose the connotation of the RIM mechanism, an in‐depth study to elucidate the dark state of AIE molecules is needed. In this review, the recent progress of luminescence quenching mechanisms for AIE molecules is summarized and compendiously categorized into four parts, which are: restriction of access to dark state (RADS), restricted access to a conical intersection (RACI), restrict molecules from entering twisted intramolecular charge transfer (TICT) state, and excited state intramolecular proton transfer (ESIPT) coupled with TICT state, respectively. These insights and systematical elucidation of the emission quenching in the view of dark state are of great significance for fundamental understanding. It is hoped that this feature article will attract more researcher's interests and open up new vistas for the development of aggregate science.
Giant Bulk Photostriction and Accurate Photomechanical Actuation in Hybrid Perovskites
Authors: Lv Xingjie , Dong Shuai , Huang Xin , Cao Bo , Zeng Shouxin , Wang Yaojin , Wu Tom , Chen Lang , Wang Junling , Yuan Guoliang , Liu Jun‐Ming 
Published: August 2021

AbstractIt is well known that a material may be strained by mechanical, thermal, electric, magnetic, and light stimuli, and this effect has been extensively utilized in industries. However, the observed photostrictive effect usually occurs in the very thin surface layer and the photostriction of most bulk materials has been too small to be applied in a device until now. Here, a giant bulk photostriction is achieved, evidenced by the measured linear strain ε ≈ 0.72–0.43% for MAPbI3 single crystal plates of 0.05–0.5 mm in thickness under the 532 nm illumination. More importantly, the MAPbI3 single crystals also exhibit accurate photomechanical actuation functionality and the actuator can precisely adjust the displacement from hundreds of pm to tens of μm or the angle of a hard mirror from ≈10−6 to 0.2 degree. The present work not only unveils the huge bulk photostriction in lead halide perovskite single crystals but also demonstrates a wireless photomechanical actuator which is much simpler and smaller than conventional piezoelectric actuators.
Revealing Ammonia Quantification Minefield in Photo/Electrocatalysis
Authors: Zhao Yunxuan , Wu Fan , Miao Yingxuan , Zhou Chao , Xu Ning , Shi Run , Wu Li‐Zhu , Tang Junwang , Zhang Tierui 
Published: August 2021

AbstractPhoto/electrocatalytic ammonia synthesis has recently developed fast while the ammonia yields over state‐of‐the‐art photo/electrocatalysts are still very moderate. Such low concentration of synthesized NH3 brings about a challenge to the reliable quantification of the product in photo/electrocatalysis. Notably, we found that the quantitative detection of ammonia concentration below 0.2 ppm is error‐prone, which is likely the case happening in the majority of photo/electrocatalytic NH3 synthesis, thus arising concerns about the rationality and accuracy for low‐concentration ammonia quantification in these processes. Herein, we discuss the methodology used and analyze the reliability of various detection methods for the detection of trace ammonia in aqueous media. The challenges facing the detection of low concentration of ammonia in photo/electrocatalysis can be overcome by integration with multiple detection methods. According to the data presented, we also propose an effective criterion for precise quantification of ammonia, avoiding the unreasonable comparisons in photo/electrocatalytic ammonia synthesis.
Radically Enhanced Dual Recognition
Authors: Chen Xiao‐Yang , Mao Haochuan , Feng Yuanning , Cai Kang , Shen Dengke , Wu Huang , Zhang Long , Zhao Xingang , Chen Hongliang , Song Bo , Jiao Yang , Wu Yong , Stern Charlotte L. , Wasielewski Michael R. , Stoddart J. Fraser 
Published: August 2021

AbstractComplexation between a viologen radical cation (V.+) and cyclobis(paraquat‐p‐phenylene) diradical dication (CBPQT2(.+)) has been investigated and utilized extensively in the construction of mechanically interlocked molecules (MIMs) and artificial molecular machines (AMMs). The selective recognition of a pair of V.+ using radical‐pairing interactions, however, remains a formidable challenge. Herein, we report the efficient encapsulation of two methyl viologen radical cations (MV.+) in a size‐matched bisradical dicationic host — namely, cyclobis(paraquat‐2,6‐naphthalene)2(.+), i.e., CBPQN2(.+). Central to this dual recognition process was the choice of 2,6‐bismethylenenaphthalene linkers for incorporation into the bisradical dicationic host. They provide the space between the two bipyridinium radical cations in CBPQN2(.+) suitable for binding two MV.+ with relatively short (3.05–3.25 Å) radical‐pairing distances. The size‐matched bisradical dicationic host was found to exhibit highly selective and cooperative association with the two MV.+ in MeCN at room temperature. The formation of the tetrakisradical tetracationic inclusion complex — namely, [(MV)2⊂CBPQN]4(.+) – in MeCN was confirmed by VT 1H NMR, as well as by EPR spectroscopy. The solid‐state superstructure of [(MV)2⊂CBPQN]4(.+) reveals an uneven distribution of the binding distances (3.05, 3.24, 3.05 Å) between the three different V.+, suggesting that localization of the radical‐pairing interactions has a strong influence on the packing of the two MV.+ inside the bisradical dicationic host. Our findings constitute a rare example of binding two radical guests with high affinity and cooperativity using host‐guest radical‐pairing interactions. Moreover, they open up possibilities of harnessing the tetrakisradical tetracationic inclusion complex as a new, orthogonal and redox‐switchable recognition motif for the construction of MIMs and AMMs.
Bead‐free and tough electrospun PCL/gelatin/PGS ternary nanofibrous scaffolds for tissue engineering application
Authors: Behtouei Ebrahim , Zandi Mojgan , Askari Fahimeh , Daemi Hamed , Zamanlui Soheila , Arabsorkhi‐Mishabi Amirhesam , Pezeshki‐Modaress Mohamad 
Published: August 2021

AbstractPoly(glycerol sebacate) (PGS) is a biodegradable and biocompatible polyester that is increasingly used in the biomedical field. Herein, a novel ternary poly(ε‐caprolactone)/gelatin/PGS (PCL/gelatin/PGS) blend nanofibers were designed and fabricated with a wide range of chemical compositions, mechanical properties, and modulated degradability levels. PGS blends with gelatin are commonly used for enhancing electrospinability but their low‐mechanical properties, lack of structural stability in an aqueous medium, and unmodulated degradation behavior limited their application. Blending PGS and gelatin with PCL could improve their properties in a ternary structure. In addition, considering ternary blends of PCL/gelatin/PGS, an enhancement of hydrophilicity due to the presence of gelatin in the system is expected, resulting in better biocompatibility and controlled biodegradation. By increasing the polymer concentration, voltage, and distance of the needle to the collector, the bead‐free electrospun nanofibers were obtained. The ternary blend nanofibers with an equal weight ratio of polymers, T33 (containing 33 wt% PGS, 33 wt% gelatin, and 33 wt% PCL), possess more than a 4‐fold increase in tensile strength (7 MPa) and 89‐fold increase in elongation at break (1760.6%) compared to gelatin/PGS binary nanofibers. In vitro studies on glioma cells showed well attachment and proliferation of C6 glioma cells. The obtained results demonstrated the potential of these scaffolds for nerve tissue engineering applications.
Carboxylated nanocellulose superabsorbent: Biodegradation and soil water retention properties
Authors: Barajas‐Ledesma Ruth M. , Wong Vanessa N. L. , Little Karen , Patti Antonio F. , Garnier Gil 
Published: August 2021

AbstractIn this study, TEMPO (2,2,6,6‐tetramethylpiperidine‐1‐oxyl)‐oxidized nanocellulose superabsorbents are prepared using three different drying techniques: freeze‐dried, and oven‐dried at low and high temperatures. The benefits are investigated by evaluating the superabsorbent structure, composition and application rate. The absorption performance of nanocellulose superabsorbents is affected by the concentration and type of salts in the soil water extracts. Oven‐dried at 50°C SAP presents the highest ionic sensitivity attributed to its large number of accessible carboxylate groups. The water retention of the soil treatments increases with increasing application rate. Soil treated with the freeze‐dried superabsorbent shows the highest water retention, whereas those amended with the 50°C oven‐dried SAP remain moist the longest. The biodegradation rate of these materials depends on the application rate and nutrient availability. Carboxylated nanocellulose superabsorbents emerge as high‐performance biodegradable materials for agricultural use, able to replace the current non‐biodegradable petrochemical‐based superabsorbents.
Locust bean gum‐polyvinyl alcohol hydrogels: Synthesis, characterization, swelling behaviors, and mathematical models
Authors: Matar Ghassan H. , Andac Muberra , Elmas Aykut 
Published: August 2021

AbstractIn this study, locust bean gum/polyvinyl alcohol (LBG/PVA) hydrogels were synthesized by the gel casting method without using toxic crosslinking agents. Infrared spectroscopy (FTIR), X‐ray diffraction (XRD), and thermogravimetric analysis (TGA) methods were used for characterization of the synthesized hydrogels. Scanning electron microscopy (SEM) was used for observation surface morphology of the hydrogel and swelled hydrogels. The Swelling behavior of prepared hydrogels was investigated and the data were interpreted by various kinetic models. The prepared hydrogels showed pH and temperature‐responsive behavior. The maximum swelling ratio was evaluated as 607.72 at 37°C. The diffusional exponent values (n) were found as 0.5946, 0.5028, and 0.2785 at 4, 25, and 37°C, respectively. According to the n values, it was found that non‐Fickian diffusion dominates the swelling process. The obtained diffusion prediction curves were fitted to three different models: Higuchi, Peppas, and Elmas models. Among the results, Elmas model has better fits at 277 K and 298 K while Peppas model is better at 310 K. The results indicated that LBG/PVA hydrogels could be a candidate biomaterial for drug delivery applications.
Recent advances of environmental pollutants detection via paper‐based sensing strategy
Authors: Zou Xue , Ji Yayun , Li Hangzhou , Wang Zhaoli , Shi Linhong , Zhang Shengli , Wang Tengfei , Gong Zhengjun 
Published: August 2021

AbstractPaper has become one of the most promising substrates for building low‐cost and powerful sensing platforms due to its self‐pumping ability and compatibility with multiple patterning methods. Paper‐based sensors have been greatly developed in the field of environmental monitoring. In this review, we introduced the research and application of paper‐based sensors in environmental monitoring, focusing on the deposition and patterning methods of building paper‐based sensors, and summarized the applications of detecting environmental pollutants, including metal ions, anions, explosives, neurotoxins, volatile organic compounds, and small molecules. In addition, the development prospects and challenges of promoting paper‐based sensors are also discussed. The current review will provide references for the construction of portable paper‐based sensors, and has implications for the field of on‐site real‐time detection of the environment.
Increased modularity of the resting‐state network in children with nonsyndromic cleft lip and palate after speech rehabilitation
Authors: Cheng Hua , Rao Bo , Zhang Wenjing , Chen Renji , Peng Yun 
Published: August 2021

AbstractIntroductionSpeech therapy is the primary management followed the physical management through surgery for children with nonsyndromic cleft lip and palate (NSCLP). However, the topological pattern of the resting‐state network after rehabilitation remains poorly understood. We aimed to explore the functional topological pattern of children with NSCLP after speech rehabilitation compared with healthy controls.MethodsWe examined 28 children with NSCLP after speech rehabilitation (age = 10.0 ± 2.3 years) and 28 healthy controls for resting‐state functional MRI. We calculated functional connections and the degree strength, betweenness centrality, network clustering coefficient (Cp), characteristic path length (Lp), global network efficiency (Eg), local network efficiency (Eloc), modularity index (Q), module number, and participation coefficient for the between‐group differences using two‐sample t tests (corrected p < .05). Additionally, we performed a correlation analysis between the Chinese language clear degree scale (CLCDS) scores and topological properties in children with NSCLP.ResultsWe detected significant between‐group differences in the areas under the curve (AUCs) of degree strength and betweenness centrality in language‐related brain regions. There were no significant between‐group differences in module number, participation coefficient, Cp, Lp, Eg, or Eloc. However, the Q (density: 0.05–0.30) and QAUC (t = 2.46, p = .02) showed significant between‐group differences. Additionally, there was no significant correlation between topological properties of statistical between‐group differences and CLCDS scores.ConclusionsAlthough nodal metric differences existed in the language‐related brain regions, the children with NSCLP after speech rehabilitation had similar global network properties, module numbers, and participation coefficient, but increased modularity. Our results suggested that children with NSCLP achieved speech rehabilitation through function specialization in the language‐related brain regions. The resting‐state topology pattern could be of substantive neurobiological importance and potential imaging biomarkers for speech rehabilitation.
Vasopressors independently associated with mortality in acute myocardial infarction and cardiogenic shock
Authors: Basir Mir B. , Lemor Alejandro , Gorgis Sarah , Taylor Angela M. , Tehrani Behnam , Truesdell Alexander G. , Bharadwaj Aditya , Kolski Brian , Patel Kirit , Gelormini Joseph , Todd Josh , Lasorda David , Smith Craig , Riley Robert , Marso Steve , Federici Robert , Kapur Navin K. , O'Neill William W. ,   The National Cardiogenic Shock Initiative Investigators
Published: August 2021

AbstractBackgroundIncreasing vasopressor dose is associated with increasing mortality in patients presenting with acute myocardial infarction and cardiogenic shock (AMICS). It is unknown whether the use of vasopressors is independently harmful or if their use is secondary to decreasing intrinsic cardiac power output (CPO). Mechanical circulatory support (MCS) devices enhance CPO. We sought to evaluate the independent impact of increasing vasopressor dose on survival in the National Cardiogenic Shock Initiative (NCSI).MethodsThe NCSI is a single arm prospective trial evaluating outcomes associated with the use of MCS using Impella in patients with AMICS. Early initiation of MCS placement before percutaneous coronary intervention (PCI) and rapid de‐escalation of vasopressors guided by systematic use of invasive hemodynamic measures led to 70% in‐hospital survival for the first 300 patients enrolled from July 2016 to December 2019 in 57 U.S. sites.ResultsHemodynamic measures were obtained immediately after MCS and PCI. Survival curves were constructed based on CPO and use of vasopressors. For patients with CPO ≤0.6 W, survival was 77.3%, 45.0%, and 35.3% when 0, 1, or ≥ 2 vasopressors were used (p = 0.02). Similarly, for patients with CPO >0.6 W survival was 81.7%, 72.6%, and 56.8%, respectively (p = 0.01). Logistic regression analysis demonstrated that increasing vasopressor requirements were independently associated with increasing mortality (p = 0.02).ConclusionIncreasing vasopressor requirement is associated with increased mortality in AMICS independent of underlying CPO. Methods to decrease the need for vasopressors may enhance survival in AMICS.