bluuebunny/crossref_metadata_2025_split huggingface dataset:
Nanoengineering Palladium Plasmonic Nanosheets Inside Polymer Nanospheres for Photothermal Therapy and Targeted Drug Delivery
Authors: Uson Laura , Yus Cristina , Mendoza Gracia , Leroy Eric , Irusta Silvia , Alejo Teresa , García‐Domingo David , Larrea Ane , Arruebo Manuel , Arenal Raul , Sebastian Victor 
Published: November 2021

AbstractThe incorporation of plasmonic nanoconstructs in biodegradable polymeric nanoparticles (NPs), together with therapeutic drugs in a controlled procedure is of interest for different applications in Nanomedicine. Advanced hybrid nanomaterials can be engineered by combining the in situ formation of plasmonic palladium nanosheets (NSs) and the proper ionic nature of the encapsulated drug. This study presents a new procedure to synthesize hybrid nanostructures by a Pickering double emulsion. Anisotropic palladium (Pd) NSs with unique near‐infrared (NIR)‐optical properties can be assembled within a poly lactic‐co‐glycolic acid matrix of < 200 nm NPs, when Pd precursors are in situ reduced via a gas‐phase procedure. The hybrid nanomaterials respond to external NIR light stimulus. The unprecedented precision to assemble, in a single stage, plasmonic nanoconstructs having a total loading selectivity, when encapsulated in combination with hydrophobic drugs, offers new opportunities in the new class of theragnostics, in particular when triggered drug delivery and photothermal therapies are required.
Stretchable MoS2 Artificial Photoreceptors for E‐Skin
Authors: Zhang Weifeng , Liu Yulong , Pei Xue , Yuan Zhihong , Zhang Yan , Zhao Zihan , Hao He , Long Run , Liu Nan 
Published: November 2021

Abstract2D materials have been widely applied in flexible electronics but only with limited stretchability, because the metal‐halide bonding is so strong that the materials’ electronic properties will be severely influenced upon tensile strain. Here, a strategy is proposed for the fabrication of ultrastretchable MoS2 photoreceptors based on chemical vapor deposition‐grown or manually stacked multilayer MoS2. Strain‐dependent spectroscopic comparisons of multilayer versus monolayer MoS2 indicate that the strain transfer is suppressed from bottom to top layers owing to interlayer sliding, which is consistent with the density functional theory and molecular dynamics simulations. Thus, the optoelectronic properties of multilayer MoS2 can withstand larger mechanical strain than monolayer MoS2. Leveraging this mechanical feature, ten‐layer MoS2 photodetector is fabricated on polystyrene‐b‐poly (ethylene‐co‐butylene)‐b‐polystyrene elastomer, withstanding ≈50% tensile strain and presenting 32 times higher photoresponsivity than that of monolayer MoS2 under the same stretching condition. Based on large‐area bilayer MoS2 film, 5 × 5 stretchable photodetector array is demonstrated and is capable of working as artificial photoreceptors to control a robotic hand under 16% tensile strain, showing great potential in applications for 2D material‐based electronic skin.
Spatiotemporally Controlled Access to Photoluminescence Dark State of 2D Monolayer Semiconductor by FRAP Microscopy
Authors: Su Hua , Nie Yufeng , Sun Qianlu , Yin Linliang , Li Jian , Xia Xing‐Hua , Xu Weigao , Wang Wei 
Published: November 2021

AbstractTailoring the photoluminescence (PL) of semiconductors through spatiotemporal manipulation of dynamics of photoexcited carriers is of paramount importance for understanding the emitting mechanism and developing high‐performance devices. Herein, fluorescence recovery after photobleaching (FRAP) microscopy, a powerful tool in biology, is first utilized to simultaneously manipulate and monitor the dynamics of photoexcited carrier in attractive 2D transition metal dichalcogenide monolayers (1L‐TMDs). This allows on‐demand access to the PL dark state of 1L‐TMDs, based on the triggered exciton–exciton annihilation by pump beam‐initiated photodoping. Using a 0.7‐µm‐diametered pump laser, the PL dark region can be facilely tailored from ≈0.5 to ≈5 µm over a 10‐µm‐1L‐WS2 flake. An interesting photoinduced dedoping effect in 1L‐TMDs after photodoping is discovered by FRAP, which has not been observed before and might account for the non‐blinking emission of 1L‐TMDs. The revealed mono‐exponential photo‐dedoping can also be kinetically tailored by ≈170‐fold (k: 0.11–19.00 s‐1) by humidity, power of incident laser and type of 1L‐TMDs. This study demonstrates the power of FRAP microscopy in exploring the effect of photoexcited carrier dynamics on the PL property of semiconductors, holding promises for understanding light‐emitting mechanism and optimizing operational parameters for optoelectronic devices.
Covalent Organic Framework Membrane with Turing Structures for Deacidification of Highly Acidic Solutions
Authors: Zhou Lihong , Li Xiaofeng , Cao Kecheng , Jia Zhimin , Long Honghan , Li Yang , Tao Guohong , Liu Ning , Zhang Jie , Ma Lijian 
Published: November 2021

AbstractThe deacidification of highly acidic industrial wastewater, such as the spent fuel reprocessing feed liquid, is of great significance for the smooth progress of the subsequent treatment processes. Herein, a novel covalent organic framework (COF) membrane with bidirectional anisotropic Turing structures is synthesized for the first time and used for deacidification. The COF membrane presents linear and hydrophobic properties on one side and porous and superhydrophilic properties on the other side, which makes the water permeability of hydrophilic side 45 times higher than that of the hydrophobic side and effectively prevents the reverse osmosis of water. Impressively, the COF membrane has excellent thermal, acid, and irradiation stabilities, and an extraordinarily high ability to intercept metal ions in a complex multi‐ion solution containing 5 m HNO3, with the interception rate up to 100%. However, H+ can easily pass through the membrane with the permeation flux of 1015.7 mol L−1 m−2, which realizes the efficient deacidification of high acidic solutions. This study provides not only a new idea for the design and preparation of Turing‐structural membranes, but also a feasible strategy for the deacidification and process simplification of spent fuel reprocessing feed liquid and other industrial wastewater with high acidity.
A New End Group on Nonfullerene Acceptors Endows Efficient Organic Solar Cells with Low Energy Losses
Authors: Pan Youwen , Zheng Xiangjun , Guo Jing , Chen Zeng , Li Shuixing , He Chengliang , Ye Shounuan , Xia Xinxin , Wang Shanlu , Lu Xinhui , Zhu Haiming , Min Jie , Zuo Lijian , Shi Minmin , Chen Hongzheng 
Published: November 2021

AbstractLarge energy loss is one of the main limiting factors for power conversion efficiencies (PCEs) of organic solar cells (OSCs). To this effect, the chemical modifications of the famous Y‐series nonfullerene acceptor (NFA) BTP‐4Cl‐BO with a new end group, TPC‐Cl, whose π‐conjugation is extended through the fusing of 3‐(dicyanomethylene)indanone (IC) group with a chlorinated thiophene ring, to synthesize two novel NFAs, BTP‐T‐2Cl and BTP‐T‐3Cl are performed. For BTP‐T‐2Cl with two TPC‐Cl groups, the resulting OSC exhibits a modest PCE of 14.89% but an extraordinary low energy loss of 0.49 eV, because its superior electroluminescence quantum efficiency of 0.0606% mitigates significantly the nonradiative loss (0.191 eV). For BTP‐T‐3Cl with one TPC‐Cl group, the corresponding device shows a higher PCE of 17.61% accompanied by a slightly bigger energy loss of 0.51 eV, which can be ascribed to the optimized morphology and/or efficient charge generation. Furthermore, the ternary OSC adopting two NFAs of BTP‐T‐3Cl and BTP‐4Cl‐BO achieves an impressive PCE of 18.21% (certified value of 17.9%), which is among the highest values for OSCs to date. The above results demonstrate that expanding end groups of NFAs with electron‐donating rings is an effective strategy to realize lower energy losses for OSCs.
Surface Electronic Structure Modulation of Cobalt Nitride Nanowire Arrays via Selenium Deposition for Efficient Hydrogen Evolution
Authors: Sun Yiqiang , Mao Keke , Shen Qi , Zhao Lei , Shi Chuanxin , Li Xiuling , Gao Yanan , Li Cuncheng , Xu Kun , Xie Yi 
Published: November 2021

AbstractNonmetal heteroatom incorporation into the lattice of host materials is a common way to regulate the surface electronic structure of electrocatalysts to boost their electrocatalytic performance. However, the heteroatom incorporation will inevitably trigger lattice strain and vacancy, which may lead to large changes in the structure of host materials. In this situation, the reconstruction of doped catalysts easily occurs during the catalytic process under harsh alkaline media, which hinders understanding the structure–activity correlation between catalysts and catalytic performance. Herein, taking cobalt nitride as an example, it is promulgated that a low‐temperature selenium sublimation strategy can effectively optimize the surface electronic structure in Co4N nanowire arrays with no significant change of bulk phase structure. Benefiting from surface selenium modification, the optimized SeCo4N nanowire arrays exhibit a 6.5 times enhancement of catalytic activity with structural phase stability for hydrogen evolution reaction in basic media. These findings may provide a new concept to design stable structured catalysts for energy‐related applications.
Machine Learning‐Evolutionary Algorithm Enabled Design for 4D‐Printed Active Composite Structures
Authors: Sun Xiaohao , Yue Liang , Yu Luxia , Shao Han , Peng Xirui , Zhou Kun , Demoly Frédéric , Zhao Ruike , Qi H. Jerry 
Published: November 2021

AbstractActive composites consisting of materials that respond differently to environmental stimuli can transform their shapes. Integrating active composites and 4D printing allows the printed structure to have a pre‐designed complex material or property distribution on numerous small voxels, offering enormous design flexibility. However, this tremendous design space also poses a challenge in efficiently finding appropriate designs to achieve a target shape change. Here, a novel machine learning (ML) and evolutionary algorithm (EA) based approach is presented to guide the design process. Inspired by the beam deformation characteristics, a recurrent neural network (RNN) based ML model whose training dataset is acquired by finite element simulations is developed for the forward shape‐change prediction. EA empowered with ML is then used to solve the inverse problem of finding the optimal design. For multiple target shapes with different complexities, the ML‐EA approach demonstrates high efficiency. Combining the ML‐EA with computer vision algorithms, a new paradigm is presented that streamlines design and 4D printing process where active straight beams can be designed based on hand‐drawn lines and be 4D printed that transform into the drawn profiles under the stimulus. The approach thus provides a highly efficient tool for the design of 4D‐printed active composites.
3D Printed Scaffolds Incorporated with Platelet‐Rich Plasma Show Enhanced Angiogenic Potential while not Inducing Fibrosis
Authors: Ibanez Rita I. R. , do Amaral Ronaldo J. F. C. , Simpson Christopher R. , Casey Sarah M. , Reis Rui L. , Marques Alexandra P. , Murphy Ciara M. , O'Brien Fergal J. 
Published: November 2021

AbstractSuccessful therapeutic strategies for wound healing rely on proper vascularization while inhibiting fibrosis. However, scaffolds designed for skin tissue engineering generally lack the biochemical cues that can enhance their vascularization without inducing fibrosis. Therefore, the objective of this work is to incorporate platelet‐rich plasma (PRP), a natural source of angiogenic growth factors, into a gelatin methacrylate (GelMA) hydrogel, yielding a bioink that can subsequently be used to 3D print a novel regenerative scaffold with defined architecture for skin wound healing. A PRP‐activated bioink is successfully 3D printed, and the resulting scaffolds present similar structural, rheological, and mechanical properties compared to GelMA‐only scaffolds. Furthermore, 3D printed PRP‐activated scaffolds facilitate controlled release of PRP‐derived growth factors for up to 14 days, presenting superior angiogenic potential in vitro (e.g., tubulogenesis assay) and in vivo (chick chorioallantoic membrane) compared to GelMA‐only scaffolds, while not inducing a myofibroblastic phenotype in fibroblasts (e.g., α‐smooth muscle actin expression). This disruptive technology offers the opportunity for a patient's autologous growth factors to be incorporated into a tailored 3D‐printed scaffold in theatre prior to implantation, as part of a single‐stage procedure, and has potential in other tissue engineering applications in which enhanced vascularization with limited fibrosis is desired.
High‐Speed Ionic Synaptic Memory Based on 2D Titanium Carbide MXene
Authors: Melianas Armantas , Kang Min‐A , VahidMohammadi Armin , Quill Tyler James , Tian Weiqian , Gogotsi Yury , Salleo Alberto , Hamedi Mahiar Max 
Published: November 2021

AbstractSynaptic devices with linear high‐speed switching can accelerate learning in artificial neural networks (ANNs) embodied in hardware. Conventional resistive memories however suffer from high write noise and asymmetric conductance tuning, preventing parallel programming of ANN arrays. Electrochemical random‐access memories (ECRAMs), where resistive switching occurs by ion insertion into a redox‐active channel, aim to address these challenges due to their linear switching and low noise. ECRAMs using 2D materials and metal oxides however suffer from slow ion kinetics, whereas organic ECRAMs enable high‐speed operation but face challenges toward on‐chip integration due to poor temperature stability of polymers. Here, ECRAMs using 2D titanium carbide (Ti3C2Tx) MXene that combine the high speed of organics and the integration compatibility of inorganic materials in a single high‐performance device are demonstrated. These ECRAMs combine the speed, linearity, write noise, switching energy, and endurance metrics essential for parallel acceleration of ANNs, and importantly, they are stable after heat treatment needed for back‐end‐of‐line integration with Si electronics. The high speed and performance of these ECRAMs introduces MXenes, a large family of 2D carbides and nitrides with more than 30 stoichiometric compositions synthesized to date, as promising candidates for devices operating at the nexus of electrochemistry and electronics.
An Ultrahigh‐Power Mesocarbon Microbeads|Na+‐Diglyme|Na3V2(PO4)3 Sodium‐Ion Battery
Authors: Wei Qiulong , Chang Xiaoqing , Wang Jian , Huang Tingyi , Huang Xiaojuan , Yu Jiayu , Zheng Hongfei , Chen Jin‐hui , Peng Dong‐Liang 
Published: November 2021

AbstractSodium‐ion batteries (SIBs) show practical applications in large‐scale energy storage systems. But, their power density is limited by the sluggish Na+ diffusion into the cathode and anode materials. Herein, the authors demonstrate a prototype of ultrahigh power SIB, consisting of the high‐rate Na3V2(PO4)3 (NVP) cathode, graphite‐type mesocarbon microbeads (MCMB) anode, and Na+‐diglyme electrolyte. It is found that the overpotential of the NVP cathode obeys the Ohmic rule. Thus, the as‐synthesized NVP@C@carbon nanotubes (CNTs) cathode with the high conductive CNTs networks displays high electronic conductivity, reducing the overpotential and charge transfer resistances and leading to the remarkable rate capability over 1000C. For the MCMB anode, the initial [Na‐diglyme]+ co‐intercalation step is pseudocapacitive dominated, and then the expanded graphite's layers ensure the subsequent fast ions diffusion. The rapid (de)intercalation kinetics in between the cathode and anode are well‐matched. Thus, the assembled MCMB|1 m NaPF6 in diglyme|NVP@C@CNTs full‐cell SIB delivers the energy density of 88 Wh kg−1 at the high power density of ≈10 kW kg−1. Even at the ultrahigh power density of 23 kW kg−1, an energy density of 58 Wh kg−1 is obtained. The encouraging results of the full cell will promote the development of high‐power SIB for large‐scale applications in the future.
Mechanical Behavior and Dendrite Resistance of closo‐Hydroborate Solid Electrolyte
Authors: Brighi Matteo , Murgia Fabrizio , Černý Radovan 
Published: November 2021

AbstractStack pressure and mechanical robustness are two important parameters needed to tackle the interfacial instability of solid‐state batteries. Here, the mechanical behavior of Na4(CB11H12)2(B12H12), as solid electrolyte at the interface with Na anode, is reported. The solid electrolyte is tested as function of stack pressure and different current densities, revealing a critical current density of 0.6 mA cm−2 at room temperature and an optimal stack pressure of 1.5 MPa. These findings are achieved, thanks to the adoption of a multilayer approach, demonstrating the powerfulness of hydroborates to compensate chemical and electrochemical instability, simply employing different complex hydride polyanions that change locally the electrochemical properties while preserving structural and chemical coherence.
Lightweight Cellulose Nanofibril/Reduced Graphene Oxide Aerogels with Unidirectional Pores for Efficient Electromagnetic Interference Shielding
Authors: Li Mengmeng , Han Fuyi , Jiang Shuai , Zhang Meiling , Xu Qiuyu , Zhu Jianhua , Ge Aixiong , Liu Lifang 
Published: November 2021

AbstractLightweight and compressible aerogels have been widely considered as promising materials for electromagnetic interference (EMI) shielding. Herein, a lightweight cellulose nanofibril/reduced graphene oxide carbon aerogel fabricated by unidirectional freeze‐drying and pyrolysis processes is reported. The results show that the aerogels with unidirectionally aligned pores possess better compression resilience and EMI shielding performance in the radial direction. The unidirectional aerogel with low density (≈0.0058 g cm−3) exhibits a high EMI shielding effectiveness (SE) of ≈33 dB at 8.2–12.4 GHz and a specific EMI SE of 5759 dB cm3 g−1. Therefore, the fabricated aerogel demonstrates a promising potential in the field of next‐generation EMI shielding materials.
In Situ Construction of Oriented Pt‐PANI Needle‐Like Nanoarrays‐Based Label‐Free Aptasensor for Ultrafast and Ultrasensitive Recognition of Cardiac Troponin I
Authors: Zhang Wei , Liu Tao , Shan Yuansheng , Hou Bailing , Chu Zhenyu , Gu Xiaoping , Ma Zhengliang , Jin Wanqin 
Published: November 2021

AbstractDue to the short course and high mortality of acute myocardial infarction (AMI) which will cause irreversible myocardial necrosis to induce cardiac arrest, its early diagnosis within minutes is always a challenge in clinical emergency. In this work, an ultrafast and ultrasensitive aptasensor is designed to achieve quantitatively detection of cardiac troponin I (cTnI) which is proved as a highly specific and sensitive biomarker to AMI, and within only 4 min, the cTnI concentration can be accurately reported. This aptasensor is constructed via an in situ growth of the oriented Pt‐polyaniline (PANI) needle‐like nanoarrays providing both high electrocatalysis and abundant active sites as the signal magnifier and DNA carrier. A target‐induced strand release strategy is proposed to remarkably accelerate the recognition process of cTnI through the specific design of DNA stand for binding. The as‐prepared aptasensor can exhibit an ultrawide linear detection range of cTnI from 1 pg mL−1 to 100 ng mL−1 satisfying the clinical demand for AMI diagnosis, together with excellent selectivity among various biomarkers. Based on its fast recognition ability, this aptasensor presents a high accuracy in the practical detection of human serum to prove its promising ability in the early and on‐site diagnosis of AMI.
Enhanced GeSn Microdisk Lasers Directly Released on Si
Authors: Kim Youngmin , Assali Simone , Burt Daniel , Jung Yongduck , Joo Hyo‐Jun , Chen Melvina , Ikonic Zoran , Moutanabbir Oussama , Nam Donguk 
Published: November 2021

AbstractGeSn alloys are promising candidates for complementary metal‐oxide‐semiconductor‐compatible, tunable lasers. Relaxation of residual compressive strain in epitaxial GeSn has recently shown promise in improving the lasing performance. However, the suspended device configuration that is thus far introduced to relax the strain is destined to limit heat dissipation, thus hindering the device performance. Herein is demonstrated that strain‐free GeSn microdisk laser devices fully released on Si outperform the canonical suspended devices. This approach allows to simultaneously relax the limiting compressive strain while offering excellent thermal conduction. Optical simulations confirm that, despite a relatively small refractive index contrast between GeSn and Si, optical confinement in strain‐free GeSn optical cavities on Si is superior to that in conventional strain‐free GeSn cavities suspended in the air. Moreover, thermal simulations indicate a negligible temperature increase in the device. Conversely, the temperature in the suspended devices increases substantially reaching, for instance, 120 K at a base temperature of 75 K under the employed optical pumping conditions. Such improvements enable increasing the operation temperature by ≈40 K and reducing the lasing threshold by 30%. This approach lays the groundwork to implement new designs in the quest for room temperature GeSn lasers on Si.
Metal–Organic Framework Based Thermally Activated Delayed Fluorescence Emitter with Oxygen‐Insensitivity for Cell Imaging
Authors: Bie Binglin , Guo Linshuo , Zhang Mengxun , Ma Yanhang , Yang Chuluo 
Published: November 2021

AbstractTo achieve better resolution and contrast in fluorescence techniques, time‐resolved fluorophores are promising constituents for probes in imaging and sensing, allowing for the elimination of background signals from scattering and short‐lived autofluorescence. Here a metal–organic framework (MOF) named Spiro‐MOF‐1 is designed with high thermally activated delayed fluorescence (TADF) persistence using a strategy of high rigidity to achieve a lifetime more than two times longer than that of pure linker. The rigid structure originated from spiro‐bi‐acridine unit is unambiguously revealed through 3D electron diffraction tomography (3D‐EDT). Furthermore, nanocrystals of Spiro‐MOF‐1 are successfully developed and modified with polyethylene glycol (PEG) as a biocompatible, time‐resolved fluorescent fluorophore with high TADF persistence, which exhibits a lifetime around 1 μs with no obvious decay under various bio‐mimicking environments, which has not been achieved by any other MOF‐based TADF emitter and small organic molecules. In further cell experiments, PEG‐modified nanocrystals exhibit a fluorescent signal that is more than 30 times longer than that of autofluorescence background in BGC823 cell line.
Catalytic Ability Comparison of Five Transition Metal Clusters (Zn, Cu, Fe, Ni, and Ru) for Heat‐Induced Graphene Etching by Ab Initio Molecular Dynamics Simulations
Authors: Bie Jie , Wang Jinlan , Chen Shuang , Fa Wei 
Published: November 2021

AbstractGraphene can be widely utilized as a substrate to support various transition metal (TM) nanoclusters or nanoparticles for surfaced‐supported catalysis, such as electrocatalysis or photovoltaics. The subtle interactions between TM and graphene carbon atoms are expected to be crucial in TM–graphene nanocomposites to affect their growth morphologies and final functionalities. Here, the morphology evolution and catalytic ability of five ultrafine TM (Zn, Cu, Fe, Ni, and Ru) clusters with 48 atoms on graphene etching are investigated by using ab initio molecular dynamics (AIMD) simulations. It is found that three factors, i.e., TM cluster type, operation temperature, and graphene edge type, play important roles in the catalytic behaviors of TM clusters for heat‐induced graphene etching. The results are helpful in locating the catalytic performance of TM clusters in graphene cutting and ensuring stability of TM–graphene nanocomposites in device applications.