bluuebunny/crossref_metadata_2025_split huggingface dataset:
2D, Metal‐Free Electrocatalysts for the Nitrogen Reduction Reaction
Authors: Liu Chuangwei , Tian Ang , Li Qinye , Wang Tianyi , Qin Gaowu , Li Song , Sun Chenghua 
Published: December 2022

AbstractEnvironmentally friendly ammonia production is important for addressing the carbon emissions and substantial energy consumption that are currently associated with the chemical industry. In recent decades, many achievements are made in this area; however, low production yield, poor selectivity, and unsatisfactory Faradaic efficiency hinder large‐scale applications. 2D, metal‐free electrocatalysts stand out from other candidates because of their physical, electronic, and chemical properties. In this study, recent developments of 2D‐based electrochemical materials for converting dinitrogen into ammonia in ambient conditions are systematically reviewed. First, recent unique progress and challenges on novel 2D electrocatalysts for the nitrogen reduction reaction are summarized. Then, various synthetic strategies for electrochemical materials and the influence of these methods have on the intrinsic material performance are highlighted. Last, by comparing current engineering strategies, electrochemical tests, and computational calculations, the opportunities, critical issues, and scientific challenges for 2D nanomaterials as stable, efficient catalysts, are analyzed. On the basis of this comparison, technology solutions are provided and rational principles for future studies are proposed.
Recent Developments of Optoelectronic Synaptic Devices Based on Metal Halide Perovskites
Authors: Hao Dandan , Yang Zhenyu , Huang Jia , Shan Fukai 
Published: December 2022

AbstractMassive data processing with high computing efficiency and low operating power is required owing to the rapid development of artificial intelligence and information technology. However, the von Neumann structure computing system with the separated memory and processor can cause large energy consumption and a low running speed during massive data processing. Therefore, the brain‐inspired neuromorphic computing system is developed, that can provide hardware support for emulating biological synaptic functions and realizing highly intensive data processing with low power consumption. As a neuromorphic device, the optoelectronic synaptic device (OSD) is regarded as an ideal device to replace the von Neumann‐based computer because of its ultrafast signal transmission, large bandwidth, low energy consumption, and wireless communication. Owing to their unique optoelectronic property, metal halide perovskites (MHPs) have received growing attention as effective photosensitive materials in OSDs. Therefore, the review introduces the recent progress on OSDs based on MHPs (MHPs‐OSDs) including the structures and properties of MHPs, and the architectures and performance characteristics of MHPs‐OSDs. Furthermore, applications of MHPs‐OSDs are presented. Finally, the outlook and opportunity of MHPs‐OSDs are discussed.
Interface Engineering of Biomass‐Derived Carbon used as Ultrahigh‐Energy‐Density and Practical Mass‐Loading Supercapacitor Electrodes
Authors: Chen Ruwei , Tang Hao , He Peng , Zhang Wei , Dai Yuhang , Zong Wei , Guo Fei , He Guanjie , Wang Xiaohui 
Published: December 2022

AbstractThe development of flexible electrodes with high mass loading and efficient electron/ion transport is of great significance but still remains the challenge of innovating suitable electrode structures for high energy density application. Herein, for the first time, lignosulfonate‐derived N/S‐co‐doped graphene‐like carbon is in situ formed within an interface engineered cellulose textile through a sacrificial template method. Both experimental and theoretical calculations disclose that the formed pomegranate‐like structure with continuous conductive pathways and porous characteristics allows sufficient ion/electron transport throughout the entire structures. As a result, the obtained flexible electrode delivers a remarkable integrated capacitance of 6534 mF cm−2 (335.1 F g−1) and a superior stability at an industrially applicable mass loading of 19.5 mg cm−2. A pseudocapacitive cathode with ultrahigh capacitance of 7000 mF cm−2 can also be obtained based on the same electrode structure engineering. The as‐assembled asymmetric supercapacitor achieves a high areal capacitance of 3625 mF cm−2, and a maximum energy density of 1.06 mWh cm−2, outperforms most of other reported high‐loading supercapacitors. This synthesis method and structural engineering strategy can provide materials design concepts and a wide range of applications in the fields of energy storage beyond supercapacitors.
Exploring the Potential of PEG‐Heparin Hydrogels to Support Long‐Term Ex Vivo Culture of Patient‐Derived Breast Explant Tissues
Authors: Koch Maria K. , Ravichandran Akhilandeshwari , Murekatete Berline , Clegg Julien , Joseph Mary Teresa , Hampson Madison , Jenkinson Mitchell , Bauer Hannah S. , Snell Cameron , Liu Cheng , Gough Madeline , Thompson Erik W. , Werner Carsten , Hutmacher Dietmar W. , Haupt Larisa M. , Bray Laura J. 
Published: December 2022

AbstractBreast cancer is a complex, highly heterogenous, and dynamic disease and the leading cause of cancer‐related death in women worldwide. Evaluation of the heterogeneity of breast cancer and its various subtypes is crucial to identify novel treatment strategies that can overcome the limitations of currently available options. Explant cultures of human mammary tissue have been known to provide important insights for the study of breast cancer structure and phenotype as they include the context of the surrounding microenvironment, allowing for the comprehensive exploration of patient heterogeneity. However, the major limitation of currently available techniques remains the short‐term viability of the tissue owing to loss of structural integrity. Here, an ex vivo culture model using star‐shaped poly(ethylene glycol) and maleimide‐functionalized heparin (PEG‐HM) hydrogels to provide structural support to the explant cultures is presented. The mechanical support allows the culture of the human mammary tissue for up to 3 weeks and prevent disintegration of the cellular structures including the epithelium and surrounding stromal tissue. Further, maintenance of epithelial phenotype and hormonal receptors is observed for up to 2 weeks of culture which makes them relevant for testing therapeutic interventions. Through this study, the importance of donor‐to‐donor variability and intra‐patient tissue heterogeneity is reiterated.
Toward 3D Bioprinting of Osseous Tissue of Predefined Shape Using Single‐Matrix Cell‐Bioink Constructs
Authors: Gu Yawei , Pigeot Sebastien , Ahrens Lucas , Tribukait‐Riemenschneider Fabian , Sarem Melika , Wolf Francine , García‐García Andres , Barbero Andrea , Martin Ivan , Shastri V. Prasad 
Published: December 2022

AbstractEngineering living bone tissue of defined shape on‐demand has remained a challenge. 3D bioprinting (3DBP), a biofabrication process capable of yielding cell constructs of defined shape, when combined with developmental engineering can provide a possible path forward. Through the development of a bioink possessing appropriate rheological properties to carry a high cell load and concurrently yield physically stable structures, printing of stable, cell‐laden, single‐matrix constructs of anatomical shapes is realized without the need for fugitive or support phases. Using this bioink system, constructs of hypertrophic cartilage of predesigned geometry are engineered in vitro by printing human mesenchymal stromal cells at a high density to drive spontaneous condensation and implanted in nude mice to evoke endochondral ossification. The implanted constructs retain their prescribed shape over a 12‐week period and undergo remodeling to yield ossicles of the designed shape with neovascularization. Microcomputed tomography, histological, and immunohistochemistry assessments confirm bone tissue characteristics and the presence of human cells. These results demonstrate the potential of 3DBP to fabricate complex bone tissue for clinical application.
Control of Molecular Orbital Ordering Using a van der Waals Monolayer Ferroelectric
Authors: Amini Mohammad , Silveira Orlando J. , Vaňo Viliam , Lado Jose L. , Foster Adam S. , Liljeroth Peter , Kezilebieke Shawulienu 
Published: December 2022

Abstract2D ferroelectric materials provide a promising platform for the electrical control of quantum states. In particular, due to their 2D nature, they are suitable for influencing the quantum states of deposited molecules via the proximity effect. Here, electrically controllable molecular states in phthalocyanine molecules adsorbed on monolayer ferroelectric material SnTe are reported. The strain and ferroelectric order in SnTe are found to create a transition between two distinct orbital orders in the adsorbed phthalocyanine molecules. By controlling the polarization of the ferroelectric domain using scanning tunneling microscopy (STM), it is successfully demonstrated that orbital order can be manipulated electrically. The results show how ferroelastic coupling in 2D systems allows for control of molecular states, providing a starting point for ferroelectrically switchable molecular orbital ordering and ultimately, electrical control of molecular magnetism.
Cooperative Electronic Structure Modulator of Fe Single‐Atom Electrocatalyst for High Energy and Long Cycle Li–S Pouch Cell
Authors: Lim Won‐Gwang , Park Cheol‐Young , Jung Hyeonjung , Kim Seoa , Kang Seok Hun , Lee Young‐Gi , Jeong Yo Chan , Yang Seung Bo , Sohn Kwonnam , Han Jeong Woo , Lee Jinwoo 
Published: December 2022

AbstractHigh‐energy and long cycle lithium–sulfur (Li–S) pouch cells are limited by the insufficient capacities and stabilities of their cathodes under practical electrolyte/sulfur (E/S), electrolyte/capacity (E/C), and negative/positive (N/P) ratios. Herein, an advanced cathode comprising highly active Fe single‐atom catalysts (SACs) is reported to form 320.2 W h kg−1 multistacked Li–S pouch cells with total capacity of ≈1 A h level, satisfying low E/S (3.0), E/C (2.8), and N/P (2.3) ratios and high sulfur loadings (8.4 mg cm−2). The high‐activity Fe SAC is designed by manipulating its local environments using electron‐exchangeable binding (EEB) sites. Introducing EEB sites comprising two different types of S species, namely, thiophene‐like‐S (–S) and oxidized‐S (–SO2), adjacent to Fe SACs promotes the kinetics of the Li2S redox reaction by providing additional binding sites and modulating the Fe d‐orbital levels via electron exchange with Fe. The –S donates the electrons to the Fe SACs, whereas –SO2 withdraws electrons from the Fe SACs. Thus, the Fe d‐orbital energy level can be modulated by the different –SO2/–S ratios of the EEB site, controlling the electron donating/withdrawing characteristics. This desirable electrocatalysis is maximized by the intimate contact of the Fe SACs with the S species, which are confined together in porous carbon.
On‐Surface Synthesis of Chiral Graphene Nanoribbon Segments via the Quarter‐Anthryl on Au(111) Surface
Authors: Zhang Hui , Lu Jianchen , Li Baijin , Zhao Xin‐Jing , Zhou Hangjing , Niu Gefei , Xiong Wei , Zhang Yong , Fu Boyu , Gao Lei , Tan Yuan‐Zhi , Cai Jinming 
Published: December 2022

AbstractQuarteranthene is predicted to manifest nontrivial edge states as the competition from the hybridization of localized frontier states and the Coulomb repulsion between valence electrons, which hosts much research potential in memory, spintronic devices fabrication, and quantum computation. The fabrication of ribbon‐like structures with up‐mentioned edge states, such as chiral graphene nanoribbon, possesses a high significance in the topological phase transition investigation. However, the synthesis of chiral graphene nanoribbon is limited in reactive substrate or with the edge‐brominated precursor. Here, the fabrication of quarteranthene and its chiral graphene nanoribbon segment on Au(111) substrate is reported. A combined bond‐resolved scanning tunneling microscopy, noncontact atomic force microscopy characterization, and corresponding density functional theory calculations confirm the chemical structure of fabricated products on the Au(111) substrate. The detailed analysis of the laterally extended products reveals that the lateral‐extended structures are acquired via the linkage of the hydrocarbon quarter‐anthryl. In addition, several strategies are used to modulate the yield of quarteranthene and its lateral‐extended products. These findings provide a new insight into the lateral extension strategy on metal substrates and provide another possible fabrication strategy of chiral graphene nanoribbons on the relative inert Au(111) substrate.
Plasma Activation and its Nanoconfinement Effects Boost Surface Anti‐Biofouling Performance
Authors: Mahmoodi Nasim , Bazzoli Dario G. , Overton Tim W. , Mendes Paula M. 
Published: December 2022

AbstractAlthough plasma treatment can alter polymer surface wettability and adhesiveness, scant attention has been given to plasma effects across scales and their anti‐fouling performance. Herein, the discovery that plasma‐activated polydimethylsiloxane (PDMS) nanopillar arrays remarkably enhance anti‐fouling behavior, yielding a 98.7% reduction in Escherichia coli adhesion compared to native planar surfaces. The plasma‐activated nanopillar arrays can hold to their anti‐fouling properties for extended periods of storage, still exhibiting more than 65.1% less bacterial colonization than their native planar counterparts after 50 days. The anti‐fouling behavior promoted by plasma activation is significantly enhanced as the structure features reduce in size from macroscale to microscale to nanoscale, revealing an altered plasma activation effect upon confinement at the nanoscale level. It is anticipated that the findings will improve the ability to achieve non‐fouling effects in polymeric materials for a broad range of applications in clinical and industrial settings.
Real‐Space Observation of Potential Reconstruction at Metallic/Insulating Oxide Interface
Authors: Jia Qingxuan , Gloter Alexandre 
Published: December 2022

AbstractElectric field reconstruction at interfaces plays a crucial role in device performances controlling, for example, Schottky potential barrier and interfacial Rashba effect. Here, scanning transmission electron microscopy (STEM) and ab‐initio calculation are used to estimate the atomic‐scale and large‐scale potential reconstruction at the interface between a metallic oxide SrRuO3 (SRO) thin film and an insulating DyScO3 (DSO) substrate. The intensity and the symmetry of the large‐scale electrostatic reconstruction at the interface is probed by 4D‐STEM discussing the center‐of‐mass shift for different angular ranges detection. Numerical simulations indicate that thermal diffuse scattered (TDS) electrons can be sensitive to large‐scale electric field and experiments based on these diffused electrons near the interface confirm that the electric field extends more in the insulating DyScO3 (DSO) side. The magnitude of the electrostatic drop at the interface estimated by the 4D‐STEM experiment is in accordance with the ab‐initio values for a p‐type reconstruction of the interface plane. Furthermore, an atomically resolved TDS potential asymmetry is observed in real‐space at the SRO/DSO interface by 4D‐STEM. This asymmetry is associated with the formation of a local ferroelectric type dipole at the interfacial unit‐cell revealing unambiguously the balance evolution between antiferrodistortive and ferroelectric instabilities at the interface between a metallic SRO and an insulating DSO.
High‐Efficiency Reclamation of Oscillating Energy During Multiple Droplets Impact on Bionic Lotus Surface
Authors: Li Jingbo , Zhu Zewei , Luo Yimin , Li Xia , Tan Sheng , Luo Zhuangzhu 
Published: December 2022

AbstractDroplet bouncing on special wettability surface is common and important in daily life and engineering applications (anti‐icing and drag reduction, etc.). However, there are few studies on the multiple droplets impact and there is a lack of systematic research on the interaction of oscillation and bounce. Here, the impact and oscillation of multiple droplets on the porous superhydrophobic bionic lotus surface are studied by a high‐speed camera system. On the bionic lotus surface (Surf‐1), an impacting droplet can merge another larger sessile droplet and bounce off. Comparing with single droplet impact, it is suggested that multiple droplets impact make more efficient use of the air cushion on the micrometer‐nanometer‐scale binary structure (MNBS) and show the self‐cleaning performance of Surf‐1 better. Moreover, with the theory for damped harmonic oscillators, it is found that Surf‐1 can prolong the oscillation of droplets (last >250 ms) and slow down the attenuation of energy. The energy can be efficiently recycled to the bounce by shortening the droplet impact interval (ti). The fundamental understanding of multiple droplets impact and the reclamation of oscillating energy are beneficial for scientific design of new surface and engineering applications.
An Efficient Perovskite‐Like Phosphor with Peak Emission Wavelength at 850 nm for High‐Performance NIR LEDs
Authors: Tang Wenqiang , Wu Dan , Xiao Yu , Dong Xiaoling , Wang Yue , Zhou Wenping , Liu Yifan , Zhang Liangliang 
Published: December 2022

AbstractNear‐infrared (NIR) phosphor‐converted light‐emitting diodes (pc‐LEDs) are an emerging light source demanded for the miniaturization of NIR spectroscopy. However, the photoelectric efficiency and spectral properties of NIR pc‐LEDs are still very limited due to a lack of efficient broadband NIR phosphors with peak emission wavelength >850 nm. Here, a novel Cr3+‐activated perovskite‐like Mg4Ta2O9 phosphor is reported, which exhibits a broad NIR emission band peaking at 850 nm with a high internal (external) quantum efficiency of 72% (33.4%). The fabricated NIR pc‐LED shows a broad emission band covering the whole 700–1100 nm spectrum range with a photoelectric conversion efficiency of 22.1% at 10 mA. This work may provide a new paradigm for the discovery of Cr3+ singly doped NIR phosphors with excellent performance.
High‐Sensitivity Organic Photodetector Based on Surface‐Concentrated Nonfused Ring Electron Acceptor
Authors: Kim Min Soo , Luo Dou , Jang Woongsik , Kim Byung Gi , Shan Chengwei , Kyaw Aung Ko Ko , Wang Dong Hwan 
Published: December 2022

AbstractOrganic photodetectors (OPDs) with high photodetection abilities are essential requirements for ubiquitous light‐sensing devices. This work presents a simple nonfused ring electron acceptor (NFREA) named “TPDC‐4F” having optical bandgap of 1.42 eV, being designed as an efficient OPD via thickness control and additive engineering of the photosensitive layer. The optimized photosensitive layer composed of poly[(2,6‐(4,8‐bis(5‐(2‐ethylhexyl‐3‐fluoro)thiophen‐2‐yl)‐benzo[1,2‐b:4,5‐b′]dithiophene))‐alt‐(5,5‐(1′,3′‐di‐2‐thienyl‐5′,7′‐bis(2‐ethylhexyl)benzo[1′,2′‐c:4′,5′‐c′]dithiophene‐4,8‐dione))] (PM6) donors and TPDC‐4F acceptors shows a dramatically suppressed dark current of 3.55 × 10−9 A cm−2. Moreover, it shows improved photoelectric properties and fast charge transfer even though the photosensitive layer thickness is as large as 330 nm. OPDs based on the 330‐nm‐thick PM6:TPDC‐4F with 1‐chloronaphthalene additive exhibit a high specific detectivity (D*) of 1.27 × 1013 cm Hz1/2 W−1 at 800 nm and a linear dynamic range of 122 dB under a bias of −0.1 V. The device also exhibits fast rise and fall times of 6.81 and 5.41 µs, respectively. This work demonstrates that the NFREA‐based OPDs offer competitive device performance compared to those based on fused‐ring electron acceptors.
Cathode–Electrolyte Interface Modification by Binder Engineering for High‐Performance Aqueous Zinc‐Ion Batteries
Authors: Dong Haobo , Liu Ruirui , Hu Xueying , Zhao Fangjia , Kang Liqun , Liu Longxiang , Li Jianwei , Tan Yeshu , Zhou Yongquan , Brett Dan J.L. , He Guanjie , Parkin Ivan P. 
Published: December 2022

AbstractA stable cathode–electrolyte interface (CEI) is crucial for aqueous zinc‐ion batteries (AZIBs), but it is less investigated. Commercial binder poly(vinylidene fluoride) (PVDF) is widely used without scrutinizing its suitability and cathode‐electrolyte interface (CEI) in AZIBs. A water‐soluble binder is developed that facilitated the in situ formation of a CEI protecting layer tuning the interfacial morphology. By combining a polysaccharide sodium alginate (SA) with a hydrophobic polytetrafluoroethylene (PTFE), the surface morphology, and charge storage kinetics can be confined from diffusion‐dominated to capacitance‐controlled processes. The underpinning mechanism investigates experimentally in both kinetic and thermodynamic perspectives demonstrate that the COO− from SA acts as an anionic polyelectrolyte facilitating the adsorption of Zn2+; meanwhile fluoride atoms on PTFE backbone provide hydrophobicity to break desolvation penalty. The hybrid binder is beneficial in providing a higher areal flux of Zn2+ at the CEI, where the Zn‐Birnessite MnO2 battery with the hybrid binder exhibits an average specific capacity 45.6% higher than that with conventional PVDF binders; moreover, a reduced interface activation energy attained fosters a superior rate capability and a capacity retention of 99.1% in 1000 cycles. The hybrid binder also reduces the cost compared to the PVDF/NMP, which is a universal strategy to modify interface morphology.
High‐Throughput Metal 3D Printing Pen Enabled by a Continuous Molten Droplet Transfer
Authors: Kim Chan Kyu , Cho Dae‐Won , Kim Seok , Song Sang Woo , Seo Kang Myung , Cho Young Tae 
Published: December 2022

AbstractIn metal additive manufacturing (AM), arc plasma is attracting attention as an alternative heat source to expensive lasers to enable the use of various metal wire materials with a high deposition efficiency. However, the stepwise material deposition and resulting limited number of degrees of freedom limit their potential for high‐throughput and large‐scale production for industrial applications. Herein, a high‐throughput metal 3D printing pen (M3DPen) strategy is proposed based on an arc plasma heat source by harnessing the surface tension of the molten metal for enabling continuous material deposition without a downward flow by gravity. The proposed approach differs from conventional arc‐based metal AM in that it controls the solidification and cooling time between interlayers of a point‐by‐point deposition path, thereby allowing for continuous metal 3D printing of freestanding and overhanging structures at once. The resulting mechanical properties and unique microstructures by continuous metal deposition that occur due to the difference in the thermal conditions of the molten metal under cooling are also investigated. This technology can be applied to a wide range of alloy systems and industrial manufacturing, thereby providing new possibilities for metal 3D printing.