bluuebunny/crossref_metadata_2025_split huggingface dataset:
Nanoporous NiSb to Enhance Nitrogen Electroreduction via Tailoring Competitive Adsorption Sites
Authors: Fan Guilan , Xu Wence , Li Jinhan , Chen Jia‐Liang , Yu Meng , Ni Youxuan , Zhu Shengli , Su Xun‐Cheng , Cheng Fangyi 
Published: September 2021

AbstractAmbient nitrogen reduction reaction (NRR) is attracting extensive interest but still suffers from sluggish kinetics owing to competitive rapid hydrogen evolution and difficult nitrogen activation. Herein, nanoporous NiSb alloy is reported as an efficient electrocatalyst for N2 fixation, achieving a high ammonia yield rate of 56.9 µg h−1 mg−1 with a Faradaic efficiency of 48.0%. Density functional theory calculations reveal that in NiSb alloy, Ni favors N2 hydrogenation while the neighboring Sb separates active sites for proton and N2 adsorption, which optimizes the adsorption/desorption of intermediates and enables an energetically favorable NRR pathway. This work indicates promising electrocatalytic application of the alloys of 3d and p block metals toward the NRR and provides an intriguing strategy to enhance the reduction of inert molecules by restraining the competitive hydrogen adsorption.
Crystallographic‐Site‐Specific Structural Engineering Enables Extraordinary Electrochemical Performance of High‐Voltage LiNi0.5Mn1.5O4 Spinel Cathodes for Lithium‐Ion Batteries
Authors: Liang Gemeng , Peterson Vanessa K. , Wu Zhibin , Zhang Shilin , Hao Junnan , Lu Cheng‐Zhang , Chuang Cheng‐Hao , Lee Jyh‐Fu , Liu Jue , Leniec Grzegorz , Kaczmarek Sławomir Maksymilian , D'Angelo Anita M. , Johannessen Bernt , Thomsen Lars , Pang Wei Kong , Guo Zaiping 
Published: September 2021

AbstractThe development of reliable and safe high‐energy‐density lithium‐ion batteries is hindered by the structural instability of cathode materials during cycling, arising as a result of detrimental phase transformations occurring at high operating voltages alongside the loss of active materials induced by transition metal dissolution. Originating from the fundamental structure/function relation of battery materials, the authors purposefully perform crystallographic‐site‐specific structural engineering on electrode material structure, using the high‐voltage LiNi0.5Mn1.5O4 (LNMO) cathode as a representative, which directly addresses the root source of structural instability of the Fdm structure. By employing Sb as a dopant to modify the specific issue‐involved 16c and 16d sites simultaneously, the authors successfully transform the detrimental two‐phase reaction occurring at high‐voltage into a preferential solid‐solution reaction and significantly suppress the loss of Mn from the LNMO structure. The modified LNMO material delivers an impressive 99% of its theoretical specific capacity at 1 C, and maintains 87.6% and 72.4% of initial capacity after 1500 and 3000 cycles, respectively. The issue‐tracing site‐specific structural tailoring demonstrated for this material will facilitate the rapid development of high‐energy‐density materials for lithium‐ion batteries.
Suppressing Interface Strain for Eliminating Double‐Slope Behaviors: Towards Ideal Conformable Polymer Field‐Effect Transistors
Authors: Wang Shuya , Zhao Xiaoli , Zhang Cong , Yang Yahan , Liang Jing , Ni Yanping , Zhang Mingxin , Li Juntong , Ye Xiaolin , Zhang Jidong , Tong Yanhong , Tang Qingxin , Liu Yichun 
Published: September 2021

AbstractHigh‐mobility polymer field‐effect transistors (PFETs) are being actively explored for applications in soft electronic skin and low‐cost flexible displays because of their superior solution processability, mechanical flexibility, and stretchability. However, most of high‐mobility PFETs often deviate from the idealized behavior with variable mobility, large threshold voltage, and high off‐state current, which masks their intrinsic properties and significantly impedes their practical applications. Here, it is first revealed that interface strain between polymer thin film and rigid substrate plays a crucial role in determining the ideality of PFETs, and demonstrate that various ideal conformable PFETs can be successfully fabricated by releasing strain. It is found that strain in film can be released by one‐step peeling strategy, which can reduce π‐π stacking distance and suppress generation of oxygen doped carriers, thereby obtaining linearly injected charge carriers and decreased carrier concentration in channel, eventually realizing ideal PFETs. More impressively, the fabricated ideal conformable PFET array displays outstanding conformability to curved objects, and meanwhile showing excellent organic light‐emitting display driving capability. The work clarifies the effect of the interface strain on the device ideality, and strain can be effectively released by a facile peeling strategy, thus offering useful guidance for the construction of ideal conformable PFETs.
Biodegradable Small‐Scale Swimmers for Biomedical Applications
Authors: Llacer‐Wintle Joaquin , Rivas‐Dapena Antón , Chen Xiang‐Zhong , Pellicer Eva , Nelson Bradley J. , Puigmartí‐Luis Josep , Pané Salvador 
Published: September 2021

AbstractMost forms of biomatter are ephemeral, which means they transform or deteriorate after a certain time. From this perspective, implantable healthcare devices designed for temporary treatments should exhibit the ability to degrade and either blend in with healthy tissues, or be cleared from the body with minimal disruption after accomplishing their designated tasks. This topic is currently being investigated in the field of biomedical micro‐ and nanoswimmers. These tiny devices have the ability to move through fluids by converting physical or chemical energy into motion. Several architectures of these devices have been designed to mimic the motion strategies of nature's motile microorganisms and cells. Due to their motion abilities, these devices have been proposed as minimally invasive tools for precision healthcare applications. Hence, a natural progression in this field is to produce motile structures that can adopt, or even surpass, similar transient features as biological systems. The fate of small‐scale swimmers after accomplishing their therapeutic mission is critical for the successful translation of small‐scale swimmers’ technologies into clinical applications. In this review, recent research efforts are summarized on the topic of biodegradable micro‐ and nanoswimmers for biomedical applications, with a focus on targeted therapeutic delivery.
Lithium Fluoride in Electrolyte for Stable and Safe Lithium‐Metal Batteries
Authors: Tan Yi‐Hong , Lu Gong‐Xun , Zheng Jian‐Hui , Zhou Fei , Chen Mei , Ma Tao , Lu Lei‐Lei , Song Yong‐Hui , Guan Yong , Wang Junxiong , Liang Zheng , Xu Wen‐Shan , Zhang Yuegang , Tao Xinyong , Yao Hong‐Bin 
Published: September 2021

AbstractElectrolyte engineering via fluorinated additives is promising to improve cycling stability and safety of high‐energy Li‐metal batteries. Here, an electrolyte is reported in a porous lithium fluoride (LiF) strategy to enable efficient carbonate electrolyte engineering for stable and safe Li‐metal batteries. Unlike traditionally engineered electrolytes, the prepared electrolyte in the porous LiF nanobox exhibits nonflammability and high electrochemical performance owing to strong interactions between the electrolyte solvent molecules and numerous exposed active LiF (111) crystal planes. Via cryogenic transmission electron microscopy and X‐ray photoelectron spectroscopy depth analysis, it is revealed that the electrolyte in active porous LiF nanobox involves the formation of a high‐fluorine‐content (>30%) solid electrolyte interphase layer, which enables very stable Li‐metal anode cycling over one thousand cycles under high current density (4 mA cm−2). More importantly, employing the porous LiF nanobox engineered electrolyte, a Li || LiNi0.8Co0.1Mn0.1O2 pouch cell is achieved with a specific energy of 380 Wh kg−1 for stable cycling over 80 cycles, representing the excellent performance of the Li‐metal pouch cell using practical carbonate electrolyte. This study provides a new electrolyte engineering strategy for stable and safe Li‐metal batteries.
The Interfacial Electronic Engineering in Binary Sulfiphilic Cobalt Boride Heterostructure Nanosheets for Upgrading Energy Density and Longevity of Lithium‐Sulfur Batteries
Authors: Li Zhonglin , Li Pengyue , Meng Xueping , Lin Zhang , Wang Ruihu 
Published: September 2021

AbstractHigh gravimetric, areal and volumetric capacities together with long lifetime are key indexes for the applications of lithium–sulfur (Li‐S) batteries in compact space. The sulfur host materials play pivotal roles in the practical deployment. Herein, one type of new heterostructure nanosheets composed of cobalt boride (CoB) on nitrogen, boron‐codoped porous carbon (NBC), which is constructed through molten salt‐assisted strategy using ZIF‐67‐encapsulated ZIF‐8 as precursors is reported on. Benefiting from strong interfacial electronic interactions between binary sulfiphilic CoB and porous NBC, the CoB/NBC‐S electrode exhibits the excellent cycling stability with low average capacity decay of 0.013% in ultralong 1500 cycles at high rate of 5 C. Remarkably, the electrode with high sulfur content of 82 wt% and high sulfur loading of 5.8 mg cm−2 delivers gravimetric capacity of 1309 mA h g−1, areal capacity of 7.59 mA h cm−2, and volumetric capacity of 1355 mA h cm−3 at 0.1 C. The favorable electrochemical performance can rival with the state‐of‐the‐art of those in the reported nanosheets‐based sulfur cathodes. This study provides new methodology for the design of heterostructure nanosheets of metal borides to achieve energy density and longevity of Li‐S batteries.
Uncovering the Promotion of CeO2/CoS1.97 Heterostructure with Specific Spatial Architectures on Oxygen Evolution Reaction
Authors: Dai Tengyuan , Zhang Xin , Sun Mingzi , Huang Bolong , Zhang Nan , Da Pengfei , Yang Rui , He Zidong , Wang Wei , Xi Pinxian , Yan Chun‐Hua 
Published: September 2021

AbstractStructural engineering and compositional controlling are extensively applied in rationally designing and fabricating advanced freestanding electrocatalysts. The key relationship between the spatial distribution of components and enhanced electrocatalysis performance still needs further elaborate elucidation. Here, CeO2 substrate supported CoS1.97 (CeO2‐CoS1.97) and CoS1.97 with CeO2 surface decorated (CoS1.97‐CeO2) materials are constructed to comprehensively investigate the origin of spatial architectures for the oxygen evolution reaction (OER). CeO2‐CoS1.97 exhibits a low overpotential of 264 mV at 10 mA cm−2 due to the stable heterostructure and faster mass transfer. Meanwhile, CoS1.97‐CeO2 has a smaller Tafel slope of 49 mV dec−1 through enhanced adsorption of OH−, fast electron transfer, and in situ formation of Co(IV)O2 species under the OER condition. Furthermore, operando spectroscopic characterizations combined with theoretical calculations demonstrate that spatial architectures play a distinguished role in modulating the electronic structure and promoting the reconstruction from sulfide to oxyhydroxide toward higher chemical valence. The findings highlight spatial architectures and surface reconstruction in designing advanced electrocatalytic materials.
Multichannel Piezo‐Ultrasound Implant with Hybrid Waterborne Acoustic Metastructure for Selective Wireless Energy Transfer at Megahertz Frequencies
Authors: Jiang Laiming , Lu Gengxi , Yang Yang , Xu Yang , Qi Fangjie , Li Jiapu , Zhu Benpeng , Chen Yong 
Published: September 2021

AbstractUltrasound energy transfer (UET) is developed and integrated into various bioelectronics with diagnostic, therapeutic, and monitoring capabilities. However, existing UET platforms generally enable one function at a time due to the single ultrasound channel architecture, limiting the full potential of bioelectronics that requires multicontrol modes. Here, a multichannel piezo‐ultrasound implant (MC‐PUI) is presented that integrates a hybrid waterborne acoustic metastructure (HWAM), multiple piezo‐harvesters, and a miniaturized circuit with electronic components for selective wireless control via ultrasound frequency switching. The HWAM that utilizes both a 3D‐printed air‐diffraction matrix and a half‐lambda Fabry–Perot resonator is optimized to provide the advantage of ultrasound selectivity at megahertz frequencies. Complying with U.S. Food and Drug Administration regulations, frequency‐controlled multifunctional operations, such as wireless charging (≈11.08 µW) at 3.3 MHz and high‐sensitivity wireless switch/control (threshold ≈0.55 MPa) of micro‐light‐emitting diode/motor at 1 MHz, are demonstrated ex vivo using porcine tissue and in vivo in a rat. The developed MC‐PUI enhances UET versatility and opens up a new pathway for wireless implant design.
Tunable 2D Group‐III Metal Alloys
Authors: Rajabpour Siavash , Vera Alexander , He Wen , Katz Benjamin N. , Koch Roland J. , Lassaunière Margaux , Chen Xuegang , Li Cequn , Nisi Katharina , El‐Sherif Hesham , Wetherington Maxwell T. , Dong Chengye , Bostwick Aaron , Jozwiak Chris , van Duin Adri C. T. , Bassim Nabil , Zhu Jun , Wang Gwo‐Ching , Wurstbauer Ursula , Rotenberg Eli , Crespi Vincent , Quek Su Ying , Robinson Joshua A. 
Published: September 2021

AbstractChemically stable quantum‐confined 2D metals are of interest in next‐generation nanoscale quantum devices. Bottom‐up design and synthesis of such metals could enable the creation of materials with tailored, on‐demand, electronic and optical properties for applications that utilize tunable plasmonic coupling, optical nonlinearity, epsilon‐near‐zero behavior, or wavelength‐specific light trapping. In this work, it is demonstrated that the electronic, superconducting, and optical properties of air‐stable 2D metals can be controllably tuned by the formation of alloys. Environmentally robust large‐area 2D‐InxGa1−x alloys are synthesized byConfinement Heteroepitaxy (CHet). Near‐complete solid solubility is achieved with no evidence of phase segregation, and the composition is tunable over the full range of x by changing the relative elemental composition of the precursor. The optical and electronic properties directly correlate with alloy composition, wherein the dielectric function, band structure, superconductivity, and charge transfer from the metal to graphene are all controlled by the indium/gallium ratio in the 2D metal layer.
Hyperbolic Metamaterials Fabricated Using 3D Assembled Nanorod Arrays and Enhanced Photocatalytic Performance
Authors: Li Caixia , Liu Jiatong , Wu Zheli , Chen Zhe , Jiang Jingwen , Dou Zhengkang , Liu Xiaoyu , Fu Ming , He Dawei , Wang Yongsheng 
Published: September 2021

AbstractIt is significant but challenging to develop a 3D colloidal assembly method for optical metamaterials. Hyperbolic metamaterials (HMMs) with 3D porous periodic morphologies are suitable for loading functional components for energy harvesting and biosensing and for providing a tunable range of indefinite permittivity. In this study, porous HMMs with 3D periodicities are constructed from directionally assembled silica nanorods with conformal coating of metal. The indefinite dielectric ranges around visible wavelength are formed from the anisotropic geometry induced anisotropic effective permittivity along different directions and are tunable according to the rod length, rod diameter, and thickness of metal coating. The negative refraction of rod array based metamaterials is verified using the transmission ratio between the part beam and full beam in microscope–spectrum system with incident light beam. The rod‐based metamaterials show a higher optical absorption in near‐ultraviolet and visible wavelengths than the compared colloidal sphere assembled structures. The porous HMMs loaded with TiO2 can provide enhanced optical absorption and photocatalytic performances. The structures coated with 180–190 atomic‐layer‐deposition cycles of TiO2 and 8–9 min deposition of silver provide the best performance.
2,6‐Dicarbonitrile Diphenyl‐1λ5‐Phosphinine (DCNP)—A Robust Conjugated Building Block for Multi‐Functional Dyes Exhibiting Tunable Amplified Spontaneous Emission
Authors: Balijapalli Umamahesh , Tang Xun , Okada Daichi , Lee Yi‐Ting , Karunathilaka Buddhika S. B. , Auffray Morgan , Tumen‐Ulzii Ganbaatar , Tsuchiya Youichi , Sandanayaka Atula S. D. , Matsushima Toshinori , Nakanotani Hajime , Adachi Chihaya 
Published: September 2021

AbstractHighly efficient organic light‐emitting diodes (OLEDs) with the concurrent achievement of high external electroluminescence quantum efficiency (EQE) and low light amplification thresholds under optical excitation have been considered as a crucial evolution towards the development of high‐performance electrically pumped organic semiconductor laser diodes. Herein, a series of 2,6‐dicarbonitrile‐diphenyl‐1λ5‐phosphinine (DCNP) based donor (D)‐acceptor (A) type dyes with different electron‐withdrawing and donating moieties have been designed and characterized. The well‐manipulated D‐A strength with tunable optical properties guaranteed the low amplified spontaneous emission (ASE) thresholds of below 10 µJ cm−2 and furnished a wide‐range color‐tuning capability in the visible region (485–595 nm). Furthermore, employing a thermally‐activated delayed fluorescence (TADF) molecule as a triplet harvester boosted the performance of OLEDs based on mDMCz that exhibits an exceptional EQE value of 18.4% which is an eightfold enhancement as compared with that of standard fluorescence OLEDs. Also, the TADF‐assistant fluorescence (TAF) system enables a reduction of the ASE threshold to 3 µJ cm−2 and excellent ASE stability. These results provide a rational design strategy to construct color‐tunable lasing dyes with reduced ASE thresholds and clarify their potentiality as the fluorescent dopant in the TAF system to utilize up‐converted triplet excitons via efficient energy transfer.
Reversibly Photoswitchable Tristate Fluorescence within a Single Polymeric Nanoparticle
Authors: Yu Maolin , Zhang Peisheng , Liu Le , Wang Han , Wang Hong , Zhang Chonghua , Gao Yong , Yang Chuluo , Cui Jiaxi , Chen Jian 
Published: September 2021

AbstractHerein, a class of novel photoswitchable tristate fluorescent polymeric nanoparticles (TS‐PFPNs) consisting of a well‐designed perylenediimide‐spiropyran conjugate (PDI‐SP), two energy‐matched photochromics as spiropyran‐linked methacrylate and diarylethene (DTE) derivative (DTEo‐1) is described. By optimizing the feed ratio of three dyes and controllable switching fluorescence resonance energy transfer from excited PDI to SP or DTE moiety with different lights stimuli, the emission of these TS‐PFPNs can be reversibly switched among distinguishable green, red, and quenching states. In addition, these TS‐PFPNs exhibit high brightness, high contrast, excellent water‐dispersibility, and photoreversibility as well as outstanding long‐term storage stability and processability. It is also demonstrated that these TS‐PFPNs can be directly used for advanced anticounterfeiting, high‐density data storage, and multilevel information encryption.
Breaking Classic Heavy‐Atom Effect to Achieve Heavy‐Atom‐Induced Dramatic Emission Enhancement of Silole‐Based AIEgens with Through‐Bond and Through‐Space Conjugation
Authors: Xiong Zuping , Wang Zhenni , Liu Longxiang , Jiang Mengyi , Zhang Xiaoxiao , Zhu Qiaozhi , Feng Hui , Qian Zhaosheng 
Published: September 2021

AbstractClassic heavy‐atom effect is well known on traditional luminophores, but its usability for newly developed AIEgens with through‐bond and through‐space conjugation leaves a question open. Herein, an interesting heavy‐atom‐induced emission enhancement against classic heavy‐atom effect is reported by examining unique photophysical behaviors of aggregation‐induced emission (AIE)‐active silole compounds both experimentally and theoretically. It is revealed that heavy atoms exert an insignificant impact on the fluorescence of AIEgens due to their through‐space conjugation nature, and weak intermolecular interactions and heavy‐atom‐caused vibration restriction collaboratively contribute to the emission enhancement of these AIEgens via restricting intramolecular motions. The breaking of classic heavy‐atom effect on silole‐based AIEgens not only proves its usability scope only on through‐bond conjugated dyes, it also provides an effective and simple strategy to dramatically improve the emission efficiency of AIEgens.
Ionic Conductivity of Nanopores with Electrically Conductive Surface: Comparison Between 1D and 2D Models
Authors: Krom Artur I. , Ryzhkov Ilya I. 
Published: September 2021

AbstractNanoporous membranes with high ionic conductivity are advantageous in such electrochemical processes as (reverse) electrodialysis, capacitive deionization, and hydrogen energy conversion. In membranes with electrically conductive surface, the conductivity can be regulated by varying the surface potential. This work is devoted to the theoretical study of switchable ionic conductivity. The transport of ions is described by the 2D space charge model and 1D uniform potential model taking into account the Stern layer. The conductivity decreases with lowering the Stern layer permittivity due to enhanced screening of electronic surface charge. The growth of surface potential leads to the conductivity enhancement due to accumulation of more counter‐ions inside the nanopore. For nanopores with constant surface charge density, the ionic conductivity follows the bulk electrolyte conductivity at high ion concentrations, and becomes independent of concentration when the latter is low. In contrast, the nanopores with constant surface potential demonstrate a linear decrease of conductivity with lowering the logarithm of ion concentration. The deviation between 1D and 2D models becomes noticeable at higher values of Stern layer permittivity, pore radius, electrolyte concentration, and surface potential. The proposed models are verified by comparison with experimental data on pure water conductivity in charged porous matrix.
The Interfacial Effect on the Open Circuit Voltage of Ionic Thermoelectric Devices with Conducting Polymer Electrodes
Authors: Mardi Saeed , Zhao Dan , Kim Nara , Petsagkourakis Ioannis , Tybrandt Klas , Reale Andrea , Crispin Xavier 
Published: September 2021

AbstractOrganic‐based energy harvesting devices can contribute to a sustainable solution for the transition to renewable energy sources. The concept of ionic thermoelectrics (iTE) has been recently proposed and motivated by the high values of thermo‐voltage in electrolytes. So far, most research has focused on developing new electrolytes with high Seebeck coefficient. Despite the major role of the electrode materials in supercapacitors and batteries, the effect of various electrodes on energy harvesting in iTE devices has not been widely studied. In this work, the conducting polymer poly(3,4‐ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) is investigated as the functional electrodes in iTE supercapacitors. Through investigating the thermo‐voltage of iTEs of the same electrolyte with varying composition of PEDOT electrodes, it is identified that the different PSS content greatly affects the overall thermo‐induced voltage coefficient, Seff (i.e., effective thermopower). The permselective polyanion in the electrode causes cation concentration differences at the electrode/electrolyte interface and contributes to an interfacial potential drop that is temperature dependent. As a result, the overall thermo‐voltage of the device possesses both an interfacial and a bulk contribution. The findings extend the fundamental understanding of iTE effect with functional electrodes, which could lead a new direction to enhance the heat‐to‐electricity conversion.