bluuebunny/crossref_metadata_2025_split huggingface dataset:
An Inorganic‐Dominate Molecular Diluent Enables Safe Localized High Concentration Electrolyte for High‐Voltage Lithium‐Metal Batteries
Authors: Liu Qianqian , Liu Yan , Chen Zerui , Ma Qiang , Hong Youran , Wang Jianghao , Xu Yifei , Zhao Wei , Hu Zhikun , Hong Xiang , Wang Jiangwei , Fan Xiulin , Wu Hao Bin 
Published: November 2022

AbstractThe development of high‐voltage Lithium‐metal batteries (LMBs) is hindered by suitable electrolytes that are simultaneously compatible with both high‐voltage cathodes and Li anodes. Herein, a novel localized high‐concentration electrolyte with ethoxy(pentafluoro)cyclotriphosphazene (PFPN) as a nonflammable diluent is developed. The inorganic‐dominate diluent improves the safety of the organic electrolyte, and helps to construct robust passivation interphases on both electrodes. Specifically, PFPN accelerates the complete reduction of anions, leading to a stable anion‐derived interphase layer on Li anode. Meanwhile, PFPN and anions co‐participate in the formation of cathode‐electrolyte interphase, suppressing side reactions and the structural damage of high‐voltage Ni‐rich cathodes. As a result, PFPN‐based electrolyte prolongs the cycling life of LMBs based on high‐voltage LiNi0.6Co0.2Mn0.2 (NCM622) and LiNi0.8Co0.1Mn0.1 (NCM811) cathodes. Specially, 25‐µm‐thick Li paired with NCM622 with a N/P ratio of 1.3 (4.4 V) exhibits excellent capacity retention of above 90% after 200 cycles. This study highlights the important role of diluent in tailoring electrode/electrolyte interphases and provides a new strategy for designing high‐safety electrolytes toward high‐voltage LMBs.
Lithiation‐Induced Defect Engineering to Promote Oxygen Evolution Reaction
Authors: Liu Jingjie , Zheng Mengting , Li Jiantao , Yuan Yifei , Li Chenghang , Zhang Shanqing , Yang Lin , Bai Zhengyu , Lu Jun 
Published: November 2022

AbstractExploring efficient electrocatalysts for oxygen evolution reaction (OER) is an urgent need to advance the development of sustainable energy conversion. Though defect engineering is considered an effective strategy to regulate catalyst activity for enhanced OER performance, the controllable synthesis of defective oxides electrocatalysts remains challenging. Here, oxygen defects are introduced into NiCo2O4 nanorods by an electrochemical lithiation strategy. By tuning in situ lithiation potentials, the concentration of oxygen defects and the corresponding catalytic activity can be feasibly regulated. In addition, the relationship between the changes in the defect density and electronic structure and the lithiation cut‐off voltages is revealed. The results show that NiCo2O4 nanorods undertook intercalation and two‐step conversion reaction, in which the lithiation‐induced conversion reaction gives rise to a CoO@NiO‐based structure with higher defect density and lower oxidation states. As a result, the defective CoO@NiO‐based catalyst exhibits exceptional OER activity with an overpotential of 270 mV at 10 mA cm−2, which is about 74 mV below the pristine nanomaterials. This research proposes a novel strategy to explore high‐performance catalysts with structural stability and defect control.
Engineering Polarization in the Ferroelectric Electrocatalysts to Boost Water Electrolysis
Authors: Li Xiaoning , Du Yumeng , Ge Liangbing , Hao Chongyan , Bai Ying , Fu Zhengping , Lu Yalin , Cheng Zhenxiang 
Published: November 2022

AbstractWater splitting is the most important process for making green hydrogen. The positive effects of ferroelectric polarization in various kinds of water splitting are well recognized, but the study of electrocatalytic water splitting is still in its infancy. Herein, a family of intrinsic ferroelectrics with a flexible tetragonal tungsten bronze structure is chosen to accommodate oxygen evolution reaction (OER) active sites together with its freedom for tuning the ferroelectric polarization. It is found that the OER performance is positively correlated with the ferroelectric polarization, with a significant reduction in the overpotential of ≈40 mV at 10 mA cm−2, coming from two trade‐off effects, i.e., enhancement of the surface adsorption and band tilting for fast electron transfer. This study not only fills the gap between electrocatalytic water splitting and the band structure but also proposes ferroelectric polarization as a powerful tool to enhance water splitting for clean hydrogen in several ways.
Enhanced Cycle Stability of Low‐Cost Na‐Rich Metallic NaCl Electrode for Advanced Na‐Ion Batteries
Authors: Moeez Iqra , Susanto Dieky , Park Jae‐Ho , Kim Ji‐Young , Lim Hee‐Dae , Chung Kyung Yoon 
Published: November 2022

AbstractSodium‐rich metallic Nax+z has received significant attention as a low‐cost alternative to the conventional electrode materials used in Li‐ion batteries. However, the poor cyclability of NaxCl remains a major challenge to its practical application. Here, a simple method is developed for improving the electrochemical performance of NaxCl by controlling the upper limit of cut‐off voltage. It is demonstrated that additional Na‐vacancy defects can be introduced in the NaCl structure during the high‐voltage activation process at 4.5 V. The structure then accommodates more sodium ions during the next discharge, resulting in increased capacity. At the same time, Cl‐ions released by NaCl decomposition are oxidized to form Cl‐based organic species at the active material interfaces. This plays a crucial role in protecting the NaCl electrode from undesired side reactions at high voltage. In short, this control of the charging protocol helps to induce more vacancies in the NaCl structure, as well as form stable interphases on the electrode surface, contributing to the increased capacity and enhanced cycle stability. This study will help in exploring a new approach for developing low‐cost and high‐capacity electrode material, which can potentially be applied in future energy‐storage systems.
Engineering Transition Metal Layers for Long Lasting Anionic Redox in Layered Sodium Manganese Oxide
Authors: Voronina Natalia , Yu Jun Ho , Kim Hee Jae , Yaqoob Najma , Guillon Olivier , Kim Hyungsub , Jung Min‐Gi , Jung Hun‐Gi , Yazawa Koji , Yashiro Hitoshi , Kaghazchi Payam , Myung Seung‐Taek 
Published: November 2022

AbstractOxygen‐redox‐based‐layered cathode materials are of great importance in realizing high‐energy‐density sodium‐ion batteries (SIBs) that can satisfy the demands of next‐generation energy storage technologies. However, Mn‐based‐layered materials (P2‐type Na‐poor Nay[AxMn1−x]O2, where A = alkali ions) still suffer from poor reversibility during oxygen‐redox reactions and low conductivity. In this work, the dual Li and Co replacement is investigated in P2‐type‐layered NaxMnO2. Experimentally and theoretically, it is demonstrated that the efficacy of the dual Li and Co replacement in Na0.6[Li0.15Co0.15Mn0.7]O2 is that it improves the structural and cycling stability despite the reversible Li migration from the transition metal layer during de‐/sodiation. Operando X‐ray diffraction and ex situ neutron diffraction analysis prove that the material maintains a P2‐type structure during the entire range of Na+ extraction and insertion with a small volume change of ≈4.3%. In Na0.6[Li0.15Co0.15Mn0.7]O2, the reversible electrochemical activity of Co3+/Co4+, Mn3+/Mn4+, and O2‐/(O2)n‐ redox is identified as a reliable mechanism for the remarkable stable electrochemical performance. From a broader perspective, this study highlights a possible design roadmap for developing cathode materials with optimized cationic and anionic activities and excellent structural stabilities for SIBs.
Light‐Mediated Multi‐Level Flexible Copper Iodide Resistive Random Access Memory for Forming‐Free, Ultra‐Low Power Data Storage Application
Authors: Mishra Dhananjay , Mokurala Krishnaiah , Kumar Ajit , Seo Seung Gi , Jo Hyeon Bin , Jin Sung Hun 
Published: November 2022

AbstractThis study demonstrates the efficacy of an emerging p‐type copper iodide (CuI) semiconductor in a flexible, low‐voltage resistive random‐access memory (RRAM), which can be readily integrated with metal‐oxide n‐type counterparts for complementary circuit systems. Herein, CuI RRAM devices are implemented via a room‐temperature solid iodination process, exhibiting a consistent On/Off ratio (≈104), excellent endurance of more than ≈103 cycles, together with a long retention period (> 5 × 104 s). Furthermore, a scheme of light‐mediated multi‐level data storage is demonstrated using blue light illumination (λ = 455 nm), to exploit possible photonic memristive functionality through notable photo‐response of CuI. In addition, the current conduction and resistive switching behaviors are systematically studied via low‐temperature measurements from 203 to 343 K, validating thermal stability and the governing key switching mechanism in CuI RRAM devices. The longstanding problem with CuI device longevity is effectively addressed via PMMA encapsulation, resulting in a 15‐fold improvement in the lifespan of devices even in air, as compared with non‐passivated devices. These findings suggest that flexible optoelectronic systems, combined with reliable, ultra‐low power CuI RRAM devices with photo memristive functionality, can leverage the enhancement of multifunctional selectors required in process‐in‐memories and the synaptic elements of neuromorphic applications.
Tailoring Rational Crystal Orientation and Tunable Sulfur Vacancy on Metal‐Sulfides toward Advanced Ultrafast Ion‐Storage Capability
Authors: Zhao Wenqing , Yuan Shaohui , Lei Shuya , Zeng Zihao , Dong Jinfeng , Jiang Feng , Yang Yue , Sun Wei , Ji Xiaobo , Ge Peng 
Published: November 2022

AbstractAttracted by high energy density and power density, metal‐sulfides anodes have promising application prospects in fast charging batteries. However, they still suffer from low electrical conductivity and sluggish electrochemical kinetics, resulting in poor fast charging capacity. Herein, spindle‐like antimony sulfide (Sb2S3) is rationally tailored with favorable (hk1) crystal orientation and rich S‐vacancies using a simple hydrothermal method, which improve electric conductivity significantly. Triggered by S‐vacancies lattice defects, SbOC interfacial bonds and S‐doped carbon layer are built successfully. Under their multiple‐controlling synergistic effects, electrochemical kinetics and reaction reversibility are promoted effectively. As expected, Sb2S3/HTAB@C show high average initial coulombic efficiency of 86.12%, and deliver 624.5 and 428.4 mAh g−1 after cycling 100 cycles at 10.0 and 30.0 A g−1 respectively in Li‐ion batteries (LIBs). Electrochemical kinetic analysis and theoretical calculations indicate that superior ultrafast charging capacity originates from quickened interfacial electron/ions transferring and alleviates electrochemical polarization. Ex situ technologies powerfully prove good stability of (hk1) orientation, SbOC bonds and S‐doped carbon layer. Notably, full LIBs of SS/H@C versus LiFePO4@C display 500.9 and 398.3 mAh g−1 at 5.0 and 10.0 A g−1, respectively. This study is anticipated to open avenue to develop advanced metal‐sulfides anodes for fast charging batteries.
Regulating Charge Carrier Recombination in the Interconnecting Layer to Boost the Efficiency and Stability of Monolithic Perovskite/Organic Tandem Solar Cells
Authors: Yang Haidi , Chen Weijie , Yu Yuan , Shen Yunxiu , Yang Heyi , Li Xinqi , Zhang Ben , Chen Haiyang , Cheng Qinrong , Zhang Zhichao , Qin Wei , Chen Jing‐De , Tang Jian‐Xin , Li Yaowen , Li Yongfang 
Published: November 2022

AbstractThe charge carriers of single‐junction solar cells can be fluently extracted and then collected by electrodes, leading to weak charge carrier accumulation and low energy loss (Eloss). However, in tandem solar cells (TSCs), it is a considerable challenge to obtain a balance between the densities of the holes and electrons extracted from the two respective subcells to facilitate an efficient recombination in the interconnecting layer (ICL). Herein, a charge‐carrier‐dynamic management strategy for inorganic perovskite/organic TSCs is proposed, centered on the simultaneous regulation of the defect states of CsPbI1.9Br1.1 perovskite in the front subcell and hole transport ability from the perovskite to ICL. The target hole density on the perovskite surface and the hole loss before reaching the ICL are significantly improved. As a result, the hole/electron density offset in the ICL can be effectively narrowed, leading to a balanced charge carrier recombination, which reduces the Eloss in TSCs. The resulting inorganic perovskite/organic 0.062‐cm2 TSC exhibits a remarkable power conversion efficiency (PCE) of 23.17% with an ultrahigh open‐circuit voltage (Voc) of 2.15 V, and the PCE of the 1.004‐cm2 device (21.69%) exhibited a weak size‐dependence. This charge‐carrier‐dynamic management strategy can also effectively enhance the operational and ultraviolet‐light stabilities of the TSCs.
CeOx as Surface Passivation and Hole Transfer Catalyst Layer Boosting Solar Water Oxidation of ZnFe2O4 Nanorods Photoanode
Authors: Maity Dipanjan , Pal Debashish , Saha Soham , Punetha Pooja , Sarkar Debasish , De Debasis , Khan Gobinda Gopal , Mandal Kalyan 
Published: November 2022

AbstractSevere surface photocarrier recombination and poor electronic conductivity are the major factors behind the sluggish photoelectrochemical water oxidation kinetics of the ZnFe2O4 photoanode. Here, the CeOx catalyst overlayer has been coupled with the reduced ZnFe2O4 nanorods (NRs) to reduce the surface charge recombination on the photoanode significantly. The density functional theory (DFT) studies indicate that the oxygen vacancy defect‐rich CeOx catalyst constructs a favorable band alignment with ZnFe2O4 promoting rapid photocarrier separation and serves as a conducting photocarrier transfer pathway accelerating the hole transportation toward the electrode/electrolyte interface. The ZnFe2O4/CeOx nano‐heterostructure photoanode exhibits a current density of 0.64 mA cm−2 at 1.23 V versus RHE under AM 1.5 G illumination, which corresponds to >167% increase over that of the ZnFe2O4 NRs photoanode. The CeOx coupling reduces the onset potential cathodically by 180 mV over the ZnFe2O4 NRs photoanode. The ZnFe2O4/CeOx nano‐heterostructure photoanode also exhibits excellent charge transfer efficiency (≈64% at 1.23 V vs RHE) and photostability. The results indicate the superior catalytic performance of oxygen vacancy defect‐rich CeOx in the PEC process. This work demonstrates the multifunctional role of CeOx as a surface passivation overlayer, hole transfer layer, and efficient oxygen evolution reaction catalyst.
Enhanced Electron Correlation and Significantly Suppressed Thermal Conductivity in Dirac Nodal‐Line Metal Nanowires by Chemical Doping
Authors: Coughlin Amanda L. , Pan Zhiliang , Hong Jeonghoon , Zhang Tongxie , Zhan Xun , Wu Wenqian , Xie Dongyue , Tong Tian , Ruch Thomas , Heremans Jean J. , Bao Jiming , Fertig Herbert A. , Wang Jian , Kim Jeongwoo , Zhu Hanyu , Li Deyu , Zhang Shixiong 
Published: November 2022

AbstractEnhancing electron correlation in a weakly interacting topological system has great potential to promote correlated topological states of matter with extraordinary quantum properties. Here, the enhancement of electron correlation in a prototypical topological metal, namely iridium dioxide (IrO2), via doping with 3d transition metal vanadium is demonstrated. Single‐crystalline vanadium‐doped IrO2 nanowires are synthesized through chemical vapor deposition where the nanowire yield and morphology are improved by creating rough surfaces on substrates. Vanadium doping leads to a dramatic decrease in Raman intensity without notable peak broadening, signifying the enhancement of electron correlation. The enhanced electron correlation is further evidenced by transport studies where the electrical resistivity is greatly increased and follows an unusual dependence on the temperature (T). The lattice thermal conductivity is suppressed by an order of magnitude via doping even at room temperature where phonon‐impurity scattering becomes less important. Density functional theory calculations suggest that the remarkable reduction of thermal conductivity arises from the complex phonon dispersion and reduced energy gap between phonon branches, which greatly enhances phase space for phonon–phonon Umklapp scattering. This work demonstrates a unique system combining 3d and 5d transition metals in isostructural materials to enrich the system with various types of interactions.
Ultrasound‐Driven On‐Demand Transient Triboelectric Nanogenerator for Subcutaneous Antibacterial Activity
Authors: Imani Iman M. , Kim Bosung , Xiao Xiao , Rubab Najaf , Park Byung‐Joon , Kim Young‐Jun , Zhao Pin , Kang Minki , Kim Sang‐Woo 
Published: November 2022

AbstractTo prevent surgical site infection (SSI), which significantly increases the rate morbidity and mortality, eliminating microorganisms is prominent. Antimicrobial resistance is identified as a global health challenge. This work proposes a new strategy to eliminate microorganisms of deep tissue through electrical stimulation with an ultrasound (US)‐driven implantable, biodegradable, and vibrant triboelectric nanogenerator (IBV‐TENG). After a programmed lifetime, the IBV‐TENG can be eliminated by provoking the on‐demand device dissolution by controlling US intensity with no surgical removal of the device from the body. A voltage of ≈4 V and current of ≈22 µA generated from IBV‐TENG under ultrasound in vitro, confirming inactivating ≈100% of Staphylococcus aureus and ≈99% of Escherichia coli. Furthermore, ex vivo results show that IBV‐TENG implanted under porcine tissue successfully inactivates bacteria. This antibacterial technology is expected to be a countermeasure strategy against SSIs, increasing life expectancy and healthcare quality by preventing microorganisms of deep tissue.
Laser‐Induced Graphene Enabled Additive Manufacturing of Multifunctional 3D Architectures with Freeform Structures
Authors: Liu Fu , Gao Yan , Wang Guantao , Wang Dan , Wang Yanan , He Meihong , Ding Xilun , Duan Haibin , Luo Sida 
Published: November 2022

Abstract3D printing has become an important strategy for constructing graphene smart structures with arbitrary shapes and complexities. Compared with graphene oxide ink/gel/resin based manners, laser‐induced graphene (LIG) is unique for facile and scalable assembly of 1D and 2D structures but still faces size and shape obstacles for constructing 3D macrostructures. In this work, a brand‐new LIG based additive manufacturing (LIG‐AM) protocol is developed to form bulk 3D graphene with freeform structures without introducing extra binders, templates, and catalysts. On the basis of selective laser sintering, LIG‐AM creatively irradiates polyimide (PI) powder‐bed for triggering both particle‐sintering and graphene‐converting processes layer‐by‐layer, which is unique for assembling varied types of graphene architectures including identical‐section, variable‐section, and graphene/PI hybrid structures. In addition to exploring combined graphitizing and fusing discipline, processing efficiency and assembling resolution of LIG‐AM are also balanceable through synergistic control of lasing power and powder‐feeding thickness. By further studying various process dependent properties, a LIG‐AM enabled aircraft‐wing section model is finally printed to comprehensively demonstrate its shiftable process, hybridizable structure, and multifunctional performance including force‐sensing, anti‐icing/deicing, and microwave shielding and absorption.
Ternary Synergism of Heterogeneous M1N4‐C‐M2N4‐C‐M3N4Single‐Atom Sites to Manipulate the Electrocatalytic Pathway for Zn‐Air Battery and Water Splitting
Authors: Yang Anzhou , Su Keying , Lei Wu , Tang Yawen , Qiu Xiaoyu 
Published: November 2022

AbstractTernary metal catalysts hold great promise in complementary functionality and synergistic interplay, which are promising for combined reactions involving multi‐intermediates. However, simultaneously downscaling all three metal species into single‐atom level still remains challenge. Herein, a universal metal encapsulation‐segregation‐overlay strategy is designed to realize the fabrication of heterogeneous M1N4‐C‐M2N4‐C‐M3N4ternary single‐atoms (TSAs)‐based catalysts, with well‐defined configuration and threefold enhancement of single‐atom loading (IrPtCu TSAs, up to 21.24 wt%). Taking non‐precious‐metallic CoN4‐C‐NiN4‐C‐FeN4TSAs for instance, the integration of triple‐decker single‐atoms affords strong electronic reciprocity, with interbedded Ni donating electrons for both Fe and Co, thereby simultaneously enhancing the catalytic activity for oxygen reduction, oxygen evolution, and hydrogen evolution through a “site‐selective master‐servant” mechanism. Thanks to the mutually assisted tri‐functionality, the CoN4‐C‐NiN4‐C‐FeN4TSAs‐electrode takes on alternatating master/servant roles to enable outstanding recyclability for energy devices. This work breaks the obstructions in synthesis and fundamental study of TSAs, providing insights into atomic material design for complicated catalytic reactions.
Selective Lanthanide‐Organic Catalyzed Depolymerization of Nylon‐6 to ϵ‐Caprolactam
Authors: Wursthorn Lukas , Beckett Kristen , Rothbaum Jacob O. , Cywar Robin M. , Lincoln Clarissa , Kratish Yosi , Marks Tobin J. 
Published: November 2022

AbstractNylon‐6 is selectively depolymerized to the parent monomer ϵ‐caprolactam by the readily accessible and commercially available lanthanide trisamido catalysts Ln(N(TMS)2)3(Ln=lanthanide). The depolymerization process is solvent‐free, near quantitative, highly selective, and operates at the lowest Nylon‐6 to ϵ‐caprolactam depolymerization temperature reported to date. The catalytic activity of the different lanthanide trisamides scales with the Ln3+ionic radius, and this process is effective with post‐consumer Nylon‐6 as well as with Nylon‐6+polyethylene, polypropylene or polyethylene terephthalate mixtures. Experimental kinetic data and theoretical (DFT) mechanistic analyses suggest initial deprotonation of a Nylon terminal amido N−H bond, which covalently binds the catalyst to the polymer, followed by a chain‐end back‐biting process in which ϵ‐caprolactam units are sequentially extruded from the chain end.
Towards a Cradle‐to‐Cradle Polyolefin Lifecycle
Authors: Thevenon Arnaud , Vollmer Ina 
Published: November 2022

AbstractAchieving efficient chemical depolymerization of waste polyolefins to monomers remains an unsolved challenge, while it could be an effective means to avoid further waste accumulation in the environment and generate economic benefits. In a recent publication by Conk et al., polyethylene (PE) is converted to propylene, the second most used monomer in the polymer industry. The conversion is achieved via a tandem catalysis approach in which partially unsaturated PE chains react with ethylene to generate propylene with yields as high as 87 %. The study is a first proof of concept showcasing a selective chemical depolymerization of PE to a monomer. Future research is expected to focus on the catalyst optimization, process design, and compatibility with contaminated and multi‐polymer waste streams.