bluuebunny/crossref_metadata_2025_split huggingface dataset:
In Situ Non‐Topotactic Reconstruction‐Induced Synergistic Active Centers for Polysulfide Cascade Catalysis
Authors: Zeng Pan , Zou Hao , Cheng Chen , Wang Lei , Yuan Cheng , Liu Genlin , Mao Jing , Chan Ting‐Shan , Wang Qingyuan , Zhang Liang 
Published: January 2023

AbstractMost reported catalysts for lithium‐sulfur battery can work for only one of the multiple elementary reactions, thereby resulting in the gradual enrichment of unconverted polysulfides at the catalytic centers and aggravating the shuttle effect. Herein, the concept of cascade catalysis based on a ternary heterostructure, which divides sulfur redox reactions into distinct steps by multiple catalytic centers, is proposed to realize the tandem reduction of Li2S8 to Li2S. As a proof of concept, the ternary heterostructure Na0.67Ni0.25Mn0.75O2(NNMO)‐MnS2‐Ni3S4 achieved by in situ non‐topotactic electrochemical reconstruction successfully integrates three types of active centers into one structure to achieve cascade catalysis. More specifically, NNMO acts as an adsorption mediator to effectively capture polysulfides, MnS2 functions better in catalyzing the conversion of polysulfides into Li2S4 and Ni3S4 demonstrates an enhanced catalytic effect for Li2S precipitation. This synergistic cascade catalysis originates primarily from the dynamic energy‐level matching between the metal d‐band center and the lowest unoccupied molecular orbital of the polysulfides, affording appropriate molecular orbital hybridization and facile interfacial electron transition and thus endowing favorable sulfur reduction kinetics. Eventually, the NNMO‐MnS2‐Ni3S4/S composite electrode exhibits excellent rate performance and high restraining ability toward the polysulfide shuttle under long cycling, high sulfur loading and low electrolyte conditions.
Dynamic Assembly of Cascade Enzymes by the Shape Transformation of a DNA Scaffold
Authors: Lin Peng , Dinh Huyen , Morita Yuki , Nakata Eiji , Morii Takashi 
Published: January 2023

AbstractWithin cells, the close spatial arrangement of cascade enzymes facilitates the channeling of intermediates and enhances cascade reaction efficiency. Reconfigurable DNA nanostructures, owing to their structural controllability and precise spatial addressability, are promising tools for mimicking such processes. In this study, a 3D DNA origami scaffold, with a dynamic shape transformation from its open boat form to a closed hexagonal prism induced by toehold‐mediated strand displacement, is designed to investigate the enzyme cascade reaction of xylose reductase and xylitol dehydrogenase from D‐xylose metabolic pathway. Enzymes are assembled on the DNA scaffold in its open state, which is subsequently closed by the assistance of DNA sequence‐specific closing keys. The enzyme cascade efficiency is much higher in the static encapsulated closed state than in the open state due not only to the enzyme proximity but also the environmental factors of 3D DNA structure. These results provide novel insights into controlling enzyme cascade reactions by inducing the shape transformation of DNA nanostructures and how environmental factors affect the action of multi‐enzyme complexes in the cell.
Hierarchical Topography with Tunable Micro‐ and Nanoarchitectonics for Highly Enhanced Cardiomyocyte Maturation via Multi‐Scale Mechanotransduction
Authors: Ahn Hyunah , Cho Younghak , Yun Geun‐Tae , Jung Kwang Bo , Jeong Wonji , Kim Yesol , Son Mi‐Young , Lee Eunjung , Im Sung Gap , Jung Hee‐Tae 
Published: January 2023

AbstractEnhancing cardiomyocyte (CM) maturation by topographical cues is a critical issue in cardiac tissue engineering. Thus far, single‐scale topographies with a broad range of feature shapes and dimensions have been utilized including grooves, pillars, and fibers. This study reports for the first time a hierarchical structure composed of nano‐pillars (nPs) on micro‐wrinkles (µWs) for effective maturation of CMs. Through capillary force lithography followed by a wrinkling process, vast size ranges of topographies are fabricated, and the responses of CMs are systematically investigated. Maturation of CMs on the hierarchical structures is highly enhanced compared to a single‐scale topography: cardiac differentiation of H9C2s (rat cardiomyocytes) on the hierarchical topography is ≈ 2.8 and ≈ 1.9 times higher than those consisting of single‐scale µWs and nPs. Both nPs and µWs have important roles in cardiac maturation, and the aspect ratio (height/diameter) of the nPs and the wavelength of the µWs are important in CM maturation. This enhancement is caused by strong focal adhesion and nucleus mediated mechanotransduction of CMs from the confinement effects of the different wavelengths of µWs and the cellular membrane protrusion on the nPs. This study demonstrates how a large family of hierarchical structures is used for cardiac maturation.
Metasurface‐Enabled Holographic Lithography for Impact‐Absorbing Nanoarchitected Sheets
Authors: Kagias Matias , Lee Seola , Friedman Andrew C. , Zheng Tianzhe , Veysset David , Faraon Andrei , Greer Julia R. 
Published: January 2023

AbstractNanoarchitected materials represent a class of structural meta‐materials that utilze nanoscale features to achieve unconventional material properties such as ultralow density and high energy absorption. A dearth of fabrication methods capable of producing architected materials with sub‐micrometer resolution over large areas in a scalable manner exists. A fabrication technique is presented that employs holographic patterns generated by laser exposure of phase metasurface masks in negative‐tone photoresists to produce 30–40 µm‐thick nanoarchitected sheets with 2.1 × 2.4 cm2 lateral dimensions and ≈500 nm‐wide struts organized in layered 3D brick‐and‐mortar‐like patterns to result in ≈50–70% porosity. Nanoindentation arrays over the entire sample area reveal the out‐of‐plane elastic modulus to vary between 300 MPa and 4 GPa, with irrecoverable post‐elastic material deformation commencing via individual nanostrut buckling, densification within layers, shearing along perturbation perimeter, and tensile cracking. Laser induced particle impact tests (LIPIT) indicate specific inelastic energy dissipation of 0.51–2.61 MJ kg−1, which is comparable to other high impact energy absorbing composites and nanomaterials, such as Kevlar/poly(vinyl butyral) (PVB) composite, polystyrene, and pyrolized carbon nanolattices with 23% relative density. These results demonstrate that holographic lithography offers a promising platform for scalable manufacturing of nanoarchitected materials with impact resistant capabilities.
Conjugated Coordination Polymer as a New Platform for Efficient and Selective Electroreduction of Nitrate into Ammonia
Authors: Zhang Yizhe , Zheng Hui , Zhou Kangjie , Ye Jinyu , Chu Kaibin , Zhou Zhiyou , Zhang Longsheng , Liu Tianxi 
Published: January 2023

AbstractElectroreduction of nitrate into ammonia (NRA) provides a sustainable route to convert the widespread nitrate pollutants into high‐value‐added products under ambient conditions, which unfortunately suffers from unsatisfactory selectivity due to the competitive hydrogen evolution reaction (HER). Previous strategies of modifying the metal sites of catalysts often met a dilemma for simultaneously promoting activity and selectivity toward NRA. Here, a general strategy is reported to enable an efficient and selective NRA process through coordination modulation of single‐atom catalysts to tailor the local proton concentration at the catalyst surface. By contrast, two analogous Ni‐single‐atom enriched conjugated coordination polymers (NiO4‐CCP and NiN4‐CCP) with different coordination motifs are investigated for the proof‐of‐concept study. The NiO4‐CCP catalyst exhibits an ammonia yield rate as high as 1.83 mmol h−1 mg−1 with a Faradaic efficiency of 94.7% under a current density of 125 mA cm−2, outperforming the NiN4‐CCP catalyst. These experimental and theoretical studies both suggest that the strategy of coordination modulation can not only accelerate the NRA by adjusting the adsorption energies of NRA intermediates on the metal sites but also inhibit the HER through regulating the proton migration with contributions from the metal‐hydrated cations adsorbed at the catalyst surface, thus achieving simultaneous enhancement of NRA selectivity and activity.
Lasing by Template‐Assisted Self‐Assembled Quantum Dots
Authors: Aftenieva Olha , Sudzius Markas , Prudnikau Anatol , Adnan Mohammad , Sarkar Swagato , Lesnyak Vladimir , Leo Karl , Fery Andreas , König Tobias A.F. 
Published: January 2023

AbstractMiniaturized laser sources with low threshold power are required for integrated photonic devices. Photostable core/shell nanocrystals are well suited as gain material and their laser properties can be exploited by direct patterning as distributed feedback (DFB) lasers. Here, the 2nd‐order DFB resonators tuned to the photoluminescence wavelength of the QDs are used. Soft lithography based on template‐assisted colloidal self‐assembly enables pattern resolution in the subwavelength range. Combined with the directional Langmuir–Blodgett arrangement, control of the waveguide layer thickness is further achieved. It is shown that a lasing threshold of 5.5 mJ cm−2 is reached by a direct printing method, which can be further reduced by a factor of ten (0.6 mJ cm−2) at an optimal waveguide thickness. Moreover, it is discussed how one can adjust the DFB geometries to any working wavelength. This colloidal approach offers prospects for applications in bioimaging, biomedical sensing, anti‐counterfeiting, or displays.
Light‐Triggered and Polarity‐Switchable Homojunctions for Optoelectronic Logic Devices
Authors: Li Kangjie , He Ting , Guo Nan , Xu Tengfei , Fu Xiao , Wang Fang , Xu Hangyu , Li Guohua , Liu Shuning , Deng Ke , Xiao Yunlong , Miao Jinshui , Hu Weida 
Published: January 2023

AbstractSemiconductor homojunctions based on 2D materials are promising candidates for optoelectronic logic devices due to their excellent electrostatic tunability and photoelectric characteristic. However, to reach programmable logic functions, the 2D homojunctions usually suffer from compulsory combinations of electrical and optical inputs. Here, a light‐triggered and polarity‐switchable homojunction made from the vertically stacked MoTe2/CuInP2S6/Au layers in a dual‐floating gate transistor configuration, is demonstrated. Utilizing the band alignment between MoTe2 and CuInP2S6, the photocarriers in MoTe2 can be excited to Au layer across the insulating CuInP2S6 efficiently, serving as floating gate to modulate the polarity of the MoTe2 homojunctions which produce photocurrents simultaneously in photovoltaic mode. A logic gate XOR is achieved in one single device without the need for any applied voltage. Moreover, the devices exhibit both anomalous photoresponse and optical memory behaviors in photoconductive mode. The results provide a potential route for the development of optoelectronic logic devices with fully light‐actuated sensing capability.
Photoluminescence Enhancement for Efficient Mixed‐Halide Blue Perovskite Light‐Emitting Diodes
Authors: Chen Zhan , Liu Xiao‐Ke , Wang Heyong , Liu Xianjie , Hou Lintao , Gao Feng 
Published: January 2023

AbstractThe development of highly efficient blue perovskite light‐emitting diodes (PeLEDs) remains a big challenge, requiring more fundamental investigations. In this work, significant photoluminescence enhancement in mixed halide blue perovskite films is demonstrated by using a molecule, benzylphosphonic acid, which eventually doubles the external quantum efficiency to 6.3% in sky‐blue PeLEDs. The photoluminescence enhancement is achieved by forming an oxide‐bonded perovskite surface at grain boundaries and suppressing electron–phonon interaction, which enhances the radiative recombination rate and reduces the nonradiative recombination rate, respectively. Moreover, severe thermal quenching is observed in the blue perovskite films, which can be explained by a two‐step mechanism involving exciton dissociation and electron–phonon interaction. The results suggest that enhancing the radiative recombination rate and reducing the electron–phonon interaction‐induced nonradiative recombination rate are crucial for achieving blue perovskite films with strong emission at or above room temperature.
Deep Eutectic Solvents Synthesis of A2Sb(C2O4)Cl3 (A = NH4, K, Rb) with Superior Optical Performance
Authors: Zhang Die , Wang Qiang , Luo Han , Cao Liling , Dong Xuehua , Huang Ling , Gao Daojiang , Zou Guohong 
Published: January 2023

AbstractDeep eutectic solvents (DESs), which are considered as a new kind of green solvents, have been adopted for the synthesis of diverse functional materials. Herein, DESs synthesis is used to solve the problem of easy hydrolysis and oxidation of the emerging optical functional groups Sb3+ cations, producing three novel antimony chloride oxalates named A2Sb(C2O4)Cl3 (A = NH4, K, Rb). The three title compounds feature noncentrosymmetric structures consisted of [Sb(C2O4)Cl3]2– anionic clusters, which induce excellent linear and nonlinear optical properties of them. Particularly, Rb2Sb(C2O4)Cl3 exhibits a strong nonlinear optical response that is 2.1 times that of KH2PO4, as well as large calculated birefringence of 0.22@546 nm, indicating that antimony oxalates are promising optical materials. This work affords an effective strategy to settle the difficulties in crystallization of the materials including cations with low oxidation state and easy hydrolysis.
A Facile yet Versatile Strategy to Construct Liquid Hybrid Energy‐Saving Windows for Strong Solar Modulation
Authors: Li Jichang , Gu Pengyu , Pan Hongyu , Qiao Zhiyuan , Wang Jianfeng , Cao Yanxia , Wang Wanjie , Yang Yanyu 
Published: January 2023

AbstractSmart windows with light management and indoor solar heating modulation capacities are of paramount importance for building energy conservation. Thermochromic poly(N‐isopropylacrylamide) (PNIPAm) hydrogel smart windows exhibit advantages of the relatively suitable transition temperature of 32 °C, high cost‐effective and automatic passive sunlight regulation, but sustain slow response rate and unsatisfactory solar modulation efficiency. Herein, a strategy of one‐step copolymerization of NIPAm and different olefine acids (OA) using reverse atom transfer radical polymerization method is developed to fabricate various chain/microparticle hybrids (CMH) for liquid energy‐saving windows. Synergetic mechanisms of thermal‐induced dissolution and aggregation of linear polymer chains integrated with water capture and release of microgel particles contribute to tunable light‐scattering behaviors and adaptive solar modulation. Without any post‐treatment, the as‐prepared poly(N‐isopropylacrylamide‐co‐acrylic acid) (P(NIPAm‐co‐AA))‐based CMH suspension is injected into sandwich glass to construct energy‐saving windows, which exhibits appreciated near‐room‐temperature transition (26.7 °C), rapid response (5 s), extraordinary luminous transmittance (91.5%), and solar modulation efficiency (85.8%), resulting in a substantial decline of indoor temperature of 24.5 °C in simulation experiment. Combining the versatile strategy with flexible adjustment on transition temperature, multifarious P(NIPAm‐co‐OA)‐based CMH windows with eminent light management capacity are obtained. This work will powerfully promote the development and renovation of energy‐efficient windows.
Ein praktikabler und robuster zwitterionischer kooperativer Lewis‐Säure‐/Acetat‐/Benzimidazolium‐Katalysator für direkte 1,4‐Additionen
Authors: Hans Andreas C. , Becker Patrick M. , Haußmann Johanna , Suhr Simon , Wanner Daniel M. , Lederer Vera , Willig Felix , Frey Wolfgang , Sarkar Biprajit , Kästner Johannes , Peters René 
Published: January 2023

AbstractEin Katalysatortyp wird vorgestellt, der eine außergewöhnliche Effizienz bei direkten 1,4‐Additionen ermöglicht. Der Katalysator ist eine zwitterionische Einheit, in der Acetat an CuII bindet, das formal negativ geladen ist und als Gegenion für eine Benzimidazolium‐Einheit dient. Alle 3 Funktionalitäten sind an der katalytischen Aktivierung beteiligt. Für Maleimide wurde die Produktivität im Vergleich zur Literatur um einen Faktor >300 gesteigert (Umsatzzahlen bis zu 6700). Eine hohe Stereoselektivität und Produktivität wurde auch für ein breites Spektrum anderer Michael‐Akzeptoren erreicht. Der polyfunktionelle Katalysator ist in nur 4 Stufen ausgehend von N−Ph‐Benzimidazol mit einer Gesamtausbeute von 96 % zugänglich und stabil während der Katalyse. Dies ermöglichte die mehrfache Wiederverwendung des gleichen Katalysators mit nahezu konstanter Effizienz. Mechanistische Studien, insbesondere durch DFT, liefern ein detailliertes Bild der Funktionsweise des Katalysators. Die Benzimidazolium‐Einheit stabilisiert das koordinierte Enolat‐Nucleophil und verhindert, dass Acetat/Essigsäure vom Katalysator dissoziieren.
Enantioselective N‐Heterocyclic Carbene Catalyzed α‐Oxidative Coupling of Enals with Carboxylic Acids Using an Iodine(III) Reagent
Authors: Xu Yuan‐Yuan , Gao Zhong‐Hua , Li Cao‐Bo , Ye Song 
Published: January 2023

AbstractThe enantioselective α‐oxidative coupling of enals with carboxylic acids was developed via the umpolung of an NHC‐bound enolate with an iodine(III) reagent. The corresponding α‐acyloxyl‐β,γ‐unsaturated esters were afforded in good yields, with high regio‐ and enantioselectivities. The key step of the reaction involves the formation of enol iodine(III) intermediate from the enolate with iodosobenzene, which changes the polarity of α‐carbon of the enal from nucleophilic to electrophilic, and thus facilitates the subsequent addition of carboxylate.
Electron‐Rich Bi Nanosheets Promote CO2⋅− Formation for High‐Performance and pH‐Universal Electrocatalytic CO2 Reduction
Authors: Li Zaiqi , Sun Bin , Xiao Difei , Wang Zeyan , Liu Yuanyuan , Zheng Zhaoke , Wang Peng , Dai Ying , Cheng Hefeng , Huang Baibiao 
Published: January 2023

AbstractElectrochemical CO2 reduction reaction (CO2RR) to chemical fuels such as formate offers a promising pathway to carbon‐neutral future, but its practical application is largely inhibited by the lack of effective activation of CO2 molecules and pH‐universal feasibility. Here, we report an electronic structure manipulation strategy to electron‐rich Bi nanosheets, where electrons transfer from Cu donor to Bi acceptor in bimetallic Cu−Bi, enabling CO2RR towards formate with concurrent high activity, selectivity and stability in pH‐universal (acidic, neutral and alkaline) electrolytes. Combined in situ Raman spectra and computational calculations unravel that electron‐rich Bi promotes CO2⋅− formation to activate CO2 molecules, and enhance the adsorption strength of *OCHO intermediate with an up‐shifted p‐band center, thus leading to its superior activity and selectivity of formate. Further integration of the robust electron‐rich Bi nanosheets into III–V‐based photovoltaic solar cell results in an unassisted artificial leaf with a high solar‐to‐formate (STF) efficiency of 13.7 %.
In Situ Polymerized 1,3‐Dioxolane Electrolyte for Integrated Solid‐State Lithium Batteries
Authors: Mi Ye Qian , Deng Wei , He Chaohui , Eksik Osman , Zheng Yi Ping , Yao De Kun , Liu Xian Bin , Yin Yan Hong , Li Ye Sheng , Xia Bao Yu , Wu Zi Ping 
Published: January 2023

AbstractSolid‐state lithium batteries are promising and safe energy storage devices for mobile electronics and electric vehicles. In this work, we report a facile in situ polymerization of 1,3‐dioxolane electrolytes to fabricate integrated solid‐state lithium batteries. The in situ polymerization and formation of solid‐state dioxolane electrolytes on interconnected carbon nanotubes (CNTs) and active materials is the key to realizing a high‐performance battery with excellent interfacial contact among CNTs, active materials and electrolytes. Therefore, the electrodes could be tightly integrated into batteries through the CNTs and electrolyte. Electrons/ions enable full access to active materials in the whole electrode. Electrodes with a low resistance of 4.5 Ω □−1 and high lithium‐ion diffusion efficiency of 2.5×10−11 cm2 s−1 can significantly improve the electrochemical kinetics. Subsequently, the batteries demonstrated high energy density, amazing charge/discharge rate and long cycle life.
Integrated Micro Space Electrostatic Field in Aqueous Zn‐Ion Battery: Scalable Electrospray Fabrication of Porous Crystalline Anode Coating
Authors: Guo Can , Zhou Jie , Chen Yuting , Zhuang Huifen , Li Jie , Huang Jianlin , Zhang Yuluan , Chen Yifa , Li Shun‐Li , Lan Ya‐Qian 
Published: January 2023

AbstractThe inhomogeneous consumption of anions and direct contact between electrolyte and anode during the Zn‐deposition process generate Zn‐dendrites and side reactions that can aggravate the space‐charge effect to hinder the practical implementation of zinc‐metal batteries (ZMBs). Herein, electrospray has been applied for the scalable fabrication (>10 000 cm2 in a batch‐experiment) of hetero‐metallic cluster covalent‐organic‐frameworks (MCOF‐Ti6Cu3) nanosheet‐coating (MNC) with integrated micro space electrostatic field for ZMBs anode protection. The MNC@Zn symmetric cell presents ultralow overpotential (≈72.8 mV) over 10 000 cycles at 1 mAh cm−2 with 20 mA cm−2, which is superior to bare Zn and state‐of‐the‐art porous crystalline materials. Theoretical calculations reveal that MNC with integrated micro space electrostatic field can facilitate the deposition‐kinetic and homogenize the electric field of anode to significantly promote the lifespan of ZMBs.
Embedding Lanthanide Organic Polyhedra into Mesoporous Silica Nanoparticles for the Photocatalytic Degradation of Organic Dyes
Authors: Lin Xiao‐Shan , Liao Wen‐Hua , Zhou Li‐Peng , Sun Qing‐Fu 
Published: January 2023

AbstractOrganic pollutants cause severe environmental problems because of their damage to human health and ecological systems. Photocatalytic degradation of persistent organic pollutants is of great importance to address these hazards. Herein, we report a lanthanide organic polyhedra‐based hybrid material Gd8L12⊂MSN with the capability of photocatalytic dye degradation. Gd8L12⊂MSN was prepared by embedding the Gd8L12 complex into mesoporous silica nanoparticles (MSNs) using a “ship‐in‐a‐bottle” strategy. Photocurrent response tests revealed that this hybrid material is a potential semiconductor and could generate a rapid and steady photocurrent upon irradiation. Further dye degradation experiments indicated that it could photocatalyze the degradation of familiar organic dyes. Thereinto, compared with the critical Gd8L12 complex, the hybrid material exhibited an acceleration of 2.4 times and realized reusability. This not only offers a potential advanced photocatalyst for degrading persistent organic pollutants, but also provides a strategy for the application of supramolecular materials in environmental science.