bluuebunny/crossref_metadata_2025_split huggingface dataset:
Investigating the Role of Fe‐Pyrrolic N4 Configuration in the Oxygen Reduction Reaction via Covalently Bound Porphyrin Functionalized Carbon Nanotubes
Authors: Li Qi , Xu Yue , Pedersen Angus , Wang Mengnan , Zhang Mi , Feng Jingyu , Luo Hui , Titirici Maria‐Magdalena , Jones Christopher R. 
Published: January 2024

AbstractAtomically dispersed iron–nitrogen–carbon catalysts are promised, low‐cost, and high‐performance electrocatalysts for the Oxygen Reduction Reaction (ORR) in fuel cells. However, most Fe–N–C materials are produced via pyrolysis at a high temperature and it is difficult to characterise the precise Fe–N configurations. This can lead to confusion surrounding the best chemical and coordination environment for Fe and understanding the subsequent ORR mechanisms. In this work, Fe porphyrin is used to produce a specific Fe–N environment, therefore allowing the role and activity of this environment to be studied. Carbon nanotubes (CNTs) are covalently functionalized with iron 5,10,15,20‐triphenylporphyrin (FeTPP) motifs via aryl diazonium methodology, enabling the exact role of only the Fe‐Pyrrolic N4 configuration of FeTPP in ORR to be studied and better understood. Upon covalent functionalization, a high electrochemical active site density of 1.12 × 1015 sites cm−2, approximately six‐fold more than that of noncovalently functionalized samples with 12.7% electrochemical active site. The heightened active site density and superior electrochemical active site utilization (12.7%) lead to the more favorable 4‐electron pathway for the ORR. Furthermore, a preliminary discussion regarding the selectivity of the ORR pathway is initiated.
Hierarchically Structured Hydrogel Composites with Ultra‐High Conductivity for Soft Electronics
Authors: Wang Zhuang , Xu Xiaoyun , Tan Renjie , Zhang Shuai , Zhang Ke , Hu Jinlian 
Published: January 2024

AbstractConductive hydrogels possessing high conductivity, stretchability, and biocompatibility are promising materials for underwater devices and bioelectronics. However, typical hydrogels often exhibit low electrical conductivity, which is insufficient for applications requiring high electronic communication. A common approach to increase hydrogel conductivity is to introduce conductive fillers; however, this usually implies a partial sacrifice of stretchability, biocompatibility, and water content. In addition, the electrical properties of hydrogels tend to be unstable due to rehydration in aqueous environments. In this study, a conductive hydrogel composite is fabricated from silver nanowires (AgNWs) and poly(vinyl alcohol) (PVA) employing a synergistic method of freezing and salting‐out treatments. This combined method constructs a hierarchical hydrogel structure and increases the local concentration of AgNWs by inducing continuous phase separation. The resultant conductive hydrogel composites exhibit ultra‐high electrical conductivity (≈1739 S cm−1) and electrical stability in aqueous environments while maintaining high water content (≈87%), stretchability (≈480%), and excellent biocompatibility. To illustrate the capabilities of the conductive hydrogel composites, they are applied to bionic sharks, underwater soft circuitry, and electrocardiogram electrodes.
On‐Chip Direction‐Multiplexed Meta‐Optics for High‐Capacity 3D Holography
Authors: Li Zhe , Liu Yang , Zhang Chen , Qiao Yuqi , Deng Rong , Shi Yangyang , Li Zhongyang 
Published: January 2024

AbstractMetasurfaces are recently incorporated with waveguides for in‐plane wave manipulation and extraction, enhancing the capability and design flexibility of integrated photonic devices. However, the unique guided‐wave‐driven scheme poses challenges in achieving multiplexed functionality for on‐chip integrated metasurfaces. Here, an on‐chip direction‐multiplexing strategy is proposed and demonstrated for high‐capacity 3D multiplane projection in free space. By exploring and utilizing the direction‐dependence of the guided‐wave‐driven detour phase manipulation, a 16‐channel on‐chip holography is realized with different images independently encoded at distinct z planes for all four illumination directions. Moreover, the on‐chip full‐space 3D holography is demonstrated by exploiting the conjugated relation of the optical responses driven by the opposite on‐chip illuminations, enabling observation of a total of 16 holographic images in full‐space. The demonstrated on‐chip direction‐multiplexed holography exhibits low background noise or crosstalk and offers high information density and quality, which shows promise for practical applications in data storage, 3D display, and virtual/augmented reality.
Simultaneously Generating Redox Mediator and Hybrid SEI for Lithium–oxygen Batteries by Lewis Acid Catalyzed Ring‐opening Reaction of Organic Iodine
Authors: Wang Qian‐Yan , Zheng Meng‐Ting , Gao Meng‐Lin , Liao Ya‐Ling , Zhang Xiao‐Ping , Fan Cong , Chen Wei‐Rong , Lu Jun 
Published: January 2024

AbstractFacing high overpotential, severe Li corrosion and degradation of electrolytes caused by the reactive oxygen species, the development of lithium–oxygen batteries is seriously limited. Although the iodine species have been considered to be effective redox mediators (RMs) for lowering the charging overpotential, the shuttling of oxidized I3− may attack the Li metal anode, compromising the number of RMs, cycling stability and energy efficiency. Here the intend to introduce 3‐Iodooxetane (C3H5OI, IOD) into TEGDME‐based electrolyte to form a protective SEI layer on the Li surface for defending against the attack of I3−. However, the iodine in IOD is found difficult to dissociate. To solve this problem, hard Lewis acid, aluminum trichloride (AlCl3) is proposed as the catalytic agent for dissociating the I− and triggering the ring‐opening reaction of the detached C3H5O+ ions. The former can dissociate redox couple I3−/I− while the latter can form oligomers or polymers under the attack of a nucleophile. Meanwhile, AlCl3 can form Al2O3 and LiCl inorganic species. Taking together, the introduction of IOD and AlCl3 into electrolytes can effectively derive reduced overpotential and in situ SEI layers consisting of flexible organics and rigid inorganics, endowing lithium–oxygen batteries over 150 cycles with significantly enhanced stability and lifespan.
Flexible Film Constructed by Asymmetrically‐Coordinated La1N4Cl1 Moieties on Interconnected Nitrogen‐Doped Graphene Nanocages for High‐Efficiency Electromagnetic Wave Absorption
Authors: Shi Yanan , Ma Zheng , Zhang Xiao , Yan Feng , Zhao Yingying , Zhu Chunling , Chen Yujin 
Published: January 2024

AbstractThe microenvironments of metal single‐atoms (SAs) have important effects on their physicochemical properties. However, the understanding of the relationship between the coordination configuration of SAs and their properties is insufficient. Here, a sacrificing template strategy is developed to anchor La‐SAs on interconnected graphene nanocages (La‐N‐Cl/GNC), where La‐SAs are located above the graphene plane and one La atom coordinated with four N atoms in the graphene plane and with one Cl atom along the axial direction. Theoretical calculations demonstrated that asymmetrically La‐SAs are more conducive to breaking local charge symmetry. Consequently, additional electrical dipoles along the axial direction are generated, leading to unprecedented dipolar polarization loss and strong electromagnetic wave absorption properties. Moreover, the film constructed by asymmetrically‐coordinated La‐N‐Cl/GNC with a mass density of 0.084 g cm−3 exhibits superior flexibility, excellent mechanical strength, and moderate thermal insulation properties, guaranteeing its practical applications in harsh environments. These findings not only shed light on the relationships between asymmetrically coordinated SAs and their dielectric properties at the atomic level but also provide an efficient method for preparing multifunctional films.
Defect Strategy‐Regulated MoSe2‐Modified Self‐Supporting Graphene Aerogels Serving as Both Cathode and Interlayer of Lithium‐Sulfur Batteries
Authors: Zhai Shengjun , Ye Zimujun , Liu Ran , Xu Hongyuan , Li Changwen , Liu Weiyi , Wang Xianbao , Mei Tao 
Published: January 2024

AbstractThe severe shuttle effect and the sluggish redox reaction kinetics are the two most urgent issues with lithium‐sulfur batteries (LSBs). In this work, Se vacancy‐rich molybdenum selenide‐modified graphene aerogels are designed to serve as both cathode host (MoSe2‐x@GA/S) and freestanding interlayers (MoSe2‐x@GA) for LSBs. The graphene network‐supported binder‐free sulfur host maximizes electron conductivity/Li+ migration rate and alleviates bulk expansion. The defect‐rich MoSe2‐x with sulfiphilic‐lithiophilic properties accelerates the nucleation and dissociation of Li2S, while the insertion of a bifunctional interlayer not only facilitates the adsorption and conversion of polysulfides but also regulates the uniform lithium deposition and inhibit the growth of lithium dendrites. As a result, the assembled MoSe2‐x@GA/S+interlayer electrode obtains good feedback in terms of capacity enhancement and cycling stability, possessing a high initial discharge capacity of 1256.9 mA h g−1 at 0.2 C and a slow decay ratio of 0.024% per cycle at a high current density of 1 C after 1000 long‐term cycling, and achieve high specific capacity (720.6 mA h g−1) at high sulfur loading (4.8 mg cm−2) and lean electrolyte (5.5 µL mg−1) conditions. This insightful work contributes new ideas for the design of binder‐free sulfur host and the application of defective electrocatalytic engineering.
Electrochromic Reflective Displays Based on In Situ Photo‐Crosslinked PEDOT:PSS Patterns
Authors: Yang Guojian , Fan Junpeng , Zhang Kai , Gu Chang , Li Jing , Kang Kai , Xiang Chaoyu , Qian Lei , Zhang Ting 
Published: January 2024

AbstractElectrochromic (EC) technology is regarded as one of the most promising candidates for next‐generation reflective displays, owing to its advantages of outstanding color adjustability, low energy consumption, vivid color, and flexibility, etc. However, current EC reflective displays are seriously restricted by the complicated and expensive patterned methods. Herein, a facile and low‐cost route is developed to achieve the EC reflective displays, which is fabricated based on the combination of an easily‐obtained EC material of poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) and an efficient photo‐crosslinked additive (2,4‐hexadiyne‐1,6‐diol, HDDO). The micrometer‐scale patterns (<50 µm) can be achieved by the in situ photo‐crosslinked process. As‐prepared EC devices show great performances containing fast response (<0.5 s), good reversibility (>10 000 cycles) and high coloration efficiency (274.75 cm2 C−1). More importantly, the applications in the EC logo, QR code, and price tag are demonstrated successfully. Overall, the current exploration suggests an efficient, low‐cost, and facile method to produce patterned EC devices with high performance, which can undoubtedly promote the further development and application of EC reflective displays.
Activation‐Induced Senescent Cell Death based on Chiral CoHAu Nanoassemblies with Enantioselective Cascade‐Catalytic Ability
Authors: Li Si , Wang Fang , Xing Xinhe , Yue Xiaoyong , Sun Shan , Lin Hengwei , Xu Chuanlai 
Published: January 2024

AbstractChirality is common in nature, which determines the high enantioselectivity of living systems. Selecting suitable chiral configurations is of great meaning for nanostructures to function better in biological systems. In this study, chiral Co3O4‐H2TPPS‐Au (CoHAu) nanoassemblies are constructed to accelerate the production ∙OH by consuming D‐glucose (D‐Glu, widely spread in nature) based on their outstanding enantioselective cascade‐catalytic abilities. In particular, D‐CoHAu nanoassemblies are more effective in the catalytic conversion of D‐Glu than L‐CoHAu nanoassemblies. This phenomenon is due to the stronger binding affinity of D‐CoHAu nanoassemblies indicated by the lower Km value. Moreover, D‐CoHAu nanoassemblies display excellent consumption‐ability of D‐Glu and production of ∙OH in living cells, which can eliminate senescent cells effectively based on their intracellular enantioselective cascade‐catalysis. This research establishes the foundation for bio‐mimicking nanostructures with unique functionalities to regulate abnormal biological activities better.
Electroluminescence, Mechanoluminescence, and Triboelectric from Superior Multimode Systems Based on Flexible Hydrogels for Human Motion Sensing
Authors: Yu Yongjie , Xu Haibo , Song Enhai , Peng Dengfeng , Han Keyu , Xu Shiqing , Bai Gongxun 
Published: January 2024

AbstractFlexible sensors have attracted extensive research interest due to their great application potential in biodetection, flexible display, and wearable devices. However, they still have a lot of room for improvement in terms of luminous color, flexibility, and self‐powered systems. A wearable, antifreeze, and discoloration sensing system based on electroluminescence, mechanoluminescence, and tribo‐power generation is developed in this paper. Triboelectric nanogenerator systems can harvest biomechanical energy from hand clapping and knee/elbow bending to generate real‐time electrical signals. The use of dielectric materials reduces the initial voltage and frequency of light‐emitting devices, enabling them to be driven by Triboelectric nanogenerators. At the same time, the device can produce red, blue, white, and other multicolor light. In addition, the system can produce an optical signal output due to external mechanical stimulation. As a result, the sensor system is simple to manufacture and unique to operate, proving its potential applications in areas such as cold‐resistant displays, wearable optoelectronics, soft robotics, and electronic skin.
High‐performance Self‐powered Ultraviolet‐visible‐near infrared Broadband Photodetectors Based on Sb2Se3/TiO2 Heterojunctions and Multifunctional Applications
Authors: Gao Songyao , Xu Jianping , Shi Shaobo , Chen Jing , Xu Jianghua , Kong Lina , Zhang Xiaosong , Li Lan 
Published: January 2024

AbstractHigh‐performance broadband photodetectors (PDs) are essential components in spectroscopy, remote sensing, imaging, and light communication applications. In this paper, Sb2Se3 nanoparticles (NPs) are uniformly deposited on TiO2 nanorod arrays (NRs) to construct a type II heterojunction with good interfacial contact by a simple two‐step potentiostatic electrochemical deposition method combined with N2 atmosphere annealing at 280, 290 and 300 °C to control the amount of Se in Sb2Se3. A good interfacial contact between Sb2Se3 and TiO2 is conducive to the separation and transport of photogenerated carriers. Sb2Se3/TiO2 PDs exhibit excellent self‐powered photoresponse in a broad spectral range from ultraviolet‐visible‐near infrared (UV‐VIS‐NIR) due to the combined effects of high light absorption, low defect density, and more suitable band alignment. The optimal parameters with a responsivity of 13.48 A W−1, detectivity of 7.9 × 1011 Jones, and response time of 18/20 µs are demonstrated for the PDs annealed at 290 °C. The excellent performance broadband Sb2Se3/TiO2 PDs are used to construct the application models in the light communication for light encryption and flaw detection. This work opens up a new strategy for Sb2Se3/TiO2 PDs in multifunctional applications.
Deep Learning Design for Multiwavelength Infrared Image Sensors Based on Dielectric Freeform Metasurface
Authors: Xiong Bo , Xu Yihao , Li Wenwen , Ma Wei , Chu Tao , Liu Yongmin 
Published: January 2024

AbstractNear‐infrared multispectral imaging technology enhances target detection and recognition by distinguishing the spectral characteristics of various targets. However, traditional imaging systems heavily rely on complex optical filter designs that are often bulky and mechanically unstable, posing significant challenges for miniaturization and integration challenging. In this study, a freeform dielectric metasurface with the wavelength‐multiplexing focusing effect based on a deep learning model is designed, which can separate the mixed near‐infrared light into distinct wavelengths. To effectively modulate the complex amplitude of the transmitted light at three distinct near‐infrared wavelengths (1150, 1350, and 1550 nm), high‐index silicon freeform nanostructures supporting rich resonant modes are proposed. An inverse design model based on deep learning is utilized to generate individual freeform nanostructures pixel by pixel, satisfying the complex amplitude requirement for a multiplexed metalens design. Both the simulated and experimental results show that the wavelength‐multiplexing effect of the devices is in good agreement with the target with negligible crosstalk. Finally, a metasurface is employed to realize near‐infrared multispectral imaging, which allows for the distinct detection and decoding of images at the three target wavelengths. The proposed technology has a wide range of applications in clinical medicine, biological tissue imaging, and deep‐space exploration.
Vertical Van Der Waals Epitaxy of p‐MoxRe1‐Xs2 on GaN for Ultrahigh Detectivity Uv–vis–NIR Photodetector
Authors: Jiang Zhongwei , Zhou Jie , Li Bo , Ma Zhengweng , Huang Zheng , Yang Yongkai , Zhang Yating , Huang Yeying , Zhang Huile , Fan Kangkai , Li Yu , Liu Xinke 
Published: January 2024

Abstractvan der Waals (vdW) heterogeneous integration and doping engineering have emerged as crucial factors in advancing the development of functional device systems. This work presents a fully vertical 2D/3D vdW stacking p‐MoxRe1‐xS2/GaN (x = 0.10 ± 0.02) heterojunction photodetector, integrating multiple strategies for enhanced performance, such as mixed‐dimensional stacking, p‐type doping, vertical device design, and type‐II band alignment. By integrating horizontal, vertical, and quasi‐vertical devices on a Free‐standing (FS)‐GaN substrate, the vertical p‐MoxRe1‐xS2/GaN device demonstrates superior performance, including high Ilight/Idark ratio (1.48 × 106), large Responsivity (888.69 AW−1), high specific detectivity (D*) (6.13 × 1014 Jones), and fast response speed (rise/decay time of 181 ms/259 ms). Moreover, the spectral response encompasses the ultraviolet (UV), visible, and near‐infrared (NIR) regions through energy band integration and bandgap modulation. This design surpasses previous devices, highlighting the potential of highly sensitive and micro‐integrated optoelectronic devices enabled by vertical vdW heterogeneous integration.
In Situ Glass Crystallization Enables Narrowband Blue Luminescence for Full‐Spectrum Lighting and Transparent Display
Authors: Li Xinyue , Feng Weigang , You Fengluan , Pang Tao , Zhu Jiwen , Lin Jidong , Fang Yongzheng , Chen Daqin 
Published: January 2024

AbstractCurrently, narrowband light‐convertor is critically urgent for preeminent color representation in lighting and display fields, however, the development of target materials still remains challenging. Herein, glass ceramic (GC) composite based on in situ glass crystallization, where the condense glass network structure acts as effective obstructors for long distance ion diffusion, is elaborately designed to inhibit activators’ multi‐sites occupation for acquiring narrowband emitting. Following this strategy, an unprecedented narrowband blue emission of Eu2+‐activators with a peak at 447 nm and full‐width of half maximum (FWHM) of ≈30 nm is developed in a new type of Sr5(PO4)3Cl (SPOCl) GC composite. The Eu2+‐activators’ hindered diffusion inside the GC composite makes preferential and limit occupation of the [Sr1O9] sites, enabling narrowband blue luminescence. Furthermore, the GC composite highlights remarkable performance in high‐power violet‐excitable full‐spectrum lighting and transparent display (TD) prototype fields, due to its high color purity (≈98.1%), photoluminescence quantum field (PLQY, ≈80.5%) and thermal stability (≈82.1%@150 °C). This work not only promotes the profound understanding of the relationship between light manipulation and glass crystallization, but also paves the way toward the implementation of high‐quality lighting and display of GC composites.
Organocatalytic Stereoselective Decarboxylative Addition of α‐Amido Malonic Acid Half Oxyesters to Isatins
Authors: Fujita Kazuki , Kumazawa Ibuki , Yokoi Jyunpei , Abe Kazuki , Takehara Tsunayoshi , Suzuki Takeyuki , Yasukawa Naoki , Nakamura Shuichi 
Published: January 2024

AbstractThe stereoselective reaction of α‐amido‐substituted malonic acid half oxyesters (α‐amido‐MAHOs) with isatins was developed. A cinchona alkaloid thiourea catalyst gave products bearing a tetrasubstituted stereogenic centre in high yields with high diastereo‐ and enantioselectivities (75–99% yield, 83:17–97:3 dr, 92:8–99:1 er). The obtained products can be converted into some chiral compounds without loss of enantiopurity. Density functional theory (DFT) calculations were conducted to clarify the origin of stereoselectivities, and suggested that the first stereogenic centre is set in the decarboxylation, the second in the protonation.
Continuous Manufacturing of Active Pharmaceutical Ingredients: Current Trends and Perspectives
Authors: Hyer Andres , Gregory Daniel , Kay Kaitlin , Le Quang , Turnage Justin , Gupton Frank , Ferri James K. 
Published: January 2024

AbstractThe pharmaceutical industry has traditionally employed batch processing as a means of synthesizing active pharmaceutical ingredients (APIs) on a commercial scale. Batch manufacturing enables API synthesis in large quantities in order to meet regulations. Yet, this strategy remains cumbersome, is labor‐intensive, and creates complex logistical networks. In recent decades, batch API processing has gradually eroded American economic competitiveness and has led to the offshoring of API manufacturing from the United States. Today it is estimated that +80% of APIs are manufactured overseas.[1] Meanwhile, disruptions from the Coronavirus Disease (SARS‐CoV‐2) have exacerbated weaknesses in the global supply chain, culminating with widespread shortages of critical life‐saving drugs.[2] These shortages have emphasized the importance of reshoring drug manufacturing to the U.S. and fostered a regulatory landscape that seeks advanced methods of API manufacturing in order to bolster America's supply chain resiliency.[3] Recently, increased attention has been directed towards continuous drug manufacturing to enable nonstop API production within modular stand‐alone flow systems. Continuous manufacturing (CM) facilitates modular automation, offers new avenues towards process intensification, and even enables in‐line analytical monitoring from raw materials to packaged products. This strategy offers better conversion, increased safety, reduced waste, and overall cost savings versus traditional batch‐style processing. The rise of advanced API manufacturing, coupled with the current regulatory landscape, offers a rare window of opportunity to convert traditional batch pharmaceutical processes into continuous, streamlined production systems to on‐shore API manufacturing and eliminate drug shortages. This review will outline the current state‐of‐the‐art in the CM of APIs and will highlight the translation of chemistry and unit operations from batch processes to modular CM systems.
Copper‐Catalyzed Diazidation of Allenes: Access to 3‐(Azidomethyl)‐2H‐Azirines
Authors: Zhang Shen‐Yuan , Hu Li‐Yan , Li Yang , Li Yuan , Luo Kai , Wu Lei 
Published: January 2024

AbstractA class of 3‐(azidomethyl)‐2H‐azirine has been obtained through a copper‐catalyzed diazidation of allenes and a subsequent azirination involving vinyl azides. A variety of functional groups in the allenes are well tolerated, providing a series of 3‐(azidomethyl)‐2H‐azirine motifs in 51%‐93% yields (26 examples).