bluuebunny/crossref_metadata_2025 huggingface dataset:
Significant Dark Current Suppression in Organic Photodetectors Using Side Chain Fluorination of Conjugated Polymer
Authors: Park Byoungwook , Jung Juhyoung , Lim Dae‐Hee , Lee Hanbee , Park Sungjun , Kyeong Minju , Ko Seo‐Jin , Eom Seung Hun , Lee Seung‐Hoon , Lee Changjin , Yoon Sung Cheol
Published: October 2021

Dark current density (Jdark) is the most important factors determining signal‐to‐noise ratio, linear dynamic range and detectivity (D*) of organic photodetectors (OPDs). However, the solution‐processed OPDs generally suffer from high Jdark under bias because the origin of Jdark still remains unclear and related to complicate factors. In this work, the effect of fluorinated alkyl side chain (FAC) of conjugated polymers (CPs) on the OPD performance is systematically investigated according to the number of fluorine atom. The OPDs, comprising the CPs with a FAC (CP‐FAC), exhibit at least two orders lower Jdark (≈3.73 × 10‐10 A cm‐2 at ‐2 V) compared to that without FAC while significantly maintaining high external quantum efficiency (≈78%). This is because the side chain fluorination leads to the formation of a more ordered molecular structure of the CPs, which reduces the trap density and energetic disorder, thus resulting in the effective suppression of Jdark and in the enhancement of charge carrier mobility. The CP‐FAC based OPD exhibits an exceptionally high D* (≈3.39 × 1013 cm Hz1/2 W‐1 at ‐2 V) and a reasonable response speed (f‐3db = ≈56.31 kHz). Furthermore, a photoplethysmography sensor comprising the CP‐FAC based OPD in a transmission mode is demonstrated.
Fabricating Tissues In Situ with the Controlled Cellular Alignments
Authors: He Chuanjiang , Liu Mengxue , Jiang Deming , Wu Jianguo , Qin Chunlian , Liang Tao , Wu Pan , Han Chunmao , Huang Liquan , Hsia K. Jimmy , Wang Ping
Published: October 2021

Tissue engineering techniques have enabled to replicate the geometrical architecture of native tissues but usually fail to reproduce their exact cellular arrangements during the fabricating process, while it is critical for manufacturing physiologically relevant tissues. To address this problem, a “sewing‐like” method of controlling cellular alignment during the fabricating process is reported here. By integrating the stretching step into the fabricating process, a static mechanical environment is created which, in turn, regulates the subsequent cellular alignment, elongation, and differentiation in the generated tissues. With this method, patterned cellular constructs can be fabricated with controlled cellular alignment. Moreover, this method shows a potent capability to fabricate physiologically relevant skeletal muscle constructs in vitro by mechanically inducing myoblast fusion and maturation. As a potential clinical application, aligned myofibers are directly fabricated onto injured muscles in vivo, which repair the damaged tissues effectively. This study shows that the “sewing‐like” method can produce engineered tissues with precise control of cellular arrangements and more clinically viable functionalities.
Extracellular Matrix‐Based Conductive Interpenetrating Network Hydrogels with Enhanced Neurovascular Regeneration Properties for Diabetic Wounds Repair
Authors: Fan Lei , Xiao Cairong , Guan Pengfei , Zou Yan , Wen Huiquan , Liu Can , Luo Yian , Tan Guoxin , Wang Qiyou , Li Yangfan , Yu Peng , Zhou Lei , Ning Chengyun
Published: October 2021

The critical effects that impair diabetic wound healing are characterized by poor vascularization and severe peripheral neuropathy. Current management strategies for diabetic wound healing are unsatisfactory, due to the paucity of neurovascular regeneration at the wound site. Importantly, conductivity in skin tissue is reported to be essential for modulating myriad biological processes especially vascular and nerve regeneration. Herein, an extracellular matrix (ECM)‐based conductive dressing is synthesized from an interpenetrating polymer network hydrogel composed of gelatin methacryloyl, oxidized chondroitin sulfate (OCS), and OCS‐polypyrrole conductive nanoparticles that can promote diabetic wound repairing by enhancing local neurovascular regeneration. The conductive hydrogels combine the advantageous features of water‐swollen hydrogels with conductive polymers (CPs) to provide tissue‐matching electrical conductivity and mechanical properties for neurovascular regeneration. In vitro and in vivo studies show that the conductive hydrogel can promote neurovascular regeneration by increasing intracellular Ca2+ concentration, which subsequently promotes phosphorylation of proteins in the phosphatidylinositol 3‐kinase (PI3K)/protein kinase B (AKT) and mitogen‐activated protein kinase kinase (MEK)/extracellular signal‐regulated kinase (ERK) pathways. Furthermore, the conductive hydrogel stimulates full‐thickness diabetic wound repair on day 14 by promoting local neurovascular regeneration and collagen deposition. These findings corroborate that the ECM‐based conductive interpenetrating network hydrogel dressing significantly promotes wound repairing due to its neurovascular regeneration properties, suggesting that they are suitable candidates for diabetic wound repair.
Atmospheric Hygroscopic Ionogels with Dynamically Stable Cooling Interfaces Enable a Durable Thermoelectric Performance Enhancement
Authors: Ni Feng , Xiao Peng , Zhang Chang , Zhou Wei , Liu Depeng , Kuo Shiao‐Wei , Chen Tao
Published: October 2021

In thermoelectric generator (TEG) systems, heat dissipation from their cold sides is an accessible, low‐cost, and effective way to increase the temperature gap for their thermoelectric performance enhancement. Although significant efforts have been dedicated mediated by hygroscopic hydrogel coolers as self‐sustained alternatives for effective heat removal, it still remains a challenge for overcoming instabilities in their cooling process. The inevitable mechanical deformation of these conventional hydrogels induced by excessive water desorption may cause a detached cooling interface with the targeted substrates, leading to undesirable cooling failure. Herein, a self‐sustained and durable evaporative cooling approach for TEG enabled by atmospheric hygroscopic ionogels (RIGs) with stable interfaces to efficiently improve its thermoelectric performance is proposed. Owing to its superior hygroscopicity, the RIGs can achieve higher heat dissipation for TEG through water evaporation than that of common commercial metal heat sinks. Moreover, its favorable adhesion enables the RIG closely interact with the TEG surface either in static or dynamic conditions for a durable thermoelectric performance enhancement. It is believed that such a self‐sustained evaporative cooling strategy based on the RIG will have great implications for the enhancement of TEG's efficiency, demonstrating a great promise in intermittent thermal‐energy utilizations.
A Schottky‐Barrier‐Free Plasmonic Semiconductor Photocatalyst for Nitrogen Fixation in a “One‐Stone‐Two‐Birds” Manner
Authors: Bai Haoyuan , Lam Shiu Hei , Yang Jianhua , Cheng Xizhe , Li Shasha , Jiang Ruibin , Shao Lei , Wang Jianfang
Published: October 2021

Plasmonic photocatalysis has received much attention owing to attractive plasmonic enhancement effects in improving the solar‐to‐chemical conversion efficiency. However, the photocatalytic efficiencies have remained low mainly due to the short carrier lifetime caused by the rapid recombination of plasmon‐generated hot charge carriers. Although plasmonic metal–semiconductor heterostructures can improve the separation of hot charge carriers, a large portion of the hot charge carriers are lost when they cross the Schottky barrier. Herein, a Schottky‐barrier‐free plasmonic semiconductor photocatalyst, MoO3−x, which allows for efficient N2 photofixation in a “one‐stone‐two‐birds” manner, is demonstrated. The oxygen vacancies in MoO3−x serve as the “stone.” They “kill two birds” by functioning as the active sites for the chemisorption of N2 molecules and inducing localized surface plasmon resonance for the generation of hot charge carriers. Benefiting from this unique strategy, plasmonic MoO3−x exhibits a remarkable photoreactivity for NH3 production up to the wavelength of 1064 nm with apparent quantum efficiencies over 1%, and a solar‐to‐ammonia conversion efficiency of 0.057% without any hole scavenger. This work shows the great potential of plasmonic semiconductors to be directly used for photocatalysis. The concept of the Schottky‐barrier‐free design will pave a new path for the rational design of efficient photocatalysts.
Magnetic and Optical Field Multi‐Assisted Li–O2 Batteries with Ultrahigh Energy Efficiency and Cycle Stability
Authors: Wang Xiao‐Xue , Guan De‐Hui , Li Fei , Li Ma‐Lin , Zheng Li‐Jun , Xu Ji‐Jing
Published: October 2021

The photoassisted lithium–oxygen (Li–O2) system has emerged as an important direction for future development by effectively reducing the large overpotential in Li–O2 batteries. However, the advancement is greatly hindered by the rapidly recombined photoexcited electrons and holes upon the discharging and charging processes. Herein, a breakthrough is made in overcoming these challenges by developing a new magnetic and optical field multi‐assisted Li–O2 battery with 3D porous NiO nanosheets on the Ni foam (NiO/FNi) as a photoelectrode. Under illumination, the photogenerated electrons and holes of the NiO/FNi photoelectrode play a key role in reducing the overpotential during discharging and charging, respectively. By introducing the external magnetic field, the Lorentz force acts oppositely on the photogenerated electrons and holes, thereby suppressing the recombination of charge carriers. The magnetic and optical field multi‐assisted Li–O2 battery achieves an ultralow charge potential of 2.73 V, a high energy efficiency of 96.7%, and good cycling stability. This external magnetic and optical field multi‐assisted technology paves a new way of developing high‐performance Li–O2 batteries and other energy storage systems.
Fiber‐Based Biopolymer Processing as a Route toward Sustainability
Authors: Li Chunmei , Wu Junqi , Shi Haoyuan , Xia Zhiyu , Sahoo Jugal Kishore , Yeo Jingjie , Kaplan David L.
Published: October 2021

Some of the most abundant biomass on earth is sequestered in fibrous biopolymers like cellulose, chitin, and silk. These types of natural materials offer unique and striking mechanical and functional features that have driven strong interest in their utility for a range of applications, while also matching environmental sustainability needs. However, these material systems are challenging to process in cost‐competitive ways to compete with synthetic plastics due to the limited options for thermal processing. This results in the dominance of solution‐based processing for fibrous biopolymers, which presents challenges for scaling, cost, and consistency in outcomes. However, new opportunities to utilize thermal processing with these types of biopolymers, as well as fibrillation approaches, can drive renewed opportunities to bridge this gap between synthetic plastic processing and fibrous biopolymers, while also holding sustainability goals as critical to long‐term successful outcomes.
A Transparent, Highly Stretchable, Solvent‐Resistant, Recyclable Multifunctional Ionogel with Underwater Self‐Healing and Adhesion for Reliable Strain Sensors
Authors: Xu Liguo , Huang Zhenkai , Deng Zhishuang , Du Zhukang , Sun Tao Lin , Guo Zi‐Hao , Yue Kan
Published: October 2021

Ionogels have gained increasing attentions as a flexible conductive material. However, it remains a big challenge to integrate multiple functions into one gel that can be widely applied in various complex scenes. Herein, a kind of multifunctional ionogels with a combination of desirable properties, including transparency, high stretchability, solvent and temperature resistance, recyclability, high conductivity, underwater self‐healing ability, and underwater adhesiveness is reported. The ionogels are prepared via one‐step photoinitiated polymerization of 2,2,2‐trifluoroethyl acrylate and acrylamide in a hydrophobic ionic liquid. The abundant noncovalent interactions including hydrogen bonding and ion–dipole interactions endow the ionogels with excellent mechanical strength, resilience, and rapid self‐healing capability at room temperature, while the fluorine‐rich polymeric matrix brings in high tolerance against water and various organic solvents, as well as tough underwater adhesion on different substrates. Wearable strain sensors based on the ionogels can sensitively detect and differentiate large body motions, such as bending of limbs, walking and jumping, as well as subtle muscle movements, such as pronunciation and pulse. It is believed that the designed ionogels will show great promises in wearable devices and ionotronics.
Guiding Drug Through Interrupted Bloodstream for Potentiated Thrombolysis by C‐Shaped Magnetic Actuation System In Vivo
Authors: Wang Longchen , Wang Jienan , Hao Junnian , Dong Ziliang , Wu Jianrong , Shen Guofeng , Ying Tao , Feng Liangzhu , Cai Xiaojun , Liu Zhuang , Zheng Yuanyi
Published: October 2021

Fast and effective thrombolysis using tissue plasminogen activator (tPA) is limited by the poor delivery efficiency of thrombolytic drugs, which is induced by an interrupted bloodstream and delayed recanalization. Existing magnetic micro/nanodrug‐loaded robots used for targeted thrombotic therapy are limited by the complexity of the clinical verification of nanodrugs and the limited space of magnetic actuation systems. Herein, a general drug delivery strategy based on mass transportation theory for thrombolysis is presented, and an open space C‐shaped magnetic actuation system with laser location and ultrasound imaging navigation for in vivo evaluation is developed. tPA can be guided through an interrupted bloodstream to the thrombi by the locomotion of magnetic nanoparticle swarms (MNSs), thereby improving the thrombolysis efficacy. Notably, this strategy is able to quickly establish a life channel to achieve time‐critical recanalization, which is typically inaccessible using native tPA. Both in vitro and in vivo thrombolysis experiments demonstrate that the thrombus lysis efficacy significantly increases after the application of the MNS under a rotating magnetic field. This study provides an anticipated C‐shaped magnetic actuation system for in vivo validation and also presents a clinically feasible drug delivery strategy for targeted thrombolytic therapy with minimal systemic tPA exposure.
Metal–Organic‐Framework‐Based Hydrogen‐Release Platform for MultieffectiveHelicobacter PyloriTargeting Therapy and Intestinal Flora Protective Capabilities
Authors: Zhang Wei , Zhou Yanan , Fan Yating , Cao Rui , Xu Yingying , Weng Zhenzhen , Ye Jing , He Cong , Zhu Yin , Wang Xiaolei
Published: October 2021

Helicobacter pylori(H. pylori) infection is the leading cause of chronic gastritis, peptic ulcer, and gastric cancer. Antibiotics, as traditional method for eliminatingH. pylori, have no targeting effect, which causes serious bacterial resistance and gut dysbacteriosis. Moreover, antibiotics can hardly address hyperactive inflammatory response or damaged gastric mucosal barrier caused byH. pyloriinfection. Here, a pH‐responsive metal–organic framework hydrogen‐generation nanoparticle (Pd(H) @ ZIF‐8) is reported, which is encapsulated with ascorbate palmitate (AP) hydrogel. Both in vitro and in vivo experiments demonstrate that the outer AP hydrogel can target and adhere to the inflammatory site through electrostatic interactions, and is then hydrolyzed by matrix metalloproteinase (MMP) enriching in inflammatory sites. The released Pd(H) @ ZIF‐8 nanoparticles are further decomposed by gastric acid to generate zinc ions (Zn2+) and hydrogen, thus effectively killingH. pylori, alleviating inflammation and restoring impaired gastric mucosa simultaneously. Unexpectedly, this metal–organic framework hydrogen‐generation platform (Pd(H) @ ZIF‐8 @ AP) also has an effect toward avoiding the imbalance of intestinal flora, which thus provides a more precise, effective, and healthy strategy for the treatment ofH. pyloriinfection.
The Quest for Stable Potassium‐Ion Battery Chemistry
Authors: Wu Xianyong , Qiu Shen , Liu Yao , Xu Yunkai , Jian Zelang , Yang Jihui , Ji Xiulei , Liu Jun
Published: October 2021

Potassium‐ion batteries (KIBs) have attracted wide interest for energy storage because of the abundance of the electrode materials involved; however, their electrochemical performances are far behind what can be achieved from lithium‐ion batteries (LIBs) or sodium‐ion batteries (SIBs). Herein, key promising electrode and electrolyte materials for potassium‐ion batteries are identified, the coupled electrochemical reactions in the cell are investigated, and the compatibility between different materials is demonstrated to play the most important role. K2Mn[Fe(CN)6] cathode can deliver a high capacity of ≈125 mAh g−1 and exceptional cycling stability over 61 000 cycles (≈9 months) if the side reactions from the anode can be prevented. Graphite is a good anode material but is subjected to degradation in traditional carbonate electrolytes. New concentrated electrolytes are developed and evaluated. A stable KIB system is demonstrated by coupling a stable K2Mn[Fe(CN)6] cathode, a prepotassiated graphite anode with a concentrated electrolyte to achieve a high energy density of ≈260 Wh kg−1 (based on the active mass of cathode and anode) and good cycling of over 1000 cycles.
2D MoS2 Heterostructures on Epitaxial and Self‐Standing Graphene for Energy Storage: From Growth Mechanism to Application
Authors: Zebardastan Negar , Bradford Jonathan , Gupta Bharati , Lipton‐Duffin Josh , MacLeod Jennifer , Pham Hong Duc , Dubal Deepak , Ostrikov Kostya , Wolff Annalena , Hu Kailong , Ito Yoshikazu , Mariani Carlo , Betti Maria Grazia , Motta Nunzio
Published: October 2021

Layered molybdenum disulphide (MoS2) crystals in combination with graphene create the opportunity for the development of heterostructures with tailored surface and structural properties for energy storage applications. Herein, 2D heterostructures are developed by growing MoS2 on epitaxial and self‐standing nanoporous graphene (NPG) using chemical vapor deposition (CVD). The effect of substrate as well as different CVD growth parameters such as temperature, amount of sulfur and MoO3 precursors, and argon flow on the growth of MoS2 is systematically investigated. Interestingly, various structures of MoS2 such as monolayer triangular islands, spirals, standing sheets, and irregular stacked multilayered MoS2 are successfully developed. The growth mechanism is proposed using different advanced characterization techniques. The formation of a continuous wetting layer with grain boundaries over the surface prior to formation of any other structures is detected. As a proof of principle, MoS2/NPG is employed for the first time as anode material in potassium ion battery. The electrode delivers a specific capacity of 389 mAh g−1 with over 98% stability after 200 cycles. The porous structures clearly facilitate the ion transport which is beneficial for the ion battery. These encouraging results open new opportunities to develop hierarchical heterostructures of 2D‐materials for next‐generation energy storage technologies.
Multi‐Object Detector YOLOv4‐Tiny Enables High‐Throughput Combinatorial and Spatially‐Resolved Sorting of Cells in Microdroplets
Authors: Howell Lewis , Anagnostidis Vasileios , Gielen Fabrice
Published: October 2021

The encapsulation of cells together with micro‐objects in monodispersed water‐in‐oil microdroplets offers a powerful means to perform quantitative biological studies within large cell populations. In such applications, accurate object detection is crucial to ensure control over the content for every compartment. In particular, the ability to rapidly count and localize objects is key to future applications in single‐cell ‐omics, cellular aggregation, and cell‐to‐cell interactions. In this paper, the authors combine the Deep Learning object detector YOLOv4‐tiny with microfluidic Image‐Activated Droplet Sorting (DL‐IADS), to perform flexible, label‐free classification, counting, and localization of multiple micro‐objects simultaneously and at high‐throughput. They trained YOLOv4‐tiny to detect SH‐SY5Y cells, polyacrylamide beads, and cellular aggregates in a single model, with a precision of 92% for cells, 98% for beads, and 81% for aggregates. They exploit this accuracy and counting ability to implement a closed‐loop feedback that enables controlled loading of microbeads via the automated adjustment of flow rates. They subsequently demonstrate the combinatorial sorting of co‐encapsulated single cells and single beads based on real‐time classification at up to 111 Hz, with enrichment factors of up to 145. Finally, they demonstrate spatially‐resolved sorts by evaluating cell‐to‐cell distances in real‐time to isolate cell doublets with high purity.
Construction of Novel Biomass‐Based Solar Evaporator with Asymmetric Dual‐Layer Structure for Water Desalination
Authors: Liu Jinhua , Xu Linqiong , Li Yongchao , Zhao Jingjing , Jia Xichen , Chao Jiabao , Lv Bizhi , Zhao Yongqing
Published: October 2021

Solar desalination technology is regarded as a low‐carbon and environment‐friendly technology to address the water crisis. The current challenge is that sunlight irradiates directly the entire water body, resulting in a low photothermal conversion efficiency. Herein, a novel photothermal compound material with dual‐layer structure for solar‐steam‐generation is developed by depositing multi‐walled carbon nanotubes (MWCNTs) and carbon black nanoparticles (CB) onto a biomass reed straw (RS) skeleton. With respect to the lower layer of the resultant generator, the porous RS skeleton with open‐cell vessel channels and closed‐cell porous basic tissues can not only supply the water to the upper layer through the capillary force, but also insulate the heat transport. Additionally, the MWCNTs‐CB hybrid photothermal composite on the upper layer with large specific surface and roughness facilitates the evaporation of water by the generated heat from the absorbed solar light. The composite generator possesses an extremely high spectral absorption of ≈99% in wet state, along with a superb evaporation rate of ≈1.45 kg m−2 h−1 and photothermal conversion efficiency of ≈87.58% under one sunlight irradiation. Thus, the deposition of MWCNTs‐CB on a renewable biomass RS skeleton develops an ideal candidate generator that hold a desirable promise for applications in seawater desalination.
Light‐Triggered Drug Release from Red Blood Cells Suppresses Arthritic Inflammation
Authors: Zywot Emilia M. , Orlova Natalia , Ding Song , Rampersad Rishi R. , Rabjohns Emily M. , Wickenheisser Victoria A. , Wang Qunzhao , Welfare Joshua G. , Haar Lauren , Eudy Amanda M. , Tarrant Teresa K. , Lawrence David S.
Published: October 2021

Arthritis is a leading cause of disability in adults, which can be intensely incapacitating. The location and intensity of the pain is both subjective and challenging to manage. Consequently, patient‐directed delivery of anti‐inflammatories is an essential component of future therapeutic strategies for the management of this disorder. The design and application of a light‐responsive red blood cell (RBC)‐conveyed dexamethasone (Dex) construct that enables targeted drug delivery upon illumination of the inflamed site is described. The red wavelength (650 nm) responsive nature of the phototherapeutic is validated using tissue phantoms mimicking the light absorbing properties of various skin types. Furthermore, photoreleased Dex has the same impact on cellular responses as conventional Dex. Murine RBCs containing the photoactivatable therapeutic display comparable circulation properties as fluorescently labeled RBCs. In addition, a single dose of light‐targeted Dex delivery is fivefold more effective in suppressing inflammation than the parent drug, delivered serially over multiple days. These results are consistent with the notion that the circulatory system be used as an on‐command drug depot, providing the means to therapeutically target diseased sites both efficiently and effectively.
Atomic Identification of Interfaces in Individual Core@shell Quantum Dots
Authors: Liu Guiju , Liang Wenshuang , Xue Xuyan , Rosei Federico , Wang Yiqian
Published: October 2021

CdSe@CdS Core@shell quantum dots (QDs) have been widely studied in recent years, due to their architecture which allows to tailor properties by controlling structure and composition. However, since CdSe and CdS have the same crystal structure, same cations, and similar lattice parameters, it is very challenging to image the interface. Herein, high‐resolution transmission electron microscopy, high‐angle annular dark‐field imaging, and energy‐dispersive X‐ray spectroscopy elemental mapping are combined to characterize the core@shell structure and identify the interface in the CdSe@CdS QDs with different CdS shell thicknesses. By examining changes in lattice spacing in an individual CdSe@CdS quantum dot, the atomic core@shell interface is identified. For thin‐shelled QDs, an ideal coherent interface forms between core and shell due to the small lattice mismatch, and the lattice spacing remains unchanged at the core and shell regions. For thick‐shelled QDs, the lattice spacing is different at the core and shell regions, while the heterostructured interface is still coherent and cannot be clearly imaged. As the shell thickness further increases, a sharp core@shell interface appears. The results define an approach to characterize the heterostructure of two materials with the same crystalline structure and cations.
Stretchable Zn‐Ion Hybrid Battery with Reconfigurable V2CTx and Ti3C2Tx MXene Electrodes as a Magnetically Actuated Soft Robot
Authors: Li Yang , Yang Haitao , Zhang Tianran , Li Shuo , Li Shuai , He Shuaiming , Chen Tianle , Lee Jim Yang , Zhao Yusheng , Chen Po‐Yen
Published: October 2021

Stretchable energy storage devices have become indispensable components toward energy autonomy for wearable electronic, implantable medical devices, and untethered soft machines. A Zn‐based battery with a neutral electrolyte could act as a competitive candidate for wearable/implantable electronics because of its intrinsic safety and high energy density. Therefore, it is highly desired to develop a synergistic combination of stretchable anodes/cathodes and neutral electrolytes for stretchable Zn‐based batteries. Herein, a scalable fabrication process is developed to produce stretchable Zn‐ion hybrid batteries composed of V2CTx MXene cathodes and zinc‐decorated Ti3C2Tx MXene anodes. To endow high stretchability to the Zn‐ion hybrid battery, both MXene‐based electrodes are fabricated with crumple‐like microtextures enabling reversible folding/unfolding behaviors to attenuate in‐plane stress while stretching. In comparison with the state‐of‐the‐art work, the as‐fabricated Zn‐ion hybrid battery features large deformability (50% strain), ultrathin device (≈170 µm), low areal weight (≈20 mg cm−2), and an ultralow self‐discharge rate (0.7 mV h−1), and demonstrates rechargeable and strain‐insensitive specific capacities of 118.5 and 103.6 mAh g−1 under 0% and 50% strains, respectively. Finally, with ultrathin and lightweight merits, the stretchable battery is further fabricated into a magnetically actuated soft robot with remote control, capable of crawling between two designated points for charging/discharging tasks.
Essentials of High Performance Water Electrolyzers – From Catalyst Layer Materials to Electrode Engineering
Authors: Pham Chuyen Van , Escalera‐López Daniel , Mayrhofer Karl , Cherevko Serhiy , Thiele Simon
Published: October 2021

Proton‐exchange membrane water electrolyzers (PEMWEs) will play a key role in future sustainable hydrogen production for mobility, households or chemical industry. Yet, the anode in PEMWEs, where the pivotal oxygen evolution reaction takes place, needs further improvement in terms of performance and cost. Both catalyst materials and electrode structure have to be optimized in order to inhibit degradation and reduce noble metal loadings. This review focuses on a holistic approach, covering all catalyst material, electrode structure, and transport layers within the framework of an overall electrode design, which not only optimizes the catalyst but also, all components of the electrode in conjunction. This review defines the goals for performance metrics of future PEMWEs in terms of power density and durability of the anode. Moreover, it summarizes manufacturing techniques and approaches that have a chance to be upscaled to meet the megawatt deployment of PEMWEs. The different aspects described jointly in this review such as novel catalyst system with higher intrinsic and structural performance or graded porous transport layers shall help to advance a next generation of electrodes.
Doctor‐Blade Casting Fabrication of Ultrathin Li Metal Electrode for High‐Energy‐Density Batteries
Authors: Du Junmou , Wang Wenyu , Wan Mintao , Wang Xiancheng , Li Guocheng , Tan Yucheng , Li Chunhao , Tu Shuibin , Sun Yongming
Published: October 2021

The employment of ultrathin Li metal electrodes with matched capacity with current cathodes and improved electrochemical stripping/plating behaviors plays a key role in the realization of high‐energy‐density batteries. However, their fabrication remains challenging using regular cold rolling processing due to inferior processibility of metallic Li. Herein, a facile molten metal doctor‐blade casting approach is explored to fabricate uniform metallic Li layers with thickness ranging from 10 to 50 µm on regular battery Cu current collectors with a lithiophilic Sn interphase layer. The enhanced surface wettability between Li and the spontaneously formed Li–Sn alloy helps to realize uniform spreading, and formation of an ultrathin and uniform metallic Li layer. The existence of the Li–Sn alloy in the bulk of metallic Li electrode helps to reduce the nucleation barrier and improve the electrochemical performance of the Li metal. With a cathode areal capacity of 2.8 mA h cm−2 the LiCoO2||Li/Li–Sn full cell shows improved capacity retention from 58% to 77% after 100 cycles at a lower Negative/Positive ratio of 2/1, offering a high energy density of 662.4 W h kg−1. The enhanced electrochemical performance of the as‐fabricated ultrathin Li metal electrode with high energy density opens up a promising pathway for realizing next‐generation high‐energy‐density batteries.
Processing Rusty Metals into Versatile Prussian Blue for Sustainable Energy Storage
Authors: Peng Jian , Zhang Wang , Wang Jinsong , Li Lin , Lai Weihong , Yang Qiuran , Zhang Binwei , Li Xiaoning , Du Yumeng , Liu Hanwen , Wang Jianli , Cheng Zhenxiang , Wang Lizhen , Wang Shiwen , Wang Jiazhao , Chou Shulei , Liu Huakun , Dou Shixue
Published: October 2021

To reach a closed‐loop material system and meet the urgent requirement of sustainable energy storage technologies, it is essential to incorporate efficient waste management into designing new energy storage materials. Here, a “two birds with one stone” strategy to transform rusty iron products into Prussian blue as high‐performance cathode materials, and recover the rusty iron products to their original status, is reported. Owing to the high crystalline and Na+ content, the rusty iron derived Prussian blue shows a high specific capacity of 145 mAh g−1 and excellent cycling stability over 3500 cycles. Through the in situ X‐ray diffraction and in situ Raman spectra, it is found that the impressive ion storage capability and stability are strongly related to the suppressed structure distortion during the charge/discharge process. The ion migration mechanism and the possibility to serve as a universal host for other kinds of ions are further illuminated by density functional theory calculations. This work provides a new strategy for recycling wasted materials into high value‐added materials for sustainable battery systems, and is adaptable in the nanomedicine, catalysis, sensors, and gas storage applications.
Thermally Activated P2‐O3 Mixed Layered Cathodes toward Synergistic Electrochemical Enhancement for Na Ion Batteries
Authors: Yang Junghoon , Lim Jin‐Myoung , Park Mihui , Lee Gi‐Hyeok , Lee Suwon , Cho Maenghyo , Kang Yong‐Mook
Published: October 2021

Layer‐structured oxide cathodes have a lot of phases, which can be varied depending on Na ion contents and finally determine their electrochemical properties. Therefore, the off‐stoichiometry of layer‐structured oxides with the Na ions may differentiate not only their capacities but also the cyclic stabilities, kinetics, and so on, highlighting the importance of Na ion content. However, Na2CO3 tends to be irreversibly formed on surface by making use of the Na ions lost from the lattice. Thereby, the O3 phase with stoichiometric Na content changes into the off‐stoichiometric P2 phase bringing about significant disadvantages. To address this issue, a thermal activation process is suggested to simultaneously decompose Na2CO3 into electrochemically active Na ions and modulate the off‐stoichiometric P2 phase into the stoichiometric O3 phase. This study indicates that minimizing the loss of Na ions and maintaining the lattice framework with higher contents of Na ions during the synthesis of Na‐incorporating layered cathodes should be a key toward attaining electrochemical superiority.
Presence of Maximal Characteristic Time in Photoluminescence Blinking of MAPbI3 Perovskite
Authors: Seth Sudipta , Podshivaylov Eduard A. , Li Jun , Gerhard Marina , Kiligaridis Alexander , Frantsuzov Pavel A. , Scheblykin Ivan G.
Published: October 2021

Photoluminescence (PL) blinking is a common phenomenon in nanostructured semiconductors associated with charge trapping and defect dynamics. PL blinking kinetics exhibit very broadly distributed timescales. The traditionally employed analysis of probability distribution of ON and OFF events suffers from ambiguities in their determination in complex PL traces making its suitability questionable. Here, the statistically correct power spectral density (PSD) estimation method applicable for fluctuations of any complexity is employed. PSDs of the blinking traces of submicrometer MAPbI3 crystals at high frequencies follow power law with excitation power density dependent parameters. However, at frequencies less than 0.3 Hz, the majority of the PSDs saturate revealing the presence of a maximal characteristic timescale of blinking in the range of 0.5–10 s independently of the excitation power density. Super‐resolution optical microscopy shows the characteristic timescale to be an inherent material property independent of polycrystallinity. Thus, for the first time the maximum timescale of the multiscale blinking behavior of nanoparticles is observed demonstrating that the power law statistics are not universal for semiconductors. It is proposed that the viscoelasticity of metal‐halide perovskites can limit the maximum timescale for the PL fluctuations by limiting the memory of preceded deformations/re‐arrangements of the crystal lattice.
High‐performance nano‐splitters containing aggregation‐induced emission luminogens for stereoselective crystallization obtained via polymerization‐induced self‐assembly
Authors: Li Bowen , Li Na , Wang Zhaoxu , Ye Xichong , Zhang Jie , Wan Xinhua
Published: October 2021

Collecting both enantiomorphs with high optical purity and yield in a single crystallization process can be achieved by adding aggregated polymeric “tailor‐made” additives, known as nano‐splitters. Inefficient preparation and large addition amount have hindered the practical application of such amazing nanoparticles. Herein, we report the first nano‐splitters containing aggregation‐induced emission luminogens prepared via polymerization‐induced self‐assembly of block copolymer, poly[(S)‐2‐(tert‐butoxycarbonylamino)‐6‐(methacrylamido)hexanoic acid]‐b‐polystyrene, followed by the removal of tert‐butoxycarbonyl groups. When added into the supersaturated solution of racemic amino acids (a.a.) with seeds, the fluorescent labeled nano‐assemblies enantioselectivity dyed the crystals of S‐a.a. and enabled the separation from colorless R‐a.a. crystals in terms of fluorescent difference. Both enantiomers were obtained with high optical purity and yield (e.g., R‐ asparagine monohydrate, >99 ee%; S‐ asparagine monohydrate, ∼94 ee%; 88% total yield). Owing to a low detection limit of fluorescence, the addition amount was reduced to 0.03 wt% without remarkably compromising the ee values of both enantiomorphs. Due to the low addition amount and efficient synthesis, the output–input ratio was increased greatly.
Real‐world experience of adalimumab therapy for patients with ulcerative colitis: A single tertiary medical center experience in Central Taiwan
Authors: Yen Hsu‐Heng , Hsu Yu‐Chun , Kuo Chu‐Hsuan , Hsu Tsui‐Chun , Chen Yang‐Yuan
Published: October 2021

There are few studies on the treatment outcomes of adalimumab therapy in Taiwanese patients with ulcerative colitis (UC). A total of 102 patients with ulcerative colitis were identified from the electronic clinical database of the Changhua Christian Hospital. The demographic data and clinical features of the disease pattern of the UC patients receiving adalimumab therapy were retrospectively reviewed. Between January 2015 and June 2020, 18 patients with UC received adalimumab therapy. Due to the absence of a response, 5 of the 18 patients (27.7%) only received the induction therapy. Of the 13 patients who received maintenance adalimumab therapy, four discontinued the therapy: three (23.1%) stopped due to a loss of response, and one (7.7%) stopped due to a cutaneous reaction to adalimumab. Because of Taiwan's 1‐year limit on the use of adalimumab, seven patients relapsed and required a second course of therapy. The median period between course completion and relapse was 31 weeks. Two (20%) of the ten patients who finished the first course of therapy did not experience a relapse. The treatment response of patients with UC to adalimumab therapy appears to be comparable to those in previously published Western studies. The majority of patients who responded to adalimumab will relapse following a limited duration of adalimumab therapy in Taiwan.
Mechanically‐Guided 4D Printing of Magnetoresponsive Soft Materials across Different Length Scale
Authors: Zhu Hanlin , He Yifeng , Wang Yuan , Zhao Yan , Jiang Chao
Published: October 2021

Untethered magnetoresponsive soft materials that can transform between various complex 3D shapes are of growing interests in diverse areas such as soft robotics, flexible electronics, and biomedical engineering. Previous approaches are difficult to precisely encode continuous 3D magnetization profiles in small‐scale 3D structures. Herein, a novel method to produce magnetoresponsive soft materials for shape‐morphing systems across different length scale is reported. The magnetization profiles are programmed by the mechanically‐guided 4D printing with high precision and time‐cost efficiency. A theoretical model and model‐based simulation method are developed to quantitatively predict shape‐morphing of printed structures under applied magnetic fields, and guide the design of complex 3D shapes. A broad set of structures with complex transformations are fabricated to illustrate the capability of the methods. Diverse typical functional applications from centimeter‐ to millimeter‐scale, including soft crawling robots, flexible grippers, bionic butterfly, and multistate magnetic switch, are further demonstrated.
A eudicot leaf from the Lower Cretaceous (Aptian, Araripe Basin) Crato Konservat‐Lagerstätte
Authors: Pessoa Edlley M. , Ribeiro Alexandre C. , Jud Nathan A.
Published: October 2021

Premise

The Crato Konservat‐Lagerstätte in Brazil preserves an exceptionally rich assemblage of plant macrofossils from the Early Cretaceous (late Aptian), including rare early angiosperm fossils related to Nymphaeales, monocots, and magnoliids, and a variety of angiosperms of uncertain affinities. Macrofossils of eudicot angiosperms have not been described previously, despite the presence of tricolpate pollen. We describe a fossil leaf with morphology characteristic of eudicot angiosperms.

Methods

The fossil was collected from a quarry in the Lower Cretaceous (late Aptian) Crato Formation of northeastern Brazil in the state of Ceará. We compared the leaf architecture with that of ferns, gymnosperms, and similar living and fossil angiosperms.

Results

The leaf ofBaderadea pinnatissectagen. et sp. nov. is simple and petiolate, with leaf architecture similar to that of some herbaceous Ranunculales. The blade is 5 cm long and the margin is untoothed and twice pinnately lobed with narrow lobes (pinnatisect). The primary vein framework is pinnate and there are multiple orders of reticulate venation.

Conclusions

The combination of characters preserved in the fossil supports the interpretation thatB. pinnatissectawas an herbaceous eudicot similar to some members of Ranunculales and distinguished from other lobate Aptian angiosperms by leaf shape, presence of multiple orders of reticulate venation, and the absence of glandular teeth. The presence of eudicots in the flora of the Crato was already supported by pollen; the discovery of macrofossils like these provides additional information about their morphology and ecological role in low‐latitude Early Cretaceous plant communities.
Genotype‐cardiac phenotype correlations in a large single‐center cohort of patients affected by RASopathies: Clinical implications and literature review
Authors: Leoni Chiara , Blandino Rita , Delogu Angelica Bibiana , De Rosa Gabriella , Onesimo Roberta , Verusio Valeria , Marino Maria Vittoria , Lanza Gaetano Antonio , Rigante Donato , Tartaglia Marco , Zampino Giuseppe
Published: October 2021

Congenital heart disease (CHD) and hypertrophic cardiomyopathy (HCM) are common features in patients affected by RASopathies. The aim of this study was to assess genotype‐ phenotype correlations, focusing on the cardiac features and outcomes of interventions for cardiac conditions, in a single‐center cohort of 116 patients with molecularly confirmed diagnosis of RASopathy, and compare these findings with previously published data. All enrolled patients underwent a comprehensive echocardiographic examination. Relevant information was also retrospectively collected through the analysis of clinical records. As expected, significant associations were found between PTPN11 mutations and pulmonary stenosis (both valvular and supravalvular) and pulmonary valve dysplasia, and between SOS1 mutations and valvular defects. Similarly, HRAS mutations were significantly associated with HCM. Potential associations between less prevalent mutations and cardiac defects were also observed, including RIT1 mutations and HCM, SOS2 mutations and septal defects, and SHOC2 mutations and septal and valve abnormalities. Patients with PTPN11 mutations were the most likely to require both a primary treatment (transcatheter or surgical) and surgical reintervention. Other cardiac anomalies less reported until recently in this population, such as isolated functional and structural mitral valve diseases, as well as a sigmoid‐shaped interventricular septum in the absence of HCM, were also reported. In conclusion, our study confirms previous data but also provides new insights on cardiac involvement in RASopathies. Further research concerning genotype/phenotype associations in RASopathies could lead to a more rational approach to surgery and the consideration of drug therapy in patients at higher risk due to age, severity, anatomy, and comorbidities.
Aortic root dilatation and dilated cardiomyopathy in an adult with Tatton‐Brown‐Rahman syndrome
Authors: Cecchi Alana C. , Haidar Amier , Marin Isabella , Kwartler Callie S. , Prakash Siddharth K. , Milewicz Dianna M.
Published: October 2021

Tatton‐Brown‐Rahman syndrome is an autosomal dominant overgrowth syndrome caused by pathogenic DNMT3A variants in the germline. Clinical findings of tall stature due to postnatal overgrowth, intellectual disability, and characteristic facial features, are the most consistent findings observed in patients with Tatton‐Brown‐Rahman syndrome (TBRS). Since the syndrome was first described in 2014, an expanding spectrum of neuropsychiatric, musculoskeletal, neurological, and cardiovascular manifestations have been reported. However, most TBRS cases described in the literature are children with de novo DNMT3A variants, signaling a need to better characterize the phenotypes in adults. In this report, we describe a 34 year old referred to genetics for possible Marfan syndrome with aortic root dilatation, mitral valve prolapse, and dilated cardiomyopathy, who was diagnosed with TBRS due to a heterozygous de novo DNMT3A variant. This represents the third reported TBRS case with aortic root dilation and the second with cardiomyopathy. Collectively, these data provide evidence for an association with aortic disease and cardiomyopathy, highlight the clinical overlap with Marfan syndrome, and suggest that cardiovascular surveillance into adulthood is indicated.
On‐Surface Synthesis and Collective Spin Excitations of a Triangulene‐Based Nanostar
Authors: Hieulle Jeremy , Castro Silvia , Friedrich Niklas , Vegliante Alessio , Lara Francisco Romero , Sanz Sofía , Rey Dulce , Corso Martina , Frederiksen Thomas , Pascual Jose Ignacio , Peña Diego
Published: October 2021

Triangulene nanographenes are open‐shell molecules with predicted high spin state due to the frustration of their conjugated network. Their long‐sought synthesis became recently possible over a metal surface. Here, we present a macrocycle formed by six [3]triangulenes, which was obtained by combining the solution synthesis of a dimethylphenyl‐anthracene cyclic hexamer and the on‐surface cyclodehydrogenation of this precursor over a gold substrate. The resulting triangulene nanostar exhibits a collective spin state generated by the interaction of its 12 unpaired π‐electrons along the conjugated lattice, corresponding to the antiferromagnetic ordering of six S=1 sites (one per triangulene unit). Inelastic electron tunneling spectroscopy resolved three spin excitations connecting the singlet ground state with triplet states. The nanostar behaves close to predictions from the Heisenberg model of an S=1 spin ring, representing a unique system to test collective spin modes in cyclic systems.
Multivariate Synergistic Flexible Metal‐Organic Frameworks with Superproton Conductivity for Direct Methanol Fuel Cells
Authors: Li Zhen‐Hua , Zeng Hui , Zeng Guang , Ru Chunyu , Li Guanghua , Yan Wenfu , Shi Zhan , Feng Shouhua
Published: October 2021

Improving proton conductivity and fabricating viable metal‐organic frameworks (MOFs) based proton exchange membranes (PEMs) are central issues exploiting electrolyte MOFs. We aim to design multivariate flexibility synergistic strategy to achieve Flexible MOFs (FMOFs) with high conductivity at a wide range of humidity. In situ powder X‐ray diffraction (PXRD) and temperature‐dependent Fourier transform infrared spectra (FT‐IR) prove the synergistic self‐adaption between dynamic torsion of alkyl sulfonic acid and dynamic breathing of FMOF, forming a continuous hydrogen‐bonding networks to maintain high conductivity. Based on the convincing proton conductivity, we construct a series of long‐term durable MOF‐based PEMs that serve as a bridge between MOF and fuel cell. Consequently, the membrane electrode assembly (MEA) of the flexible PMNS1‐40 exhibits a maximum single‐cell power density of 34.76 mW cm−2 and hopefully opens doors to evaluate the practical application of proton‐conducting MOFs in direct methanol fuel cells.