bluuebunny/crossref_metadata_2025 huggingface dataset:
Surface Protonic Conduction on Oxide Ceramics: Mechanism, Materials, and Method for Characterization
Authors: Gu Jie , Jiang Lulu , Ismail Sara Adeeba , Guo Hui , Han Donglin
Published: December 2022

Surface protonic conduction originates from a common phenomenon of surface adsorption of water, which occurs almost everywhere when the temperature and humidity are properly controlled. Different from the volume transport of protons inside the oxide ceramics, which exhibits an Arrhenius relationship with the temperature and asks for at least 500 °C to activate sufficiently high proton conductivity, the surface protonic conduction exhibits an anti‐Arrhenius behavior, enabling to achieve high surface proton conductivity at much lower temperature (e.g., close to room temperature). Therefore, the surface protonic conduction is attracting increasing attention due to its promising application in the areas of low temperature catalysis and solid‐state electrochemical devices. This review paper summarizes recent progress on the mechanism, materials, influential factors, and characterization methods of the protonic conduction on the surface of oxide ceramics, and discusses present problems and future perspectives.
Extended Work Function Shift of Large‐Area Biofunctionalized Surfaces Triggered by a Few Single‐Molecule Affinity Binding Events
Authors: Di Franco Cinzia , Macchia Eleonora , Sarcina Lucia , Ditaranto Nicoletta , Khaliq Aniqa , Torsi Luisa , Scamarcio Gaetano
Published: December 2022

Few binding events are here shown to elicit an extended work function change in a large‐area Au‐surface biofunctionalized with ≈108 capturing antibodies. This is demonstrated by Kelvin probe force microscopy (KPFM), imaging a ≈105 µm2 wide Au‐electrodes covered by a dense layer (≈104 µm−2) of physisorbed anti‐immunoglobulin‐M (anti‐IgM). A 10 min incubation in 100 µL phosphate buffer saline solution encompassing ≈10 IgM antigens (10−19 mole L−1  102 × 10−21 m) produces a work function shift ΔW ≈ –60 meV. KPFM images prove that this shift involves the whole inspected area. Notably, no work function change occurs upon incubation in highly concentrated (3 × 10−15 m) nonbinding IgG solutions. The ΔW measured by KPFM is in quantitative agreement with the threshold voltage shift of an electrolyte‐gated single‐molecule large‐area transistor (SiMoT). The findings provide direct experimental evidence for the SiMoT ultrahigh sensitivity, by imaging the extensive shift of the gate work function, likely arising from collective surface phenomena, elicited by single‐molecule binding events.
Capillary Evaporation‐Induced Fabrication of Compact Flake Graphite Anode with High Volumetric Performance for Potassium Ion Batteries
Authors: Chang Xiaqing , Sun Ning , Li Guang , Yang Botao , Soomro Razium A. , Xu Bin
Published: December 2022

Improvement in volumetric performance is growing requirements for rechargeable batteries of lightweight and compact size. Flake graphite (FG) with thin lamellar structure realizes a satisfactory K‐ion storage performance, but its low packing density leads to poor volumetric capacity. Herein, this work fabricates an FG anode with improved packing density by hydrothermal treatment of the FG with graphene oxide and subsequent capillary evaporation‐induced drying process. A three‐dimensional flake graphite/reduced graphene oxide (FG/rGO) hydrogel is formed after hydrothermal treatment, which can be compressed during drying process via the capillary force generated by water evaporation, resulting in a compact structure with enhanced packing density. Compared to the pristine FG electrode (106.0 mAh cm−3), the FG/rGO‐82 anode realizes an ultrahigh volumetric capacity of 218.9 mAh cm−3 and good rate performance with a retained capacity of 152.3 mAh cm−3 at 2 C. Moreover, the FG/rGO‐82 exhibits excellent cycle stability with a capacity retention of 90.1% after 300 cycles. Even under a high mass loading of 7.4 mg cm−2, it still remains a volumetric capacity of 145.4 mAh cm−3 after 300 cycles at 1 C. The results prove that the capillary evaporation induced drying of hydrogel is an effective way to prepare electrode material with high volumetric capacity.
Dynamic Coordination Structure Evolutions of Atomically Dispersed Metal Catalysts for Electrocatalytic Reactions
Authors: Tan Hui‐Ying , Wang Jiali , Lin Sheng‐Chih , Kuo Tsung‐Rong , Chen Hao Ming
Published: December 2022

Single‐atom catalysts (SACs) are regarded as promising electrocatalysts for various reactions in the field of energy conversion and storage owing to their maximized atom utilization efficiency and unique electronic properties. The modifications of local coordination structures of single metal centers play significant roles in dominating catalytic performances, thus the SACs are resurveyed with different local coordination environments in order to explore such a paramount structure–performance relationship in various energy‐conversion reactions, including O2/CO2 reduction reaction and hydrogen evolution reaction. Notably, the atomically dispersed metal atoms that are subject to working conditions will undergo dynamic changes and then affect the catalytic properties, consequently, understanding the dynamic nature of SACs during reactions is highly significant but is still lacking to date. To this endeavor, this review particularly summarizes the dynamic evolutions of local coordination structures of SACs in various electrochemical reactions based on advanced operando/in situ techniques, aiming to precisely demonstrate the correlation between the dynamic coordination environment of SACs and the electrocatalytic activity. Finally, the challenges and perspectives are highlighted in the mechanistic studying for understanding the accurate active sites of SACs under realistic working conditions.
Electropolymerized Triphenylamine Network Films for High‐Performance Transparent to Black Electrochromism and Capacitance
Authors: Wang Bohan , Wang Lingyu , Chen Haoyan , Jia Yanhua , Ma Yuguang
Published: December 2022

The polytriphenylamine films are prepared by electropolymerization from a precursor HPB‐6TPA with hexaphenylbenzene (HPB) core bearing six triphenylamine (TPA) units. The abundant and valuable electrochromism from transparent to black and from no to strong near‐infrared absorption are achieved from this TPA network film. The presence of residual TPA and dimeric TPA (N,N,N′,N′‐tetraphenylbenzidine) units in network film and their independent potential response attain the electrochromic behaviors. The network film possesses short response time and can realize high doping level (72%), attributed to favorable dopant ion channel caused by the twisting structure of HPB core and TPA units. The network film also shows large lightness changes and high specific capacitance (788.9 F g−1@1.4 A g−1), attributed to multiple active units due to HPB core with high functionality. By regulating the voltammetric cycle number of electropolymerization, films with different lightness black colored states can be prepared conveniently to satisfy different practical needs.
A Novel Strategy to Construct Artificial Light‐Harvesting System Based on Aggregation‐Induced Emission Surfactants for Photocatalysis
Authors: Xing Ling‐Bao , Wang Ying , Li Xin‐Long , Han Ning , Ma Chao‐Qun , Liu Hui , Yu Shengsheng , Wang Rongzhou , Zhuo Shuping
Published: December 2022

Herein, a novel strategy to construct artificial light‐harvesting systems (LHSs) based on micelles is proposed. Two efficient artificial LHSs are fabricated in water based on tetraphenylethene (TPE) modified surfactants (TPE‐SAA). TPE‐SAA can self‐assemble into spherical micelles in an aqueous solution through noncovalent interactions. Due to the aggregation‐induced emission effect of the TPE unit, TPE‐SAA micelles exhibit strong emission and directly act as donors to achieve the energy transfer process. Firstly, two fluorescent dyes (4,7‐bis(thien‐2‐yl)‐2,1,3‐benzothiadiazole (DBT) and amphoteric sulforhodamine 101 (SR101)), which are localized in the hydrophobic interior and positively charged surface of TPE‐SAA respectively, are chosen as energy acceptors to realize the two‐step sequential energy transfer process with high efficiency. In addition, energy transfer can also take place from TPE‐SAA to SR101, and bright white‐light emission with a CIE coordinate of (0.31, 0.33) can be achieved by adjusting the ratio of donor to acceptor. Furthermore, to utilize the harvested energy, the micelle‐based artificial LHSs are employed to promote the aerobic cross‐dehydrogenative coupling reaction. Moreover, the dehalogenation reaction of α‐bromoacetophenone can also be catalyzed by the TPE‐SAA+DBT+SR101 system in water.
Advances, Challenges, and Perspectives for Heavy‐Metal‐Free Blue‐Emitting Indium Phosphide Quantum Dot Light‐Emitting Diodes
Authors: Cui Zhongjie , Yang Dan , Qin Shuaitao , Wen Zhuoqi , He Haiyang , Mei Shiliang , Zhang Wanlu , Xing Guichuan , Liang Chao , Guo Ruiqian
Published: December 2022

Quantum dot light‐emitting diodes (QLEDs), regarded as promising candidates in the next‐generation display, have attracted much attention recently. In spite of the outstanding performance of cadmium‐based (Cd‐based) QLEDs, the toxicity of Cd hinders their wide application. Indium phosphide quantum dots (InP QDs) with heavy‐metal‐free feature and competitive performance are considered to be able to replace Cd‐based QDs as emitting layer in the QLEDs. Much progress is obtained in the red‐emitting and green‐emitting InP‐based QLEDs. However, the blue‐emitting ones are faced with great challenges and are demanded on full‐color display urgently, which is limited by the inferior performance of blue‐emitting InP QDs and lack of investigations about their QLED devices. In this review, the encountered challenges for high‐quality blue‐emitting InP QDs are presented. Common strategies for blue‐emitting InP QDs, including size engineering, composition engineering, and surface engineering are presented and analyzed. The progress of blue‐emitting InP‐based QLEDs, which strongly relies on the advances of materials, is also summarized. Finally, some perspectives from device physics are provided and discussed to inspire more efficient strategies toward blue‐emitting InP‐based QLEDs.
Mid‐Infrared Silicon‐on‐Lithium‐Niobate Electro‐Optic Modulators Toward Integrated Spectroscopic Sensing Systems
Authors: Xu Siyu , Ren Zhihao , Dong Bowei , Zhou Jingkai , Liu Weixin , Lee Chengkuo
Published: December 2022

Mid‐infrared spectroscopy is an emerging technique in various applications such as molecule identification and label‐free chemical sensing. Integrated photonic platforms have a promising potential to perform miniaturized spectroscopic sensing with the advantage of compact footprint, low cost, and low power consumption. As an essential building block for integrated photonics, on‐chip phase shifter plays an important role in mid‐infrared spectroscopic systems, enabling signal processing and spectrum analysis. However, the implementation of effective pure phase modulation in mid‐infrared photonics remains challenging due to the unavoidable electroabsorption in the plasma dispersion effect at a long wavelength. Here, silicon photonic devices are built on lithium niobate substrates to simultaneously leverage the prominent electro‐optic effect and circumvent the absorption originating from the oxide layer. In particular, a reliable transfer printing method is presented for flexibly integrating the monocrystalline silicon waveguides with foreign substrates. In the fabricated silicon‐on‐lithium‐niobate platform, the electro‐optic performance is exploited via Mach–Zehnder interferometer for operation in the mid‐infrared regime. The modulator achieves half‐wave voltage length product of 12.3 V∙cm at the wavelength of 3.78 µm, with a maximum extinction ratio of 25.2 dB. These results indicate the potential of the proposed technology for the implementation of integrated mid‐infrared spectroscopic sensing systems.
Laser‐Triggered Vapor‐Phase Anion Exchange on All‐Inorganic Perovskites for Multicolor Patterns and Microfabrications
Authors: Sheng Yuhang , Zha Yanfang , Feng Xuying , Xing Fangjian , Di Yunsong , Liu Cihui , Zhang Xiaowei , Gan Zhixing
Published: December 2022

Anion exchange reaction is a facile postsynthesis approach to modulate the bandgaps of perovskites to meet the demands in full visible spectrum. However, conventional anion exchanges are usually conducted in solutions, limiting their applications in fabricating high‐quality blue‐emitting perovskites and multicolor fluorescent patterns. Herein, a laser‐triggered vapor‐phase anion exchange (LTVAE) method is developed to convert CsPbBr3 perovskites with different morphologies (nanocrystal films/solution, microcrystals, and microplatelets) into CsPb(BrxCl1‐x)3 and CsPb(BrxI1‐x)3 perovskites. Thus, the green fluorescence is converted into blue and red fluorescence. Moreover, the deep‐blue fluorescence obtained by LTVAE shows a high quantum yield (QY) of 67.2%. Based on the mask‐assistant LTVAE, multicolor fluorescent patterns are fabricated, which are very significant for anticounterfeit and multicolor displays. Furthermore, a polymer‐assistant LTVAE method is developed to improve the stability of the multicolor fluorescent patterns. More importantly, micro‐heterojunctions with two different fluorescent colors are successfully constructed on a single CsPbBr3 microplatelet, which paves the way for microfabrications.
Tunable Luminescence on Indium Halide Hybrid Regulated by Sb3+ Doping Concentration
Authors: Shi Cui‐Mi , Xuan Hong‐Li , Wu Yue , Xu Liang‐Jin , Chen Zhong‐Ning
Published: December 2022

Sb3+ doping strategy has proved to be an effective way to regulate the band gap and improve the photophysical properties of metal halides. Herein, Sb3+‐doped lead‐free indium halide hybrid InCl6(C4H12N2)2Cl·H2O:xSb3+ (0 ≤ x ≤ 1) is reported. Upon Sb3+‐doping, the weak emission of InCl6(C4H12N2)2Cl experiences a significant enhancement in emission intensity with near‐unity photoluminescence quantum yield (PLQY). The photophysical data fitted by the power‐law equation verifies self‐trapped exciton emission for the broadband emission. Interestingly, the emission experiences a gradual red‐shift with emission color changing from green to yellow and finally to orange as the Sb3+‐doped concentration increases. The single crystal X‐ray diffraction, excitation wavelengths‐dependent emission spectra, and the distortion degree calculation of InCl6(C4H12N2)2Cl·H2O:xSb3+ (0 ≤ x ≤ 1) indicate that the Sb3+ concentration dependent luminescence results from the synergistic effect of crystal phase transition, change of luminescence center, and the distortion of crystal structure. This achievement represents a successful strategy to achieve the photophysical properties modulation of metal halides for versatile optical applications.
Digitally Printed Liquid Metal Composite Antenna for Energy Harvesting: Toward Energy‐Autonomous Battery‐Free Wearable Bioelectronics
Authors: Maranha Miguel , Silva André F. , Lopes Pedro Alhais , de Almeida Aníbal T. , Tavakoli Mahmoud
Published: December 2022

Rapid progress on wearable bioelectronics holds the promise for remote patient monitoring. However, there are concerns related with the use of batteries, including the need for frequent charging, user safety, and environmental pollution. The development of rapidly deployable battery‐free patches that harvest their energy from external sources is highly desired. Here, untethered battery‐free patches through far‐field energy harvesting are demonstrated. Taking advantage of a stretchable biphasic liquid metal‐based ink and digital fabrication techniques, that is, direct printing, and laser patterning, tailor‐made customized antennas are fabricated over various substrates, including polydimethylsiloxane, Kapton, and wound‐dressing medical‐grade adhesives. Folded dipole and planar inverted‐F antennas (PIFA) are evaluated and they are optimized for an over‐the‐body scenario. Compared to previous works that only show communication of data at <1 Hz, here, battery‐free acquisition and transmission of electrocardiogram (ECG) data at 100 Hz via Bluetooth is demonstrated. It is shown that using 3 parallel PIFA antennas, it is possible to harvest ≈10 mW at 30 cm from the transmitter, which is ≈7× the required power by the ECG circuit. This study proves the feasibility of next generation of battery‐free wearable biomonitoring patches/e‐textiles and demonstrates materials and methods for fabrication of optimized printed antennas.
One‐Pot MOFs‐Encapsulation Derived In‐Doped ZnO@In2O3Hybrid Photocatalyst for Enhanced Visible‐Light‐Driven Photocatalytic Hydrogen Evolution
Authors: Yang Hongli , Gao Junlun , Yang Man , Hou Huilin , Gao Fengmei , Luo Yong , Yang Weiyou
Published: December 2022

The development of visible‐light‐induced photocatalysts is one of the critically important issues because it offers a green and sustainable route for solar energy conversion. Herein, In‐doped ZnO@In2O3hybrid photocatalysts are designed and constructed through a one‐pot metal‐organic frameworks (MOFs)‐encapsulation‐derived method. The photocatalytic activity of the sample photocatalysts is systematically investigated by photocatalytic hydrogen evolution under visible light irradiation. The composition of the hybrid photocatalysts is also controlled to find the best photocatalytic activities. Interestingly, using a visible‐light irradiation source, the optimized In‐doped ZnO@In2O3photocatalyst shows an H2evolution rate of 417 µmol∙g−1∙h−1, which is nearly 20 times higher than that of the In‐doped ZnO sample and also exceeds most ZnO‐based catalysts ever reported. The enhanced catalytic performance is ascribed to the increased visible‐light response and enhanced charge separation efficiency by the synergistic effects of electron‐trapped In doping and electron‐donated In2O3coupling. This work presents a promising pathway for fabricating MOFs‐encapsulation derived visible‐light‐driven composites for high photocatalytic performance towards hydrogen evolution.
Framework Dimensional Control Boosting Charge Storage in Conjugated Coordination Polymers
Authors: Fan Kun , Fu Cheng , Chen Yuan , Zhang Chenyang , Zhang Guoqun , Guan Linnan , Mao Minglei , Ma Jing , Hu Wenping , Wang Chengliang
Published: December 2022

Conjugated coordination polymers (CCPs) with extended π–d conjugation, which can effectively promote long‐range delocalization of electrons and enhance conductivity, are superior to traditional metal‐organic frameworks (MOFs) and attracted great attention for potential applications in chemical sensors, electronics, energy conversion/storage devices, etc. However, the precise construction of CCPs is still challenging due to the complex and uncontrollable reactions of CCPs. Herein, two different framework dimensions of CCPs are controllably realized by employing the same ligand (2,3,5,6‐tetraaminobenzoquinone (TABQ)) and the same metal (copper) as center ions. The manipulation of reaction leads to different valences of ligands and metal ions, different coordination geometries, and thereby 1D‐CuTABQ and 2D‐CuTABQ frameworks, respectively. High performance of charge storage is hence achieved involving the storage of both cations and anions, and therein, 2D‐CuTABQ shows a high reversible capacity of ≈305 mAh g−1, good rate capability and high capacity retention (≈170 mAh g−1 after 2000 cycles at 5 A g−1 with 0.01% decay per cycle), which outperforms 1D‐CuTABQ and almost all of the reported MOFs as cathodes for batteries. These results highlight the delicate structural control of CCPs for high‐performance batteries and other various applications.
Highly Efficient and Stable Self‐Powered Mixed Tin‐Lead Perovskite Photodetector Used in Remote Wearable Health Monitoring Technology
Authors: Liu Fengcai , Liu Kai , Rafique Saqib , Xu Zengyi , Niu Wenqing , Li Xiaoguo , Wang Yifan , Deng Liangliang , Wang Jiao , Yue Xiaofei , Li Tao , Wang Jun , Ayala Paola , Cong Chunxiao , Qin Yajie , Yu Anran , Chi Nan , Zhan Yiqiang
Published: December 2022

Realization of remote wearable health monitoring (RWHM) technology for the flexible photodiodes is highly desirable in remote‐sensing healthcare systems used in space stations, oceans, and forecasting warning, which demands high external quantum efficiency (EQE) and detectivity in NIR region. Traditional inorganic photodetectors (PDs) are mechanically rigid and expensive while the widely reported solution‐processed mixed tin‐lead (MSP) perovskite photodetectors (PPDs) exhibit a trade‐off between EQE and detectivity in the NIR region. Herein, a novel functional passivating antioxidant (FPA) strategy has been introduced for the first time to simultaneously improve crystallization, restrain Sn2+ oxidization, and reduce defects in MSP perovskite films by multiple interactions between thiophene‐2‐carbohydrazide (TAH) molecules and cations/anions in MSP perovskite. The resultant solution‐processed rigid mixed Sn–Pb PPD simultaneously achieves high EQE (75.4% at 840 nm), detectivity (1.8 × 1012 Jones at 840 nm), ultrafast response time (trise/tfall = 94 ns/97 ns), and improved stability. This work also highlights the demonstration of the first flexible photodiode using MSP perovskite and FPA strategy with remarkably high EQE (75% at 840 nm), and operational stability. Most importantly, the RWHM is implemented for the first time in the PIN MSP perovskite photodiodes to remotely monitor the heart rate of humans at rest and after‐run conditions.
Axial Phosphate Coordination in Co Single Atoms Boosts Electrochemical Oxygen Evolution
Authors: Liu Yan , Zhang Shuangshuang , Jiao Chi , Chen Huimei , Wang Gang , Wu Wenjie , Zhuo Zhiwen , Mao Junjie
Published: December 2022

Cobalt single atoms coordinated with planar four nitrogen atoms (Co1N4) represent an efficient electrocatalyst for oxygen evolution reaction (OER), whereas the large energy barrier of CoOH dehydrogenation limits the OER activity. Herein, axial phosphate (PO4) coordination is incorporated in Co1N4 single atoms of cobalt phthalocyanine@carbon nanotubes (P‐CoPc@CNT), so as to boost the intrinsic OER performance through manipulating the reaction pathway. With a relative low mass loading of Co (2.7%), the P‐CoPc@CNT shows remarkable alkaline OER activity with the overpotential of 300 mV and Tafel slope of 41.7 mV dec−1, which dramatically outperforms the CoPc@CNT without axial PO4 coordination. Based on mechanistic analysis, the axial PO4 coordination directly participates in the OER cycle by the transformation of axial ligand. Specially, the CoOH dehydrogenation process is replaced by the dehydrogenation of HPO4‐Co1N4 intermediate, which largely decreases the energy barrier and thus benefits the whole OER process.
Ultraflexible and Energy‐Efficient Artificial Synapses Based on Molecular/Atomic Layer Deposited Organic–Inorganic Hybrid Thin Films
Authors: Liu Chang , Zhu Lin , Weng Jing‐Kai , Li Yu‐Chen , Chen Zhuo , Lei Jin , Zi Tao‐Qing , Wu Di , Fa Wei , Chen Shuang , Liang Bin , Li Ai‐Dong
Published: December 2022

Flexible artificial synapses, a conjunctive product of brain‐inspired neuromorphic computing and wearable electronics, arouse enormous interest in highly connected and energy‐efficient neural networks. The organic–inorganic hybrid materials hold great potential in flexible devices due to versatile properties. Here, an organic–inorganic hybrid synaptic device consisting of 2 nm Al2O3 and 22 nm Al‐based hydroquinone (Al‐HQ) sandwiched between Pt and poly(3,4‐ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) electrodes is prepared on highly flexible cellophane by molecular/atomic layer deposition (MLD/ALD). The vertically integrated Pt/Al2O3/Al‐HQ/PEDOT:PSS device exhibits reliable resistive switching with an ON/OFF ratio greater than 103. Several important bio‐synaptic functions, such as long‐term potentiation, long‐term depression, paired‐pulse facilitation, and spike‐time‐dependent plasticity, are realized in this device with the extremely low energy consumption of ≈25.2 fJ per reset operation, which is ascribed to the unique electron trapping/detrapping and tunneling mechanism. Remarkably, the excellent flexibility and robustness of this hybrid synaptic device is confirmed under the minimum curvature radius of ≈0.7 mm after 104 bending cycles. A pattern recognition computation based on these hybrid synapse devices shows a 90.2% learning accuracy. This research paves a way for the MLD/ALD‐derived organic–inorganic‐hybrid‐based artificial synapse applications in flexible energy‐efficient neuron network systems toward system‐on‐plastics.
Activated Internetwork Pathways in Partially‐Disordered Spinel Cathode Materials with Ultrahigh Rate Performance
Authors: Yang Julia H. , Ceder Gerbrand
Published: December 2022

In this study, a class of earth‐abundant, cation‐excess partially disordered spinel materials which demonstrate superior rate performance as Li‐ion cathodes compared to disordered rocksalt materials is computationally investigated. These results show that the partial disorder creates solid solution lithiation with spinel‐like features at the atomic level. A low‐voltage capacity gain is possible with lithiation past the rock salt stoichiometry. It is argued that high rate in partially disordered spinel materials comes from newly activated 16c/16d internetwork pathways which are not possible in normal spinel where only 16c intranetwork diffusion occurs. The assessment and understandings motivate the incorporation of some degree of partial spinel ordering in future disordered rocksalt electrodes to enable superior rate performance.
Molecular determinants for the layering and coarsening of biological condensates
Authors: Latham Andrew P. , Zhang Bin
Published: December 2022

Many membraneless organelles, or biological condensates, form through phase separation, and play key roles in signal sensing and transcriptional regulation. While the functional importance of these condensates has inspired many studies to characterize their stability and spatial organization, the underlying principles that dictate these emergent properties are still being uncovered. In this review, we examine recent work on biological condensates, especially multicomponent systems. We focus on connecting molecular factors such as binding energy, valency, and stoichiometry with the interfacial tension, explaining the nontrivial interior organization in many condensates. We further discuss mechanisms that arrest condensate coalescence by lowering the surface tension or introducing kinetic barriers to stabilize the multidroplet state.
Propulsion efficiency of achiral microswimmers in viscoelastic polymer fluids
Authors: Quashie David , Gordon David , Nielsen Paige , Kelley Shannon , Jermyn Sophie , Ali Jamel
Published: December 2022

We report the effects of polymer size, concentration, and polymer fluid viscoelasticity on the propulsion kinematics of achiral microswimmers. Magnetically driven swimmer's step‐out frequency, orientation angle, and propulsion efficiency are shown to be dependent on fluid microstructure, viscosity, and viscoelasticity. Additionally, by exploring the swimming dynamics of two geometrically distinct achiral structures, we observe differences in propulsion efficiencies of swimmers. Results indicate that larger four‐bead swimmers are more efficiently propelled in fluids with significant elasticity in contrast to smaller 3‐bead swimmers, which are able to use shear thinning behavior for efficient propulsion. Insights gained from these investigations will assist the development of future microswimmer designs and control strategies targeting applications in complex fluids.
Partial least squares, steepest descent, and conjugate gradient for regularized predictive modeling
Authors: Qin S. Joe , Liu Yiren , Tang Shiqin
Published: December 2022

In this article, we explore the connection of partial least squares (PLS) to other regularized regression algorithms including the Lasso and ridge regression, and consider a steepest descent alternative to the PLS algorithm. First, the PLS latent variable analysis is emphasized and formulated as a standalone procedure. The PLS connections to the conjugate gradient, Krylov space, and the Cayley–Hamilton theorem for matrix pseudo‐inverse are explored based on known results in the literature. Comparison of PLS with the Lasso and ridge regression are given in terms of the different resolutions along the regularization paths, leading to an explanation of why PLS sometimes does not outperform the Lasso and ridge regression. As an attempt to increase resolutions along the regularization paths, a steepest descent PLS is formulated as a regularized regression alternative to PLS and is compared to other regularized algorithms via simulations and an industrial case study.
Discriminative Transition Sequences of Origami Metamaterials for Mechanologic
Authors: Liu Zuolin , Fang Hongbin , Xu Jian , Wang Kon-Well
Published: December 2022

Transitions of multistability in materials are exploited for various functions and applications, such as spectral gap tuning, impact energy trapping, and wave steering. However, a fundamental and comprehensive understanding of the transitions, either quasistatic or dynamic transitions, has not yet been acquired, especially in terms of the sequence predictability and tailoring mechanisms. This research, utilizing the stacked Miura‐ori‐variant (SMOV) structure that has multistable shape reconfigurability as a platform, uncovers the deep knowledge of quasistatic and dynamic transitions and proposes the corresponding versatile formation and tuning of mechanical logic gates. Through theoretical, numerical, and experimental means, discriminative and deterministic quasistatic transition sequences, including reversible and irreversible ones, are uncovered, where they constitute a transition map that is editable upon adjusting the design parameters. Via applying dynamic excitations and tailoring the excitation conditions, reversible transitions between all stable configurations become attainable, generating a fully connected transition map. Benefiting from the nonlinearity of the quasistatic and dynamic transitions, basic and compound mechanical logic gates are achieved. The versatility of the scheme is demonstrated using a single SMOV to realize different complex logic operations without increasing structural complexity, showing its unique computing power and inspiring the avenue for efficient physical intelligence.
Radon exposure and risk of neurodegenerative diseases among male miners in Ontario, Canada: A cohort study
Authors: Zeng Xiaoke , Berriault Colin , Arrandale Victoria H. , DeBono Nathan L. , Harris M. Anne , Demers Paul A.
Published: December 2022

Background

Environmental radon has been examined as a risk factor for neurodegenerative diseases in a small number of previous studies, but the findings have been inconsistent. This study aims to investigate the association between occupational radon exposure and neurodegenerative disease in a cohort of male miners with work experience in multiple ore types in Ontario, Canada.

Methods

Radon exposure (1915–1988) was assessed using two job‐exposure matrices (JEM) constructed from using historical records for 34,536 Ontario male miners. Neurodegenerative outcomes were ascertained between 1992 and 2018. Poisson regression models were used to estimate incidence rate ratios (RR) and 95% confidence intervals (CI) between cumulative radon exposure in working level months (WLM) and each neurodegenerative outcome.

Results

Levels of cumulative radon exposure showed variability among cohort members with a mean of 7.5 WLM (standard deviation 24.4). Miners in uranium mines or underground jobs had higher levels and more variability in exposure than workers in non‐uranium work or surface jobs. Compared to the reference group (radon < 1 WLM), increased rates of Alzheimer's (RR 1.23, 95% CI 1.05–1.45) and Parkinson's disease (RR 1.43, 95% CI 1.08–1.89) were observed among workers with >1–5 WLM and >5–10 WLM, respectively, but not among higher exposed workers (>10 WLM).

Conclusion

This study did not observe a positive monotonic dose–response relationship between cumulative radon exposure and Alzheimer's or Parkinson's disease in Ontario mining workers. There was no association observed with motor neuron disease.
Inversions on human chromosomes
Authors: Kosuthova Klara , Solc Roman
Published: December 2022

Human chromosome inversions are types of balanced structural variations, making them difficult to analyze. Thanks to PEM (paired‐end sequencing and mapping), there has been tremendous progress in studying inversions. Inversions play an important role as an evolutionary factor, contributing to the formation of gonosomes, speciation of chimpanzees and humans, and inv17q21.3 or inv8p23.1 exhibit the features of natural selection. Both inversions have been related to pathogenic phenotype by directly affecting a gene structure (e.g., inv5p15.1q14.1), regulating gene expression (e.g., inv7q21.3q35) and by predisposing to other secondary arrangements (e.g., inv7q11.23). A polymorphism of human inversions is documented by the InvFEST database (a database that stores information about clinical predictions, validations, frequency of inversions, etc.), but only a small fraction of these inversions is validated, and a detailed analysis is complicated by the frequent location of breakpoints within regions of repetitive sequences.
Fetal akinesia deformation sequence syndrome associated with recessive TTN variants
Authors: Alkhunaizi Ebba , Martin Nicole , Jelin Angie C. , Rosner Mara , Bailey Diana J. , Steiner Laurie A. , Lakhani Saquib , Ji Weizhen , Katzman Philip J. , Forster Katherine R. , Jarinova Olga , Shannon Patrick , Chitayat David ,   Care4Rare Canada Consortium
Published: December 2022

Arthrogryposis multiplex congenita (AMC) [also known as multiple joints contracture or Fetal Akinesia Deformation Sequence (FADS)] is etiologically a heterogeneous condition with an estimated incidence of approximately 1 in 3000 live births and much higher incidence when prenatally diagnosed cases are included. The condition can be acquired or secondary to fetal exposures and can also be caused by a variety of single‐gene disorders affecting the brain, spinal cord, peripheral nerves, neuromuscular junction, muscle, and a variety of disorders affecting the connective tissues (Niles et al., Prenatal Diagnosis, 2019; 39:720–731). The introduction of next‐generation gene sequencing uncovered many genes and causative variants of AMC but also identified genes that cause both dominant and recessive inherited conditions with the variability of clinical manifestations depending on the genes and variants. Molecular diagnosis in these cases is not only important for prognostication but also for the determination of recurrence risk and for providing reproductive options including preimplantation and prenatal diagnosis. TTN, the largest known gene in the human genome, has been known to be associated with autosomal dominant dilated cardiomyopathy. However, homozygote and compound heterozygote pathogenic variants with recessive inheritance have rarely been reported. We report the effect of recessive variants located within the fetal IC and/or N2BA isoforms in association with severe FADS in three families. All parents were healthy obligate carriers and none of them had cardiac or skeletal muscle abnormalities. This report solidifies FADS as an alternative phenotypic presentation associated with homozygote/compound heterozygous pathogenic variants in the TTN.
Stable Operation of Aqueous Organic Redox Flow Batteries in Air Atmosphere
Authors: Kong Taoyi , Liu Jun , Zhou Xing , Xu Jie , Xie Yihua , Chen Jiawei , Li Xianfeng , Wang Yonggang
Published: December 2022

As a green route for large‐scale energy storage, aqueous organic redox flow batteries (AORFBs) are attracting extensive attention. However, most of the reported AORFBs were operated in an inert atmosphere. Herein, we clarify this issue by using the reported AORFB (i.e., 3, 3′‐(9,10‐anthraquinone‐diyl)bis(3‐methylbutanoicacid) (DPivOHAQ)||Ferrocyanide) as an example. We demonstrate that the dissolved O2 can oxidize the discharged DPivOHAQ in anolyte, leading to capacity‐imbalance between anolyte and catholyte. Therefore, this cell shows continuous capacity fading when operated in an air atmosphere. We propose a simple strategy for this challenge, in which the oxygen evolution reaction (OER) in catholyte is employed to balance oxygen reduction reaction (ORR) in anolyte. When using the Ni(OH)2‐modifed carbon felt (CF) as a current collector for catholyte, this cell shows an excellent stability in air atmosphere because the Ni(OH)2‐induced OER capacity in catholyte exactly balances the ORR capacity in anolyte. Such O2‐balance strategy facilitates AORFBs’ practical application.
Electronic Control of the Scholl Reaction: Selective Synthesis of Spiro vs Helical Nanographenes
Authors: Izquierdo‐García Patricia , Fernández‐García Jesús M. , Perles Josefina , Fernández Israel , Martín Nazario
Published: December 2022

Scholl oxidation has become an essential reaction in the bottom‐up synthesis of molecular nanographenes. Herein, we describe a Scholl reaction controlled by the electronic effects on the starting substrate (1 a, b). Anthracene‐based polyphenylenes lead to spironanographenes under Scholl conditions. In contrast, an electron‐deficient anthracene substrate affords a helically arranged molecular nanographene formed by two orthogonal dibenzo[fg,ij]phenanthro‐[9,10,1,2,3‐pqrst]pentaphene (DBPP) moieties linked through an octafluoroanthracene core. Density Functional Theory (DFT) calculations predict that electronic effects control either the first formation of spirocycles and subsequent Scholl reaction to form spironanographene 2, or the expected dehydrogenation reaction leading solely to the helical nanographene 3. The crystal structures of four of the new spiro compounds (syn 2, syn 9, anti 9 and syn 10) were solved by single crystal X‐ray diffraction. The photophysical properties of the new molecular nanographene 3 reveal a remarkable dual fluorescent emission.
Controlled Construction of Heteroleptic [Pd2(LA)2(LB)(LC)]4+Cages: A Facile Approach for Site‐Selective endo‐Functionalization of Supramolecular Cavities
Authors: Liu Yan , Liao Shou‐Heng , Dai Wen‐Tao , Bai Qixia , Lu Shuai , Wang Heng , Li Xiaopeng , Zhang Zhe , Wang Pingshan , Lu Wei , Zhang Qi
Published: December 2022

Construction of supramolecular structures with internal functionalities is a promising approach to build enzyme‐like cavities. The endo‐functionalized [Pd12L24] and [Pd2L4] coordination cages represent the most successful systems in this regard. However, these systems mainly contain one type of endo‐moiety. We herein provide a solution for the controlled endo‐functionalization of [Pd2L4] cages. Site‐selective introduction of the endo‐functional group was achieved through the formation of heteroleptic [Pd2(LA)2(LB)(LC)] cages. Using two orthogonal steric control elements is the key for the selective formation of the hetero‐assemblies. We demonstrated the construction of two hetero‐cages with a single internal functional group as well as a hetero‐cage with two distinct endohedral functionalities. The endo‐functionalized hetero‐cages bound sulfonate guests with fast‐exchange dynamics. This strategy provides a new solution for the controlled endo‐functionalization of supramolecular cavities.
Circularly Polarized Lasing from a Microcavity Filled with Achiral Single‐Crystalline Microribbons
Authors: Liang Qian , Ma Xuekai , Long Teng , Yao Jiannian , Liao Qing , Fu Hongbing
Published: December 2022

Organic circularly polarized (CP) lasers have received increasing attention due to their future photoelectric applications. Here, we demonstrate a CP laser from a pure organic crystal‐filled microcavity without any chiral molecules or chiral structures. Benefited from the giant anisotropy and excellent laser gain of organic crystals, optical Rashba‐Dresselhaus spin‐orbit coupling effect can be induced and is conductive to the CP laser in such microcavities. The maximum dissymmetry factor of the CP lasing with opposite helicities reachs 1.2. Our strategy may provide a new idea for the design of CP lasers towards future 3D laser displays, information storage and other fields.
Tuning the low rolling resistance, wet grip, and heat build‐up properties of tyre tread formulations using carbon black/thermally exfoliated graphite hybrid fillers
Authors: Bijina Vijayan , Jandas Ponnath Janardhanan , Jose Jesvin , Muhammed Ajnas Nellorammal , Abhitha Kozhikodan Parambil , John Honey
Published: December 2022

Ecofriendly green tyre tread compounds were developed with low rolling resistance, low heat buildup, and improved wet grip properties. A standard formulation of natural rubber (NR) and butadiene (BR) with 50 phr carbon black was prepared in a brabender plasticoder. Based on the processability, successful reduction of carbon black and aromatic oil content was done up to a minimum value of 32 and 3 phr respectively. Partial replacement of graphite with carbon black was done to achieve the optimized formulation. A binary filler system with 10 phr graphite and 22 phr carbon black was optimized based on the mechanical properties and further addition of graphite leads to reduction in properties due to agglomeration. To enhance the properties further, the graphite was thermally treated to get an exfoliated structure which can significantly improve the area of the filler/matrix macromolecules interface. This ultimately had a positive impact on targeted properties. A sudden thermal shock for 15 min at various temperatures ranging from 400 to 550°C was given and prepared the optimized binary formulation and evaluated the properties. Excellent results in terms of low rolling resistance (0.039) and heat build‐up (18°C) were recorded for final formulation. The flex fatigue resistance was enhanced and the thermal stability improved by 29°C.
A fabrication strategy for porous carbon spheres based on cross‐linked chitosan/poly(γ‐glutamic acid) colloidal particles
Authors: Sun Jingru , Liu Huan , Xu Sheng , Zhu Ying , Xia Chunmiao , Gan Lei , Zhang Rongli , Zhang Cuige , Miao Zongcheng
Published: December 2022

A new strategy was developed to prepare nanoscale porous carbon spheres (PCSs) using cross‐linked chitosan/poly(γ‐glutamic acid) colloidal particles as precursor. The fabricated cross‐linked chitosan/poly(γ‐glutamic acid) colloidal particles (Ca2+/CS/γ‐PGA CPs) were prepared from the self‐assembly of negatively charged poly(γ‐glutamic acid) and positively charged chitosan, and the cross‐linking of Ca2+ in aqueous solution, via the electrostatic interaction. After lyophilization, the Ca2+/CS/γ‐PGA CPs power was obtained, followed by carbonization in a tube furnace under N2 atmosphere. Finally, the products were washed by hydrochloric acid, obtaining PCSs with hierarchical pore structure and super‐hydrophobicity. The prepared PCSs exhibited excellent separation performance for oil‐in‐water emulsions.
Moxibustion improved the effect of fecal microbiota transplantation donor to dextran sulfate sodium‐induced colitis in mice
Authors: Wang Xinting , Wu Jihong , Huang Rui , Wang Shenglan
Published: December 2022

Fecal microbiota transplantation (FMT) is beneficial for several gastrointestinal diseases because it alters the intestinal microbiota of recipients. The efficacy of FMT is related to the microbial structure and composition of the donor. Mild moxibustion is a non‐invasive and safe traditional Chinese therapy that can regulate the gut microbiota. In this study, we investigated whether moxibustion improved the efficacy of FMT in donors using a dextran sulfate sodium (DSS)‐induced colitis mouse model. Normal mice were treated with mild moxibustion at acupoints ST25 and ST36 for 7 days. DSS (2%) was administered for 7 days to induce colitis. FMT was performed on Day 8 and lasted for 7 days. The effect of FMT on mice with DSS was observed on Day 21. Using hematoxylin and eosin staining and immunofluorescence, we analyzed the pathology and cell proliferation after FMT in DSS mice. In addition, using 16 S rDNA sequencing analysis, we investigated the gut microbiota of mice. The results indicated that moxibustion altered the colonic microbial community and increased the relative abundance of specific bacteria without changes in morphology and physiological function in normal mice. FMT using donors with moxibustion reduced body weight loss, inflammation, abnormal microbial community structure, and the relative abundance of some bacteria. These results provide potential strategies for the safe and targeted improvement of FMT donors.
Enalapril increases the urinary excretion of metformin in rats by inducing multidrug and toxin excretion protein 1 in the kidney
Authors: Gou Xue‐yan , Wu Yan‐fang , Ran Feng‐lin , Ma Yan‐rong , Wu Xin‐an
Published: December 2022

Two‐thirds of patients with type 2 diabetes mellitus have hypertension, and thus the combination of two or more drugs to treat these diseases is common. It has been shown that the combination of metformin and enalapril has beneficial effects, but few studies have evaluated the interactions between these two drugs. This study investigated the effects of enalapril on the pharmacokinetics and urinary excretion of metformin in rats, with a focus on transporter‐mediated drug interactions. Rats were dosed orally with metformin alone (100 mg/kg) or in combination with enalapril (4 mg/kg). The concentration of metformin was measured by high performance liquid chromatography and the level of organic cation transporters (rOCTs) and multidrug and toxin excretion protein 1 (rMATE1), which mediate the uptake and efflux of metformin, respectively, were evaluated by immunoblotting. After single and 7‐day dosing, the plasma concentration of metformin in the co‐administration group was significantly lower than that in the metformin‐only group, and the CL/F and urinary excretion were increased in the co‐administration group. Enalapril did not affect the Kp of metformin but reduced renal slice‐uptake of metformin. The expression of rMATE1 was increased, whereas rOCT2 expression was decreased in rat kidney. Importantly, long‐term co‐administration of metformin and enalapril markedly decreased the level of lactic acid and uric acid in the blood. Enalapril increases the urinary excretion of metformin through the up‐regulation of rMATE1. This reveals a new mechanism of drug interactions and provides a basis for drug dosage adjustment when these drugs are co‐administered.
Determination of pioglitazone hydrochloride by flow injection chemiluminescence tris(2,2′‐bipyridyl)ruthenium(II)–silver(III) complex system
Authors: Rehman Habib Ur , Kakar Attiq Ur Rehman , Yaqoob Mohammed , Asghar Muhammad , Saeed Ahmed Syed , Nisa Khair Un
Published: December 2022

A novel flow injection‐chemiluminescence (FI–CL) approach is proposed for the assay of pioglitazone hydrochloride (PG‐HCl) based on its enhancing influence on the tris(2,2′‐bipyridyl)ruthenium(II)–silver(III) complex (Ru(bipy)32+‐DPA) CL system in sulfuric acid medium. The possible CL reaction mechanism is discussed with CL and ultraviolet (UV) spectra. The optimum experimental conditions were found as: Ru(bipy)32+, 5.0 × 10−5 M; sulfuric acid, 1.0 × 10−3 M; diperiodatoargentate(III) (DPA), 1.0 × 10−4 M; potassium hydroxide, 1.0 × 10−3 M; flow rate 4.0 ml min−1for each flow stream and sample loop volume, 180 μl. The CL intensity of PG‐HCl was linear in the range of 1.0 × 10−3to 5.0 mg L−1(R2 = 0.9998,n = 10) with limit of detection [LOD, signal‐to‐noise ratio (S/N) = 3] of 2.2 × 10−4 mg L−1, limit of quantification (LOQ,S/N = 10) of 6.7 × 10−4 mg L−1, relative standard deviation (RSD) of 1.0 to 3.3% and sampling rate of 106 h−1. The methodology was satisfactorily used to quantify PG‐HCl in pharmaceutical tablets with recoveries ranging from 93.17 to 102.77 and RSD from 1.9 to 2.8%.