bluuebunny/crossref_metadata_2025 huggingface dataset:
Surface Charge Modification on 2D Nanofluidic Membrane for Regulating Ion Transport
Authors: Xie Linhan , Tang Jiadong , Qin Runan , Zhang Qianqian , Liu Jingbing , Jin Yuhong , Wang Hao
Published: November 2022

2D nanofluidic membranes are capable of regulating ion transport toward various applications concerning energy and environment, which is primarily contributed by the excess charge on the interior surface of narrow nanoscale pores. However, there is still a lack of comprehensive summaries and discussions on the surface charge modification principles and strategies of 2D nanofluidic membranes, as well as the practical applications of charge‐modified 2D nanofluidic membranes for regulating ion transport. In this review, the surface charge modification principles and charge modification methods of 2D nanofluidic membranes are first introduced in detail, which is of great significance for improving the ion regulation capability of membranes and realizing the design of nanochannel materials. Next, recent advances in the two typical applications of concentration cells and water treatment based on charge‐modified 2D nanofluidic membranes are summarized. Finally, some challenges and prospects related to charge‐modified 2D nanofluidic membranes are discussed to indicate directions for future research in this field. It is anticipated that this review will provide valuable strategies for the development of high‐performance charge‐modified 2D nanofluidic membranes toward energy and environment applications.
Probabilistic Neural Computing with Stochastic Devices
Authors: Misra Shashank , Bland Leslie C. , Cardwell Suma G. , Incorvia Jean Anne C. , James Conrad D. , Kent Andrew D. , Schuman Catherine D. , Smith J. Darby , Aimone James B.
Published: November 2022

The brain has effectively proven a powerful inspiration for the development of computing architectures in which processing is tightly integrated with memory, communication is event‐driven, and analog computation can be performed at scale. These neuromorphic systems increasingly show an ability to improve the efficiency and speed of scientific computing and artificial intelligence applications. Herein, it is proposed that the brain's ubiquitous stochasticity represents an additional source of inspiration for expanding the reach of neuromorphic computing to probabilistic applications. To date, many efforts exploring probabilistic computing have focused primarily on one scale of the microelectronics stack, such as implementing probabilistic algorithms on deterministic hardware or developing probabilistic devices and circuits with the expectation that they will be leveraged by eventual probabilistic architectures. A co‐design vision is described by which large numbers of devices, such as magnetic tunnel junctions and tunnel diodes, can be operated in a stochastic regime and incorporated into a scalable neuromorphic architecture that can impact a number of probabilistic computing applications, such as Monte Carlo simulations and Bayesian neural networks. Finally, a framework is presented to categorize increasingly advanced hardware‐based probabilistic computing technologies.
Tethered Small‐Molecule Acceptors Simultaneously Enhance the Efficiency and Stability of Polymer Solar Cells
Authors: Li Shangyu , Zhang Rui , Zhang Ming , Yao Jia , Peng Zhengxing , Chen Qi , Zhang Cen , Chang Bowen , Bai Yang , Fu Hongyuan , Ouyang Yanni , Zhang Chunfeng , Steele Julian A. , Alshahrani Thamraa , Roeffaers Maarten B.J. , Solano Eduardo , Meng Lei , Gao Feng , Li Yongfang , Zhang Zhi‐Guo
Published: November 2022

For polymer solar cells (PSCs), the mixture of polymer donors and small‐molecule acceptors (SMAs) is fine‐tuned to realize a favorable kinetically trapped morphology and thus a commercially viable device efficiency. However, the thermodynamic relaxation of the mixed domains within the blend raises concerns related to the long‐term operational stability of the devices, especially in the record‐holding Y‐series SMAs. Here, a new class of dimeric Y6‐based SMAs tethered with differential flexible spacers is reported to regulate their aggregation and relaxation behavior. In their polymer blends with PM6, it is found that they favor an improved structural order relative to that of Y6 counterpart. Most importantly, the tethered SMAs show large glass transition temperatures to suppress the thermodynamic relaxation in mixed domains. For the high‐performing dimeric blend, an unprecedented open circuit voltage of 0.87 V is realized with a conversion efficiency of 17.85%, while those of regular Y6‐base devices only reach 0.84 V and 16.93%, respectively. Most importantly, the dimer‐based device possesses substantially reduced burn‐in efficiency loss, retaining more than 80% of the initial efficiency after operating at the maximum power point under continuous illumination for 700 h. The tethering approach provides a new direction to develop PSCs with high efficiency and excellent operating stability.
Low‐Voltage Intrinsically Stretchable Organic Transistor Amplifiers for Ultrasensitive Electrophysiological Signal Detection
Authors: Liu Kai , Wang Chengyu , Liu Bowen , Bian Yangshuang , Kuang Junhua , Hou Yangkun , Pan Zhichao , Liu Guocai , Huang Xin , Zhu Zhiheng , Qin Mingcong , Zhao Zhiyuan , Jiang Chen , Liu Yunqi , Guo Yunlong
Published: November 2022

Stretchability is a prerequisite for electronic skin devices. However, state‐of‐the‐art stretchable thin‐film transistors do not possess sufficiently low operating voltages and good stability, significantly limiting their use in real‐world biomedical applications. Herein, a van der Waals‐controlling elastomer/carbon quantum dot interfacial polarization methodology is proposed to form a hybrid polymer dielectric with 620% tensile strain and large‐area film uniformity (>A4 paper size). Using the hybrid polymer dielectrics, the prepared intrinsically stretchable organic thin‐film transistors demonstrate a low operating voltage below 5 V, 100% strain tolerance, and excellent operational stability, as well as a high on‐current/off‐current ratio of 105 and a steep subthreshold slope of 500 mV dec−1. Based on this device technology, an amplifier with a high gain of 90 V V−1 among the highest values of reported stretchable transistors is realized. This amplifier is at the first time applied to detect human electrophysical signals with an output signal amplitude of over 0.2 V, which even outperforms other types of the state‐of‐the‐art organic amplifiers for human electrophysiology monitoring. This stretchable device technology sufficiently meets the safety and portability requirements of wearable biomedical applications, opening a new opportunity to e‐skin with signal control and amplification capabilities.
Mechanical Janus Structures by Soft–Hard Material Integration
Authors: Zhang Haozhe , Yang Weizhu , Liu Qingchang , Gao Yuan , Yue Zhufeng , Xu Baoxing
Published: November 2022

Engineering Janus structures that possess anisotropic features in functions have attracted growing attention for a wide range of applications in sensors, catalysis, and biomedicine, and are yet usually designed at the nanoscale with distinct physical or chemical functionalities in their opposite sides. Inspired by the seamless integration of soft and hard materials in biological structures, here a mechanical Janus structure composed of soft and hard materials with a dramatic difference in mechanical properties at an additively manufacturable macroscale is presented. In the combination of extensive experimental, theoretical, and computational studies, the design principle of soft–hard materials integrated mechanical Janus structures is established and their unique rotation mechanism is addressed. The systematic studies of assembling the Janus structure units into superstructures with well‐ordered organizations by programming the local rotations are further shown, providing a direct route of designing superstructures by leveraging mechanical Janus structures with unique soft–hard material integration. Applications are conducted to demonstrate the features and functionalities of assembled superstructures with local ordered organizations in regulating and filtering acoustic wave propagations, thereby providing exemplification applications of mechanical Janus design in functional structures and devices.
Bifunctional Integration Performed by a Broadband High‐Efficiency Spin‐Decoupled Metasurface
Authors: Yang Ling‐Jun , Sun Sheng , Sha Wei E. I. , Hu Jun
Published: November 2022

Achieving broadband multitasked integration on an ultrathin interface is pivotal to increasing data capacity. However, broadband bifunctional metasurfaces exhibiting high‐efficiency and crosstalk‐free characteristics are rarely seen. Here, three broadband spin‐decoupled criteria are developed to design the meta‐atoms of high‐efficiency bifunctional metasurfaces. Specifically, six dipole‐loaded quasi‐I‐shaped meta‐atoms are proposed to satisfy the broadband spin‐decoupled criteria in radio band from 8.6 to 17.8 GHz (about 70% bandwidth) with more than 90% efficiency. The metasurface equipped with the proposed meta‐atoms can keep dispersionless phase gradients and crosstalk‐free characteristics in two orthogonal circular polarizations. This work demonstrates the broadband scheme with spin‐decoupled bifunctional metasurface, yielding two independent broadband multimode vortex beams in two completely decoupled helicities. Besides, other possible applications of the proposed meta‐atoms are illustrated from the perspective of the half‐wave plant (polarization control). Accordingly, the other multitasked‐type bifunctional metasurface is fabricated to achieve the broadband integration of two different functionalities: polarization conversion and full‐polarization anomalous refraction. The proposed schemes offer broadband, polarization‐multiplexing, and multitasked‐integration routes for complex electromagnetic wave manipulations within a subwavelength thickness, which can stimulate the development of electromagnetic/optical integration devices with broadband multiplexing techniques.
Crystal Growth of 3D Poly(ε‐caprolactone) Based Bone Scaffolds and Its Effects on the Physical Properties and Cellular Interactions
Authors: Huang Boyang , Wang Yaxin , Vyas Cian , Bartolo Paulo
Published: November 2022

Extrusion additive manufacturing is widely used to fabricate polymer‐based 3D bone scaffolds. However, the insight views of crystal growths, scaffold features and eventually cell‐scaffold interactions are still unknown. In this work, melt and solvent extrusion additive manufacturing techniques are used to produce scaffolds considering highly analogous printing conditions. Results show that the scaffolds produced by these two techniques present distinct physiochemical properties, with melt‐printed scaffolds showing stronger mechanical properties and solvent‐printed scaffolds showing rougher surface, higher degradation rate, and faster stress relaxation. These differences are attributed to the two different crystal growth kinetics, temperature‐induced crystallization (TIC) and strain‐induced crystallization (SIC), forming large/integrated spherulite‐like and a small/fragmented lamella‐like crystal regions respectively. The stiffer substrate of melt‐printed scaffolds contributes to higher ratio of nuclear Yes‐associated protein (YAP) allocation, favoring cell proliferation and differentiation. Faster relaxation and degradation of solvent‐printed scaffolds result in dynamic surface, contributing to an early‐stage faster osteogenesis differentiation.
Boosted Heterogeneous Catalysis by Surface‐Accumulated Excess Electrons of Non‐Oxidized Bare Copper Nanoparticles on Electride Support
Authors: Han Sung Su , Thacharon Athira , Kim Jun , Chung Kyungwha , Liu Xinghui , Jang Woo‐Sung , Jetybayeva Albina , Hong Seungbum , Lee Kyu Hyoung , Kim Young‐Min , Cho Eun Jin , Kim Sung Wng
Published: November 2022

Engineering active sites of metal nanoparticle‐based heterogeneous catalysts is one of the most prerequisite approaches for the efficient production of chemicals, but the limited active sites and undesired oxidation on the metal nanoparticles still remain as key challenges. Here, it is reported that the negatively charged surface of copper nanoparticles on the 2D [Ca2N]+∙e− electride provides the unrestricted active sites for catalytic selective sulfenylation of indoles and azaindoles with diaryl disulfides. Substantial electron transfer from the electride support to copper nanoparticles via electronic metal–support interactions results in the accumulation of excess electrons at the surface of copper nanoparticles. Moreover, the surface‐accumulated excess electrons prohibit the oxidation of copper nanoparticle, thereby maintaining the metallic surface in a negatively charged state and activating both (aza)indoles and disulfides under mild conditions in the absence of any further additives. This study defines the role of excess electrons on the nanoparticle‐based heterogeneous catalyst that can be rationalized in versatile systems.
Ultra‐Narrowband Blue Multi‐Resonance Thermally Activated Delayed Fluorescence Materials
Authors: Oda Susumu , Kawakami Bungo , Horiuchi Masaru , Yamasaki Yuki , Kawasumi Ryosuke , Hatakeyama Takuji
Published: November 2022

Ultra‐narrowband blue multi‐resonance‐induced thermally activated delayed fluorescence (MR‐TADF) materials (V‐DABNA and V‐DABNA‐F), consisting of three DABNA subunits possessing phenyl or 2,6‐difluorophenyl substituents on the peripheral nitrogen atoms are synthesized by one‐shot triple borylation. Benefiting from the inductive effect of fluorine atoms, the emission maximum of V‐DABNA‐F (464 nm) is blueshifted from that of the parent V‐DABNA (481 nm), while maintaining a small full width at half maximum (FWHM, 16 nm) and a high rate constant for reverse intersystem crossing (6.5 × 105 s−1). The organic light‐emitting diodes (OLEDs) using V‐DABNA and V‐DABNA‐F as emitters are fabricated by vapor deposition and exhibit blue emission at 483 and 468 nm with small FWHMs of 17 and 15 nm, corresponding to Commission Internationale d’Éclairage coordinates of (0.09, 0.27) and (0.12, 0.10), respectively. Both devices achieve high external quantum efficiencies of 26.2% and 26.6% at the maximum with minimum efficiency roll‐offs of 0.9% and 3.2%, respectively, even at 1000 cd m−2, which are record‐setting values for blue MR‐TADF OLEDs.
The molecular genetics of RASopathies: An update on novel disease genes and new disorders
Authors: Tartaglia Marco , Aoki Yoko , Gelb Bruce D.
Published: November 2022

Enhanced signaling through RAS and the mitogen‐associated protein kinase (MAPK) cascade underlies the RASopathies, a family of clinically related disorders affecting development and growth. In RASopathies, increased RAS‐MAPK signaling can result from the upregulated activity of various RAS GTPases, enhanced function of proteins positively controlling RAS function or favoring the efficient transmission of RAS signaling to downstream transducers, functional upregulation of RAS effectors belonging to the MAPK cascade, or inefficient signaling switch‐off operated by feedback mechanisms acting at different levels. The massive effort in RASopathy gene discovery performed in the last 20 years has identified more than 20 genes implicated in these disorders. It has also facilitated the characterization of several molecular activating mechanisms that had remained unappreciated due to their minor impact in oncogenesis. Here, we provide an overview on the discoveries collected during the last 5 years that have delivered unexpected insights (e.g., Noonan syndrome as a recessive disease) and allowed to profile new RASopathies, novel disease genes and new molecular circuits contributing to the control of RAS‐MAPK signaling.
COVID‐19: Impact on children living in out‐of‐home care and their carers
Authors: Townsend Michelle L. , Tarren‐Sweeney Michael , Hopkins Joanna , Paxman Marina , Dey Proshanta , Katz Ilan
Published: November 2022

Children enter out‐of‐home care (OOHC) having experienced significant childhood adversities and trauma. Little is known about the short‐term impacts of the COVID‐19 pandemic on this vulnerable group. To gain some insights, we analysed the early impacts on the well‐being and experiences of children in OOHC and their carers using the Pathways of Care Longitudinal Study data prior to and post the first lockdown restrictions. A total of 862 children, young people and their carers were interviewed either pre‐COVID‐19 restrictions (n = 567) (April 2019–March 2020) or post‐COVID‐19 restrictions (n = 295) (June–December 2020). While the two groups showed no significant differences in socio‐emotional well‐being, both the pre‐ and the post‐COVID‐19 restriction groups of children in OOHC had slight reductions in socio‐emotional well‐being. The interviews with the post‐COVID‐19 group showed that the pandemic restrictions affected children's well‐being and behaviour, education, social and physical activities, as well as time spent with their birth family. Likewise, interviews with carers post‐COVID‐19 found a negative effect on carers' well‐being, their ability to manage financially and their capacity to care and access services and support. The article contributes new evidence to inform OOHC policy and practice to support service systems facing unique challenges arising from a pandemic.
Tenecteplase Improves Reperfusion across Time in Large Vessel Stroke
Authors: Yogendrakumar Vignan , Beharry James , Churilov Leonid , Alidin Khairunnisa , Ugalde Melissa , Pesavento Lauren , Weir Louise , Mitchell Peter J. , Kleinig Timothy J. , Yassi Nawaf , Thijs Vincent , Wu Teddy Y. , Shah Darshan G. , Dewey Helen M. , Wijeratne Tissa , Yan Bernard , Desmond Patricia M. , Sharma Gagan , Parsons Mark W. , Donnan Geoffrey A. , Davis Stephen M. , Campbell Bruce C. V. ,   for the Royal Melbourne Stroke Registry and EXTEND‐IA TNK Collaborators
Published: November 2022

Objective

Tenecteplase improves reperfusion compared to alteplase in patients with large vessel occlusions. To determine whether this improvement varies across the spectrum of thrombolytic agent to reperfusion assessment times, we performed a comparative analysis of tenecteplase and alteplase reperfusion rates.

Methods

Patients with large vessel occlusion and treatment with thrombolysis were pooled from the Melbourne Stroke Registry, and the EXTEND‐IA and EXTEND‐IA TNK trials. The primary outcome, thrombolytic‐induced reperfusion, was defined as the absence of retrievable thrombus or >50% reperfusion at imaging reassessment. We compared the treatment effect of tenecteplase and alteplase, accounting for thrombolytic to assessment exposure times, via Poisson modeling. We compared 90‐day outcomes of patients who achieved reperfusion with a thrombolytic to patients who achieved reperfusion via endovascular therapy using ordinal logistic regression.

Results

Among 893 patients included in the primary analysis, thrombolytic‐induced reperfusion was observed in 184 (21%) patients. Tenecteplase was associated with higher rates of reperfusion (adjusted incidence rate ratio [aIRR] = 1.50, 95% confidence interval [CI] = 1.09–2.07, p = 0.01). Findings were consistent in patient subgroups with first segment (aIRR = 1.41, 95% CI = 0.93–2.14) and second segment (aIRR = 2.07, 95% CI = 0.98–4.37) middle cerebral artery occlusions. Increased thrombolytic to reperfusion assessment times were associated with reperfusion (tenecteplase: adjusted risk ratio [aRR] = 1.08 per 15 minutes, 95% CI = 1.04–1.13 vs alteplase: aRR = 1.06 per 15 minutes, 95% CI = 1.00–1.13). No significant treatment‐by‐time interaction was observed (p = 0.87). Reperfusion via thrombolysis was associated with improved 90‐day modified Rankin Scale scores (adjusted common odds ratio = 2.15, 95% CI = 1.54–3.01) compared to patients who achieved reperfusion following endovascular therapy.

Interpretation

Tenecteplase, compared to alteplase, increases prethrombectomy reperfusion, regardless of the time from administration to reperfusion assessment. Prethrombectomy reperfusion is associated with better clinical outcomes. ANN NEUROL 2023;93:489–499
A Combined Panel of Salivary Biomarkers in de novo Parkinson's Disease
Authors: De Bartolo Maria Ilenia , Vivacqua Giorgio , Belvisi Daniele , Mancinelli Romina , Fabbrini Andrea , Manzo Nicoletta , Costanzo Matteo , Leodori Giorgio , Conte Antonella , Fabbrini Giovanni , Morini Sergio , Berardelli Alfredo
Published: November 2022

Objective

To investigate molecular biomarkers of a‐synuclein and tau aggregation, autophagy, and inflammation in the saliva of de novo Parkinson's disease (PD) patients in comparison to healthy subjects (HS), and to correlate molecular data with clinical features of PD patients, in order to establish whether abnormalities of these parameters are associated with specific clusters of de novo PD patients, and their potential diagnostic power in differentiating PD patients from HS.

Methods

We measured total and oligomeric a‐synuclein, total‐tau and phosphorylated‐tau, microtubule‐associated protein light chain 3 beta (MAP‐LC3beta), and tumor necrosis factor alpha (TNFalpha) in the saliva of 80 de novo PD patients and 62 HS, using quantitative enzyme‐linked immunosorbent Assay analysis.

Results

Oligomeric a‐synuclein, total‐tau, MAP‐LC3beta, and TNFalpha levels resulted significantly higher in patients with respect to HS, while no significant differences were detected for total a‐synuclein or phosphorylated‐tau. Phosphorylated‐tau directly correlated with MAP‐LC3beta, whereas it inversely correlated with TNFalpha in PD patients. An inverse correlation was detected between MAP‐LC3beta and non‐motor symptoms severity. Principal Component Analysis showed that molecular and clinical parameters were independent of each other in de novo PD patients. Receiver operating characteristic curve analysis reported an accurate diagnostic performance of oligomeric a‐synuclein and MAP‐LC3beta. The diagnostic accuracy of total a‐synuclein increased when it was combined with other salivary biomarkers targeting different molecular pathways.

Interpretation

Our study proposes a novel biomarker panel using saliva, a non‐invasive biofluid, in de novo PD patients, with implications in understanding the molecular pathways involved in PD pathogenesis and the relevance of different molecular pathways in determining clinical PD subtypes. ANN NEUROL 2023;93:446–459
Chemical Upcycling of Conventional Polyureas into Dynamic Covalent Poly(aminoketoenamide)s
Authors: Ma Youwei , Jiang Xuesong , Yin Jie , Weder Christoph , Berrocal José Augusto , Shi Zixing
Published: November 2022

The chemical upcycling of polymers is an emerging strategy to transform post‐consumer waste into higher‐value chemicals and materials. However, on account of the high stability of the chemical bonds that constitute their main chains, the chemical modification of many polymers proves to be difficult. Here, we report a versatile approach for the upcycling of linear and cross‐linked polyureas, which are widely used because of their high chemical stability. The treatment of these polymers or their composites with acetylacetone affords di‐vinylogous amide‐terminated compounds in good yield. These products can be reacted with aromatic isocyanates, and the resulting aminoketoenamide bonds are highly dynamic at elevated temperatures. We show here that this conversion scheme can be exploited for the preparation of dynamic covalent poly(aminoketoenamide) networks, which are healable and reprocessable through thermal treatment without any catalyst.
Off‐center Mechanophore Activation in Block Copolymers
Authors: Zhang Hang , Diesendruck Charles E.
Published: November 2022

Block copolymers (BCPs) are used in numerous applications in modern materials science. Yet, like homopolymers, BCPs can undergo covalent bond scission when mechanically stressed (mechanochemistry), which could lead to unexpected consequences in such applications. BCPs’ heterogeneity may affect force transduction, perhaps changing force distribution and localization. To verify this, agem‐dichlorocyclopropane (gDCC) embedded linear chain is prepared and extended with a poly(methyl methacrylate) block. When stressed in solution, the mechanochemical ring‐opening ofgDCC is accelerated compared to homopolymers, even though the mechanophores are at the chain ends. Moreover, a higher mechanophore activation selectivity is obtained. These results indicate that mechanochemical response outside, and even far from the chain center is quite prominent in BCPs, and that forces along the polymer chain can efficiently activate multi‐mechanophores regions, even when far from the polymer midchain.
Regulating the Mechanical and Optical Properties of Polymer‐based Nanocomposites by Sub‐Nanowires
Authors: Yuan Feng , Ouyang Chen , Yang Minzheng , Shi Wenxiong , Ren Weibin , Shen Yang , Wei Yan , Deng Xuliang , Wang Xun
Published: November 2022

Sub‐nanowires (SNWs) exhibit great potential applications in nanocomposites owing to their high specific surface area, high flexibility, and similarity to polymer chains in dimension, which are a good entry point to bridge inorganic materials and polymer materials. Herein, we synthesized hydroxyapatite sub‐nanowires (HAP SNWs) and engineered hydroxyapatite sub‐nanowires/polyimide (HSP) gels and films by simple mixing of HAP SNWs and polyimide (PI). Benefiting from the interactions between HAP SNWs and PI, these nanocomposites were a continuous hybrid network. As the increase of HAP SNWs contents, the viscosity and modulus of HSP gels were greatly improved by one or two orders of magnitude compared with PI gel. HSP films not only maintained high transparency but also gained high haze, as well as exhibited enhanced Young's modulus. Thus, both HSP gels and films developed in this work are promising for various applications in coatings and high‐performance films.
Polyphosphinoborane Block Copolymer Synthesis Using Catalytic Reversible Chain‐Transfer Dehydropolymerization
Authors: Race James J. , Heyam Alex , Wiebe Matthew A. , Diego‐Garcia Hernandez J. , Ellis Charlotte E. , Lei Shixing , Manners Ian , Weller Andrew S.
Published: November 2022

An amphiphilic block copolymer of polyphosphinoborane has been prepared by a mechanism‐led strategy of the sequential catalytic dehydropolymerization of precursor monomers, H3B ⋅ PRH2(R=Ph, n‐hexyl), using the simple pre‐catalyst [Rh(Ph2PCH2CH2PPh2)2]Cl. Speciation, mechanism and polymer chain growth studies support a step‐growth process where reversible chain transfer occurs, i.e. H3B ⋅ PRH2/oligomer/polymer can all coordinate with, and be activated by, the catalyst. Block copolymer [H2BPPhH]110‐b‐[H2BP(n‐hexyl)H]11can be synthesized and self‐assembles in solution to form either rod‐like micelles or vesicles depending on solvent polarity.
Single Solution‐Phase Synthesis of Charged Covalent Organic Framework Nanosheets with High Volume Yield
Authors: Huang Tong , Jiang Haifei , Douglin John C. , Chen Yu , Yin Shuoyao , Zhang Junfeng , Deng Xiaojuan , Wu Hong , Yin Yan , Dekel Dario R. , Guiver Michael D. , Jiang Zhongyi
Published: November 2022

Covalent organic framework nanosheets (COF‐NSs) are emerging building blocks for functional materials, and their scalable fabrication is highly desirable. Current synthetic methods suffer from low volume yields resulting from confined on‐surface/at‐interface growth space and complex multiple‐phase synthesis systems. Herein, we report the synthesis of charged COF‐NSs in open space using a single‐phase organic solution system, achieving magnitudes higher volume yields of up to 18.7 mg mL−1. Charge‐induced electrostatic repulsion forces enable in‐plane anisotropic secondary growth from initial discrete and disordered polymers into large and crystalline COF‐NSs. The charged COF‐NS colloidal suspensions are cast into thin and compact proton exchange membranes (PEMs) with lamellar morphology and oriented crystallinity, displaying outstanding proton conductivity, negligible dimensional swelling, and good H2/O2 fuel cell performance.
Chemically crosslinked polyvinyl alcohol for water shut‐off and conformance control treatments during oil production: The effect of silica nanoparticles
Authors: Rajabi M. Sadegh , Moradi Rasoul , Andrade L. Omar
Published: November 2022

Polyvinyl alcohol (PVA) is a synthetic commercial polymer with the inherent hydrophilicity, thermal and chemical resistance, ecofriendly, and a high anti‐fouling potential making it an attractive choice for water treatment applications, but has been less studied for oil and gas industry applications. On the other hands, nowadays nanotechnology has gained an important space within most core areas in upstream oil and gas operations. The present work, first PVA at various concentrations, was added to 5 wt% NaCl solution and then, crosslinked by formaldehyde 37% at two different concentration ratios. To compare, a nanocomposite hydrogel was fabricated in the same way with 1 wt% silica nanoparticles (NPs). Contact angle and filtration test were performed to confirm the ability of PVA hydrogel and nanocomposite hydrogel for oil and water adsorption. Following this, a rheology measurement was made to realize the gelation time of samples and their performance for water shutoff applications. Finally, an experimental flooding setup was designed to inject the fluids into carbonate plugs in order to estimate of oil and water effective permeability, and oil recovery factor (RF) before and after the PVA hydrogel and nanocomposite hydrogel injection. Both samples wettability tests showed a super‐hydrophilic state for brine droplets and neutral state for synthetic oil droplets by using nanocomposite hydrogel. The flooding tests revealed that the PVA hydrogel was clogged the plug with blocking efficiency of 32.83% for water effective permeability and 14.60% for oil effective permeability. This value was calculated to be 50.37% for water effective permeability and 31.36% for oil effective permeability in the case of nanocomposite hydrogel injection. Oil RF was also reported to be 64.58% after injecting PVA hydrogel which was higher than nanocomposite hydrogel injection with RF of 52.08%.
Population dynamics and biorational management of sucking insect vectors on chili (Capsicum annuumL.) in Bangladesh
Authors: Khatun Mst. Fatema , Jahan Mashrat , Das Keya R. , Lee Kyeong‐Yeoll , Kil Eui‐Joon
Published: November 2022

To evaluate population fluctuations in relation to weather parameters and biorational management of sucking insect vectors in chili (Capsicum annuumL.), we conducted a study at the experimental field of Bangabandhu Sheikh Mujibur Rahman Agricultural University, Gazipur, in 2020 and 2021. It has been shown in this study that sucking insects (aphids, jassids, whiteflies, and thrips) were active throughout the study period. The highest count of sucking insect vectors (24.67 aphids, 13.72 whitefly, and 56.56 thrips) in March and (14.83 jassid) in April was recorded at average temperatures of 34–36°C and 31°C, respectively. There was a positive correlation between pest abundance and temperature, relative humidity, and rainfall for all insects, with the exception of a negative correlation between whiteflies and temperature and rainfall. The results of linear regression models showed that abiotic factors contribute to pest abundance levels, with 100R2values of 14.9 (thrips), 46.3 (jassids), 7.1 (whiteflies), and 0.67 (aphids); the results were statistically significant for all models in the case of thrips, jassids, and whiteflies, but not significant in the case of aphids. The most effective treatment was spinosad 45SC, a bacterium‐derived pesticide recommended for the control of sucking insect vector complexes in chili. The results from the spinosad‐treated plot, in terms of insect counts and corresponding mortality rates, were as follows: aphids (3.68), 68.89%; jassids (3.52), 72.01%; whiteflies (3.00), 66.69%; and thrips (3.40), 69.20%. The results of this study will aid in developing predictive models of different control agents against sucking insect vectors in vegetable crops.
Director's network location and corporate environmental investment in the carbon neutrality age
Authors: Wang Liukai , Su Yun , Huang Heshu , Gong Yu , Wang Weiqin
Published: November 2022

Although carbon neutrality is a global aim, the potential drivers and influence mechanisms of corporate governance communities are unclear. This study examines the impact of director's network location on corporate environmental investment (CEI) and explores potential channels for CEI performance changes. Using a sample of 495 listed firms in China from 2015 to 2019, we construct a director‐based network using contacts of independent company directors. Results indicate that director's network location has positive economic impacts on CEI performance and that financing constraints are an important mechanism of director's networks affecting CEI. Director's networks positively affect corporate performance by improving CEI. Results are robust to endogeneity concerns and contribute to the CEI literature by showing a positive effect between director's network and CEI, as well as between director's network and enterprise value. This paves the way for policymakers, managers, and investors to understand the influence of director's network on CEI performance.
Peptide‐functionalized double network hydrogel with compressible shape memory effect for intervertebral disc regeneration
Authors: Ho Chia‐Yu , Wang Chen‐Chie , Wu Tsung‐Chiao , Kuan Chen‐Hsiang , Liu Yu‐Chung , Wang Tzu‐Wei
Published: November 2022

As a prominent approach to treat intervertebral disc (IVD) degeneration, disc transplantation still falls short to fully reconstruct and restore the function of native IVD. Here, we introduce an IVD scaffold consists of a cellulose‐alginate double network hydrogel‐based annulus fibrosus (AF) and a cellulose hydrogel‐based nucleus pulposus (NP). This scaffold mimics native IVD structure and controls the delivery of Growth Differentiation Factor‐5 (GDF‐5), which induces differentiation of endogenous mesenchymal stem cells (MSCs). In addition, this IVD scaffold has modifications on MSC homing peptide and RGD peptide which facilitate the recruitment of MSCs to injured area and enhances their cell adhesion property. The benefits of this double network hydrogel are high compressibility, shape memory effect, and mechanical strength comparable to native IVD. In vivo animal study demonstrates successful reconstruction of injured IVD including both AF and NP. These findings suggest that this double network hydrogel can serve as a promising approach to IVD regeneration with other potential biomedical applications.
Recent advances in surgical strategies and liver transplantation for hepatoblastoma
Authors: Honda Masaki , Uchida Koushi , Irie Tomoaki , Hirukawa Kazuya , Kadohisa Masashi , Shimata Keita , Isono Kaori , Shimojima Naoki , Sugawara Yasuhiko , Hibi Taizo
Published: November 2022

Hepatoblastoma (HB) is the most common malignant liver tumor in children. Although the development of treatment strategies with advances in chemotherapy has greatly improved the prognosis of HB, surgical resection and liver transplantation still play a vital role in the treatment of HB. In recent years, technological innovations have led to the development of new surgical approaches for HB. In this review, we describe the latest research on the surgical management of HB, including new imaging technologies, minimally invasive approaches, and the application of associating liver partition portal vein ligation for staged hepatectomy. We also discuss the current role of liver transplantation, use of ante‐situm or ex‐situ liver resection with auto‐transplantation, and management of metastatic HB.
Long‐term outcomes after paclitaxel‐coated balloon angioplasty of femoropopliteal arteries in Asian patients of the IN.PACT Global Study
Authors: Ko Young‐Guk , Choi Donghoon , Rha Seung‐Woon , Won Je Hwan , Do Young‐Soo , Lee Seung‐Whan , Menk Jeremiah S. , Kum Steven
Published: November 2022

Objectives

The long‐term data on the use of drug‐coated balloons (DCBs) for femoropopliteal atherosclerotic lesions in the real‐world setting are limited, even more so for racially and geographically distinct populations. The present analysis reports the 5‐year safety and effectiveness outcomes of a DCB in the Asian subset of the prospective, real‐world IN.PACT Global Study.

Methods

The IN.PACT Global Study was a prospective, multicenter, international, single‐arm study designed to assess the long‐term safety and effectiveness of the IN.PACT Admiral DCB in real‐world participants with femoropopliteal artery disease. The present analysis included 114 Asian participants (138 lesions) treated in South Korea and Singapore. Assessments through 5 years included freedom from clinically driven target lesion revascularization, the safety endpoint (a composite of freedom from device‐ and procedure‐related mortality through 30 days; and freedom from major target limb amputation and clinically driven target vessel revascularization within 60 months after the index procedure) and major adverse events.

Results

In this prespecified Asian subset, there was a high incidence of diabetes mellitus (54.4%), hypertension (78.1%), coronary artery disease (43.9%), and concomitant below‐the‐knee vascular disease of target leg (39.5%). Mean lesion length was 17.4 ± 12.4 cm; 26.8% were in‐stent restenosis, and more than half of the lesions were totally occluded (51.4%) and calcified (54.3%). The 5‐year Kaplan–Meier estimate of freedom from clinically driven target lesion revascularization was 77.1% (95% confidence interval: 67.0%–84.5%). The safety composite endpoint was 76.0%; the cumulative incidence of all‐cause mortality was 19.9%, and no major target limb amputations were reported through 5 years.

Conclusions

This subset analysis of Asian participants from the IN.PACT Global Study demonstrated consistent results with the previously reported data of the IN.PACT Admiral DCB. The data confirm the durable clinical effectiveness and safety profile of the DCB through 5 years for femoropopliteal atherosclerotic disease in this real‐world population.
Bail out lithotripsy to treat delayed valve‐in‐valve TAVR‐related coronary obstruction
Authors: Bingen Brian O. , Al Amri Ibtihal , Montero‐Cabezas Jose M. , van der Kley Frank
Published: November 2022

Coronary access difficulty and stent compression by the juxtaposed aortic valve leaflet hamper percutaneous management of delayed coronary artery obstruction (CAO) after valve‐in‐valve (Edwards Sapien 3 in St. Jude Trifecta) transcatheter aortic valve replacement (TAVR). Here, we present a case of delayed post‐TAVR CAO treated with intravascular lithotripsy and multistenting to overcome stent compression by the adjacent calcified leaflet.
Interdisciplinary diagnosis and treatment planning for Class III malocclusion and determining the appropriate anterior tooth positions for individual patients
Authors: Khan Ambereen , Freer Elissa , Ong Desmond
Published: November 2022

Patients presenting with Class III malocclusion often present significant challenges for the orthodontist and restorative clinician. The characteristic anterior crossbite is commonly associated with a maxillo‐mandibular skeletal base discrepancy leading to both functional and esthetic issues. Three potential incisal tooth positions are discussed using clinical examples including implants.
Localized Electric Field‐Induced Efficient Photocatalytic Oxidation over Cu‐Doped WO3 Nanofibers with Strong Dopant/Matrix Interaction
Authors: Chen Lv , Lin Yuan , Zhang Jianhua , Xiong Jinyan , Gui Yunyun , Liu Lijun
Published: November 2022

Photocatalytic oxidation technology can mineralize hazardous volatile organic compounds (VOCs), but the poor photocatalytic oxidation activity limits its practical application. Here we develop Cu‐doped WO3 electrospun nanofibers through a non‐equivalent doping strategy. The Cu dopant prefers substituting five‐coordinated W atoms atop the WO3 matrix, inducing strong dopant/matrix interaction (SDMI) effect and prominent charge rearrangement. A localized electric field (LEF) forms pointing from positively charged WO3 matrix to negatively charged Cu dopant, which triggers efficient photoexcited charge separation. Further, the Cu dopant promoted the production of ⋅OH radicals and thereby enhanced VOCs photodegradation. The 0.7 % Cu‐doped WO3 nanofibers show optimal photocatalytic oxidation performance towards formaldehyde and acetone, 5.5 and 4.8 times higher than pristine WO3 nanofibers, respectively. This work highlights the role of dopant‐induced LEF on the charge carriers separation and might shed light on developing more efficient photocatalysts with non‐equivalent dopants.
Financial literacy, the risk‐as‐feelings hypothesis, and passive income generation
Authors: Habyarimana Jean Baptiste , Kakkar Vikas
Published: November 2022

Low household wealth has been associated with the lack of participation in risky financial markets. To improve our understanding of how households decide to participate in financial markets, it is important to investigate how financial literacy heterogeneity among heads influences households' risk attitude and capacity and the propensity to invest in various financial markets. Utilizing the U.S. 2016 survey of consumer finances, this article tests the effect of the head's financial literacy on the household's risk attitude and capacity and also examines whether the household's risk tolerance leads to a greater impact of the head's financial literacy on the likelihood of investing in high‐yielding markets. Our key finding is that the head's financial literacy improves the household's risk tolerance, thereby nudging the household to invest in high‐yielding markets. The article identifies improving the head's financial literacy as an efficacious strategy for increasing household wealth via greater participation in higher‐yielding financial markets.
Structural and Functional Insight into the Mechanism of the Fe−S Cluster‐Dependent Dehydratase from Paralcaligenes ureilyticus
Authors: Bayaraa Tenuun , Lonhienne Thierry , Sutiono Samuel , Melse Okke , Brück Thomas B. , Marcellin Esteban , Bernhardt Paul V. , Boden Mikael , Harmer Jeffrey R. , Sieber Volker , Guddat Luke W. , Schenk Gerhard
Published: November 2022

Enzyme‐catalyzed reaction cascades play an increasingly important role for the sustainable manufacture of diverse chemicals from renewable feedstocks. For instance, dehydratases from the ilvD/EDD superfamily have been embedded into a cascade to convert glucose via pyruvate to isobutanol, a platform chemical for the production of aviation fuels and other valuable materials. These dehydratases depend on the presence of both a Fe−S cluster and a divalent metal ion for their function. However, they also represent the rate‐limiting step in the cascade. Here, catalytic parameters and the crystal structure of the dehydratase from Paralcaligenes ureilyticus (PuDHT, both in presence of Mg2+ and Mn2+) were investigated. Rate measurements demonstrate that the presence of stoichiometric concentrations Mn2+ promotes higher activity than Mg2+, but at high concentrations the former inhibits the activity of PuDHT. Molecular dynamics simulations identify the position of a second binding site for the divalent metal ion. Only binding of Mn2+ (not Mg2+) to this site affects the ligand environment of the catalytically essential divalent metal binding site, thus providing insight into an inhibitory mechanism of Mn2+ at higher concentrations. Furthermore, in silico docking identified residues that play a role in determining substrate binding and selectivity. The combined data inform engineering approaches to design an optimal dehydratase for the cascade.
Interplay Between Hydrogen Bonding and Electron Transfer in Mixed Valence Assemblies of Triarylamine Trisamides
Authors: Sallembien Quentin , Aoun Paméla , Blanchard Sébastien , Bouteiller Laurent , Raynal Matthieu
Published: November 2022

Hydrogen‐bonding interactions are assumed to play a critical role in the long‐range transport of light or charge recently observed in supramolecular assemblies of C3‐symmetrical discotic molecules. Herein, the structure of mixed valence assemblies formed by irradiating triarylamine trisamide (TATA) molecules was determined by multifarious techniques under various conditions with the aim of probing the interplay between the hydrogen bonding network and the rate of electron transport in different states (solution, gel, film). Irradiation was performed under initial states that vary by the degree of association of TATA monomers through hydrogen bonds. Firstly, a significant shift of the N−H and C=O stretching frequencies was observed by FTIR upon irradiation thus revealing an overlooked signature of TATA⋅+ species and interacting mixed valence aggregates. Secondly, gels and films both mostly consist of hydrogen‐bonded TATA polymers but their EPR spectra recorded at 293 K reveal very different behaviors: localized electrons in the gels versus fully delocalized electrons in the films. Hydrogen bonding thus appears as a necessary but not sufficient condition to get fast electron transfer rates and a packing of the TATA monomers particularly suitable for charge transport is assumed to exist in the solid state. Finally, defects in the hydrogen bonding network are detected upon increasing the number of radical species in the mixed valence assemblies present in the film state without impeding the delocalization of the unpaired electrons. A delicate balance between hydrogen bonds and packing is thus necessary to get supramolecular polarons in mixed valence TATA assemblies.
Organometallic Platinum(II) Photosensitisers that Demonstrate Ligand‐Modulated Triplet‐Triplet Annihilation Energy Upconversion Efficiencies
Authors: Fitzgerald Sophie A. , Xiao Xiao , Zhao Jianzhang , Horton Peter N. , Coles Simon J. , Knighton Richard C. , Ward Benjamin D. , Pope Simon J. A.
Published: November 2022

A series of 2‐phenylquinoxaline ligands have been synthesised that introduce either CF3or OCF3electron‐withdrawing groups at different positions of the phenyl ring. These ligands were investigated as cyclometalating reagents for platinum(II) to give neutral complexes of the form [Pt(C^N)(acac)] (in which C^N=cyclometalating ligand; acac=acetyl acetonate). X‐ray crystallographic studies on three examples showed that the complexes adopt an approximate square planar geometry. All examples revealed strong Pt−Pt linear contacts of 3.2041(6), 3.2199(3) and 3.2586(2) Å. The highly coloured complexes display efficient visible absorption at 400–500 nm (ϵ ≈5000 M−1 cm−1) and orange red photoluminescent characteristics (λem=603–620 nm;Φem≤37 %), which were subtly tuned by the ligand. Triplet emitting character was confirmed by microsecond luminescence lifetimes and the photogeneration of singlet oxygen with quantum efficiencies up to 57 %. Each complex was investigated as a photosensitiser for triplet–triplet annihilation energy upconversion using 9,10‐diphenylanthracene as the annihilator species: a range of good upconversion efficiencies (ΦUC5.9–14.1 %) were observed and shown to be strongly influenced by the ligand structure in each case.
Caging of a Strongly Pairing Fluorescent Thymidine Analog with Soft Nucleophiles
Authors: Eyberg Juri , Ringenberg Mark , Richert Clemens
Published: November 2022

Controlling the pairing strength of nucleobases in DNA through reactions with compounds found inside the cell is a formidable challenge. Here we report how a thiazolyl substituent turns a strongly pairing ethynylpyridoneC‐nucleoside into a reactive residue in oligonucleotides. The thiazolyl‐bearing pyridone reacts with soft nucleophiles, such as glutathione, but not with hard nucleophiles like hydroxide or carbonate. The addition products pair much more weakly with adenine in a complementary strand than the starting material, and also change their fluorescence. This makes oligonucleotides containing the new deoxynucleoside interesting for controlled release. Due to its reactivity towardN,P,S, andSe‐nucleophiles, and the visual signal accompanying chemical conversion, the fluorescent nucleotide reported here may also have applications in chemical biology, sensing and diagnostics.