bluuebunny/crossref_metadata_2025_split huggingface dataset:
Programmable Photocatalytic Activity of Multicomponent Covalent Organic Frameworks Used as Metallaphotocatalysts
Authors: Traxler Michael , Reischauer Susanne , Vogl Sarah , Roeser Jérôme , Rabeah Jabor , Penschke Christopher , Saalfrank Peter , Pieber Bartholomäus , Thomas Arne 
Published: October 2022

AbstractThe multicomponent approach allows to incorporate several functionalities into a single covalent organic framework (COF) and consequently allows the construction of bifunctional materials for cooperative catalysis. The well‐defined structure of such multicomponent COFs is furthermore ideally suited for structure‐activity relationship studies. We report a series of multicomponent COFs that contain acridine‐ and 2,2’‐bipyridine linkers connected through 1,3,5‐benzenetrialdehyde derivatives. The acridine motif is responsible for broad light absorption, while the bipyridine unit enables complexation of nickel catalysts. These features enable the usage of the framework materials as catalysts for light‐mediated carbon−heteroatom cross‐couplings. Variation of the node units shows that the catalytic activity correlates to the keto‐enamine tautomer isomerism. This allows switching between high charge‐carrier mobility and persistent, localized charge‐separated species depending on the nodes, a tool to tailor the materials for specific reactions. Moreover, nickel‐loaded COFs are recyclable and catalyze cross‐couplings even using red light irradiation.
From Lignin to Chemicals: An Expedition from Classical to Modern Catalytic Valorization Technologies
Authors: Al‐Naji Majd , Brandi Francesco , Drieß Matthias , Rosowski Frank 
Published: October 2022

AbstractFor the transition towards greener biorefineries with reduced waste, valorization of lignin to drop‐in chemicals instead of their combustion for energy purposes is a key issue for future processes. In this context, lignin should be extracted from lignocellulosic biomass (LCB) and fragmented into smaller units, followed by catalytic funneling to fine chemicals. In this review, we report on the classical approaches for lignin valorization from LCB: thermal treatments, solvolytic valorization, acid‐catalyzed process, and base‐catalyzed process. We also provide the reader with the modern approach of lignin valorization that led to an integrated LCB biorefinery. The performance of different solid catalysts in lignin‐first approach via reductive or oxidative catalytic fractionation at different conditions is discussed in detail.
Thrombus Inhibition and Neuroprotection for Ischemic Stroke Treatment through Platelet Regulation and ROS Scavenging
Authors: Ye Hongbo , Ma Zhifang , Liu Lei , Zhang Tianci , Han Qiaoyi , Xiang Zehong , Xia Yu , Ke Yue , Guan Xinghua , Shi Qiang , Ataullakhanov Fazly I. , Panteleev Mikhail 
Published: October 2022

AbstractIschemic stroke is caused by cerebrovascular stenosis or occlusion. Excessive reactive oxygen species (ROS) are the focus‐triggering factor of irreversible injury in ischemic regions, which result in harmful cascading effects to brain tissue, such as inflammation and microthrombus formation. In the present work, we designed nanodelivery systems (NDSs) based on MnO2 loaded with Ginkgolide B (GB) for restoring the intracerebral microenvironment in ischemic stroke, such as ROS scavenging, O2 elevation, thrombus inhibition and damage repair. GB can activate the endogenous antioxidant defense of cells by enhancing the nuclear factor‐E2‐related factor 2 (Nrf2) signalling pathway, thus protecting brain tissue from oxidative damage. However, the blood–brain barrier (BBB) is also a therapeutic obstacle for the delivery of these agents to ischemic regions. MnO2 nanoparticles have an inherent BBB penetration effect, which enhances the delivery of therapeutic agents within brain tissue. MnO2, with mimicking enzymatic activity, can catalyze the decomposition of overproduced H2O2 in the ischemic microenvironment to O2, meanwhile releasing platelet‐antagonizing GB molecules, thus alleviating cerebral hypoxia, oxidative stress damage, and microthrombus generation. This study may provide a promising therapeutic route for regulating the microenvironment of ischemic stroke through a combined function of ROS scavenging, microthrombus inhibition, and BBB penetration.
Recent Advances of Anticancer Studies Based on Nano‐Fluorescent Metal‐Organic Frameworks
Authors: Liang Ranxi , Liu Ning , Li Feize 
Published: October 2022

AbstractNano‐fluorescent metal‐organic frameworks (NF‐MOFs), a kind of newly emerged nano‐scaled platform, can provide visual, rapid, and highly sensitive optical imaging of cancer lesions both in vitro and in vivo. Meanwhile, the excellent porosity, structural tunability, and chemical modifiability also enable NF‐MOFs to achieve simultaneous loading of targeted molecules and therapeutic agents. These NF‐MOFs not only possess excellent targeted imaging ability, but also can guide the carried cargos to perform precise therapy, drawing considerable attention in current framework of anticancer drug design. In this review, we outline the fluorescence types and response mechanisms of NF‐MOFs, and highlight their applications in cancer diagnosis and therapy in recent years. Based on this panorama, we also discuss current issues and future trends of NF‐MOFs in biomedical fields, attempting to clarify the potential value of fluorescence imaging guided anticancer investigations.
Correlation between the Properties of Surface Lattice Oxygen on NiO and Its Reactivity and Selectivity towards the Oxidative Dehydrogenation of Propane
Authors: Tan Chunxiao , Liu Huixian , Qin Yuyao , Li Liwen , Wang Hua , Zhu Xinli , Ge Qingfeng 
Published: October 2022

AbstractModified NiO catalysts with controllable vacancies and dopants are promising for alkene production from oxidative dehydrogenation (ODH) of light alkanes, and a molecular understanding of the modification on elementary reaction steps would facilitate the design of highly efficient catalysts and catalytic processes. In this study, density functional theory (DFT) calculations was used to map out the complete reaction pathways of propane ODH on the NiO (100) surfaces with different modifiers. The results demonstrated that the presence of vacancies (O and Ni) and dopants (Li and Al) alters the electrophilicity of surface oxygen species, which in turn affects the reactivity towards C−H bond activation and the overall catalytic activity and selectivity. The strongly electrophilic O favors a radical mechanism for the first C−H activation on O followed by the second C−H activation on O−O site, whereas weak electrophilic O favors concerted C−H bond breaking over Ni−O site. The C−H bond activation proceeds through a late transition state, characterized by the almost completion of the O−H bond formation. Consequently, the adsorption energy of H adatom on O rather than p‐band center or Bader charge of O has been identified to be an accurate descriptor to predict the activation barrier for C−H breaking (activity) as well as the difference between the activation barriers of propene and CH3CCH3 (selectivity) of ODH.
Methods for Recombinant Production and Purification of Peptides as SUMO‐Peptide‐Intein Fusion Proteins to Protect from Degradation
Authors: Lamer Tess , van Belkum Marco J. , Vederas John C. 
Published: October 2022

AbstractHeterologous expression in Escherichia coli is a commonly used method to produce ribosomally synthesized peptides for further study. This generally requires expression of the target protein with an affinity fusion tag, followed by isolation of the fusion protein from a cellular lysate by affinity purification, and finally by removal of the fusion tag and purification of the desired peptide. Sometimes, however, fusion proteins may be degraded during recombinant expression in E. coli. We recently reported an expression system that sandwiches the target peptide between an N‐terminal small ubiquitin‐like modifier (SUMO) protein and a C‐terminal intein. This SUMO‐peptide‐intein (SPI) fusion protein protects the central peptide from degradation and can lead to improved peptide yield after purification. In this report, we detail the cloning, expression, and isolation procedures for the SPI fusion system, with comments on conditions that can be optimized for different peptides to obtain maximal yield for each construct. © 2022 Wiley Periodicals LLC.Basic Protocol 1: Cloning to construct SPI geneBasic Protocol 2: Expression of SPI fusion proteins in E. coli BL21(DE3)Support Protocol: Optimization of expression and induction conditionsBasic Protocol 3: Isolation and purification of SPI fusion proteins with a chitin columnAlternate Protocol: Isolation and purification of SPI fusion proteins without chitin
H2O Activity Adjustment by Hydrogen Bonding Enables High‐Performance Zn‐Organic Battery
Authors: Zhou Kang , Wang Nan , Qiu Xuan , Xie Haijiao , Wei Peng , Dong Xiaoli , Wang Yonggang 
Published: October 2022

AbstractThe advantages of low cost and high safety of zinc (Zn) metal have attracted much attention on its application in batteries, but H2O‐induced issues of hydrogen evolution reaction (HER), Zn corrosion, and Zn dendrites formation limit the application. Here, a strategy of adjusting H2O activity was provided by adding glycerol (GL) and acetonitrile (AN) into aqueous electrolyte to form hydrogen bonds between organic solvents and H2O, which alleviated the Zn corrosion. Furthermore, molecular dynamics (MD) simulation indicated that GL could exclude H2O from the Zn2+ solvation shell, thus preventing undesired HER and Zn dendrites formation. Therefore, the corresponding Zn//Zn symmetrical cell showed a ultralong lifespan (1300 h). Then, a Zn‐organic battery with 3,7‐dimorpholino‐phenothiazin‐5‐ium iodide (FD28) cathode was fabricated by using such electrolyte. Interestingly, the reduced H2O activity also ensured the stable operation of organic cathode, and thus the full cell showed superior cycle stability for over 9000 cycles (≈1100 h), which is superior to previous reports. Moreover, such electrolyte owns novel properties of nonflammability, great weatherability, and low freezing point, thus boosting the practicality of the battery.
Prognostic impact of upper and lower extremity muscle mass in heart failure
Authors: Konishi Masaaki , Akiyama Eiichi , Matsuzawa Yasushi , Sato Ryosuke , Kikuchi Shinnosuke , Nakahashi Hidefumi , Okada Kozo , Iwahashi Noriaki , Kosuge Masami , Ebina Toshiaki , Hibi Kiyoshi , Misumi Toshihiro , Tamura Kouichi , Kimura Kazuo 
Published: October 2022

AbstractAimsReduced skeletal muscle mass is a major component of sarcopenia, associated with impaired exercise capacity and poor prognosis in patients with heart failure (HF). Measurement of skeletal muscle mass by dual‐energy X‐ray absorptiometry may be affected by fluid retention, typically in the patients' lower extremities. The aim of the present study was to elucidate the association between upper and lower extremity skeletal muscle mass (USM and LSM) and all‐cause mortality in hospitalized patients with HF, after discharge.MethodsThis was a single‐centre observational cohort study of 418 patients (59% were men) admitted with a diagnosis of HF (71 ± 13 years), with a left ventricular ejection fraction of 39 ± 16%. USM and LSM were measured by dual‐energy X‐ray absorptiometry with patients in a stable state after decongestion therapy.ResultsThe USM and LSM were 5.29 ± 1.18 and 13.78 ± 3.20 kg for men and 3.37 ± 0.68 and 9.19 ± 1.80 kg for women. A positive correlation was obtained between USM and LSM with mid‐upper arm circumference (r = 0.684, P < 0.001) and calf circumference (r = 0.822, P < 0.001), respectively. During a median follow‐up of 37 months, 92 (22.0%) of the 418 patients died. A Kaplan–Meier analysis revealed that sex‐specific quartiles of USM/height2 and LSM/height2 were associated with all‐cause mortality (both P < 0.001 by the log‐rank test). In Cox models adjusted by age, sex, creatinine, haemoglobin, NYHA class, and height2, the hazard ratio with 95% confidence intervals for all‐cause mortality was 0.557 [0.393–0.783] (P < 0.001) for USM per 1 kg, and 0.783 [0.689–0.891] (P < 0.001) for LSM per 1 kg. The receiver‐operator‐characteristic curve analysis showed a comparable area under the curve between the USM/height2 and LSM/height2 (0.557 vs. 0.568, P = 0.562) in predicting all‐cause mortality. The ratio of USM to LSM was significantly lower in 37 patients with residual leg oedema than in the 360 patients without oedema (36.1% vs. 38.1%, P = 0.004), suggesting the influence of oedema on measured LSM.ConclusionsBoth USM and LSM had a prognostic implication on mortality after discharge in HF, even though LSM may have been affected by leg oedema. These findings indicate that clinicians should not ignore a patient's USM or LSM in the prognostication of patients with HF.
Carbonylative Ring Expansion of Epoxides to β‐Lactones Using Inorganic Salt as Catalytic Species Precursor
Authors: He L. , Yang J.‐C. , Song T.‐T. , Liu Y. , Lu X.‐B. 
Published: October 2022

AbstractTransition‐metal‐catalyzed carbonylative transformation is a well‐established and indispensable tool in organic chemistry, partially due to that CO is a cheap and readily available C1‐building block. The β‐lactone products via carbonylative ring expansion of epoxide are particularly attractive, because they feature broad utility in organic and polymer chemistry. One of the major challenges for this promising reaction is the usage of toxic, moderately air sensitive, unstable and pyrophoric low‐valent cobalt catalysts. Inorganic salts feature high abundance in nature, and the generation of catalytic species from in situ reduction of divalent cobalt(II) salt has received intense attention, which avoids the unnecessary storage and transport of sensitive low‐valent cobalt compounds. Herein, we have employed this strategy for the selectively carbonylative ring expansion of epoxides under an extremely mild condition, e. g. 40 °C and 1 atm CO pressure. This method eliminates the usage of extremely sensitive cobalt carbonyl catalyst. In addition, this reaction is tolerant to a variety of epoxides, and up to 15 examples of β‐lactones with excellent functionality have been isolated in moderate to excellent yields and selectivity.
Improving textural properties of gluten‐free veggie sausage with egg white proteins
Authors: Zhao Hefei , Han Aiyun , Nduwamungu Joshua J. , Nishijima Noriaki , Oda Yoshifumi , Handa Akihiro , Zhang Yue , Majumder Kaustav , Xu Changmou 
Published: October 2022

AbstractGluten and gums are usually used in veggie sausage for textural purposes; however, they are not label‐friendly for consumers with gluten sensitivity or consumers looking for clean‐label foods. Therefore, two commercial egg white proteins (P110 and M200) were studied at different levels (0%–10%) to substitute gluten or xanthan gum. The veggie sausages were subjected to color, texture, length, and weight loss evaluations. M200 significantly improved the texture of sausages and exhibited the most similar texture profile as a commercial meat sausage. The overall texture‐enhanced capability of gel materials was ranked in the order of 5% M200 > 5% P110 ≥ 3% Gluten ≥ 1.3% Xanthan Gum. Egg white proteins did not significantly affect the color, length, and weight loss of sausages. Raman spectra revealed that M200 gel had a higher α‐helix structure than P110 gel, which indicated that M200 formed an ordered gel by reforming tyrosine at Raman shift 833 and 860 cm−1 inside while P110 formed a disordered gel by exposing tyrosine. This study demonstrated that M200 would substitute both the gluten and xanthan gum for improving the texture of veggie sausages. The findings may also be applied to other meat analogs targeting gluten‐free and label‐friendly purposes.
A spectral element solution of the two‐dimensional linearized potential flow radiation problem
Authors: Visbech Jens , Engsig‐Karup Allan P. , Bingham Harry B. 
Published: October 2022

AbstractWe present a scalable two‐dimensional Galerkin spectral element method solution to the linearized potential flow radiation problem for wave induced forcing of a floating offshore structure. The pseudo‐impulsive formulation of the problem is solved in the time domain using a Gaussian displacement signal tailored to the discrete resolution. The added mass and damping coefficients are then obtained via Fourier transformation. The spectral element method is used to discretize the spatial fluid domain, whereas the classical explicit 4‐stage fourth‐order Runge–Kutta scheme is employed for the temporal integration. Spectral convergence of the proposed model is established for both affine and curvilinear elements, and the computational effort is shown to scale with , with being the total number of grid points and . The solver is used to compute the hydrodynamic coefficients for several floating bodies and compared against known public benchmark results. The results show excellent agreement, ultimately validating the solver and emphasizing the geometrical flexibility and high accuracy and efficiency of the proposed solution strategy. Lastly, an extensive investigation of nonresolved energy from the pseudo‐impulse is carried out to characterize the induced spurious oscillations of the free surface quantities leading to a robust strategy for tuning the pseudo‐impulsive motion to the spatial discretization.
Unraveling schizophrenia replicable functional connectivity disruption patterns across sites
Authors: Du Xiaotong , Wei Xiaotong , Ding Hao , Yu Ying , Xie Yingying , Ji Yi , Zhang Yu , Chai Chao , Liang Meng , Li Jie , Zhuo Chuanjun , Yu Chunshui , Qin Wen 
Published: October 2022

AbstractFunctional connectivity (FC) disruption is a remarkable characteristic of schizophrenia. However, heterogeneous patterns reported across sites severely hindered its clinical generalization. Based on qualified nodal‐based FC of 340 schizophrenia patients (SZ) and 348 normal controls (NC) acquired from seven different scanners, this study compared four commonly used site‐effect correction methods in removing the site‐related heterogeneities, and then tried to cluster the abnormal FCs into several replicable and independent disrupted subnets across sites, related them to clinical symptoms, and evaluated their potentials in schizophrenia classification. Among the four site‐related heterogeneity correction methods, ComBat harmonization (F1 score: 0.806 ± 0.145) achieved the overall best balance between sensitivity and false discovery rate in unraveling the aberrant FCs of schizophrenia in the local and public data sets. Hierarchical clustering analysis identified three replicable FC disruption subnets across the local and public data sets: hypo‐connectivity within sensory areas (Net1), hypo‐connectivity within thalamus, striatum, and ventral attention network (Net2), and hyper‐connectivity between thalamus and sensory processing system (Net3). Notably, the derived composite FC within Net1 was negatively correlated with hostility and disorientation in the public validation set (p < .05). Finally, the three subnet‐specific composite FCs (Best area under the receiver operating characteristic curve [AUC] = 0.728) can robustly and meaningfully discriminate the SZ from NC with comparable performance with the full identified FCs features (best AUC = 0.765) in the out‐of‐sample public data set (Z = −1.583, p = .114). In conclusion, ComBat harmonization was most robust in detecting aberrant connectivity for schizophrenia. Besides, the three subnet‐specific composite FC measures might be replicable neuroimaging markers for schizophrenia.
Does Renminbi internationalization matter for petroleum security in China? Evidence from a disaggregate analysis
Authors: Chen Ding , Gummi Umar Muhammad , Wang Junping 
Published: October 2022

AbstractAs the largest oil consumer and sixth largest oil producer in the world, China's growing oil import is a premise to its energy security concerns. For China, petroleum security means supply security. The paper disaggregates petroleum security into three dimensions (domestic petroleum price—DOP, petroleum supply—PS and petroleum reserve—PR) and examines the impact of Renminbi internationalization (RMBI) on these dimensions based on linear auto regressive distributed lag (ARDL) procedure, and monthly data spanning from 2011M01 to 2022M03. The empirical results reveal evidence of long run equilibrium relationship between PR, PS and RMBI. On the long run and short run dynamics, RMBI is inversely related to DOP both in the short run and long run, but the impact is less than proportionately. However, RMBI and PS co‐move in the short run with 0.24% margin. In the same vein, RMBI and PR co‐move both in the short run and long run significantly. The impact of international oil price is positive on DOP but negative on PS and PR at least in the short run. Our finding signalled to the fact that increasing acceptance of the RMB in trade settlements and crude oil invoicing serve as a comparative advantage for China to engage in oil trade and complement the oil demand growth threatening the country's energy security drive. Therefore, we suggest diversification of crude oil import sources especially to regions/countries where RMB has been widely accepted. Prominence should be given to government controlled Strategic Petroleum Reserves (SPRs) and large oil companies should be compelled to raise the level of mandatory oil reserve for sustainable supply that keep pace with the growing demand for oil.
Mechanical alterations of electrospun poly(ϵ‐caprolactone) in response to convective thermobonding
Authors: Behrangzade Ali , Keeney Hannah R. , Martinet Katarina M. , Wagner William R. , Vande Geest Jonathan P. 
Published: October 2022

AbstractVascular graft failure has persisted as a major clinical problem. Mechanical, structural, and transport properties of vascular grafts are critical factors that substantially affect their function and thus the outcome of implantation. The manufacturing method, post‐processing technique, and material of choice have a significant impact on these properties. The goal of this work is to use thermal treatment to modulate the transport properties of PCL‐based vascular engineered constructs. To this end, we electrospun PCL tubular constructs and thermally bonded the electrospun fibers in a convective oven at various temperatures (54, 57, and 60°C) and durations of treatment (15, 30, and 45 s). The effects of fiber thermal bonding (thermobonding) on the transport, mechanical, and structural properties of PCL tubular constructs were characterized. Increasing the temperature and treatment duration enhanced the degree of thermobonding by removing the interconnected void and fusing the fibers. Thermobonding at 57°C and 60°C for longer than 30 s increased the median tangential modulus (E = 126.1 MPa, [IQR = 20.7]), mean suture retention (F = 193.8 g, [SD = 18.5]), and degradation rate while it decreased the median permeability (kA = 0 m/s), and median thickness (t = 60 μm, [IQR = 2.5]). In particular, the thermobonding at 57°C allowed a finer modulation of permeability via treatment duration. We believe that the thermobonding method can be utilized to modulate the properties of vascular engineered constructs which can be useful in designing functional vascular grafts.