bluuebunny/crossref_metadata_2025_split huggingface dataset:
Strain‐Driven Mixed‐Phase Domain Architectures and Topological Transitions in Pb1−xSrxTiO3 Thin Films
Authors: Kavle Pravin , Zorn Jacob A. , Dasgupta Arvind , Wang Bo , Ramesh Maya , Chen Long‐Qing , Martin Lane W. 
Published: August 2022

AbstractThe potential for creating hierarchical domain structures, or mixtures of energetically degenerate phases with distinct patterns that can be modified continually, in ferroelectric thin films offers a pathway to control their mesoscale structure beyond lattice‐mismatch strain with a substrate. Here, it is demonstrated that varying the strontium content provides deterministic strain‐driven control of hierarchical domain structures in Pb1−xSrxTiO3 solid‐solution thin films wherein two types, c/a and a1/a2, of nanodomains can coexist. Combining phase‐field simulations, epitaxial thin‐film growth, detailed structural, domain, and physical‐property characterization, it is observed that the system undergoes a gradual transformation (with increasing strontium content) from droplet‐like a1/a2 domains in a c/a domain matrix, to a connected‐labyrinth geometry of c/a domains, to a disconnected labyrinth structure of the same, and, finally, to droplet‐like c/a domains in an a1/a2 domain matrix. A relationship between the different mixed‐phase modulation patterns and its topological nature is established. Annealing the connected‐labyrinth structure leads to domain coarsening forming distinctive regions of parallel c/a and a1/a2 domain stripes, offering additional design flexibility. Finally, it is found that the connected‐labyrinth domain patterns exhibit the highest dielectric permittivity.
Computational Biomaterials: Computational Simulations for Biomedicine
Authors: Dai Xinyue , Chen Yu 
Published: August 2022

AbstractWith the flourishing development of material simulation methods (quantum chemistry methods, molecular dynamics, Monte Carlo, phase field, etc.), extensive adoption of computing technologies (high‐throughput, artificial intelligence, machine learning, etc.), and the invention of high‐performance computing equipment, computational simulation tools have sparked the fundamental mechanism‐level explorations to predict the diverse physicochemical properties and biological effects of biomaterials and investigate their enormous application potential for disease prevention, diagnostics, and therapeutics. Herein, the term “computational biomaterials” is proposed and the computational methods currently used to explore the inherent properties of biomaterials, such as optical, magnetic, electronic, and acoustic properties, and the elucidation of corresponding biological behaviors/effects in the biomedical field are summarized/discussed. The theoretical calculation of the physiochemical properties/biological performance of biomaterials applied in disease diagnosis, drug delivery, disease therapeutics, and specific paradigms such as biomimetic biomaterials is discussed. Additionally, the biosafety evaluation applications of theoretical simulations of biomaterials are presented. Finally, the challenges and future prospects of such computational simulations for biomaterials development are clarified. It is anticipated that these simulations would offer various methodologies for facilitating the development and future clinical translations/utilization of versatile biomaterials.
The Synthesis of 5,6‐dihydrobenzo[4,5]imidazo[2,1‐a]isoquinoline Derivatives via Metal‐Free Radical Cascade Pathway
Authors: Pan Youlu , Xu Jinghao , Zhang Hongjie , Hao Rongrong , Shen Zhengrong , Huang Wenhai 
Published: July 2022

AbstractA metal‐free radical relay addition/cyclization of activated alkenes with ethers, cycloalkanes, toluenes, and alcohols has been achieved, leading to a range of functionalization of 5,6‐dihydrobenzo[4,5]imidazo[2,1‐a]isoquinolines with the yield of 43% ‐ 84%. This protocol exhibits advantages of metal‐free, base‐free, and shorter reaction time.magnified image
Cancer risk and gammopathies in 2123 adults with Gaucher disease type 1 in the International Gaucher Group Gaucher Registry
Authors: Rosenbloom Barry E. , Cappellini Maria Domenica , Weinreb Neal J. , Dragosky Marta , Revel‐Vilk Shoshana , Batista Julie L. , Sekulic Davorka , Mistry Pramod K. 
Published: August 2022

AbstractThere are numerous reports of cancers in Gaucher disease (GD) from mostly small single‐center studies; however, precise risk estimates and cancer types involved have not been delineated. We conducted a study involving 2123 patients with GD type 1 (GD1) to assess the incidence of hematological malignancies, gammopathies, and solid tumors in an international observational study, the International Cooperative Gaucher Group Gaucher Registry (Clinicaltrials.gov: NCT00358943). Risk for cancer overall and for each type of malignancy was compared to the United States (US) population using the Surveillance, Epidemiology, and End Results database. Natural history of gammopathy was determined through assessing the progression from a diagnosis of monoclonal gammopathy of unknown significance (MGUS) to multiple myeloma (MM). Risk for hematological malignancies was more than four times higher than expected compared to the general population: non‐Hodgkin lymphoma was approximately three times higher; MM was approximately nine times higher. Age‐specific incidence rates of MGUS were unexpectedly high among younger patients. The 10‐year cumulative incidence of MM after diagnosis of MGUS was 7.9%, comparable to the general population. Compared to the general US population, GD1 patients were at higher risk for solid malignancies of liver (2.9 times), kidney (2.8 times), melanoma (2.5 times), and breast (1.4 times). Colorectal, prostate, and lung cancer risks were lower than expected. These findings help advance care of patients with GD1 by supporting recommendations for individualized monitoring for malignancies and antecedents such as MGUS for MM and provoke important questions of the role of glucosylceramide and related sphingolipids in cancer biology.
Chemoselective Annulation of 2‐Benzothiazolimines Enabled by Bifunctional Phosphonium Salt: Highly Enantioselective Synthesis of Indole‐fused Cyclic Thiourea Scaffolds
Authors: Li Kehan , Lu Dongming , Tan Jian‐Ping , Ren Xiaoyu , Wang Tianli 
Published: July 2022

AbstractA highly efficient chemoselective and stereoselective annulation utilizing 2‐benzothiazolimines as unusual C2‐synthons by thiourea‐based bifunctional phosphonium salt catalysis has been developed. This asymmetric protocol provides a rapid access to highly functionalized and indole‐fused cyclic thiourea scaffolds that bear benzothiazole cores in high yields with excellent both diastereo‐ and enatioselectivities. This transformation proceeds under mild reaction conditions and expands the catalytic potential of phosphonium salt catalysts.
Engineering a ceramic piston pump to minimize particle formation for a therapeutic immunoglobulin: A combined factorial and modeling approach
Authors: Roffi Kirk , Sebastião Israel B. , Morel Alexandre 
Published: July 2022

AbstractDuring fill‐finish manufacturing, protein‐pump surface interactions can induce subvisible particle (SVP) formation which poses a risk to drug product quality and patient safety. Despite this risk, there have been no concerted efforts to understand the effects of piston pump design on SVP formation. We've systematically varied the design of the piston‐cylinder interface to minimize SVP formation for a therapeutic immunoglobulin. The clearance factor, surface roughness factor, and their combined interaction significantly affected particle concentrations, quantitated by light obscuration and microflow imaging. Optimized pump designs reduced particle levels by 1–2 orders of magnitude compared to the off‐the‐shelf equipment. At the piston surface, scanning electron microscopy revealed evidence of protein film abrasion, a process which ejects SVPs from the piston‐cylinder interface as wear debris. Computational fluid dynamics and quartz crystal microbalance were applied to simulate fluid flow and protein adsorption phenomena in the pump respectively. The risk of protein film abrasion was modeled along a hypothetical Stribeck curve, thereby interconnecting design parameters, lubrication conditions, and SVP formation. Our findings support implementation of a modular pump platform with interchangeable pistons; this approach would enable the pump design to be customized based on each protein's propensity to form SVPs. This flexible approach can benefit pharmaceutical manufacturers and patients alike by accelerating tech transfer and improving process control.
Electrocarboxylation of Aryl Epoxides with CO2for the Facile and Selective Synthesis of β‐Hydroxy Acids
Authors: Wang Yanwei , Tang Shunyao , Yang Guoqing , Wang Siyi , Ma Dengke , Qiu Youai 
Published: July 2022

AbstractHerein, an efficient and facile approach to valuable β‐hydroxy acid derivatives from readily available aryl epoxides and CO2with high chemo‐ and regioselectivity under mild and sustainable electrochemical conditions is described. This approach showed broad substrate scope and good functional‐group compatibility. In addition to aryl epoxides, four‐ to six‐membered aryl cyclic ethers could all be tolerated in the reaction to provide synthetically useful hydroxy acids with high efficiency. Further late‐stage carboxylation of complex molecules and drug derivatives demonstrated its potential application in the pharmaceutical industry. Mechanistic studies disclosed possible reaction pathways.
Photoinduced Persistent Polarization Change in a Spin Transition Crystal
Authors: Su Sheng‐Qun , Wu Shu‐Qi , Huang Yu‐Bo , Xu Wen‐Huang , Gao Kai‐Ge , Okazawa Atsushi , Okajima Hajime , Sakamoto Akira , Kanegawa Shinji , Sato Osamu 
Published: July 2022

AbstractUsing light as a local heat source to induce a temporary pyroelectric current is widely recognized as an effective way to control the polarization of crystalline materials. In contrast, harnessing light directly to modulate the polarization of a crystal via excitation of the electronic bands remains less explored. In this study, we report an FeIIspin crossover crystal that exhibits photoinduced macroscopic polarization change upon excitation by green light. When the excited crystal relaxes to the ground state, the corresponding pyroelectric current can be detected. An analysis of the structures, magnetic properties and the Mössbauer and infrared spectra of the complex, supported by calculations, revealed that the polarization change is dictated by the directional relative movement of ions during the spin transition process. The spin transition and polarization change occur simultaneously in response to light stimulus, which demonstrates the enormous potential of polar spin crossover systems in the field of optoelectronic materials.
A Conjugated Covalent Template Strategy for All‐Benzene Catenane Synthesis
Authors: Bu An , Zhao Yongye , Xiao Hongyan , Tung Chen‐Ho , Wu Li‐Zhu , Cong Huan 
Published: July 2022

AbstractMechanically interlocked molecules based on oligoparaphenylene‐derived nanohoops, particularly those without heteroatoms, are synthetically challenging and topologically intriguing targets. Herein, a π‐conjugated covalent template strategy based on azo group has been developed, which features dual intramolecular macrocyclizations directed by a tetra‐substituted azobenzene core, followed by traceless removal of the azo linker. Employing this strategy, the efficient synthesis of a novel all‐benzene [2]catenane consisting of meta‐cycloparaphenylenes has been accomplished.
Unblocking Ion‐occluded Pore Channels in Poly(triazine imide) Framework for Proton Conduction
Authors: Chi Heng‐Yu , Chen Cailing , Zhao Kangning , Villalobos Luis Francisco , Schouwink Pascal Alexander , Piveteau Laura , Marshall Kenneth Paul , Liu Qi , Han Yu , Agrawal Kumar Varoon 
Published: July 2022

AbstractPoly(triazine imide) or PTI is an ordered graphitic carbon nitride hosting Å‐scale pores attractive for selective molecular transport. AA’‐stacked PTI layers are synthesized by ionothermal route during which ions occupy the framework and occlude the pores. Synthesis of ion‐free PTI hosting AB‐stacked layers has been reported, however, pores in this configuration are blocked by the neighboring layer. The unavailability of open pore limits application of PTI in molecular transport. Herein, we demonstrate acid treatment for ion depletion which maintains AA’ stacking and results in open pore structure. We provide first direct evidence of ion‐depleted open pores by imaging with the atomic resolution using integrated differential phase‐contrast scanning transmission electron microscopy. Depending on the extent of ion‐exchange, AA’ stacking with open channels and AB stacking with closed channels are obtained and imaged for the first time. The accessibility of open channels is demonstrated by enhanced proton transport through ion depleted PTI.
In vivo Realization of Dual Photodynamic and Photothermal Therapy for Melanoma by Mitochondria Targeting Dinuclear Ruthenium Complexes under Civil Infrared Low‐power Laser
Authors: Wang Meng‐Fan , Yang Rong , Tang Shi‐Jie , Deng Yu‐Ang , Li Guo‐Kui , Zhang Dan , Chen Daomei , Ren Xiaoxia , Gao Feng 
Published: July 2022

AbstractA series of dinuclear RuII complexes with extremely high TPA cross sections in the range of 800–900 nm have been designed. The amphiphilic complex Ru3 containing tert‐butyl groups has balanced performance in singlet oxygen generation and photothermal conversion and becomes the ideal drug candidate of the series. Ru3 targets mitochondria without penetrating the nucleus, which substantially increases its photodynamic therapy activity and reduces its dark cytotoxicity. Ru3 successfully suppresses melanoma tumor growth in vitro and in vivo with combined photodynamic and photothermal therapy under low light dose irradiation of an 808 nm low‐power laser, avoiding the known PDT resistance in melanoma. The excellent therapeutic effect of Ru3 facilitates its applications in further human trials for larger or deeper buried tumors, thereby becoming a prospective candidate for a new generation of low‐power IR‐driven dual PDT/PTT drugs.
Simulation and experimental study of parameters in centrifugal electrospinning: Effects of rotor form on fiber formation
Authors: Wang Han , Feng Liang , Zeng Jun , Chen Lingmin , Chen An , Liu Maolin , Xiong Jingang 
Published: August 2022

AbstractNanofiber is a kind of high‐performance material, which has great applications. Among many preparation methods, centrifugal electrospinning combines the advantages of electrospinning and centrifugal spinning, with high yield and a wide range of application. But its influencing factors are numerous, the process is still immature, and unable to meet the needs of industrialization. Here, we design a set of centrifugal electrospinning equipment and its process, and explore the influence of rotor form on fiber formation. First, the structure and working principle of experimental equipment of centrifugal electrospinning are introduced. Then, the influence of two factors, the rotor shape and rotor material, on space electric field is studied through theoretical and simulation analysis. Finally, based on the designed equipment, the effects of different rotor forms on the fibers preparation of centrifugal electrospinning are studied. The results show that the fiber diameter of centrifugal electrospinning is greatly affected by the form of the rotor. By changing the surface shape of the rotor and the rotor material, the diameter of the fiber can be controlled. Experiments show that the average fiber diameter of the γ‐shaped rotor is the smallest, and the fiber spun with ULTEM PEI 1010 material has the best overall performance.
Soft‐template assisted preparation of hierarchically porous graphitic carbon nitride layers for high‐performance supercapacitors
Authors: Xu Zhongyun , Kong Lirong , Wang Hui , Ma Qiang , Shen Xiaoping , Wang Jianyue , Premlatha Subramanian 
Published: July 2022

AbstractStrong π–π interaction between two‐dimensional graphitic carbon nitride (CN) layers may cause the stacking phenomenon, which leads to the decrease of its surface area and thus the capacitive properties. Hard templates are usually used to avoid the stacking phenomena. However, the use of them needs redundant removing process and may cause environmental pollution. As a result, in this work, P123 was used as the soft template to expand the inter‐layer distance and create more mesopores in the CN sheets. Benefit from the synergistic effect between the unique porous structure and the high nitrogen doping level, the formed graphitic CN (P2‐g‐CN) could exhibit high specific capacitances (520.5 and 176.0 F g−1 at the current density of 0.5 and 50 A g−1), stable cyclic behavior and satisfied energy density. The superior energy storage performances and the facile synthetic approach of P2‐g‐CN indicate its promising application as high‐performance electrode for supercapacitors and other energy storage devices.
Enhanced properties of starch based foams with modified starch/polyester blend as masterbatch
Authors: Shi Huidong , Zhu Yanfeng , Ju Qing , Shen Yucai , Wang Tingwei 
Published: July 2022

AbstractStarch/PBAT blends were reactively extruded as masterbatch with the addition of tartaric acid (TA) and epoxide chain extender ADR4468 (ADR). The effects of tartaric acid and chain extender on the mechanical properties and structure of starch/PBAT blends were evaluated. The tensile strength of starch/PBAT blends with TA and TA/ADR increased by 31.4% and 85.6%, respectively. Further, starch, plasticizer, and blowing agent were melt extruded with this blend masterbatch, and the effects of masterbatch on the foamability, morphology, and properties of starch foams were investigated. When the masterbatch content was 10 phr, the obtained foam had the lowest apparent density (445.1 kg m−3), and the compressive strength, recovery, and water resistance of the foam were also improved significantly.
Investigation of the influences of the molecular weights and dosage ratios of polyvinyl alcohol on para‐aramid nanofibers/polyvinyl alcohol composite aerogels
Authors: Ren Jianhua , Hasuo Kensuke , Wei Yujun , Tabata Isao , Hori Teruo , Hirogaki Kazumasa 
Published: August 2022

AbstractPolymer‐based monolithic composite aerogels with a durable cross‐linked structure were fabricated using polyvinyl alcohol (PVA) and para‐aramid nanofibers (ANFs) as precursors, and supercritical fluid technology as a drying strategy. In order to give a clear insight into ANFs/PVA composite aerogels, we thoroughly investigated the influences of the molecular weights and dosage ratios of PVA on these composite aerogels, and clearly demonstrated the entire process of the evolution of “sol–gel‐aerogel.” The chemical composition, porous nanostructure, porosity, and mechanical performance of the ANFs/PVA composite aerogels were characterized by attenuated total reflectance‐Fourier transform‐infrared spectra (ATR‐FTIR), X‐ray photoelectron spectroscopy (XPS), field emission scanning electron microscope (FE‐SEM), nitrogen physical adsorption, and uniaxial compression, respectively. The results revealed the mechanism of the stable composition of ANFs/PVA binary system, and that both the molecular weights and dosage ratios of PVA in the ANFs/PVA composite aerogels have a significant influence on their properties. This work is beneficial to design and fabricate polymer‐based aerogels with desirable chemical and physical characteristics, and the obtained ANFs/PVA composite aerogels with appropriate molecular weight and dosage ratio of PVA possess well‐balanced comprehensive properties, which offer the potential for a wide range of applications.
Autologous blood products: Usage and preparation protocols
Authors: Palaiologou Archontia , Keeling Francis 
Published: July 2022

AbstractFocused clinical questionWhat are the appropriate preparation protocols for autologous blood products to support their clinical utilization?SummaryAutologous blood products provide a unique clinical benefit. Their popularity among the professions is growing. However, as this is a rapidly evolving field, multiple modalities are presented within the literature. Frequently there is no demonstrated superiority to previous iterations. This brief review attempts to offer a concise chronology on their evolution, preparation, and where possible, evidence to support their clinical utilization.ConclusionsThe field of autologous blood products is expanding rapidly. These products appear to yield variable clinical benefits in specific indications. However, evidence supporting their universal application is scant, and the superiority of one formulation versus another is yet to be demonstrated.
Exploring the role of practitioner lived experience of mental health issues in counselling and psychotherapy
Authors: Cleary Rua , Armour Cherie 
Published: July 2022

AbstractInsights gained from lived experience of mental health issues are increasingly utilised in the delivery of mental health services, reflecting a growing recognition of the value of experiential knowledge. Despite this recognition, there is a dearth of literature on the lived experience of counsellors and psychotherapists, and as such, insight into how counsellors and psychotherapists understand and experience their dual patient‐therapist identity is limited. This study explores the role of practitioner‐lived experience in counselling and psychotherapy. Semi‐structured interviews were conducted with two counsellors and one psychotherapist, and transcripts were analysed using interpretative phenomenological analysis. Four themes were identified: (a) identity as a practitioner; (b) self‐disclosure as enhancing therapeutic relationships; (c) importance of supervision; and (d) healing and recovery. This study adds to a growing body of research on the value of experiential knowledge in the production of mental health services, providing insight into how lived‐experience practitioners experience their dual identity within their practice, and how they can be supported in exploring and valuing their experience.
Expanding the Scope of Genetically Encoded Lysine Post‐Translational Modifications with Lactylation, β‐Hydroxybutyrylation and Lipoylation
Authors: Ren Conghui , Wu Qifan , Xiao Ruotong , Ji Yanli , Yang Xiaochen , Zhang Zhuo , Qin Hongqiang , Ma Jun‐An , Xuan Weimin 
Published: July 2022

AbstractPost‐translational modifications (PTMs) occurring on lysine residues, especially diverse forms of acylations, have seen rapid growth over the past two decades. Among them, lactylation and β‐hydroxybutyrylation of lysine side‐chains are newly identified histone marks and their implications in physiology and diseases have aroused broad research interest. Meanwhile, lysine lipoylation is highly conserved in diverse organisms and well known for its pivotal role in central metabolic pathways. Recent findings in the proteomic profiling of protein lipoylation have nonetheless suggested a pressing need for an extensive investigation. For both basic and applied research, it is necessary to prepare PTM‐bearing proteins particularly in a site‐specific manner. Herein, we use genetic code expansion to site‐specifically generate these lysine PTMs, including lactylation, β‐hydroxybutyrylation and lipoylation in proteins in E. coli and mammalian cells. Notably, using strategies including activity‐based selection, screening and rational design, unique pyrrolysyl‐tRNA synthetase variants were successfully evolved for each of the three non‐canonical amino acids, which enabled efficient production of recombinant proteins. Through encoding these ncAAs, we examined the deacylase activities of mammalian sirtuins to these modifications, and importantly we unfold the lipoamidase activity of several sirtuins.