bluuebunny/crossref_metadata_2025_split huggingface dataset:
Recyclable Copper Nanoparticles‐Catalyzed Hydroboration of Alkenes and β‐Borylation of α,β‐Unsaturated Carbonyl Compounds with Bis(Pinacolato)Diboron
Authors: Shegavi Mahadev L. , Saini Suresh , Bhawar Ramesh , Vishwantha Meghana Desai , Bose Shubhankar Kumar 
Published: March 2021

AbstractNano‐ferrite‐supported Cu nanoparticles (Fe‐dopamine‐Cu NPs) catalyzed anti‐Markovnikov‐selective hydroboration of alkenes with B2pin2 is reported under mild reaction conditions. This protocol can be applied to a broad range of substrates with high functional group compatibility. In addition, we demonstrated the use of Fe‐dopamine‐Cu NPs as a catalyst for the β‐borylation of α,β‐unsaturated ketones and ester, providing alkylboronate esters in up to 98% yield. Reuse of the magnetically recyclable catalyst resulted in no significant loss of activity in up to five reaction runs for both systems.magnified image
Palladium‐Catalyzed Thiocarbonylation of Benzyl Chlorides with Sulfonyl Chlorides for the Synthesis of Arylacetyl Thioesters
Authors: Wang Wei , Qi Xinxin , Wu Xiao‐Feng 
Published: March 2021

AbstractA convenient procedure for the synthesis of thioesters has been developed via a palladium‐catalyzed thiocarbonylation of benzyl chlorides with sulfonyl chlorides. Various arylacetyl thioesters were produced in good yields by using sulfonyl chlorides as an odorless sulfur source. Furthermore, W(CO)6 exhibited dual roles as both a solid CO surrogate and reductant here.magnified image
Soft Electronic Platforms Combining Elastomeric Stretchability and Biodegradability
Authors: Held Martin , Pichler Alexander , Chabeda Joshua , Lam Natalie , Hindenberg Philip , Romero‐Nieto Carlos , Hernandez‐Sosa Gerardo 
Published: March 2021

AbstractSoft and stretchable electronic devices are expected to offer technological advances in the field of robotics, human–machine interfacing, and healthcare. Employing biodegradable elastomers, hydrogels, and nontoxic conductors would add significant value to and minimize the ecological impact of such disposable and transient electronic applications. Here, the biodegradable and photo‐crosslinkable elastomer poly(glycerol sebacic) acrylate (PGSA) is characterized for its use in soft and stretchable electronics. Its mechanical properties are investigated in terms of their chemical composition and compared to commonly used gelatin hydrogels. Furthermore, these materials are combined with interconnects made of liquid Galinstan in order to create functional substrates with certified biodegradability under ISO standards. The combination of these materials produces elastic circuit boards that act as soft platforms for body‐mounted sensors or biodegradable stretchable light‐emitting devices. These soft platforms reveal linear elongations at a break of 130% to 350% and similar moduli to nondegradable elastomers and human tissue, without any decrease in conductivity. Advanced applications in biofriendly packaging, soft robotics, and healthcare will greatly benefit from these biodegradable devices.
Lead‐Free Halide Double Perovskite Nanocrystals for Light‐Emitting Applications: Strategies for Boosting Efficiency and Stability
Authors: Tang Huidong , Xu Yanqiao , Hu Xiaobo , Hu Qing , Chen Ting , Jiang Weihui , Wang Lianjun , Jiang Wan 
Published: March 2021

AbstractLead‐free halide double perovskite (HDP) nanocrystals are considered as one of the most promising alternatives to the lead halide perovskite nanocrystals due to their unique characteristics of nontoxicity, robust intrinsic thermodynamic stability, rich and tunable optoelectronic properties. Although lead‐free HDP variants with highly efficient emission are synthesized and characterized, the photoluminescent (PL) properties of colloidal HDP nanocrystals still have enormous challenges for application in light‐emitting diode (LED) devices due to their intrinsic and surface defects, indirect band, and disallowable optical transitions. Herein, recent progress on the synthetic strategies, ligands passivation, and metal doping/alloying for boosting efficiency and stability of HDP nanocrystals is comprehensive summarized. It begins by introducing the crystalline structure, electronic structure, and PL mechanism of lead‐free HDPs. Next, the limiting factors on PL properties and origins of instability are analyzed, followed by highlighting the effects of synthesis strategies, ligands passivation, and metal doping/alloying on the PL properties and stability of the HDPs. Then, their preliminary applications for LED devices are emphasized. Finally, the challenges and prospects concerning the development of highly efficient and stable HDP nanocrystals‐based LED devices in the future are proposed.
Engineering the Activity and Stability of MOF‐Nanocomposites for Efficient Water Oxidation
Authors: Wang Yuan , Liu Borui , Shen Xiangjian , Arandiyan Hamidreza , Zhao Tingwen , Li Yibing , Garbrecht Magnus , Su Zhen , Han Li , Tricoli Antonio , Zhao Chuan 
Published: March 2021

AbstractMetal–organic frameworks (MOFs) are considered to be promising candidates for electrochemical water splitting. However, most MOFs are characterized by low electronic conductivity limiting their use as bulk materials for anodes and cathodes. Furthermore, the understanding of the critical parameters controlling the activity and stability of MOF electrocatalysts is still insufficient. Herein, a systematic analysis is presented of the key structural parameters controlling the oxygen evolution reaction (OER) performance and stability of a representative family of bimetallic NiFe‐MOFs, where the role of the metal cations on the accessible active sites and intrinsic activity can be investigated independently from the crystal structure. The models and in‐depth structural and morphological characterizations reveal a hierarchy of properties affecting the OER activity with accessible sites and intrinsic activity playing a major role in the charge transfer efficiency. Optimization of these properties and addition of a conductive support substrate leads to efficient MOF‐nanocomposite electrocatalysts achieving a low overpotential of 258 mV at a current density of 10 mA cm−2 with a small Tafel slope of 49 mV dec−1 and excellent stability for more than 32 h of continuous OER in alkaline medium.
An Efficient, Sustainable Rhodium‐Catalyzed and Ionic Liquid‐Mediated C−H Thiolation and Selenation of Acetanilide with Diaryl Disulfides and Diaryl Diselenides
Authors: Rui Xiyan , Zhu Yueyue , Dai Rupeng , Huang Chaoqun , Wang Chao , Si Dongjuan , Wang Xi , Zhang Xiaoyuan , Wen Hongmei , Li Wei , Liu Jian 
Published: March 2021

AbstractWe established an efficient and sustainable rhodium(III)‐catalyzed and ionic liquid‐mediated C−S and C−Se formation from readily available starting material acetanilide with diaryl disulfides and diaryl diselenides. The C−H activation proceeds in ionic liquid without extra silver salt as additive, and the catalytic media can be reused for several times to accomplish the catalysts sustainable utilization. Furthermore, this synthesis protocol is suitable for a wide functional group compatibility, and the directing group can be easily removed. Most importantly it can be developed as a facile access to phenothiazine scaffold with potent biological activities, thus this strategy can be broadly applied to organic synthesis and medicinal chemistry.
Iron‐Catalyzed Oxidative Decabonylation/Radical Cyclization of Aliphatic Aldehydes with Biphenyl Isocyanides: A New Pathway For the Synthesis of 6‐Alkylphenanthridines
Authors: Luo Zaigang , Li Rui , Zhu Tao , Liu Chen‐Fu , Feng Haoran , Aboagye Nartey Kojo , Liu Qiannan , Xu Xuemei 
Published: March 2021

AbstractA facile and efficient synthetic approach to C6 functionalized phenanthridines was developed. The iron catalyzed oxidative reaction undergoes subsequent decarbonylation, radical addition and cyclization processes by using aliphatic aldehydes as the alkyl radical precursors. This protocol offers a new pathway for the synthesis of 6‐alkylphenanthridines.
Cognitive measures lacking in EHR prior to dementia or Alzheimer's disease diagnosis
Authors: Maserejian Nancy , Krzywy Henry , Eaton Susan , Galvin James E. 
Published: March 2021

AbstractIntroductionThe extent that cognitive measures are documented in electronic health records (EHR) is important for quality care and addressing disparities in timely diagnosis of dementia or Alzheimer's disease (AD).MethodsAnalysis of U.S. EHR data to describe the frequency and factors associated with cognitive measures prior to diagnosis of dementia (N = 111,125) or AD (N = 30,203).ResultsOnly 11% of dementia patients and 24% of AD patients had a cognitive measure documented in the 5 years prior to diagnosis. Black race, older age, non‐commercial health insurance, lower mean neighborhood income, greater in‐patient stays, and fewer out‐patient visits were associated with lacking cognitive measures.DiscussionExtensive missing cognitive data and differences in the availability of cognitive measures by race, age, and socioeconomic factors hinder patient care and limit utility of EHR for dementia research. Structured fields and prompts for cognitive data inputs at the point of care may help address these gaps.
Covalent Probes for Aggregated Protein Imaging via Michael Addition
Authors: Wan Wang , Huang Yanan , Xia Qiuxuan , Bai Yulong , Chen Yuwen , Jin Wenhan , Wang Mengdie , Shen Di , Lyu Haochen , Tang Yuqi , Dong Xuepeng , Gao Zhenming , Zhao Qun , Zhang Lihua , Liu Yu 
Published: March 2021

AbstractCovalent chemical reactions to modify aggregated proteins are rare. Here, we reported covalent Michael addition can generally occur upon protein aggregation. Such reactivity was initially discovered by a bioinspired fluorescent color‐switch probe mimicking the photo‐conversion mechanism of Kaede fluorescent protein. This probe was dark with folded proteins but turned on red fluorescence (620 nm) when it non‐covalently bound to misfolded proteins. Supported by the biochemical and mass spectrometry results, the probe chemoselectively reacted with the reactive cysteines of aggregated proteins via covalent Michael addition and gradually switched to green fluorescence (515 nm) upon protein aggregation. Exploiting this Michael addition chemistry in the malachite green dye derivatives demonstrated its general applicability and chemical tunability, resulting in different fluorescence color‐switch responses. Our work may offer a new avenue to explore other chemical reactions upon protein aggregation and design covalent probes for imaging, chemical proteomics, and therapeutic purposes.
Lineare gepaarte Elektrolyse – Realisierung von 200 % Stromausbeute in stöchiometrischen Umsetzungen – die elektrochemische Bromierung von Alkenen
Authors: Strehl Julia , Abraham Marvin L. , Hilt Gerhard 
Published: March 2021

AbstractDie Erzeugung von Br2durch die Oxidation von Bromid‐Ionen an der Anode und die Reduktion von molekularem Sauerstoff an der Kathode zu H2O2führte in der Summe zur Erzeugung von zwei Molekülen Br2(=Vier‐Elektronen‐Oxidation), wobei lediglich zwei Elektronen durch die Lösung geschickt wurden. Das molekulare Brom wurde zur Bromierung von Alkenen genutzt, woraufhin eine lineare gepaarte Elektrolyse verwirklicht wurde, welche Stromausbeuten von bis zu 200 % aufweist. Zudem gelangen die Diiodierung von Cyclohexen sowie die elektrophile aromatische Bromierung eines Elektronen‐reichen Aromaten mit jeweils 168 % Stromausbeute.
An Endoplasmic Reticulum Specific Pro‐amplifier of Reactive Oxygen Species in Cancer Cells
Authors: Xu Hong‐Gui , Schikora Margot , Sisa Miroslav , Daum Steffen , Klemt Insa , Janko Christina , Alexiou Christoph , Bila Galyna , Bilyy Rostyslav , Gong Wenjie , Schmitt Michael , Sellner Leopold , Mokhir Andriy 
Published: March 2021

AbstractThe folding and export of proteins and hydrolysis of unfolded proteins are disbalanced in the endoplasmic reticulum (ER) of cancer cells, leading to so‐called ER stress. Agents further augmenting this effect are used as anticancer drugs including clinically approved proteasome inhibitors bortezomib and carfilzomib. However, these drugs can affect normal cells, which also rely strongly on ER functions, leading, for example, to accumulation of reactive oxygen species (ROS). To address this problem, we have developed ER‐targeted prodrugs activated only in cancer cells in the presence of elevated ROS amounts. These compounds are conjugates of cholic acid with N‐alkylaminoferrocene‐based prodrugs. We confirmed their accumulation in the ER of cancer cells, their anticancer efficacy, and cancer cell specificity. These prodrugs induce ER stress, attenuate mitochondrial membrane potential, and generate mitochondrial ROS leading to cell death via necrosis. We also demonstrated that the new prodrugs are activated in vivo in Nemeth‐Kellner lymphoma (NK/Ly) murine model.
FRET Modulated Signaling: A Versatile Strategy to Construct Photoelectrochemical Microsensors for In Vivo Analysis
Authors: Ye Xiaoxue , Wang Xing , Kong Yao , Dai Mengjiao , Han Dongxue , Liu Zhihong 
Published: March 2021

AbstractMicroelectrode‐based electrochemical (EC) and photoelectrochemical (PEC) sensors are promising candidates for in vivo analysis of biologically important chemicals. However, limited selectivity in complicated biological systems and poor adaptability to electrochemically non‐active species restrained their applications. Herein, we propose the concept of modulating the PEC output by a fluorescence resonance energy transfer (FRET) process. The emission of energy donor was dependent on the concentration of target SO2, which in turn served as the modulator of the photocurrent signal of the photoactive material. The employment of optical modulation circumvented the problem of selectivity, and the as‐fabricated PEC microelectrode showed good stability and reproducibility in vivo. It can monitor fluctuations of SO2levels in brains of rat models of cerebral ischemia‐reperfusion and febrile seizure. More significantly, such a FRET modulated signaling strategy can be extended to diverse analytes.
Non‐Solvating and Low‐Dielectricity Cosolvent for Anion‐Derived Solid Electrolyte Interphases in Lithium Metal Batteries
Authors: Ding Jun‐Fan , Xu Rui , Yao Nan , Chen Xiang , Xiao Ye , Yao Yu‐Xing , Yan Chong , Xie Jin , Huang Jia‐Qi 
Published: March 2021

AbstractLithium (Li) metal anodes hold great promise for next‐generation high‐energy‐density batteries, while the insufficient fundamental understanding of the complex solid electrolyte interphase (SEI) is the major obstacle for the full demonstration of their potential in working batteries. The characteristics of SEI highly depend on the inner solvation structure of lithium ions (Li+). Herein, we clarify the critical significance of cosolvent properties on both Li+ solvation structure and the SEI formation on working Li metal anodes. Non‐solvating and low‐dielectricity (NL) cosolvents intrinsically enhance the interaction between anion and Li+ by affording a low dielectric environment. The abundant positively charged anion–cation aggregates generated as the introduction of NL cosolvents are preferentially brought to the negatively charged Li anode surface, inducing an anion‐derived inorganic‐rich SEI. A solvent diagram is further built to illustrate that a solvent with both proper relative binding energy toward Li+ and dielectric constant is suitable as NL cosolvent.
Bioinspired Synergistic Photochromic Luminescence and Programmable Liquid Crystal Actuators
Authors: Huang Yinliang , Bisoyi Hari Krishna , Huang Shuai , Wang Meng , Chen Xu‐Man , Liu Zhiyang , Yang Hong , Li Quan 
Published: March 2021

AbstractBioinspired smart materials with synergistic allochroic luminescence and complex deformation are expected to play an important role in many areas of science and technology. However, it is still challenging to fabricate such soft actuators with high programmability that can be manipulated in situ with high spatial resolution. Herein, we have incorporated terminally functionalized aggregation‐induced emission active tetraphenylethene derivative and photochromic spiropyran moieties into the networks of liquid crystal elastomers through covalent bonding to obtain the synergistic photochromic luminescence and programmable soft actuators. Bio‐mimic functions and light‐induced auxetic metamaterial‐like devices were shown to be feasible based on the combination of assembly and origami‐programming strategy. These bioinspired devices with synergistic photochromic luminescence and complex photodeformation abilities provide an elegant strategy to design multi‐functional liquid crystal actuators.
Ferroptosis Photoinduced by New Cyclometalated Iridium(III) Complexes and Its Synergism with Apoptosis in Tumor Cell Inhibition
Authors: Yuan Hao , Han Zhong , Chen Yuncong , Qi Fen , Fang Hongbao , Guo Zijian , Zhang Shuren , He Weijiang 
Published: March 2021

AbstractLimited therapeutic efficacy to hypoxic and refractory solid tumors has hindered the practical application of photodynamic therapy (PDT). Two new benzothiophenylisoquinoline (btiq)‐derived cyclometalated IrIII complexes, IrL1 and MitoIrL2, were constructed as potent photosensitizers, with the latter being designed for mitochondria accumulation. Both complexes demonstrated a type I PDT process and caused photoinduced ferroptosis in tumor cells under hypoxia. This ferroptosis featured lipid peroxide accumulation, mitochondria shrinkage, down‐regulation of glutathione peroxidase 4 (GPX4), and ferrostatin‐1 (Fer‐1)‐inhibited cell death. Upon photoirradiation under hypoxia, mitochondria targeting MitoIrL2 caused mitochondria membrane potential (MMP) collapse, ATP production suppression, and induced cell apoptosis. The synergetic effect of ferroptosis and apoptosis causes MitoIrL2 to outperform IrL1 in inhibiting the growth of MCF‐7, PANC‐1, MDA‐MB‐231 cells and multicellular spheroids. This study demonstrates the first example of ferroptosis induced by photosensitizing IrIII complexes. Moreover, the synergism of ferroptosis and apoptosis provides a promising approach for combating hypoxic solid tumors through type I PDT processes.
Linear Paired Electrolysis—Realising 200 % Current Efficiency for Stoichiometric Transformations—The Electrochemical Bromination of Alkenes
Authors: Strehl Julia , Abraham Marvin L. , Hilt Gerhard 
Published: March 2021

AbstractThe generation of bromine by oxidation of bromide anions at the anode and reduction of molecular oxygen at the cathode to hydrogen peroxide resulted in the overall formation of two molecules of Br2(=four electron oxidation) by passing just two electrons through the solution. The bromine was used for the bromination of alkenes and thereby a linear paired electrolysis was attained which resulted in current efficencies of up to 200 %. Also, the diiodination of cyclohexene as well as the electrophilic aromatic bromination of an electron‐rich arene were realised both in 168 % current efficiencies.
Defect Engineering in Metal–Organic Frameworks Towards Advanced Mixed Matrix Membranes for Efficient Propylene/Propane Separation
Authors: Lee Tae Hoon , Jung Jae Gu , Kim Yu Jin , Roh Ji Soo , Yoon Hee Wook , Ghanem Bader S. , Kim Hyo Won , Cho Young Hoon , Pinnau Ingo , Park Ho Bum 
Published: March 2021

AbstractHighly permselective and durable membrane materials have been sought for energy‐efficient C3H6/C3H8 separation. Mixed‐matrix membranes (MMMs) comprising a polymer matrix and metal–organic frameworks (MOFs) are promising candidates for this application; however, rational matching of filler‐matrix is challenging and their separation performances need to be further improved. Here, we propose a novel strategy of “defect engineering” in MOFs as an additional degree of freedom to design advanced MMMs. MMMs incorporated with defect‐engineered MOFs exhibit exceptionally high C3H6 permeability and maintained C3H6/C3H8 selectivity, especially with enhanced stability under industrial mixed‐gas conditions. The gas transport, sorption, and material characterizations reveal that the defect sites in MOFs provide the resulting MMMs with not only ultrafast diffusion pathways but also favorable C3H6 sorption by forming complexation with unsaturated open metal sites, confirmed by in situ FT‐IR studies. Most importantly, the concept is also valid for different polymer matrices and gas pairs, demonstrating its versatile potential in other fields.
Bedeutung der Frequenz für das Vibrationsrammen von Spundbohlen
Authors: Massarsch Karl Rainer , Wersäll Carl , Fellenius Bengt H. , Ehrmanntraut Editha 
Published: March 2021

AbstractBei modernen Vibratoren können die Vibrationsfrequenz und das exzentrische Moment während des Rammens verändert werden. Das dynamische Zusammenwirken der schwingenden Bohle mit dem umgebenden Boden kann durch Feldmessungen untersucht werden. Bisher wurde der Einfluss der Vibrationsfrequenz auf den Eindringvorgang und die Ausstrahlung von Vibrationen in die Umgebung nicht ausreichend beachtet, obwohl die Frequenz für die Rammbarkeit und die Erschütterungsausbreitung von Bedeutung sind. In vorliegendem Beitrag werden die Ergebnisse von drei Proberammungen beschrieben, bei denen Doppelbohlen in einen mitteldichten kiesigen Sandboden einvibriert wurden. Messungen wurden am Vibrator, an der Spundbohle und im Boden durchgeführt, womit u. a. die Frequenz, die Schwingungsamplitude, die Eindringgeschwindigkeit der Bohle und die Bodenerschütterungen registriert wurden. Eine Analyse der Messwerte zeigt, dass die Schwingungsfrequenz ein wichtiger Parameter ist. Wenn die Bohle nahe der Resonanzfrequenz des Vibrator‐Bohle‐Bodensystems erregt wird, schwingt die Bohle in Phase mit dem umgebenden Boden. In diesem Zustand sinkt die Eindringgeschwindigkeit ab, während die Vibrationsausstrahlung in den Boden ansteigt. Die Resonanzfrequenz kann einfach durch Messung der Bodenschwingungen bestimmt werden. Effektives Vibrationsrammen wird erreicht, wenn die Vibrationsfrequenz deutlich höher als die Resonanzfrequenz ist. Vibrationsmessungen zeigen, dass durch das Absenken des exzentrischen Moments stärkere Bodenerschütterungen verursacht werden können.
Clash of the calculators: External validation of prostate cancer risk calculators in men undergoing mpMRI and transperineal biopsy
Authors: Wei G. , Kelly B. D. , Timm B. , Perera M. , Lundon D. J. , Jack G. , Bolton D. M. 
Published: March 2021

AbstractObjectiveTo compare the accuracy of the European Randomized Study of Screening for Prostate Cancer (ERSPC) RC, MRI‐ERSPC‐RC, and Prostate Biopsy Collaborative Group (PBCG) RC in patients undergoing transperineal prostate biopsy.Patients and methodsWe identified 392 patients who underwent mpMRI before transperineal prostate biopsy across multiple public and private institutions between January 2017 and August 2019. The estimated probabilities of detecting PCa and significant PCa were calculated using the MRI‐ERSPC‐RC, ERSPC‐RC, and PBCG‐RC. Receiver operating characteristic (ROC) curves for each calculator were generated and the area underneath the curve (AUC) was compared. Calibration and clinical utility were assessed with calibration plots and decision curve analysis, respectively.ResultsPCa was detected in 285 patients (72.7%) with significant PCa found in 200 patients (51.1%). ROC curve analysis found the MRI‐ERSPC‐RC outperformed the ERSPC‐RC and PBCG‐RC. For the prediction of PCa, the AUC was 0.756, 0.696, and 0.675 for the MRI‐ERSPC‐RC, ERSPC‐RC, and PBCG‐RC, respectively. The AUC for the prediction of significant PCa was 0.803, 0.745, and 0.746 for the MRI‐ERSPC‐RC, ERSPC‐RC, and PBCG‐RC, respectively.ConclusionsOur study validated the ERSPC‐RC, MRI‐ERSPC‐RC, and PBCG‐RC in a cohort undergoing transperineal prostate biopsy with the MRI‐ERSPC‐RC performing the best. These RCs may enable improved shared decision making and help to guide patient selection for biopsy.