bluuebunny/crossref_metadata_2025_split huggingface dataset:
A Generalized Surface Chalcogenation Strategy for Boosting the Electrochemical N2 Fixation of Metal Nanocrystals
Authors: Yang Chengyong , Huang Bolong , Bai Shuxing , Feng Yonggang , Shao Qi , Huang Xiaoqing 
Published: May 2020

AbstractElectrocatalytic nitrogen reduction reaction (NRR) is a promising process relative to energy‐intensive Haber–Bosch process. While conventional electrocatalysts underperform with sluggish paths, achieving dissociation of N2 brings the key challenge for enhancing NRR. This study proposes an effective surface chalcogenation strategy to improve the NRR performance of pristine metal nanocrystals (NCs). Surprisingly, the NH3 yield and Faraday efficiency (FE) (175.6 ± 23.6 mg h–1 g–1Rh and 13.3 ± 0.4%) of Rh‐Se NCs is significantly enhanced by 16 and 15 times, respectively. Detailed investigations show that the superior activity and high FE are attributed to the effect of surface chalcogenation, which not only can decrease the apparent activation energy, but also inhibit the occurrence of the hydrogen evolution reaction (HER) process. Theoretical calculations reveal that the strong interface strain effect within core@shell system induces a critical redox inversion, resulting in a rather low valence state of Rh and Se surface sites. Such strong correlation indicates an efficient electron‐transfer minimizing NRR barrier. Significantly, the surface chalcogenation strategy is general, which can extend to create other NRR metal electrocatalysts with enhanced performance. This strategy open a new avenue for future NH3 production for breakthrough in the bottleneck of NRR.
Colossal Granular Lithium Deposits Enabled by the Grain‐Coarsening Effect for High‐Efficiency Lithium Metal Full Batteries
Authors: Zhang Weidong , Wu Qiang , Huang Jinxin , Fan Lei , Shen Zeyu , He Yi , Feng Qi , Zhu Guannan , Lu Yingying 
Published: May 2020

AbstractThe low Coulombic efficiency of the lithium metal anode is recognized as the real bottleneck to practical high‐efficiency lithium metal batteries with limited Li excess. The grain size and microstructure of deposited lithium strongly influences the lithium plating/stripping efficiency. Here, a solubilizer‐mediated carbonate electrolyte that can realize grain coarsening of lithium deposits (>20 µm in width) with oriented columnar morphology, which is in sharp contrast with conventional nanoscale dendrite‐like lithium deposits in carbonate electrolytes, is reported. It exhibits improved Li Coulombic efficiency to 98.14% at a high capacity of 3 mAh cm−2 over 150 cycles, because the colossal lithium deposition with minimal tortuosity can maintain the bulk Li with continuous electron conducting pathway during the stripping process, thus enabling efficient Li utilization. Li/NMC811 full batteries, composed of thin Li anode (45 µm) and a high‐capacity NMC811 cathode (16.7 mg cm−2), can achieve at least 12 times longer lifespan (200 cycles).
Microfluidic Synthesis of Luminescent and Plasmonic Nanoparticles: Fast, Efficient, and Data‐Rich
Authors: Nette Julia , Howes Philip D. , deMello Andrew J. 
Published: May 2020

AbstractMicrofluidic approaches to nanomaterial synthesis provide an effective means of making high quality products, with exquisite control over electronic, optical, and structural properties. Furthermore, microfluidic reactors integrating analytics and real‐time reaction control have recently emerged as powerful tools in automating materials exploration and reaction parameter mapping, with a rapidity and efficiency that is inaccessible to traditional flask‐based methods. Herein, the recent innovations in the microfluidic synthesis of photonic nanoparticles, whose varied luminescent and plasmonic properties have found great application in the biomedical and optoelectronic sciences, are presented. Special attention is placed on the achievements and promise of microfluidic approaches in automated multidimensional reaction parameter screening employing in situ optical characterization. In an extended outlook, the future of the field is explored, looking toward the integration of smart control systems and machine learning algorithms, and demonstrating how maximal positive impact can be achieved. Far from degrading or replacing the ingenuity of the experimentalist, these tools will provide new powers of exploration, augmenting the discovery process. Further, through automation and miniaturization, it is expected that such approaches will fulfill the moral imperative of maximizing the benefit derived from the natural resources consumed in conducting research.
A General Approach of Adjusting the Surface‐Free Energy of the Interfacial Layer for High‐Performance Organic Solar Cells
Authors: Alharbi Njud S. , Wang Chenyun , Alsaadi Fawaz E. , Rabah Samar O. , Tan Zhan'ao 
Published: May 2020

AbstractFor organic solar cells, the different surface‐free energies (SFE) of donors and acceptors leads to inhomogeneous distribution at the upper and bottom surfaces of the photoactive layer. Undesired distribution of donors and acceptors is unfavorable for charge collection. Adjusting the SFE of the underlying interfacial layer can effectively change the distribution of donors and acceptors within the photoactive layer. Herein, Nafion, a perfluorinated polymer containing the fluorocarbon backbone and perfluorovinyl ether branch with sulfonic acid end groups, is introduced to adjust the SFE of poly‐(3,4‐ethylenedioxythiophene):poly‐(styrenesulphonicacid) (PEDOT:PSS). The work‐function change of the PEDOT:PSS before and after doping with Nafion is explored by ultraviolet photoelectron spectroscopy. The contact angles of water and diiodomethane on the PEDOT:PSS and PEDOT:PSS‐Nafion are measured and their SFE are calculated from the Owens formula. Interfacial layer induced phase separation is investigated by energy‐dispersive spectroscopy and transmission electron microscopy. The device resistance and carrier lifetime are investigated by electrochemical impedance spectroscopy and intensity‐modulated photovoltage spectroscopy. By accurately adjusting the ratio of Nafion to PEDOT:PSS, the optimized device with PBDB‐TCL:IT‐4F achieves the power conversion efficiency (PCE) of 14.12% and the device based on PEDOT:PSS‐Nafion with PBDB‐TF:Y6 achieves the PCE of 16.31%.
Theoretical Study of Interfacial and Electronic Properties of Transition Metal Dichalcogenides and Organic Molecules Based van der Waals Heterostructures
Authors: Habib Mohammad Rezwan , Wang Weijia , Khan Afzal , Khan Yahya , Obaidulla Sk Md , Pi Xiaodong , Xu Mingsheng 
Published: May 2020

AbstractHeterostructures built from 2D materials and organic semiconductors offer a unique platform for addressing many fundamental physics and construction of functional devices. Interfaces play a crucial role in tailoring the heterostructure properties. Here, density functional theory computations are performed to explore the interfacial properties of heterostructures made of group VI transition metal dichalcogenides (TMD) and organic molecules such as perylene tetracarboxylic dianhydride (PTCDA) and pentacene. First principle calculations predict that the organic pentacene layer exhibits covalent interfacing with MoSe2 and WSe2, while the interface of other studied TMD/organic heterostructures form van der Waals (vdW) interfaces. Owing to the different molecular geometry of PTCDA and pentacene in their respective heterostructures, the work function can be modulated of the order of 1.0 eV in comparison with pure monolayer MX2 in MX2/pentacene (M = Mo, W; X = S, Se) heterostructures, while the change of work function in MX2/PTCDA (M = Mo, W; X = S, Se) is negligible (order of 0.1 eV) in comparison with pure monolayer MX2. This study will be helpful to design high‐performance optoelectronic devices based on TMDs and organic semiconductors.
Over 20% Efficient and Stable Non‐Fullerene‐Based Ternary Bulk‐Heterojunction Organic Solar Cell with WS2 Hole‐Transport Layer and Graded Refractive Index Antireflection Coating
Authors: Ram Kiran Sreedhar , Singh Jai 
Published: May 2020

AbstractThe power conversion efficiency (PCE) of a ternary organic solar cell (TOSC) with an active layer consisting of PBDB‐T‐2F and two non‐fullerene materials Y6 and SF(BR)4 is simulated. Tungsten disulphide (WS2) is used as the hole transport layer (HTL) to reduce the contact resistance between the active layer and anode which enhances the internal quantum efficiency to 91.7%. It is found that the use of a highly absorbing non‐fullerene small molecule acceptor, SF(BR)4, enhances the absorption as well as improves the stability. Finally, the incorporation of the graded refractive index coating, in the form of moth‐eye shaped nanostructures, on the top of glass reduces the reflection losses and enhances the transmission coefficient from 0.88 to 0.94. Thus, the TOSC simulated here, of the structure moth‐eye‐AR/glass/ITO/WS2/PBDB‐T‐2F:Y6:SF(BR)4/PFN‐Br/Al, produces a PCE of 20.87%. The results presented in this paper are expected to provide useful guidance for fabricating highly efficient and stable hybrid bulk‐heterojunction solar cells.
Ultralow Quiescent Power‐Consumption Wake‐Up Technology Based on the Bionic Triboelectric Nanogenerator
Authors: Zhang Chenxi , Dai Keren , Liu Di , Yi Fang , Wang Xiaofeng , Zhu Lianqing , You Zheng 
Published: May 2020

AbstractWake‐up circuits in smart microsystems make huge contributions to energy conservation of electronic networks in unmanned areas, which still require higher pressure‐triggering sensitivity and lower power consumption. In this work, a bionic triboelectric nanogenerator (bTENG) is developed to serve as a self‐powered motion sensor in the wake‐up circuit, which captures slight mechanical disturbances and overcomes the drawback of conventional self‐powered motion sensors in the wake‐up circuit that the circuit can only be triggered when a considerable pressure is applied on the sensor. The bTENG mimics the structure of plants and the addition of the leaf‐shaped tentacle structures can increase the electrical outputs by four times, which largely extends the detection range of the wake‐up circuit. The bTENG can detect both noncontact and contact mechanical disturbances; and voltages generated from both situations can trigger the wake‐up system. Moreover, the specially designed circuit that is compatible with the bTENG can help more accurately control the wake‐up system and prolong the battery life of the electronic networks to 12.4 times. An intrusion detection system is established in the wake‐up circuit to distinguish human motion and judge the scene. This work opens new horizons for wake‐up technologies, and provides new routes for persistent sensing.
Carbazole Derivatized n‐Alkyl Methacrylate Polymeric Memristors as Flexible Synaptic Substitutes
Authors: McFarlane Tucker , Bandera Yuriy , Grant Benjamin , Zdyrko Bogdan , Foulger Stephen H. , Vilčáková Jarmila , Sáha Petr , Pfleger Jiří 
Published: May 2020

AbstractA memristor is a two‐terminal electronic device whose observed conductance is dependent on the history of the voltage that has been applied across the device. In this effort, poly(11‐(9H‐carbazol‐9‐yl)undecyl methacrylate) (PUMA) is fabricated into a two‐terminal device with Al and ITO electrodes and exhibits a number of signature memristor characteristics such as an irreversible transition from an insulator to a conductor at a specific DC voltage and hysteresis in the AC response. A PUMA‐based device could transition through a multitude of conductance states with varying voltage, allowing the device to exhibit spike‐timing‐dependent‐plasticity, an essential feature in replicating the behavior of biological synapses.
The use of venetoclax‐based salvage therapy for post‐hematopoietic cell transplantation relapse of acute myeloid leukemia
Authors: Byrne Michael , Danielson Nathalie , Sengsayadeth Salyka , Rasche Adrianne , Culos Katie , Gatwood Katie , Wyatt Houston , Chinratanalab Wichai , Dholaria Bhagirathbhai , Ferrell P. Brent , Fogo Kristin , Goodman Stacey , Jagasia Madan , Jayani Reena , Kassim Adetola , Mohan Sanjay R. , Savani Bipin N. , Strickland Stephen A. , Engelhardt Brian G. , Savona Michael 
Published: May 2020

AbstractFor patients with high risk myeloid disease, allogeneic hematopoietic cell transplantation (HCT) is the only potentially curative therapy. Unfortunately, many of these patients relapse after HCT and have a limited survival. The recent approval of venetoclax, an orally bioavailable BCL‐2 inhibitor, resulted in significant responses in treatment naïve acute myeloid leukemia (AML), and off‐label use in the relapsed/refractory setting is increasing. We report the outcomes of 21 patients who underwent allogeneic HCT for myeloid disease, relapsed with AML, and were treated with venetoclax. Several patients had poor risk features including antecedent hematologic malignancy (6/21), complex karyotype (6/21), and TP53 mutations (5/21). The median age was 64.5 years and time from HCT to relapse was 5.7 months (range: 0.9 to 44.9 months). Of the 19 patients who were assessed for response, there were meaningful treatment responses seen in eight patients: five CR, three CRi, zero PR, for an ORR of 42.1%. Treatment effect was seen in six additional patients, including four in the morphologic leukemia‐free state. Nine patients maintained their response for ≥3 months and eight were receiving therapy at data cut. Post‐HCT AML relapse has an exceedingly poor outcome, and venetoclax‐based therapy is a potent therapy option that should be studied prospectively in this setting.
Adult lead exposure from ammunition reloading and indoor residential shooting
Authors: Johnson‐Arbor Kelly , Soto Pelayia , Liu Lindsy 
Published: May 2020

AbstractThe use and maintenance of firearms is a common and often preventable source of adult lead exposure that is often poorly understood by medical professionals. This case describes an elevated blood lead level (BLL) in an adult man due to the exposure sources of ammunition reloading and indoor target shooting in the basement of his home and details the challenges involved in the diagnosis and management of such cases. The elevated BLL was reduced through strict attention to personal hygiene during the reloading process and while shooting, improved ventilation and cleaning of the basement, and avoidance of vacuuming and use of dry cleaning techniques. Medical providers may be unfamiliar with the risks of indoor residential shooting and how to ameliorate them; this knowledge deficit may result in delays in diagnosis as well as an inability to successfully mitigate the risks for exposure. Time‐sensitive diagnosis and treatment, comprehensive risk assessments, and reduction of exposure sources are important facets in the care of adult patients who are exposed to lead through recreational activities. Health care professionals should be aware of the potential dangers of ammunition reloading and indoor shooting, be familiar with ways to reduce lead exposure during these activities, and understand the resources that are available for the management of lead‐exposed patients.
Preparation of Steady 3D Dark State Entanglement in Dissipative Rydberg Atoms via Electromagnetic Induced Transparency
Authors: Zhu Xiao‐Yu , Jin Zhao , Liang Erjun , Zhang Shou , Su Shi‐Lei 
Published: May 2020

AbstractA scheme to prepare a 3D entangled state between a pair of Rydberg atoms via dissipative dynamics and electromagnetic induced transparency associated with the single‐atom dark state is proposed. The prepared entangled state is the dark state of the whole system. The scheme is also feasible regardless of initial purity or mixed state. Since the proposed scheme is based on the Rydberg block regime, the Rydberg–Rydberg interaction strength does not need to satisfy a certain relation with laser detuning, which is very different to the Rydberg‐antiblock‐based dissipative schemes. One group of Rydberg states and corresponding parameters to simulate the fidelity are used, which verify the feasibility of the scheme.
Stereoselective [4+2]‐Cycloaddition with Chiral Alkenylboranes
Authors: Ni Dongshun , Witherspoon Brittany P. , Zhang Hong , Zhou Chen , Houk K. N. , Brown M. Kevin 
Published: May 2020

AbstractA method for the stereoselective [4+2]‐cycloaddition of alkenylboranes and dienes is presented. This transformation was accomplished through the introduction of a new strategy that involves the use of chiral N‐protonated alkenyl oxazaborolidines as dieneophiles. The reaction leads to the formation of products that can be readily derivatized to more complex structural motifs through stereospecific transformations of the C−B bond such as oxidation and homologation. Detailed computation evaluation of the reaction has uncovered a surprising role of the counterion on stereoselectivity.
Mechanophotonics: Flexible Single‐Crystal Organic Waveguides and Circuits
Authors: Annadhasan Mari , Agrawal Abhijeet R. , Bhunia Surojit , Pradeep Vuppu Vinay , Zade Sanjio S. , Reddy C. Malla , Chandrasekar Rajadurai 
Published: May 2020

AbstractWe present the one‐dimensional optical‐waveguiding crystal dithieno[3,2‐a:2′,3′‐c]phenazine with a high aspect ratio, high mechanical flexibility, and selective self‐absorbance of the blue part of its fluorescence (FL). While macrocrystals exhibit elasticity, microcrystals deposited at a glass surface behave more like plastic crystals due to significant surface adherence, making them suitable for constructing photonic circuits via micromechanical operation with an atomic‐force‐microscopy cantilever tip. The flexible crystalline waveguides display optical‐path‐dependent FL signals at the output termini in both straight and bent configurations, making them appropriate for wavelength‐division multiplexing technologies. A reconfigurable 2×2‐directional coupler fabricated via micromanipulation by combining two arc‐shaped crystals splits the optical signal via evanescent coupling and delivers the signals at two output terminals with different splitting ratios. The presented mechanical micromanipulation technique could also be effectively extended to other flexible crystals.
Pd(II)‐Catalyzed Tandem Enantioselective Methylene C(sp3)−H Alkenylation–Aza‐Wacker Cyclization to Access β‐Stereogenic γ‐Lactams
Authors: Ding Yi , Han Ye‐Qiang , Wu Le‐Song , Zhou Tao , Yao Qi‐Jun , Feng Ya‐Lan , Li Ya , Kong Ke‐Xin , Shi Bing‐Feng 
Published: May 2020

AbstractHerein, we describe an unprecedented cascade reaction to β‐stereogenic γ‐lactams involving Pd(II)‐catalyzed enantioselective aliphatic methylene C(sp3)−H alkenylation–aza‐Wacker cyclization through syn‐aminopalladation. Readily available 3,3′‐substituted BINOLs are used as chiral ligands, providing the corresponding γ‐lactams with broad scope and high enantioselectivities (up to 98 % ee).
Modular and Selective Arylation of Aryl Germanes (C−GeEt3) over C−Bpin, C−SiR3 and Halogens Enabled by Light‐Activated Gold Catalysis
Authors: Sherborne Grant J. , Gevondian Avetik G. , Funes‐Ardoiz Ignacio , Dahiya Amit , Fricke Christoph , Schoenebeck Franziska 
Published: May 2020

AbstractSelective C
–C
couplings are powerful strategies for the rapid and programmable construction of bi‐ or multiaryls. To this end, the next frontier of synthetic modularity will likely arise from harnessing the coupling space that is orthogonal to the powerful Pd‐catalyzed coupling regime. This report details the realization of this concept and presents the fully selective arylation of aryl germanes (which are inert under Pd0/PdII catalysis) in the presence of the valuable functionalities C−BPin, C−SiMe3, C−I, C−Br, C−Cl, which in turn offer versatile opportunities for diversification. The protocol makes use of visible light activation combined with gold catalysis, which facilitates the selective coupling of C−Ge with aryl diazonium salts. Contrary to previous light‐/gold‐catalyzed couplings of Ar–N2+, which were specialized in Ar–N2+ scope, we present conditions to efficiently couple electron‐rich, electron‐poor, heterocyclic and sterically hindered aryl diazonium salts. Our computational data suggest that while electron‐poor Ar–N2+ salts are readily activated by gold under blue‐light irradiation, there is a competing dissociative deactivation pathway for excited electron‐rich Ar–N2+, which requires an alternative photo‐redox approach to enable productive couplings.
Asymmetric Dearomative Fluorination of 2‐Naphthols with a Dicarboxylate Phase‐Transfer Catalyst
Authors: Egami Hiromichi , Rouno Taiki , Niwa Tomoki , Masuda Kousuke , Yamashita Kenji , Hamashima Yoshitaka 
Published: May 2020

AbstractA linked dicarboxylate phase‐transfer catalyst enables smooth asymmetric dearomative fluorination of 2‐naphthols with Selectfluor under mild conditions to give the corresponding 1‐fluoronaphthalenone derivatives in a highly enantioselective manner. This reaction, which is compatible with a range of functional groups, is the first example of catalytic asymmetric fluorination of 2‐naphthols, and is expected to be useful in the synthesis of bioactive molecules.
Strategies for the Syntheses of Pactamycin and Jogyamycin
Authors: Gerstner Nels C. , Nicastri Kate A. , Schomaker Jennifer M. 
Published: May 2020

AbstractPactamycin and jogyamycin are aminocyclopentitol natural products, where each core carbon bears a stereodefined alcohol or amine moiety. Their structural complexity, coupled with the diversity of functional groups coexisting in a condensed space, make them fascinating synthetic targets in their own right. Pactamycin and its derivatives bind to the 30S ribosomal subunit and display activity against parasites responsible for drug‐resistant malaria and African sleeping sickness; however, efforts to develop their therapeutic potential have been hampered by their cellular toxicity. Interestingly, bioengineered analogues display differences in selectivity and toxicity towards mammalian cells, spurring efforts to develop flexible strategies to thoroughly probe structure–activity relationships (SAR), particularly in analogues lacking the C7 hydroxyl group of pactamycin. This review compares and contrasts approaches towards pactamycin and jogyamycin, including two successful total syntheses of the former. The implications of each route for preparing analogues to inform SAR and lead to compounds with increased selectivity for binding malarial over human ribosomes are briefly discussed.
Harnessing Effective Molarity to Design an Electrochemical DNA‐based Platform for Clinically Relevant Antibody Detection
Authors: Rossetti Marianna , Brannetti Simone , Mocenigo Marco , Marini Bruna , Ippodrino Rudy , Porchetta Alessandro 
Published: May 2020

AbstractEasy‐to‐use platforms for rapid antibody detection are likely to improve molecular diagnostics and immunotherapy monitoring. However, current technologies require multi‐step, time‐consuming procedures that limit their applicability in these fields. Herein, we demonstrate effective molarity‐driven electrochemical DNA‐based detection of target antibodies. We show a highly selective, signal‐on DNA‐based sensor that takes advantage of antibody‐binding‐induced increase of local concentration to detect clinically relevant antibodies in blood serum. The sensing platform is modular, rapid, and versatile and allows the detection of both IgG and IgE antibodies. We also demonstrate the possible use of this strategy for the monitoring of therapeutic monoclonal antibodies in body fluids. Our approach highlights the potential of harnessing effective molarity for the design of electrochemical sensing strategies.