bluuebunny/crossref_metadata_2025_split huggingface dataset:
Engineering Solid Electrolyte Interface at Nano‐Scale for High‐Performance Hard Carbon in Sodium‐Ion Batteries
Authors: Ma Mengying , Cai Haoran , Xu Chenlu , Huang Renzhi , Wang Shurong , Pan Huilin , Hu Yong‐Sheng 
Published: April 2021

AbstractEngineering the structure and chemistry of solid electrolyte interface (SEI) on electrode materials is crucial for rechargeable batteries. Using hard carbon (HC) as a platform material, a correlation between Na+ storage performance, and the properties of SEI is comprehensively explored. It is found that a “good” SEI layer on HC may not be directly associated with certain kinds of SEI components, such as NaF and Na2O. Whereas, arranging nano SEI components with refined structures constructs the foundation of “good” SEI that enables fast Na+ storage and interface stability of HC in Na‐ion batteries. A layer‐by‐layer SEI on HC with inorganic‐rich inner layer and tolerant organic‐rich outer flexible layer can facilitate excellent rate and cycling life. Besides, SEI layer as the gate for Na+ from electrolyte to HC electrode can modulate interfacial crystallographic structures of HC with pillar‐solvent that function as “pseudo‐SEI” for fast and stable Na+ storage in optimal 1 m NaPF6‐TEGDME electrolytes. Such a layer‐by‐layer SEI combined with a “pseudo‐SEI” layer for HC enables an outstanding rate of 192 mAh g−1 at 2 C and stable cycling over 1100 cycles at 0.5 C. This study provides valuable guidance to improve the electrochemical performance of electrode materials through regulation of SEI in optimal electrolytes.
Biocompatibility Evolves: Phenomenology to Toxicology to Regeneration
Authors: Crawford Lars , Wyatt Meghan , Bryers James , Ratner Buddy 
Published: April 2021

AbstractThe word “biocompatibility,” is inconsistent with the observations of healing for so‐called biocompatible biomaterials. The vast majority of the millions of medical implants in humans today, presumably “biocompatible,” are walled off by a dense, avascular, crosslinked collagen capsule, hardly suggestive of life or compatibility. In contrast, one is now seeing examples of implant biomaterials that lead to a vascularized reconstruction of localized tissue, a biological reaction different from traditional biocompatible materials that generate a foreign body capsule. Both the encapsulated biomaterials and the reconstructive biomaterials qualify as “biocompatible” by present day measurements of biocompatibility. Yet, this new generation of materials would seem to heal “compatibly” with the living organism, where older biomaterials are isolated from the living organism by the dense capsule. This review/perspective article will explore this biocompatibility etymological conundrum by reviewing the history of the concepts around biocompatibility, today's standard methods for assessing biocompatibility, a contemporary view of the foreign body reaction and finally, a compendium of new biomaterials that heal without the foreign body capsule. A new definition of biocompatibility is offered here to address advances in biomaterials design leading to biomaterials that heal into the body in a facile manner.
An Adhesive‐Integrated Stretchable Silver‐Silver Chloride Electrode Array for Unobtrusive Monitoring of Gastric Neuromuscular Activity
Authors: Kurniawan Jonas F. , Tjhia Boris , Wu Vincent M. , Shin Andrew , Sit Nathan L. J. , Pham Timothy , Nguyen Andrew , Li Carleen , Kumar Rajan , Aguilar‐Rivera Marcelo , Lerman Imanuel , Kunkel David C. , Coleman Todd P. 
Published: April 2021

AbstractHere, an unobtrusive, adhesive‐integrated electrode array for continuous monitoring of stomach electric activity is introduced. This patient‐friendly, disposable peel‐and‐stick adhesive device represents an important advancement over existing arrays that require placement of each electrode individually and are thus also labor intensive and are in general more rigid and cumbersome. In comparison to other silver–silver chloride electrodes, this skin conformal array does not require gel and thus can withstand low impedance over the duration of long recordings. Interfacing these electrodes with miniaturized electronic recording and wireless telemetry systems has the potential to enable scalable population health opportunities to perform objective gastrointestinal assessment and optimization of treatment regimens.
Highly Sensitive and Selective Gas Sensor Using Heteroatom Doping Graphdiyne: A DFT Study
Authors: Wu Yang , Chen Xingzhu , Weng Kaiyi , Arramel  , Jiang Jizhou , Ong Wee‐Jun , Zhang Peng , Zhao Xiujian , Li Neng 
Published: April 2021

AbstractThe emergence of a two‐dimensional (2D) functionalized‐graphene structure, graphdiyne (GDY), promoting non‐metallic single atoms level to tailor its gas sensing performance. Herein, pristine, non‐metallic atom (N, B) doped 2D GDY is investigated for toxic and greenhouse gases sensing (CO, CO2, CH4, HCHO, H2S, SO2, SO3, NO2, NO, and NH3). The B‐doped GDY (B‐GDY) compared with pure or N doped GDY displays gas sensitivity, especially excellent sensitivity and selectivity toward NO, NO2, and NH3. Additionally, a humid environment has demonstrated no effect on the weakening selectivity of B‐GDY for the studied gases. Meanwhile, the effect of external electric field (E‐field) on sensing was calculated, indicating that the bandgap of NO‐adsorbed system reached the lowest 0.188 eV at −0.5 V Å−1 and the highest 0.363 eV at −0.1 V Å−1. This work paves the way on designing efficient and effective gas sensor toward toxic nitrogen‐based gases on GDY.
Spinterfaces Manipulate Large Magnetic Field Effects in 3D and Quasi‐2D Organic–Inorganic Hybrid Perovskites
Authors: Pan Ruiheng , Wang Kai , Li Yang , Yu Haomiao , Li Jinpeng , Xu Ling 
Published: April 2021

AbstractSpinterfaces are due to the orbital hybridization at an interface of a ferromagnet and a nonmagnetic semiconductor. Interfacial densities of states (i‐DOS) are spin‐dependent, which may offer the spin‐filter effect for enhancing spin‐polarized charge injection efficiency and magnetic field effects (MFEs). In the work, a prototypical perovskite spin valve (PeSV) comprising Ni/MAPbI3−xClx/Ni (MA = CH3NH3) is fabricated, showing a clear magnetic switching behavior in the ambient condition. It is further explored by studying the magnetophotocurrent (MPC) at the short‐circuit current density condition (magneto‐Jsc). Anomalously large magneto‐Jsc can be detected by comparing to devices with nonmagnetic Au electrodes. The effect can be more pronounced for the quasi‐2D perovskite such as (PEA)2(MA)3Pb4I13 (PEA = C6H5(CH2)2NH3). At low fields, the hyperfine field induced spin‐mixing shows remarkable magneto‐Jsc signals for it. In addition, the circularly and linearly polarized laser beam can effectively manipulate the magnitude of magneto‐Jsc for both MAPbI3−xClx and (PEA)2(MA)3Pb4I13. It is postulated that the formation of the spinterfaces may play a dominant role for the large and tunable magneto‐Jsc effect. These studies may pave the way for future experimental and theoretical studies in the field.
Guiding the Design of Heterogeneous Electrode Microstructures for Li‐Ion Batteries: Microscopic Imaging, Predictive Modeling, and Machine Learning
Authors: Xu Hongyi , Zhu Juner , Finegan Donal P. , Zhao Hongbo , Lu Xuekun , Li Wei , Hoffman Nathaniel , Bertei Antonio , Shearing Paul , Bazant Martin Z. 
Published: April 2021

AbstractElectrochemical and mechanical properties of lithium‐ion battery materials are heavily dependent on their 3D microstructure characteristics. A quantitative understanding of the role played by stochastic microstructures is critical for the prediction of material properties and for guiding synthesis processes. Furthermore, tailoring microstructure morphology is also a viable way of achieving optimal electrochemical and mechanical performances of lithium‐ion cells. To facilitate the establishment of microstructure‐resolved modeling and design methods, a review covering spatially and temporally resolved imaging of microstructure and electrochemical phenomena, microstructure statistical characterization and stochastic reconstruction, microstructure‐resolved modeling for property prediction, and machine learning for microstructure design is presented here. The perspectives on the unresolved challenges and opportunities in applying experimental data, modeling, and machine learning to improve the understanding of materials and identify paths toward enhanced performance of lithium‐ion cells are presented.
How ancestral subsistence strategies solve salmon starvation and the “protein problem” of Pacific Rim resources
Authors: Tushingham Shannon , Barton Loukas , Bettinger Robert L. 
Published: April 2021

AbstractThis article provides a theoretical treatment of hunter–gatherer diet and physiology. Through a synthesis of nutritional studies, informed by ethno‐archaeological data, we examine the risk of protein‐rich diets for human survival, and how societies circumvent "salmon starvation" in the northeastern Pacific Rim. Fundamental nutritional constraints associated with salmon storage and consumption counter long‐standing assumptions about the engine of cultural evolution in the region. Excess consumption of lean meat can lead to protein poisoning, termed by early explorers “rabbit starvation.” While consumption of fats and carbohydrates is widely portrayed as a pathway to “offsetting” protein thresholds, there are true limits to the amount of protein individuals can consume, and constraints are most extreme for smaller individuals, children, and pregnant/nursing mothers. While this problem is not usually perceived as associated with fish, the risk of protein poisoning limits the amount of low‐fat fish that people can eat safely. Compared with smaller, mass‐harvested species (e.g., eulachon), dried salmon are exceedingly lean. Under certain circumstances fattier foods (small forage fish, marine mammals, whales, and even bears) or carbohydrate‐rich plants may have been preferred not just for taste but to circumvent this “dietary protein ceiling.” Simply put, “salmon specialization” cannot evolve without access to complimentary caloric energy through fat‐rich or carbohydrate‐rich resources. By extension, the evolution of storage‐based societies requires this problem be solved prior to or in tandem with‐salmon intensification. Without such solutions, increased mortality and reproductive rates would have made salmon reliance unsustainable. This insight is in line with genomic research suggesting protein toxicity avoidance was a powerful evolutionary force, possibly linked to genetic adaptations among First Americans. It is also relevant to evaluating the plausibility of other purportedly “focal” economies and informs understanding of the many solutions varied global societies have engineered to overcome physiological protein limits.
Evidence of Mars‐Van‐Krevelen Mechanism in the Electrochemical Oxygen Evolution on Ni‐Based Catalysts
Authors: Ferreira de Araújo Jorge , Dionigi Fabio , Merzdorf Thomas , Oh Hyung‐Suk , Strasser Peter 
Published: April 2021

AbstractWater oxidation is a crucial reaction for renewable energy conversion and storage. Among the alkaline oxygen evolution reaction (OER) catalysts, NiFe based oxyhydroxides show the highest catalytic activity. However, the details of their OER mechanism are still unclear, due to the elusive nature of the OER intermediates. Here, using a novel differential electrochemical mass spectrometry (DEMS) cell interface, we performed isotope‐labelling experiments in 18O‐labelled aqueous alkaline electrolyte on Ni(OH)2 and NiFe layered double hydroxide nanocatalysts. Our experiments confirm the occurrence of Mars‐van‐Krevelen lattice oxygen evolution reaction mechanism in both catalysts to various degrees, which involves the coupling of oxygen atoms from the catalyst and the electrolyte. The quantitative charge analysis suggests that the participating lattice oxygen atoms belong exclusively to the catalyst surface, confirming DFT computational hypotheses. Also, DEMS data suggest a fundamental correlation between the magnitude of the lattice oxygen mechanism and the faradaic efficiency of oxygen controlled by pseudocapacitive oxidative metal redox charges.
Rational Design of Multicolor‐Emitting Chiral Carbonized Polymer Dots for Full‐Color and White Circularly Polarized Luminescence
Authors: Ru Yi , Sui Laizhi , Song Haoqiang , Liu Xingjiang , Tang Zhiyong , Zang Shuang‐Quan , Yang Bai , Lu Siyu 
Published: April 2021

AbstractLight‐emitting chiral carbonized polymer dots (Ch‐CPDs) are attracting great interest because of their extraordinary photonic properties, but modulating their band‐gap emission, especially at long wavelength, and maintaining their chiral structure to achieve multicolor, high‐emission Ch‐CPDs remains challenging. Reported here for the first time is the synthesis of red‐ and multicolor‐emitting Ch‐CPDs using the common precursorsL‐/D‐tryptophan ando‐phenylenediamine, and a solvothermal approach at one temperature. The quantum yield of the Ch‐CPDs was between 31 % and 54 %. Supramolecular self‐assembly provided multicolor‐emitting Ch‐CPDs showing novel circularly polarized luminescence, with the highest dissymmetric factor (glum) of 1×10−2. Importantly, circularly polarized white‐emitting CPDs were fabricated for the first time by tuning the mixing ratio of the three colored Ch‐CPDs in a gel. This strategy affords exciting opportunities for designing functional chiroptical materials.
Exciton‐Mediated Energy Transfer in Heterojunction Enables Infrared Light Photocatalysis
Authors: Li Yuanjin , Wang Hui , Zhang Xiaodong , Wang Shuhui , Jin Sen , Xu Xiaoliang , Liu Wenxiu , Zhao Zhi , Xie Yi 
Published: April 2021

AbstractAlthough a few semiconductors can directly absorb infrared light, their intrinsic properties like improper band‐edge position and strong electron–hole interaction restrict further photocatalytic applications. Herein, we propose an exciton‐mediated energy transfer strategy for realizing efficient infrared light response in heterostructures. Using black phosphorous/polymeric carbon nitride (BP/CN) heterojunction, CN could be indirectly excited by infrared light with the aid of nonradiatively exciton‐based energy transfer from BP. At the same time, excitons are dissociated into free charge carriers at the interface of BP/CN heterojunction, followed by hole injection to BP and electron retainment in CN. As a result of these unique photoexcitation processes, BP/CN heterojunction exhibits promoted conversion rate and selectivity in amine–amine oxidative coupling reaction even under infrared light irradiation. This study opens a new way for the design of efficient infrared light activating photocatalysts.
Merging Pincer Motifs and Potential Metal–Metal Cooperativity in Cobalt Dinitrogen Chemistry: Efficient Catalytic Silylation of N2 to N(SiMe3)3
Authors: Li Ming , Gupta Sandeep K. , Dechert Sebastian , Demeshko Serhiy , Meyer Franc 
Published: April 2021

AbstractUsing a pyrazolate‐bridged dinucleating ligand that provides two proximate pincer‐type PNN binding sites (“two‐in‐one pincer”), different synthetic routes have been developed towards its dicobalt(I) complex 2 that features a twice deprotonated ligand backbone and two weakly activated terminal N2 substrate ligands directed into the bimetallic pocket. Protonation of 2 is shown to occur at the ligand scaffold and to trigger conversion to a tetracobalt(I) complex 4 with two end‐on μ1,2‐bridging N2; in THF 4 is labile and undergoes temperature‐dependent N2/triflate ligand exchange. These pyrazolate‐based systems combine the potential of exhibiting both metal–metal and metal–ligand cooperativity, viz. two concepts that have emerged as promising design motifs for molecular N2 fixation catalysts. Complex 2 serves as an efficient (pre)catalyst for the reductive silylation of N2 into N(SiMe3)3 (using KC8 and Me3SiCl), yielding up to 240 equiv N(SiMe3)3 per catalyst.
Triarylmethanes and their Medium‐Ring Analogues by Unactivated Truce–Smiles Rearrangement of Benzanilides
Authors: Abrams Roman , Jesani Mehul H. , Browning Alex , Clayden Jonathan 
Published: April 2021

AbstractIntramolecular nucleophilic aromatic substitution (Truce–Smiles rearrangement) of the anions of 2‐benzyl benzanilides leads to triarylmethanes in an operationally simple manner. The reaction succeeds even without electronic activation of the ring that plays the role of electrophile in the SNAr reaction, being accelerated instead by the preferred conformation imposed by the tertiary amide tether. The amide substituent of the product may be removed or transformed into alternative functional groups. A ring‐expanding variant (n to n+4) of the reaction provided a route to doubly benzo‐fused medium ring lactams of 10 or 11 members. Hammett analysis returned a ρ value consistent with the operation of a partially concerted reaction mechanism.
A Double Deprotonation Strategy for Cascade Annulations of Palladium–Trimethylenemethanes and Morita–Baylis–Hillman Carbonates to Construct Bicyclo[3.1.0]hexane Frameworks
Authors: Yang Zhen‐Hong , Chen Peng , Chen Zhi‐Chao , Chen Zhi , Du Wei , Chen Ying‐Chun 
Published: April 2021

AbstractHere we report that the chemoselective activation of Tsuji's 2‐(cyanomethyl)allyl carbonates to generate the palladium–trimethylenemethane 1,3‐dipoles via a deprotonation strategy can be realized in the presence of Morita–Baylis–Hillman carbonates from substantial activated ketones. The following SN2′‐addition enables the formation of new 1,3‐dipole species having an activated alkene moiety through a second deprotonation process, which then undergo cascade [1+2]/[3+2] annulations to furnish complex bicyclic [3.1.0]hexane frameworks having three contiguous quaternary stereogenic centers with good to excellent enantioselectivity. Moreover, by using benzoyl aldehyde‐derived substrates, a [1+4]/[3+2] annulation sequence is similarly developed to produce fused cyclopenta[b]furan architectures.
Catalytic Asymmetric Synthesis of Silicon‐Stereogenic Dihydrodibenzosilines: Silicon Central‐to‐Axial Chirality Relay
Authors: Guo Yonghong , Liu Meng‐Meng , Zhu Xujiang , Zhu Liru , He Chuan 
Published: April 2021

AbstractA Rh‐catalyzed asymmetric synthesis of silicon‐stereogenic dihydrodibenzosilines featuring axially chiral 6‐membered bridged biaryls is demonstrated. In the presence of a RhI catalyst with a chiral diphosphine ligand, a wide range of dihydrodibenzosilines containing both silicon‐central and axial chiralities are conveniently constructed in excellent enantioselectivities via dehydrogenative C(sp3)−H silylation. Absolute configuration analysis by single‐crystal X‐ray structures revealed a novel silicon central‐to‐axial chirality relay phenomenon, which we believe will inspire further research in the field of asymmetric catalysis and chiroptical materials.
Research on rotary nozzle structure and flow field of the spinneret for centrifugal spinning
Authors: Lai Zilong , Wang Jiawei , Liu Kang , Li Wenhui , Zhang Zhiming , Chen Boya 
Published: April 2021

AbstractHigh‐speed centrifugal spinning is a novel method of fabricating nanofibers by use of centrifugal force field. The neoteric designs and proper structural parameters of spinning nozzle will change the outlet velocity and velocity distribution uniformity of spinning solution, which could affect the quality of nanofibers. Four different spinning nozzles that can be used for high‐speed centrifugal spinning are proposed. The flow of spinning solution in the different rotary nozzles is simulated based on the theoretical analysis. It can be found that the curved‐tube nozzle is better for high‐speed centrifugal spinning comparing with the velocity distribution of spinning solution in the four different spinning nozzles. The influence degree of the structure parameters of the curved‐tube nozzle on the solution outlet‐velocity is explored by orthogonal test method. The result shows that the curved‐tube nozzle with an inlet diameter of 10 mm, conical transition pipe length of 3 mm, nozzle outlet diameter of 0.8 mm, curvature radius of 4 mm, and central angle of curved tube of 30°, can effectively enhance the outlet velocity of spinning solution. Finally, it is proved by centrifugal spinning experiment that the curved‐tube nozzle after optimization can improve the morphology and quality of nanofibers.
Anatomical and developmental aspects of iatrogenic injury to the right recurrent laryngeal nerve in surgical resections of substernal goiter
Authors: Fiorelli Rossano Kepler Alvim , Duarte Alfredo Jorge Vasconcelos , de Quadros Teixeira Aline , Montenegro Thiago Scharth , Portari Filho Pedro Eder , Morard Maria Ribeiro Santos , da Silva Ascenção Agostinho Manuel , Oliveira Carlos Alberto Basílio , Novellino Pietro 
Published: April 2021

AbstractThyroid surgery is the primary treatment for substernal goiters, and iatrogenic injury to the recurrent laryngeal nerve (RNL) is always a risk. The literature suggests that iatrogenic lesions of the RNL post resection of substernal goiter are not equally distributed, being more frequent on the right recurrent laryngeal nerve (R‐RLN) in comparison to the left recurrent laryngeal nerve (L‐RLN). The relative paucity of basic anatomical and clinical reportages on R‐RLN iatrogenic injuries and on the developmental factors that may help explain its higher incidence justifies this study's undertaking. Here we compare incidence of right versus left iatrogenic injuries to the RLN in surgical resections of substernal goiters and discuss the anatomical and embryological factors involved. This report is part of a larger retrospective observational cohort study of 239 patients surgically treated for substernal goiter in the Gaffrée and Guinle University Hospital, Rio de Janeiro, from 2006 to 2018. From 239 patients, 13 presented with iatrogenic RLN injury, one patient presented bilateral lesion, totalling 15 iatrogenic lesions. Our analysis showed that the R‐RLN seems to be anatomically more vulnerable to injury due to the embryological underpinnings addressed in this review, R‐RLN = 64.29% (n = 9) and L‐RLN = 35.71% (n = 5). Pathological factors like malignancy and size of the mass are relevant issues to be considered. The knowledge of anatomical landmarks and embryological development of the thyroid and associated structures can improve our understanding and teaching of surgical anatomy, thus helping prevent and reduce the number of iatrogenic injuries on right RLNs.
Pyrimidinetrione‐imidazoles as a Unique Structural Type of Potential Agents towards Candida Albicans: Design, Synthesis and Biological Evaluation
Authors: Sui Yan‐Fei , Ansari Mohammad Fawad , Zhou Cheng‐He 
Published: April 2021

AbstractSubstantial morbidity and mortality of fungal infections have aroused concerns all over the world, and common Candida spp. currently bring about severe systemic infections. A series of pyrimidinetrione‐imidazole conjugates as potentially antifungal agents were developed. Bioassays manifested that 4‐fluobenzyl pyrimidinetrione imidazole 5 f exerted favorable inhibition towards C. albicans (MIC=0.002 mM), being 6.5 folds more active than clinical antifungal drug fluconazole (MIC=0.013 mM). Preliminary mechanism research indicated that compound 5 f could not only depolarize membrane potential but also permeabilize the membrane of C. albicans. Molecular docking was operated to simulate the interaction mode between molecule 5 f and CYP51. In addition, hybrid 5 f might form 5 f‐DNA supramolecular complex via intercalating into DNA. The interference of membrane and DNA might contribute to its fungicidal capacity with no obvious tendency to induce the resistance against C. albicans. Conjugate 5 f endowed good blood compatibility as well as low cytotoxicity towards HeLa and HEK‐293T cells.