bluuebunny/crossref_metadata_2025_split huggingface dataset:
A Crystalline Carbon Nitride Based Near‐Infrared Active Photocatalyst
Authors: Zhai Boyin , Li Hongguan , Gao Guangying , Wang Ying , Niu Ping , Wang Shulan , Li Li 
Published: September 2022

AbstractEfficient utilization of near‐infrared (NIR) light that takes a primary percentage of the solar spectrum is of great significance for practical applications of photocatalysis. However, development of singular NIR‐based photocatalysts still remains a grand challenge. Herein, a NIR‐based crystalline carbon nitride photocatalyst is proposed by using a molten‐salt assisted protocol with carbohydrazide as the oxygen‐containing precursor. Different from the doping strategy that always leads to structural damage and crystallinity decrease, structural oxygen arising from the special precursor itself is introduced into the framework of C3N4 with highly crystalline structure formed. The n→π* excitation is therefore activated with the absorption edge extended remarkably to 1400 nm. Theoretical calculations also reveal that the local internal electric field is simultaneously generated for promoting the charge separation/migration kinetics. Benefiting from structural oxygen incorporation and crystalline structure formation, the synthesized material shows a significantly enhanced visible‐light (λ > 420 nm) hydrogen production reactivity compared with the benchmark carbon nitride, and more importantly an active NIR hydrogen generation (λ > 700 nm) and long‐wavelength overall water splitting (λ = 600 nm) capability that is rarely reported for singular photocatalysts. This study showcases an illustration of promising singular NIR photocatalysts for efficient solar fuel production.
High‐Performance Perovskite Photovoltaics by Heterovalent Substituted Mixed Perovskites
Authors: Shen Lening , Chen Rui , Zhang Dong , Yilmazoglu Unal Cagatay , Gu Kai , Sarmiento Julio S. , Zhu Tao , Zheng Luyao , Zheng Jie , Wang He , Liu Chunming , Gong Xiong 
Published: September 2022

Abstract2D perovskites are relatively stable but possess poor charge transport compared to 3D perovskites. To boost charge transport, novel 2D perovskites mixed with 3D perovskites are developed, where Pb2+ are partially substituted by the heterovalent neodymium cations (Nd3+) within both 2D and 3D perovskites (termed Nd3+‐substituted 2D:3D mixed perovskites. Systematical studies reveal that the Nd3+‐substituted 2D:3D mixed perovskites possess larger crystals, superior crystallinity, suppressed non‐radiative charge recombination, and enhanced and balanced charge transport compared to the 2D:3D mixed perovskites. As a result, perovskite photovoltaics based on the Nd3+‐substituted 2D:3D mixed perovskites exhibit a power conversion efficiency of 22.11%, a photoresponsibility of over 700 mA W−1, a photodetectivity of 4.29 × 1014 cm Hz1/2 W−1, a linear dynamic range of 165 dB at room temperature, and dramatically boosted stability. These results demonstrate that, a facile way is developed to realize high‐performance perovskite photovoltaics through partially heterovalent substituted Pb2+ by Nd3+ within 2D:3D mixed perovskites.
Crystal Reconstruction of Mo:BiVO4: Improved Charge Transport for Efficient Solar Water Splitting
Authors: Jeong Yoo Jae , Seo Dong Hyun , Baek Ji hyun , Kang Min Je , Kim Bit Na , Kim Sung kyu , Zheng Xiaolin , Cho In Sun 
Published: September 2022

AbstractA multifaceted Mo:BiVO4 (mf‐BVO) photoanode is grown on F‐doped‐SnO2 substrates via achemical bath deposition, and the crystal reconstruction process of mf‐BVO is found to boost the charge transport efficiency significantly for photoelectrochemical (PEC) water splitting. The mf‐BVO exhibits columnar grains with an uncommon (121) texture with high‐index facets such as (112), (020), (132), and (204). The texture and high‐index facets facilitate rapid surface melting and grain fusion during thermal annealing, thus leading to crystal reconstructed micron‐sized BVO grains (cr‐BVO). The cr‐BVO has a photocurrent density ≈50 times larger than that of mf‐BVO. The reason is identified as the significantly improved charge transport efficiency resulting from the dopant activation (increased carrier concentration) and bulky grains (fewer defects). Additionally, the cr‐BVO exhibits improved photocorrosion resistance compared to the nanoparticle‐based BVO. After coating the oxygen evolution catalyst, the photocurrent density of cr‐BVO is further increased to 4.4 mA cm−2 for water oxidation reaction at 1.23 V versus the reversible hydrogen electrode, maintaining a high and stable faradaic efficiency of over 88% for 24 h. These results demonstrate that crystal reconstruction is a facile and effective pathway to improve the charge transport efficiency, opening a new avenue for developing efficient photoelectrodes for PEC water splitting.
Self‐Healing of Prussian Blue Analogues with Electrochemically Driven Morphological Rejuvenation
Authors: Xie Junpeng , Ma Liang , Li Jinliang , Yin Xunqing , Wen Zhaorui , Zhong Yunlei , Li Chaowei , Liu Yu , Shen Zhaoxi , Mai Wenjie , Hong Guo , Zhang Wenjun 
Published: September 2022

AbstractMaintaining the morphology of electrode materials with high invertibility contributes to the prolonged cyclic stability of battery systems. However, the majority of electrode materials tend to degrade during the charge–discharge process owing to the inevitable increase in entropy. Herein, a self‐healing strategy is designed to promote morphology rejuvenation in Prussian blue analogue (PBA) cathodes by cobalt doping. Experimental characterization and theoretical calculations demonstrate that a trace amount of cobalt can decelerate the crystallization process and restore the cracked areas to ensure perfect cubic structures of PBA cathodes. The electric field controls the kinetic dynamics, rather than the conventional thermodynamics, to realize the “electrochemically driven dissolution–recrystallization process” for the periodic self‐healing phenomenon. The properties of electron transportation and ion diffusion in bulk PBA are also improved by the doping strategy, thus boosting the cyclability with 4000 cycles in a diluent electrolyte. This discovery provides a new paradigm for the construction of self‐healing electrodes for cathodes.
Magnetic Ordering in a High‐Spin Donor–Acceptor Conjugated Polymer
Authors: Steelman Michael E. , Adams Daniel J. , Mayer Kevin S. , Mahalingavelar Paramasivam , Liu Chih‐Ting , Eedugurala Naresh , Lockart Molly , Wang Yunfei , Gu Xiaodan , Bowman Michael K. , Azoulay Jason D. 
Published: September 2022

AbstractThe development of open‐shell organic molecules that magnetically order at room temperature,which can be practically applied, remains a grand challenge in chemistry, physics, and materials science. Despite the exploration of vast chemical space, design paradigms for organic paramagnetic centers generally result in unpaired electron spins that are unstable or isotropic. Here, a high‐spin conjugated polymer is demonstrated, which is composed of alternating cyclopentadithiophene and benzo[1,2‐c;4,5‐c′]bis[1,2,5]thiadiazole heterocycles, in which macromolecular structure and topology coalesce to promote the spin center generation and intermolecular exchange coupling. Electron paramagnetic resonance (EPR) spectroscopy is consistent with spatially localized spins, while magnetic susceptibility measurements show clear anisotropic spin ordering and exchange interactions that persist at room temperature. The application of long‐range π‐correlations for spin center generation promotes remarkable stability. This work offers a fundamentally new approach to the implementation of this long‐sought‐after physical phenomenon within organic materials and the integration of manifold properties within emerging technologies.
Synthetic Nanoarchitectonics of Functional Organic–Inorganic 2D Germanane Heterostructures via Click Chemistry
Authors: Muñoz Jose , Palacios‐Corella Mario , Gómez I. Jénnifer , Zajíčková Lenka , Pumera Martin 
Published: September 2022

AbstractSucceeding graphene, 2D inorganic materials made of reactive van der Waals layers, like 2D germanane (2D‐Ge) derivatives, have attracted great attention because their physicochemical characteristics can be entirely tuned by modulating the nature of the surface substituent. Although very interesting from a scientific point of view, almost all the reported works involving 2D‐Ge derivatives are focused on computational studies. Herein, a first prototype of organic–inorganic 2D‐Ge heterostructure has been synthesized by covalently anchoring thiol‐rich carbon dots (CD–SH) onto 2D allyl germanane (2D‐aGe) via a simple and green “one‐pot” click chemistry approach. Remarkably, the implanted characteristics of the carbon nanomaterial provide new physicochemical features to the resulting 0D/2D heterostructure, making possible its implementation in yet unexplored optoelectronic tasks—e.g., as a fluorescence resonance energy transfer (FRET) sensing system triggered by supramolecular π–π interactions—that are inaccessible for the pristine 2D‐aGe counterpart. Consequently, this work builds a foundation toward the robust achievement of functional organic–inorganic 2D‐Ge nanoarchitectonics through covalently assembling thiol‐rich carbon nanoallotropes on commercially available 2D‐aGe.
A Time‐Division Position‐Sensitive Detector Image System for High‐Speed Multitarget Trajectory Tracking
Authors: Liu Kaiyang , Wan Dongyang , Wang Wenhui , Fei Cheng , Zhou Tao , Guo Dingli , Bai Lin , Li Yongfu , Ni Zhenhua , Lu Junpeng 
Published: September 2022

AbstractHigh‐speed trajectory tracking with real‐time processing capability is particularly important in the fields of pilotless automobiles, guidance systems, robotics, and filmmaking. The conventional optical approach to high‐speed trajectory tracking involves charge coupled device (CCD) or complementary metal–oxide–semiconductor (CMOS) image sensors, which suffer from trade‐offs between resolution and framerates, complexity of the system, and enormous data‐analysis processes. Here, a high‐speed trajectory tracking system is designed by using a time‐division position‐sensitive detector (TD‐PSD) based on a graphene–silicon Schottky heterojunction. Benefiting from the high‐speed optoelectronic response and sub‐micrometer positional accuracy of the TD‐PSD, multitarget real‐time trajectory tracking is realized, with a maximum image output framerate of up to 62 000 frames per second. Moreover, multichannel trajectory tracking and image‐distortion correction functionalities are realized by TD‐PSD systems through frequency‐related image preprocessing, which significantly improves the capacity of real‐time information processing and image quality in complicated light environments.
Multifunctional Ti3C2Tx MXene/Poly(Styrene‐Methacrylic Acid)@Polypyrrole Nanospheres/Thermoplastic Polyurethane Electrospinning Membrane for High Sensitivity Pressure Sensing and Pressure‐Electrothermal
Authors: Cheng Haonan , Tan Yongsong , Zhang Ningyi , Yin Yunjie , Wang Chaoxia 
Published: September 2022

AbstractThe introduction of superior conductive materials on flexible substrates with surface‐built microstructures has proven to be an effective solution for enhancing the sensitivity of pressure sensor. Thermoplastic polyurethane electrospun membrane (TPUEM) with multi‐void structure is used as substrate, and poly(styrene‐methacrylic acid)@polypyrrole nanospheres (PPNs) are pumped into the TPUEM by vacuum filtration to form a microstructure on the surface of thermoplastic polyurethane (TPU) electrospun fibers. The MXene dispersion is sprayed on the surface of PPNs/TPUEM. As it is gradually infiltrated into the material, a conductive network is formed. When the MXene/PPNs/TPUEM is subjected to pressure, its resistance decreases significantly due to the close contact between MXene and PPNs. The assembled pressure sensor shows superior sensitivity (16.72 kPa−1), broad sensing range (0–32.1 kPa), and rapid response (145 ms). The pressure sensor demonstrates the ability to detect human health signals and activities, including human pulse, breathing, and joint movements, etc. Benefiting from its excellent negative piezoresistive effect, the pressure sensor shows a significant pressure‐electrothermal function at 2.0 V and the local temperature is 48.08 °C. The MXene/PPNs/TPUEM has potential applications in human physiological signal monitoring, motion monitoring, and energy saving electric heating mats.
Tuning the Release Force of Microfibrillar Adhesives by Geometric Design
Authors: Barnefske Lena , Rundel Fabian , Moh Karsten , Hensel René , Zhang Xuan , Arzt Eduard 
Published: September 2022

AbstractSwitchable micropatterned adhesives exhibit high potential as novel resource‐efficient grippers in future pick‐and‐place systems. In contrast with the adhesion acting during the “pick” phase, the release during the “place” phase has received little research attention so far. For objects smaller than typically 1 mm, release may become difficult as gravitational and inertial forces are no longer sufficient to allow shedding of the object. A compressive overload can initiate release by elastic buckling of the fibrils, but the switching ratio (ratio between high and low adhesion force) is typically only 2–3. In this work, new microfibrillar designs are reported exhibiting directional buckling with high switching ratios in the order of 20. Their functionality is illustrated by in situ optical observation of the contact signatures. Such micropatterns can enable the successful release of small objects with high placement accuracy.
One‐Pot Covalent Functionalization of 2D Black Phosphorus by Anionic Ring Opening Polymerization
Authors: Bawadkji Obida , Cherri Mariam , Schäfer Andreas , Herziger Svenja , Nickl Philip , Achazi Katharina , Donskyi Ievgen S. , Adeli Mohsen , Haag Rainer 
Published: September 2022

AbstractIn this work, a one‐pot approach for the covalent functionalization of few‐layer black phosphorus (BP) by anionic ring opening polymerization of glycidol to obtain multifunctional BP‐polyglycerol (BP‐PG) with high amphiphilicity for near‐infrared‐responsive drug delivery and biocompatibility is reported. Straightforward synthesis in combination with exceptional biological and physicochemical properties designates functionalized BP‐PG as a promising candidate for a broad range of biomedical applications.
Ephrin Micropatterns Exogenously Modulate Cell Organization in Organoid‐Derived Intestinal Epithelial Monolayers
Authors: Larrañaga Enara , Fernández‐Majada Vanesa , Ojosnegros Samuel , Comelles Jordi , Martinez Elena 
Published: September 2022

AbstractEph‐ephrin signaling acts as spatial cue to define the tissue boundaries, the axonal growth, or the organization of compartmentalized tissues in vertebrates. By the regulation of tension, adhesion, and repulsion, intermingling of cells expressing the membrane‐tethered ligand and cells expressing the membrane‐tethered receptor is prevented. Despite being surface‐bound, most of the studies addressing Eph‐ephrin interactions use soluble ligands, which lack the spatial component needed to study tissue patterning. Here, it is shown that spatial patterns of ephrin ligands can modulate the organization of the different compartments in organoid‐derived intestinal epithelial monolayers. A modified version of the microcontact printing technique is used to create spatial cues of ephrin ligand on basement membrane surrogates. It is shown that both ligand concentration and cellular density can impact the strength of the repulsive effect triggered by Eph‐ephrin signaling. Finally, it is demonstrated that by using micropatterned ephrin spatial cues one can modify the orientation of intestinal crypts and align them in the direction set by the pattern. The approach presented here is believed to be an excellent tool to study exogenous signal with relevant spatial distribution in vivo.
From Top to Down—Recent Advances in Etching of 2D Materials
Authors: Li Minghui , Li Lin , Fan Yixuan , Jiao Fei , Geng Dechao , Hu Wenping 
Published: September 2022

AbstractEtching, considered as the reverse process of growth, has drawn intensive interests in the past decades. Rather from offering building blocks for formation of materials, etching is served as removing basic units from the matrix. Generally, etching plays a critical role in three aspects: first, it can serve as direct top‐down method to precisely make designed patterns for electronic devices. Second, it can offer an indirect way to probe the detailed growth mechanism of 2D materials, enhancing understanding of growth process. Finally, it can be an efficient and facile way to visualize grain boundaries. Herein, several commonly used etching techniques for 2D materials are presented of which chemical vapor deposition etching has attracted the most intensive attentions. Thereafter, the typical etching modes of 2D materials are demonstrated, wherein linear etching, anisotropic etching, and fractal etching are comprehensively exhibited, respectively. Furthermore, the etching mechanism of 2D materials is elucidated, thereby offering a guideline for probing their in‐depth etching dynamics and kinetics. Finally, relevant concerns regarding uniformity and reproducibility within etching process are discussed and the expected future is envisaged.
Controllable Constructing Janus Homologous Heterostructures of Transition Metal Alloys/Sulfides for Efficient Oxygen Electrocatalysis
Authors: Lu Qi , Wu Han , Zheng Xuerong , Cao Yanhui , Li Jihong , Wang Yang , Wang Haozhi , Zhi Chunyi , Deng Yida , Han Xiaopeng , Hu Wenbin 
Published: September 2022

AbstractConstructing novel heterostructures is an effective way for enhancing the oxygen electrocatalytic properties of the catalysts. In this work, a class of Janus homologous heterostructures, compositing transition metal alloys with their corresponding sulfides (TM/TMS), are controllably synthesized through an ultrafast high‐temperature shock (HTS) strategy. The ultrafast sintering rate and carbothermal reduction reaction lead to the formation of sulfides and partial reduction of sulfides to alloys, while the ultrafast cooling rate keeps the homologous heterostructure of TM/TMS stable. The components of TMs in the composites can be well controlled from unary to quaternary. Moreover, benefiting from the synergistic effect of the metallic sites in the interfaces, the adsorption and desorption energy barrier of the active intermediates are significantly optimized and thus leading to the enhanced oxygen catalytic performance. Impressively, the aqueous zinc‐air battery (ZAB) using the binary homologous nanocomposite FeCo/(FeCo)S as air cathodes achieves impressive durability (> 470 cycles) and power density (261.8 mW cm−2). The as‐assembled flexible ZAB can well power the wearable devices and can work for at least 300 cycles without obvious degradation. This work opens a new chemical space for designing homologous heterostructures for their application in energy storage and conversion systems.
Differences in faculty feedback for high, expected, and below‐expected clinically performing emergency medicine residents
Authors: Coughlin Ryan F. , Tsyrulnik Alina , Gottlieb Michael , Bod Jessica , Barnicle Ryan , Dziura James , Della‐Giustina David , Goldflam Katja 
Published: September 2022

AbstractObjectivesA lifelong pursuit such as medicine is frequently paired with a framework of “deliberate practice” for improvement. It is unclear whether the quality of feedback varies across different learner levels. Our study aims to assess whether a difference exists in the quality of feedback delivered to high‐, expected‐, and below‐expected performer emergency medicine (EM) residents based on their attending‐identified performance level.MethodsWe conducted a retrospective review of written EM resident feedback collected between November 2018 and March 2021. Clinical performance level was subjectively determined by attending faculty in their feedback. Feedback was coded on a scale from 0–5 based on the presence (1) or absence (0) of the items modified from the Ende's SMART criteria: Specific (S), Measurable (M), Achievable (A), Relevant (R), and Time‐bound (T). The primary outcome was any total modified SMART criteria score difference concerning performance level using logistic regression with Generalized Estimating Equations (GEE). Secondary outcomes were differences for individual criteria.ResultsWe analyzed 1284 evaluations (311 high performers, 930 expected performers, and 43 below‐expected performers) of 94 unique residents from 66 different evaluators. Mean total modified SMART scores were significantly higher in high and below‐expected performers than those designated as expected performers by faculty evaluators. Achievable and Relevant written feedback was provided to high performers in a significantly larger proportion than expected and below‐expected performers. Only 278 out of 1284 evaluations met criteria for Specific.ConclusionsMean total modified SMART feedback scores were significantly greater in high performers and below‐expected performers when compared to expected performers. Achievable and Relevant feedback was provided in greater proportions to high performer residents compared to expected and below‐expected performers. These findings are a challenge to academic faculty to engage in quality feedback delivery for residents at all performance levels.
A workforce study of emergency medicine medical education fellowship directors: Describing roles, responsibilities, support, and priorities
Authors: Golden Andrew , Diller David , Riddell Jeffrey , Jordan Jaime , Gisondi Michael , Ahn James 
Published: September 2022

AbstractIntroductionDespite emergency medicine (EM) medical education fellowships increasing in number, the position of the medical education fellowship director (FD) remains incompletely defined. The goal of this study was to characterize the roles, responsibilities, support, and priorities for medical education FDs.MethodsWe adapted and piloted an anonymous electronic survey consisting of 31 single‐answer, multiple‐answer, and free‐response items. The survey was distributed to FDs via listserv and individual emails from a directory compiled from multiple online resources. We used descriptive statistics to analyze data from items with discrete answer choices. Using a constructivist paradigm, we performed a thematic analysis of free‐response data.ResultsThirty‐four medical education FDs completed the survey, resulting in a response rate of 77%. Thirty‐eight percent of respondents were female. Fifty‐three percent earned master's degrees in education and 35% completed a medical education fellowship. Most respondents held other education leadership roles including program director (28%), associate/assistant program director (28%), and vice chair (25%). Sixty‐three percent received support in their role, including clinical buy‐down (90%), administrative assistants (55%), and salary (5%). There was no difference (χ2 [2, n = 32] = 1.77, p = 0.41) between availability of support and type of hospital (community, university, or public hospital). Medical education FDs dedicated a median of 12 h per month to fellowship responsibilities, include education (median 35% of time), program administration (25%), research mentorship (15%), and recruitment (10%). Medical education FDs describe priorities that can be categorized into three themes related to fellows, fellowship, and institution.ConclusionThis study provides insight into the current position and experience of medical education FDs. The results can clarify the role and responsibilities of FDs as the demand for medical education FDs increases.