bluuebunny/crossref_metadata_2025_split huggingface dataset:
Dynamic Transformation of Functionalized Bismuth to Catalytically Active Surfaces for CO2 Reduction to Formate at High Current Densities
Authors: Mahbub Muhammad Adib Abdillah , Junqueira João R. C. , Wang Xin , Zhang Jian , Dieckhöfer Stefan , Seisel Sabine , Das Debanjan , Schuhmann Wolfgang 
Published: October 2023

AbstractA facile strategy to boost the activity and preserve the selectivity of CO2 reduction to formate using organic‐functionalized metal catalysts, specifically 2‐methyl‐imidazole coordinated to Bi, Bi[2‐MeIm], is reported, and the active surfaces are investigated during structural transformation under the applied cathodic potential necessary for CO2 reduction. Operando Raman spectroscopy unveils the structure evolution during the reaction and post‐electrolysis analysis shows the formation of three phases of bismuth‐based active surfaces. As a result, Bi[2‐MeIm] achieves an excellent CO2 reduction performance with an average formate selectivity of ≈90% Faradaic efficiency and high activity reaching a current density of up to −1 A cm−2 in a narrow window of cathodic potentials from −0.46 to −0.78 V versus RHE.
Lightweight Soft Conductive Composites Embedded with Liquid Metal Fiber Networks
Authors: Ma Jiexian , Liu Zihan , Nguyen Quang‐Kha , Zhang Pu 
Published: October 2023

AbstractLiquid metal composites are promising soft conductors for applications in soft electronics, sensors, and soft robotics. Existing liquid metal composites usually have a high‐volume fraction of liquid metal, which not only increases the density but also the material cost. Future applications in soft electronics and robotics highly demand liquid metal composites with low density and high conductivity for large‐scale, low‐cost, lightweight, and more sustainable applications. In this work, lightweight and highly conductive composites embedded with liquid metal fiber networks are synthesized. This new paradigm of liquid metal composites consists of an interconnected liquid metal fiber network embedded in a compliant rubber matrix. The liquid metal fiber network serves as an ultra‐lightweight conductive pathway for electrons. Experiments indicate that this soft conductive composite also possesses nearly strain‐insensitive conductance and superior cyclic stability. Potential applications of the composite films as stretchable interconnects, electrodes, and sensors are demonstrated.
Unveiling the Impact of Organic Spacer Cations on Auger Recombination in Layered Halide Perovskites
Authors: Furuhashi Tomoki , Kanwat Anil , Ramesh Sankaran , Mathews Nripan , Sum Tze Chien 
Published: October 2023

AbstractA library of large organic cation spacers is available for engineering the performance of layered two‐dimensional (2D) halide perovskite devices. Despite extensive photophysics studies, there remains a research gap over the structure‐function relations in 2D perovskites, especially the underlying factors influencing the Auger recombination (AR) process. Herein, the contributions of exciton binding energy, exciton‐phonon coupling, and defects/film morphology to the AR process in 2D perovskites are examined. Phenyl‐alkyl‐ammonium cations with different lengths of attached alkyl groups, commonly used in blue light‐emitting diodes, are investigated. The findings reveal an order of magnitude higher threshold carrier density for the AR onset as well as a reduced AR in cations with longer alkyl chain length. Although possessing similar exciton binding energies, the exciton‐phonon coupling strength is found to play a major role in reducing the AR rate, with a smaller contribution from the defect states/film morphology. The findings can help provide further guidance on organic spacer cation engineering for highly efficient 2D perovskite light emitters.
Excitonic Degradation Mechanisms in Phosphorescent and Thermally Activated Delayed Fluorescence Organic Light‐Emitting Diodes
Authors: Jiang Jixin , Jang Ho Jin , Lee Kyung Hyung , Lim Junseop , Kim Jae‐Min , Zhao Suling , Lee Jun Yeob 
Published: October 2023

AbstractIn this study, the degradation mechanisms of triplet exciton harvesting organic light‐emitting diodes (OLEDs), namely, phosphorescent OLEDs and thermally activated delayed fluorescence (TADF) OLEDs, are investigated. Two common green emitters, fac‐tris(2‐phenylpyridine) iridium (III) (Ir(ppy)3) and 1,2,3,5‐tetrakis(carbazol‐9‐yl)‐4,6‐dicyanobenzene (4CzIPN), are doped in an exciplex‐forming cohost, and their degradation processes are comprehensively evaluated using various analytical approaches. Triplet–triplet‐annihilation induces the formation of defects, such as charge traps and exciton quenchers, triggering luminance loss during the device aging process of Ir(ppy)3‐based phosphorescent OLEDs. Electron trapping‐induced triplet‐polaron annihilation and narrow emission zone severely impair the device stability of 4CzIPN‐based TADF OLEDs, despite limited material degradation and charge trap formation.
Improving Nitrogen Retention in Algal Biochar Pyrolysis by Co‐Pyrolysis with Glucose
Authors: Vercruysse Willem , Pappa Michaela , Mangione Gianfabio , Desta Derese , Hardy An , Boyen Hans‐Gerd , Van Bael Marlies K. , Marchal Wouter , Vandamme Dries 
Published: October 2023

AbstractAlgal biomass is a promising pyrolysis feedstock, however, large amounts of nitrogen‐containing compounds (NH3, HCN,…) are emitted during its conversion. These emissions can be decreased by incorporating nitrogen in the biochar's carbon matrix via co‐pyrolysis. This study investigates whether adding glucose (GL) to the microalgae, Arthrospira sp. (SP), increases the nitrogen fixation in the solid biochar. Moreover, scalable (co‐) pyrolysis experiments are linked with micro‐scale pyrolysis. Using hyphenated pyrolysis (Py–GC–MS, TG‐IR) and characterization (CHNS, XPS, and Raman) techniques the phenomena associated with the incorporation of nitrogen in the biochars are unraveled. Co‐pyrolyzing SP and GL increased biochar yields and nitrogen retention, which is attributed to Maillard reactions occurring in the initial pyrolysis stages. In conclusion, this study provides evidence that co‐pyrolysis of microalgae and reducing sugars is a more sustainable strategy to produce algae‐based biochar.
Prediction of The Binding Mode of NP‐G2‐044 Targeting Fascin and Its Drug Resistance Mutations
Authors: Pan Jinmei , Wang Liangdong , Xu Li‐Yan , Li En‐Min , Dong Geng 
Published: October 2023

AbstractFascin is a major actin‐binding protein (ABP) in filopodia and is highly expressed in metastatic tumors. To inhibit its function, a potent inhibitor called NP‐G2‐044 is currently in phase II clinical trials. However, the binding mode of this inhibitor remains unclear. In this study, the binding mode of NP‐G2‐044 in fascin and predicted drug resistance mutations is investigated. The rough binding position and pose can be deduce based on information from its derivant NP‐G2‐029, whose crystal structure with fascin has been solved. Molecular docking, free energy perturbation (FEP) simulation and metadynamics simulation are performed to confirm the binding pose. Based on the molecular docking results, two binding modes of NP‐G2‐044, pose A and B, are obtained, with pose A being more favorable. For pose A, the planar indazole moiety has the same orientation as NP‐G2‐029 in the complex with fascin, while for pose B, it rotates ≈90°. FEP and metadynamics simulations indicate that both binding poses are possible. Relative binding free energies for mutation effects calculated by FEP predict E215A and R217A are drug resistance mutations. These findings are important for further drug development targeting fascin.
2D Light‐Weight Transition Metal Disulfide as Model Cathode for Alkali‐Ion Batteries and Beyond
Authors: Chakraborty Dwaipayan , Pandey Madhu , Johari Priya 
Published: October 2023

AbstractThe capacity of rechargeable battery is mainly controlled by two factors: maximum number of ions that can be held by an electrode material and its weight. In general, the weight and hence the specific capacity of a battery is mainly affected by the cathode material. In this context, Sc, the lightest transition metal, could prove helpful in achieving the goal of high theoretical capacity. Therefore, here the performance of two‐dimensional (2D) ScS2 nanosheets (both hexagonal‐H and trigonal‐T) as cathode materials for alkali‐ion batteries (Li, Na, and K) and other multivalent metal‐ion batteries (Mg and Al) is studied. The first‐principles calculations show that 2D H and T─ScS2 nanosheets deliver large theoretical capacity of 491.36 mA h g−1 for alkali ions and 324.29 m'A h g−1 for Mg and Al ions while maintaining good average open‐circuit voltages. Results also suggest low diffusion barriers for all metal ions except Al, with T─ScS2 exhibiting ultra‐low barriers for alkali atoms. Overall, this study provides a fundamental and a comprehensive view on the potential capabilities of both H─ScS2 and T─ScS2 by defining the underlying mechanism from the perspective of a cathode material which may prove helpful in designing light‐weight and high‐capacity transition metal sulfide‐based metal‐ion batteries in the future.
First‐Principles Study of the C‐ and Si‐Doped Buckled Honeycomb PN Monolayer
Authors: Van On Vo , Ha Chu Viet , Guerrero‐Sanchez J. , Hoat D. M. 
Published: October 2023

AbstractIn this work, the effects of doping with carbon (C) and silicon (Si) on the electronic and magnetic properties of phosphorus nitride (PN) monolayer are investigated. PN monolayer is stable, exhibiting the semiconductor nature with indirect band gap of 1.81(2.89) eV calculated by standard Perdew–Burke–Ernzerhof (hybrid HSE06) functional. C and Si impurities prefer doping at N and P sublattices, respectively. PN monolayer is slightly magnetized by doping with 25% of C with total magnetic moment of 0.20 . The magnetization is stronger in the remaining cases with total magnetic moments of 1.00 . Magnetic properties are produced mainly by C and Si impurities. In addition, C and Si codoping is also investigated, in which the magnetization depends strongly on the interatomic distance between impurities. Specifically, the inter‐dopant interactions preserve the non‐magnetic nature of PN monolayer, but significantly reduce the energy gap. However, further separating these dopants leads to the emergence of magnetism with total magnetic moment of up to 1.97 . Results may introduce doping‐based effective method to induce feature‐rich electronic and magnetic properties in buckled honeycomb PN monolayer. Such that, the C‐ and Si‐doped PN sheets are recommended for spintronic applications considering their magnetic semiconductor nature.
Landauer‐QFLPS Model for Mixed Schottky‐Ohmic Contact Two‐Dimensional Transistors
Authors: Yan Zhao‐Yi , Hou Zhan , Xue Kan‐Hao , Tian He , Lu Tian , Xue Junying , Wu Fan , Zhao Ruiting , Shao Minghao , Yan Jianlan , Yan Anzhi , Wang Zhenze , Shen Penghui , Zhao Mingyue , Miao Xiangshui , Lin Zhaoyang , Liu Houfang , Yang Yi , Ren Tian‐Ling 
Published: October 2023

AbstractTwo‐dimensional material‐based field‐effect transistors (2DM‐FETs) are playing a revolutionary role in electronic devices. However, before electronic design automation (EDA) for 2DM‐FETs can be achieved, it remains necessary to determine how to incorporate contact transports into model. Reported methods compromise between physical intelligibility and model compactness due to the heterojunction nature. To address this, quasi‐Fermi‐level phase space theory (QFLPS) is generalized to incorporate contact transports using the Landauer formula. It turns out that the Landauer‐QFLPS model effectively overcomes the issue of concern. The proposed new formula can describe 2DM‐FETs with Schottky or Ohmic contacts with superior accuracy and efficiency over previous methods, especially when describing non‐monotonic drain conductance characteristics. A three‐bit threshold inverter quantizer (TIQ) circuit is fabricated using ambipolar black phosphorus and it is demonstrated that the model accurately predicts circuit performance. The model could be very effective and valuable in the development of 2DM‐FET‐based integrated circuits.
Impact of a robotic system on intra‐abdominal infectious complications after minimally invasive gastrectomy in patients with gastric cancer: A propensity score matching analysis regarding visceral obesity
Authors: Kubo Naoshi , Sakurai Katsunobu , Hasegawa Tsuyoshi , Tamamori Yutaka , Iseki Yasuhito , Nishii Takafumi , Shimizu Sadatoshi , Inue Toru , Nishiguchi Yukio , Maeda Kiyoshi 
Published: October 2023

AbstractBackgroundThe efficacy of robotic gastrectomy (RG) on postoperative complications in patients with gastric cancer (GC) is unclear in terms of the volume of intra‐abdominal fat tissue.Patients and MethodsWe enrolled 403 patients with GC who had minimally invasive surgery between January 2015 and July 2022. During this time, 197 RG and 206 laparoscopic gastrectomies (LG) were performed on the study participants. According to the computed tomography scan, patients were defined as having or not having visceral obesity based on the visceral fatty area (VFA). In each high and low VFA group, we compared short‐term outcomes between the RG group and LG group.ResultsAfter PS matching for patients with high VFA, the two groups were well matched, with 71 cases in both the RG and LG groups. The median surgical time in the RG group was significantly longer (420 vs. 365 min, p < 0.001). However, the RG group had a significantly lower rate of severe intra‐abdominal infectious complications (IAIC), such as anastomotic leakage, pancreatic fistula, and intra‐abdominal abscess (1.4% vs. 15.4%, p = 0.004). However, among the 77 patients with low VFA values, we found no significant difference in the rate of severe IAIC between the two groups (1.1% in the RG group vs. 2.6% in the LG group, p = 1.00).ConclusionRG may be a viable alternative to LG because of the lower postoperative IAIC for patients with visceral obesity and GC. However, RG may not benefit non‐obese patients.
Selenium‐Catalyzed Electrophilic Cascade Reactions of Vinylarenes with N‐Fluorobenzenesulfonimide: A Novel Strategy for the Synthesis of β‐Keto Sulfones
Authors: Bao Fengyu 
Published: October 2023

AbstractA selenium‐catalyzed electrophilic cascade reaction of vinylarenes with N‐fluorobenzenesulfonimide for the efficient synthesis of important β‐keto sulfones via a single operation is developed. The reactions of vinylarenes bearing electron‐withdrawing groups and electron‐donating groups proceeded smoothly in the air and gave products in up to 94 % yield. Mechanistic studies suggest that vinyl amines generated by oxidative amination of vinylarenes are the intermediates, the cleavage of N−S bond and the recombination of sulfonyl radical lead to 1,3‐migration of sulfonyl, and hydrolysis affords the products β‐keto sulfones.
Development of Mitochondria‐Targeting Photosensitizers via Topoisomerase I Inhibition
Authors: Lim Bumhee , Lee Yeongcheol , In Kwon Dah , Kim Seoyoung , Oh Dong‐Chan , Kim Ikyon , Lee Jeeyeon 
Published: October 2023

AbstractPhotodynamic therapy (PDT) is an important oncologic intervention option for combating drug resistance of current chemotherapy in cancer. To improve spatiotemporal control, the development of subcellular organelle‐targeting photosensitizers is critical due to the diffusion limits of short‐lived ROS. Mitochondrial topoisomerase 1 (TOP1MT), exclusively localized in mitochondria, is emerging as a promising target for anticancer treatment. In this work, we designed and synthesized mitochondria‐targeting photosensitizers via Top1 inhibition activity of IQ6 and visualized the covalent adducts between the engaged proteins and the synthesized photoaffinity labeling probes (IQ‐Ps). Positively charged derivatives (IQ‐Ss) were also synthesized and their photo‐induced cytotoxicity was assessed to select IQ‐S1. Based on the cellular accumulation of IQ‐S1 in mitochondria and the enhanced PDT activity, we demonstrated that IQ‐S1 functions as a photosensitizer with sequential targeting of mitochondria and nucleus depending on irradiation times. Our findings suggest that the translocation of IQ‐S1 is related to the damage to mitochondrial Top1. The synthesized IQ‐S1 may contribute to the identification and tracking of cellular target proteins along with the PDT progression.
Acoustic resonance therapy is safe and effective for the treatment of nasal congestion in rhinitis: A randomized sham‐controlled trial
Authors: Luong Amber U. , Yong Michael , Hwang Peter H. , Lin Bryant Y. , Gopi Paramesh , Mohan Vivek , Ma Yifei , Johnson Jacob , Yen David M. , DeMera Richard S. , Bleier Benjamin S. 
Published: October 2023

AbstractBackgroundAcoustic resonance therapy (ART) is a novel vibrational treatment that delivers patient‐specific resonant frequency acoustic energy to the sinonasal cavities. In a pilot study, ART was effective for the acute treatment of nasal congestion. We conducted a sham‐controlled randomized trial to validate the efficacy of ART when administered daily for 2 weeks.MethodsA total of 52 adult patients were enrolled in a multi‐center, randomized, double‐blinded, sham‐controlled, interventional study evaluating ART administered by a vibrational headband. Patients received either active treatment or a non‐therapeutic sham treatment twice daily over 2 weeks. Clinical endpoints were the average change in nasal congestion sub‐score of the Total Nasal Symptom Score (TNSS) and the average change in composite TNSS.ResultsART resulted in a significantly greater mean change in the nasal congestion sub‐score compared to sham (−0.87 [95% confidence interval [CI] −1.11, −0.62] vs. −0.44 [95% CI −0.64, −0.23], p = 0.008). ART also resulted in a significantly greater reduction in the composite TNSS versus sham, (−2.85 [95% CI −3.85, −1.85], vs. −1.32 [95% CI −2.27, −0.36], p = 0.027). The response rate, determined by a nasal congestion sub‐score minimal clinically important difference of 0.23, was 80.8% for ART and 46.2% for sham, with an adjusted risk ratio of 1.95 (95% CI 1.26, 3.02, p = 0.003) in favor of ART. Safety endpoints showed no adverse events.ConclusionART is a safe and effective non‐pharmacologic alternative for the treatment of nasal congestion.
Sex‐dependent alterations in hippocampal connectivity are linked to cerebrovascular and amyloid pathologies in normal aging
Authors: Schweitzer Noah , Li Jinghang , Thurston Rebecca C. , Lopresti Brian , Klunk William E. , Snitz Beth , Tudorascu Dana , Cohen Ann , Kamboh M. Ilyas , Halligan‐Eddy Edythe , Iordanova Bistra , Villemagne Victor L. , Aizenstein Howard , Wu Minjie 
Published: October 2023

AbstractINTRODUCTIONCompared to males, females have an accelerated trajectory of cognitive decline in Alzheimer's disease (AD). The neurobiological factors underlying the more rapid cognitive decline in AD in females remain unclear. This study explored how sex‐dependent alterations in hippocampal connectivity over 2 years are associated with cerebrovascular and amyloid pathologies in normal aging.METHODSThirty‐three females and 21 males 65 to 93 years of age with no cognitive impairment performed a face‐name associative memory functional magnetic resonance imaging (fMRI) task with a 2‐year follow‐up. We acquired baseline carbon 11‐labeled Pittsburgh compound B ([11C]PiB) positron emission tomography (PET) and T2‐weighted fluid‐attenuated inversion recovery (T2‐FLAIR) MRI to quantify amyloid β (Aβ) burden and white matter hyperintensity (WMH) volume, respectively.RESULTSMales had increased hippocampal‐prefrontal connectivity over 2 years, associated with greater Aβ burden. Females had increased bilateral hippocampal functional connectivity, associated with greater WMH volume.DISCUSSIONThese findings suggest sex‐dependent compensatory mechanisms in the memory network in the presence of cerebrovascular and AD pathologies and may explain the accelerated trajectory of cognitive decline in females.
Expanding the Range of Bioorthogonal Tags for Multiplex Stimulated Raman Scattering Microscopy
Authors: Murphy Neville , Tipping William J. , Braddick Henry J. , Wilson Liam T. , Tomkinson Nicholas C. O. , Faulds Karen , Graham Duncan , Farràs Pau 
Published: October 2023

AbstractMultiplex optical detection in live cells is challenging due to overlapping signals and poor signal‐to‐noise associated with some chemical reporters. To address this, the application of spectral phasor analysis to stimulated Raman scattering (SRS) microscopy for unmixing three bioorthogonal Raman probes within cells is reported. Triplex detection of a metallacarborane using the B−H stretch at 2480–2650 cm−1, together with a bis‐alkyne and deuterated fatty acid can be achieved within the cell‐silent region of the Raman spectrum. When coupled to imaging in the high‐wavenumber region of the cellular Raman spectrum, nine discrete regions of interest can be spectrally unmixed from the hyperspectral SRS dataset, demonstrating a new capability in the toolkit of multiplexed Raman imaging of live cells.
Pushing Up the Size Limit of Boron‐doped peri‐Acenes: Modular Synthesis and Characterizations
Authors: Zhang Jin‐Jiang , Yang Lin , Liu Fupin , Serra Gianluca , Fu Yubin , Lucotti Andrea , Popov Alexey A. , Tommasini Matteo , Ma Ji , Feng Xinliang 
Published: October 2023

AbstractHeteroatom‐doped peri‐acenes (PAs) have recently attracted considerable attention considering their fascinating physical properties and chemical stability. However, the precise sole addition of boron atoms along the zigzag edges of PAs remains challenging, primarily due to the limited synthetic approach. Herein, we present a novel one‐pot modular synthetic strategy toward unprecedented boron‐doped PAs (B‐PAs), including B‐[4,2]PA (1 a‐2), B‐[4,3]PA (1 b‐2) and B‐[7,2]PA (1 c‐3) derivatives, through efficient intramolecular electrophilic borylation. Their chemical structures are unequivocally confirmed with a combination of mass spectrometry, NMR, and single‐crystal X‐ray diffraction analysis. Notably, 1 b‐2 exhibits an almost planar geometry, whereas 1 a‐2 displays a distinctive bowl‐like distortion. Furthermore, the optoelectronic properties of this series of B‐PAs are thoroughly investigated by UV/Vis absorption and fluorescence spectroscopy combined with DFT calculation. Compared with their parent all‐carbon analogs, the obtained B‐PAs exhibit high stability, wide energy gaps, and high photoluminescence quantum yields of up to 84 %. This study reveals the exceptional ability of boron doping to finely tune the physicochemical properties of PAs, showcasing their potential applications in optoelectronics.
Switchable Organocatalysis from N‐heterocyclic Carbene‐Carbodiimide Adducts with Tunable Release Temperature**
Authors: Pham Le Dung , Smith‐Sweetser Red O. , Krupinsky Briana , Dewey Carolyn E. , Lamb Jessica R. 
Published: October 2023

AbstractN‐Heterocyclic carbenes (NHCs) are powerful organocatalysts, but practical applications often require in situ generation from stable precursors that “mask” the NHC reactivity via reversible binding. Previously established “masks” are often simple small molecules, such that the NHC structure is used to control both catalytic activity and activation temperature, leading to undesirable tradeoffs. Herein, we show that NHC‐carbodiimide (CDI) adducts can be masked precursors for switchable organocatalysis and that the CDI substituents can control the reaction profile without changing the NHC structure. Large electronic variations on the CDI (e.g., alkyl versus aryl) drastically change the catalytically active temperature, whereas smaller perturbations (e.g., different para‐substituted phenyls) tune the catalyst release within a narrower window. This control was demonstrated for three classic NHC‐catalyzed reactions, each influencing the NHC‐CDI equilibrium in different ways. Our results introduce a new paradigm for controlling NHC organocatalysis as well as present practical considerations for designing appropriate masks for various reactions.