bluuebunny/crossref_metadata_2025_split huggingface dataset:
Revealing Enhanced Optoelectronic Performance of Sb2Se3‐Based Self‐Sustaining Heterostructures with Bi2Se3 and ZnSe: A Dual Polarity Photo Response
Authors: Kumar Kapil , Sharma Prince , Verma Sahil , Saini Saurabh K. , Kumar Tailor Naveen , Husale Sudhir , Singh Rajiv K. , Satapathi Soumitra , Achanta Venu Gopal , Kumar Mahesh 
Published: August 2024

AbstractThrough precise band engineering, Van der Waals heterostructures integration holds great promise for advancing high‐performance optoelectronic devices, especially photodetectors. This study presents self‐sustaining, dual‐polarity, high photo‐responsive heterostrutures (HS) photodetectors based on Sb2Se3, specifically Bi2Se3/Sb2Se3 and ZnSe/Sb2Se3. The Bi2Se3 (ZnSe) layer functions as a channel in a reconfigurable HS phototransistor configuration. These HS devices demonstrate a negative photoconductive response with bias‐modulated polarity switching of the photocurrent. The Bi2Se3/Sb2Se3 device exhibits a responsivity switch from −4 mA W−1 to 0.14 A W−1, while the ZnSe/Sb2Se3 device shows a substantially enhanced responsivity switch from ‐400 mA W−1 to 12 A W−1. This negative photo response results from a photoinduced carrier trapping mechanism at the interface of the channel layer and photosensitizer material. The bias modulation enables the switching from negative to positive responsivity. A comprehensive investigation of photoconductivity modulation provides a deeper understanding of the impact of the photogating effect and trap states under applied bias conditions. Ultrafast transient spectroscopy supports these findings, offering insights into the dynamics of charge carrier relaxation mechanisms and the trapping of photoexcited carriers in defect states, crucial for explaining the dual polarity photo response. These devices present significant advantages for switchable light imaging, optical communication, memory devices, convolution processing, and logic circuits.
In situ Ligand‐Managed SnO2 Electron Transport Layer for High‐Efficiency and Stable Perovskite Solar Cells
Authors: Sun Yulu , Xu Ruoyao , Yang Lin , Dai Jinfei , Zhu Xinyi , Cao Xiangrong , Li Peizhou , Tang Hebing , Liu Tao , Mo Daolei , Wang Yunxuan , Li Jingrui , Yuan Fang , Jiao Bo , Wu Zhaoxin , Dong Hua 
Published: August 2024

AbstractTin oxide (SnO2) with high conductivity and excellent photostability has been considered as one of the most promising materials for efficient electron transport layer (ETL) in perovskite solar cells (PSCs). Among them, SnO2 nanoparticles (NPs) dispersions have been extensively utilized due to their facile film formation. However, the inherent defects and agglomeration issues of SnO2 NPs, as well as the limited tunability and instability of the post‐treatment process for surface/interface engineering strategy, still hinder its further applications. Herein, a ligand‐management strategy implemented during the in situ synthesis of NPs that can effectively achieve uniform modification of NPs is proposed. During the synthesis of SnO2 NPs, the grafting reaction between diethyl 2‐chloromalonate (DCMA) and the surface of SnO2 NPs is completed. Compared with the post‐treatment process, this intrinsic DCMA‐passivated SnO2 (DCMA‐SnO2) effectively reduces the trap state density at the interface between perovskite and ETL while enhancing surface chemical stability. Consequently, PSCs based on DCMA‐SnO2 achieve a champion PCE of 25.39% for small cells (active area of 0.0655 cm2) and 20.61% for solar modules (active area of 23.25 cm2), demonstrating excellent shelf‐life/light soaking stability (advanced level of ISOS stability protocols). This ligand‐management strategy exhibits significant application potential in preparing high‐efficiency large‐area PSCs.
The Reinforced Separation of Intractable Gas Mixtures by Using Porous Adsorbents
Authors: Ke Quanli , Xiong Feng , Fang Guonan , Chen Jing , Niu Xiaopo , Pan Pengyun , Cui Guokai , Xing Huabin , Lu Hanfeng 
Published: August 2024

AbstractThis review focuses on the mechanism and driving force in the intractable gas separation using porous adsorbents. A variety of intractable mixtures have been discussed, including air separation, carbon capture, and hydrocarbon purification. Moreover, the separation systems are categorized according to distinctly biased modes depending on the minor differences in the kinetic diameter, dipole/quadruple moment, and polarizability of the adsorbates, or sorted by the varied separation occasions (e.g., CO2 capture from flue gas or air) and driving forces (thermodynamic and kinetic separation, molecular sieving). Each section highlights the functionalization strategies for porous materials, like synthesis condition optimization and organic group modifications for porous carbon materials, cation exchange and heteroatom doping for zeolites, and metal node‐organic ligand adjustments for MOFs. These functionalization strategies are subsequently associated with enhanced adsorption performances (capacity, selectivity, structural/thermal stability, moisture resistance, etc.) toward the analog gas mixtures. Finally, this review also discusses future challenges and prospects for using porous materials in intractable gas separation. Therein, the combination of theoretical calculation with the synthesis condition and adsorption parameters optimization of porous adsorbents may have great potential, given its fast targeting of candidate adsorbents and deeper insights into the adsorption forces in the confined pores and cages.
Zinc‐Mediated Carbamoyl Amination of Alkylidenecyclopropane‐Tethered Carbamoyl Chlorides: Synthesis of Functionalized 2‐Quinolones
Authors: Deng Jing‐Tong , Lang Ming , Peng Jin‐Bao 
Published: August 2024

AbstractThe transition metal catalyzed cyclization of alkene‐tethered carbamoyl chloride has emerged as a tool to construct oxindoles bearing quaternary centers. Most of these reactions proceed via carbometalation‐initiated 5‐exo‐trig cyclization followed by nucleophilic trapping of the resulting σ alkyl‐metal species to achieve diverse functionalized oxindoles. The 6‐endo‐trig type cyclization of alkene‐tethered carbamoyl chloride has been rarely reported. Herein, a zinc‐mediated carbamoyl amination of alkylidenecyclopropane‐tethered carbamoyl chlorides with anilines for the synthesis of functionalized 2‐quinolones was developed. A range of different substituted 2‐quinolones were prepared in 65–89% yield from alkylidenecyclopropane‐tethered carbamoyl chlorides and aniline derivatives using a Zn/TMSCl system.
Meis1 Targets Protein Tyrosine Phosphatase Receptor J in Fibroblast to Retard Chronic Kidney Disease Progression
Authors: Bai Mi , Xu Shuang , Jiang Mingzhu , Guo Yuxian , Hu Dandan , He Jia , Wang Ting , Zhang Yu , Guo Yan , Zhang Yue , Huang Songming , Jia Zhanjun , Zhang Aihua 
Published: August 2024

AbstractRenal fibrosis is a common pathological feature of chronic kidney disease (CKD) with the proliferation and activation of myofibroblasts being definite effectors and drivers. Here, increased expression of Meis1 (myeloid ecotropic viral integration site 1) is observed, predominantly in the nucleus of the kidney of CKD patients and mice, and negatively correlates with serum creatinine. Fibroblast‐specific knock‐in of Meis1 inhibits myofibroblast activation and attenuates renal fibrosis and kidney dysfunction in CKD models. Overexpression of Meis1 in NRK‐49F cells suppresses the pro‐fibrotic response induced by transforming growth factor‐β1 but accelerates by its knockdown. Mechanistically, Meis1 targets protein tyrosine phosphatase receptor J (Ptprj) to block renal fibrosis by inhibiting the proliferation and activation of fibroblasts. Finally, a new activator of Ptprj is identified through computer‐aided virtual screening, which has the effect of alleviating renal fibrosis. Collectively, these results illustrate that the Meis1/Ptprj axis has therapeutic potential for clinically treating CKD.
CRISPR Screening and Comparative LC‐MS Analysis Identify Genes Mediating Efficacy of Delamanid and Pretomanid against Mycobacterium tuberculosis
Authors: Yan Mei‐Yi , Li Haifeng , Qu Yun‐Mo , Li Si‐Shang , Zheng Dandan , Guo Xiao‐Peng , Wu Zhaojun , Lu Jie , Pang Yu , Li Weimin , Yang Jian , Zhan Lingjun , Sun Yi‐Cheng 
Published: August 2024

AbstractTuberculosis (TB), the leading cause of death from bacterial infections worldwide, results from infection with Mycobacterium tuberculosis (Mtb). The antitubercular agents delamanid (DLM) and pretomanid (PMD) are nitroimidazole prodrugs that require activation by an enzyme intrinsic to Mtb; however, the mechanism(s) of action and the associated metabolic pathways are largely unclear. Profiling of the chemical‐genetic interactions of PMD and DLM in Mtb using combined CRISPR screening reveals that the mutation of rv2073c increases susceptibility of Mtb to these nitroimidazole drugs both in vitro and in infected mice, whereas mutation of rv0078 increases drug resistance. Further assays show that Rv2073c might confer intrinsic resistance to DLM/PMD by interfering with inhibition of the drug target, decaprenylphophoryl‐2‐keto‐b‐D‐erythro‐pentose reductase (DprE2), by active nicotinamide adenine dinucleotide (NAD) adducts. Characterization of the metabolic pathways of DLM/PMD in Mtb using a combination of chemical genetics and comparative liquid chromatography‐mass spectrometry (LC‐MS) analysis of DLM/PMD metabolites reveals that Rv0077c, which is negatively regulated by Rv0078, mediates drug resistance by metabolizing activated DLM/PMD. These results might guide development of new nitroimidazole prodrugs and new regimens for TB treatment.
Trapped in Endosome PEGylated Ultra‐Small Iron Oxide Nanoparticles Enable Extraordinarily High MR Imaging Contrast for Hepatocellular Carcinomas
Authors: Zhou Dandan , Shan Shanshan , Chen Lei , Li Cang , Wang Hongzhao , Lu Kuan , Ge Jianxian , Wang Ning , Afshari Mohammad Javad , Zhang Yaqin , Zeng Jianfeng , Gao Mingyuan 
Published: August 2024

AbstractThe early diagnosis of hepatocellular carcinomas (HCCs) remains challenging in the clinic. Primovist‐enhanced magnetic resonance imaging (MRI) aids HCC diagnosis but loses sensitivity for tumors <2 cm. Therefore, developing advanced MRI contrast agents is imperative for improving the diagnostic accuracy of HCCs in very‐early‐stage. To address this challenge, PEGylated ultra‐small iron oxide nanoparticles (PUSIONPs) are synthesized and employed as liver‐specific T1 MRI contrast agents. Intravenous delivery produces simultaneous hyperintense HCC and hypointense hepatic parenchyma signals on T1 imaging, creating an extraordinarily high tumor‐to‐liver contrast. Systematic studies uncover PUSIONP distribution in hepatic parenchyma, HCC lesions at the organ, tissue, cellular, and subcellular levels, revealing endosomal confinement of PUSIONP without aggregation. By mimicking such situations, the dependency of relaxometric properties on local PUSIONP concentration is investigated, emphasizing the key role of different endosomal concentrations in liver and tumor cells for high tumor‐to‐liver contrast and clear tumor boundaries. These findings offer exceptional imaging capabilities for early HCC diagnosis, potentially benefiting real HCC patients.
Iron Corrole‐Catalyzed Intramolecular Amination Reactions of Alkyl Azides. Spectroscopic Characterization and Reactivity of [FeV(Cor)(NAd)]
Authors: You Tingjie , Shing Ka‐Pan , Wu Liangliang , Wu Kai , Wang Hua‐Hua , Liu Yungen , Du Lili , Liang Runhui , Phillips David Lee , Chang Xiao‐Yong , Huang Jie‐Sheng , Che Chi‐Ming 
Published: August 2024

AbstractAs nitrogen analogues of iron‐oxo species, high‐valent iron‐imido species have attracted great interest in the past decades. FeV‐alkylimido species are generally considered to be key reaction intermediates in Fe(III)‐catalyzed C(sp3)─H bond aminations of alkyl azides but remain underexplored. Here, it is reported that iron‐corrole (Cor) complexes can catalyze a wide range of intramolecular C─H amination reactions of alkyl azides to afford a variety of 5‐, 6‐ and 7‐membered N‐heterocycles, including alkaloids and natural product derivatives, with up to 3880 turnover numbers (TONs) and excellent diastereoselectivity (>99:1 d.r.). Mechanistic studies including density functional theory (DFT) calculations and intermolecular hydrogen atom abstraction (HAA) reactions reveal key reactive FeV‐alkylimido intermediates. The [FeV(Cor)(NAd)] (Ad = adamantyl) complex is independently prepared and characterized through electron paramagnetic resonance (EPR), resonance Raman (rR) measurement, and X‐ray photoelectron spectroscopy (XPS). This complex is reactive toward HAA reactions with kinetic isotope effects (KIEs) similar to [Fe(Cor)]‐catalyzed intramolecular C─H amination of alkyl azides.
Asymmetric Structural Engineering of Hot‐Exciton Emitters Achieving a Breakthrough in Non‐Doped BT.2020 Blue OLEDs with a Record 9.5% External Quantum Efficiency
Authors: Ma Bingzhu , Zhang Baijun , Zhang Han , Huang Yu , Liu Lu , Wang Baoling , Yang Dezhi , Ma Dongge , Tang Ben Zhong , Wang Zhiming 
Published: August 2024

AbstractHigh‐efficiency non‐doped deep‐blue organic light‐emitting diodes (OLEDs) meeting the standard of BT.2020 color gamut is desired but rarely reported. Herein, an asymmetric structural engineering based on crossed long‐short axis (CLSA) strategy is developed to obtain three new deep‐blue emitters (BICZ, PHDPYCZ, and PHPYCZ) with a hot‐exciton characteristic. Compared to 2BuCz‐CNCz featuring a symmetric single hole‐transport framework, these asymmetric emitters with the introduction of different electron‐transport units show the enhancement of photoluminescence efficiency and improvement of bipolar charge transport capacity. Further combined with high radiative exciton utilization efficiency and light outcoupling efficiency, the non‐doped OLED based on PHPYCZ exhibits the best performance with an excellent current efficiency of 3.49%, a record‐high maximum external quantum efficiency of 9.5%, and a CIE y coordinate of 0.049 approaching the BT.2020 blue point. The breakthrough obtained in this work can inspire the molecular design of deep‐blue emitters for high‐performance non‐doped BT.2020 blue OLEDs.
Programmable Analog Circuits with Neuromorphic Nanostructured Platinum Films
Authors: Radice Stefano , Profumo Filippo , Borghi Francesca , Falqui Andrea , Milani Paolo 
Published: August 2024

AbstractSelf‐assembled nanoparticle or nanowire networks have recently come under the spotlight as systems able to emulate brain‐like data processing performances by exploiting the memristive character and the wiring of the junctions connecting the nanostructured network building blocks. Recently it is demonstrated that nanostructured Au films, fabricated by the assembling of gold clusters produced in the gas phase, have non‐linear and non‐local electric conduction properties caused by the extremely high density of grain boundaries and the resulting complex arrangement of nanojunctions. These observations suggest that nanostructured metallic films can be explored and exploited as a novel class of neuromorphic systems for unconventional electronic devices. Here it is reported that nanostructured cluster‐assembled Pt films show resistive switching activity, negative differential resistance, and reversible memory effects. These properties allow the use of nanostructured Pt films in programmable analog circuits, such as gain amplifiers and relaxation oscillators with fast response.
Manipulating Multivalent Anion Intercalation for High‐Energy Aqueous Zn–Graphite Dual‐Ion Batteries
Authors: Zheng Ying , Xie Xiaolin , Ueno Hiroshi , Deng Ting , Zheng Weitao 
Published: August 2024

AbstractAnion intercalation in graphite is deemed as a promising electrode chemistry in aqueous energy storage systems due to its high onset potential. Given the limited space in graphite, multivalent anions are favorable to achieve high specific capacity. However, relevant studies are scarce so that fundamental understandings of multivalent anion intercalation remain unclear. Herein, the intercalation behaviors of ClO4−, SO42−, and PO43− in graphite are systematically investigated. High capacity and interaction between anion and graphite are proved to be contradictory as the electric charge increases. As a result, ClO4− and SO42− intercalation exhibits promising performance in primitive graphite, while PO43− intercalation is much restricted due to the intensified electronic interaction. Two Zn–graphite dual‐ion batteries based on ClO4− and SO42− intercalations display high voltages of 1.85 V, and specific energies of 106 and 112 Wh kg−1. This work provides fundamental understandings of multivalent anion intercalation and guidance to fabricate aqueous batteries (ABs) with high energy density.
Zwitterionic Nanoconfined Proton‐Sieve: Charged Casing for Accelerating Proton Conduction
Authors: Zou Wenwu , Jiang Guoxing , Li Baotao , Zhang Weifeng , Wang Liming , Cui Zhiming , Song Huiyu , Liang Zhenxing , Du Li 
Published: August 2024

AbstractSince specifying the structure during operation tends to be challenging for intrinsically proton‐conducting polymers, it becomes increasingly essential to establish a well‐defined migration path in order to predict the proton conductivity. Zwitterion covalent organic frameworks (ziCOFs) provide a platform in crystal frameworks to investigate the proton transfer mechanism, considering their specific charged channel walls, deprotonation surface, and host–guest interactions. Here, a zwitterion nanoconfined proton‐sieves (ziNPS) with “charged casing” channel of charged pathways is proposed to demonstrate theoretically the effectiveness of proton conduction. Density functional theory and molecular dynamic simulation results show that the ziNPS with different anion groups all achieve a shorter hydrogen bond to increase the dense “hydronium‐water” domain, creating a channel of hydrogen bond networks to provide a long‐range pathway for the proton to migrate. As expected, the proton conductivity test by electrochemical impedance spectroscopy demonstrates the aforementioned concept as well. This research presents a fresh view of the ion conduction mechanism originating from localized zwitterionic units, which can apply to the fabrication of COF‐based proton conductors.
Plasmagestützter Prozess mit Einzelatom‐Katalysatoren zur Nachhaltigen Umwandlung von Kunststoffabfällen
Authors: Yu Xiao , Rao Zhiqiang , Chen Guoxing , Yang Yuantao , Yoon Songhak , Liu Lina , Huang Zeai , Widenmeyer Marc , Guo Heng , Homm Gert , Kunz Ulrike , Liu Xingmin , Ionescu Emanuel , Molina‐Luna Leopoldo , Tu Xin , Zhou Ying , Weidenkaff Anke 
Published: August 2024

AbstractDie stetig steigende Menge an Kunststoffabfällen erfordert effektive Lösungen zur Bewältigung dieser Herausforderung. In dieser Studie stellen wir eine neuartige plasmagestützte Strategie zur schnellen Zersetzung verschiedener Plastikabfälle, einschließlich Mischungen, in hochwertige Kohlenstoffnanomaterialien und Wasserstoff vor. Die H2‐Ausbeute und die H2‐Selektivität, die durch die katalysatorfreien plasmagestützten Prozesse erzielt wurden, sind 14,2‐ bzw. 5,9‐mal höher als bisher unter ähnlichen Bedingungen mit konventioneller thermischer Pyrolyse erreicht wurde. Bemerkenswert ist, dass dieser katalysatorfreie Plasmaprozess einen signifikant höheren Energieertrag an H2 (gH2/kWh) im Vergleich zu anderen Pyrolyseprozessen liefert. Durch die Kopplung von Plasmapyrolyse mit thermischer Katalyse durch den Einsatz von atomar dispergierten Katalysatoren 1 Gew.‐ % M/CeO2 (M=Fe, Co und Ni) kann die Wasserstoffproduktion weiter gesteigert werden. Insbesondere der 1 Gew.– %Co/CeO2 Katalysator zeigte eine hervorragende katalytische Leistung über 10 Zyklen der Kunststoffabfallzersetzung hinweg und erreichte die höchste H2‐Ausbeute von 46,7 mmol/gplastic (entsprechend 64,4 % der theoretischen H2‐Ausbeute) und nahezu 100 % Wasserstoffatom‐Rückgewinnungseffizienz im 7. Zyklus. Atomar dispergiertes Fe auf der CeO2‐Oberfläche (1 Gew.– % Fe/CeO2) konnte im integrierten plasma‐thermischen Katalyseprozess eine H2‐Ausbeute erzielen wie sie sonst nur mit deutlich höheren Beladungen von Fe‐Partikeln auf der CeO2‐Oberfläche (10 Gew.– % Fe/CeO2) erreicht wird. Daher wurde demonstriert, dass Einzelatom‐Katalysatoren einen vielversprechenden Weg für ein kostengünstiges und effizientes chemisches Kunststoffrecycling darstellen. Durch eine Kombination aus Experiment und Modellierung haben wir ein tiefgehendes Verständnis der katalytischen Mechanismen der untersuchten Einzelatom‐Katalysatoren im entwickelten plasmagestützten Prozess erzielt. Dieser innovative und unkomplizierte Ansatz bietet eine vielversprechende und schnelle Strategie zur kontinuierlichen Umwandlung verschiedener Kunststoffabfallströme, einschließlich gemischter und kontaminierter Quellen, in hochwertige Produkte, die eine Kreislaufwirtschaft für Kunststoffe unterstützen.
High Performance Memristors Based on Imine‐Linked Covalent Organic Frameworks Obtained Using a Protonation Modification Strategy
Authors: Che Qian , Li Chenyu , Chen Zhihui , Yang Shuai , Zhang Weifeng , Yu Gui 
Published: August 2024

AbstractImine‐linked covalent organic frameworks (COFs) are garnering substantial interest in resistive random‐access memory, attributed to their superior crystallinity, excellent chemical and thermal stability, and modifiable molecular structures. However, the development of high‐performance COF‐based memristors impeded by challenges such as low conjugation degree of imine bonds and poor electron delocalization ability. Herein, we report a protonation strategy to modify the imine bonds of donor‐acceptor (D‐A) type COFs. This modification significantly enhances the electron delocalization capability of imine bonds, lowers the energy barriers for electron injection from electrodes, and stabilizes the conductive charge transfer state, thus markedly improving device performance. The protonated COF‐BTT‐BPy and COF‐BTT‐TAPT thin films‐based memristors show remarkable device performance with a high ON/OFF current ratio of 105, a low driving voltage, and outstanding endurance exceeding 600 and 1300 cycles, respectively, which is nearly twice the durability of analogous non‐protonated COFs‐based memristors. Notably, the protonated COF‐BTT‐TAPT‐based memristor exhibit the highest number of cycles reported at present. This work not only unprecedentedly enhances the performance of COF‐based memristors, but also provides a universal and promising approach for the molecular design and potential application of D‐A type imine‐linked COFs.
Enantio‐ und regiokonvergente, nickelkatalysierte Veretherung von Phenolen durch Allylierung zur Darstellung chiraler C(sp3)−O‐Allylarylether
Authors: Brösamlen Daniel , Neb Daniel , Oestreich Martin 
Published: August 2024

AbstractEs wird eine enantio‐ und regiokonvergente Allylierung von Phenolen unter Nickelkatalyse mit einem α‐/γ‐Regioisomerengemisch racemischer silylierter/germylierter Allylchloride beschrieben. Die Silyl‐/Germylgruppe steuert die Regioselektivität, und die Umwandlung liefert enantiomerenangereicherte unsymmetrische 1,3‐disubstituierte Allylarylether mit ausgezeichneter Regiokontrolle in guten Ausbeuten und mit hervorragenden Enantioselektivitäten. Bemerkenswerterweise wird keine nickelvermittelte C−O‐Bindungsaktivierung bei Raumtemperatur beobachtet. Der synthetische Wert dieser hochfunktionalisierten, siliciumhaltigen Bausteine wird in einer Reihe chemoselektiver Umwandlungen aufgezeigt, einschließlich einer [3,3]‐sigmatropen Umlagerung zur Herstellung eines α‐chiralen Silans.