bluuebunny/crossref_metadata_2025_split huggingface dataset:
Epitaxial Growth of Lead‐Free Double Perovskite Shell for CsPbX3/Cs2SnX6 (X = Cl, Br, and I) Core/Shell Perovskite Nanocrystals with Enhanced Photoelectric Properties and Stability
Authors: Lin Hanjie , Li Shuya , Zhang Yuchen , Chu Chun , MacSwain Walker , Meulenberg Robert W. , Qiao Quinn , Zhao Dong , Zheng Weiwei 
Published: November 2023

AbstractAll‐inorganic lead halide perovskite nanocrystals (NCs) have great optoelectronic properties with promising applications in light‐emitting diodes (LEDs), lasers, photodetectors, solar cells, and photocatalysis. However, the intrinsic toxicity of Pb and instability of the NCs impede their broad applications. Shell‐coating is an effective method for enhanced environmental stability while reducing toxicity by choosing non‐toxic shell materials such as metal oxides, polymers, silica, etc. However, multiple perovskite NCs can be encapsulated within the shell material and a uniform epitaxial‐type shell growth of well‐isolated NCs is still challenging. In this work, lead‐free vacancy‐ordered double perovskite Cs2SnX6 (X = Cl, Br, and I) shells are epitaxially grown on the surface of CsPbX3 NCs by a hot‐injection method. The effectiveness of the non‐toxic double perovskite shell protection is demonstrated by the enhanced environmental and phase stability against UV illumination and water. In addition, the photoluminescence quantum yields (PL QYs) increase for the CsPbCl3 and CsPbBr3 NCs after shelling because of the type I band alignment of the core/shell materials, while enhanced charge transport properties obtained from CsPbI3/Cs2SnI6 core/shell NCs are due to the efficient charge separation in the type II core/shell band alignment.
A2‐A1‐D‐A1‐A2‐Type Nonfullerene Acceptors
Authors: Tang Ailing , Cong Peiqing , Dai Tingting , Wang Zongtao , Zhou Erjun 
Published: November 2023

AbstractThe A2‐A1‐D‐A1‐A2‐type molecules consist of one electron‐donating (D) core flanked by two electron‐accepting units (A1 and A2) and have emerged as an essential branch of nonfullerene acceptors (NFAs). These molecules generally possess higher molecular energy levels and wider optical bandgaps compared with those of the classic A‐D‐A‐ and A‐DA'D‐A‐type NFAs, owing to the attenuated intramolecular charge transfer effect. These characteristics make them compelling choices for the fabrication of high‐voltage organic photovoltaics (OPVs), ternary OPVs, and indoor OPVs. Herein, the recent progress in the A2‐A1‐D‐A1‐A2‐type NFAs are reviewed, including the molecular engineering, structure‐property relationships, voltage loss (Vloss), device stability, and photovoltaic performance of binary, ternary, and indoor OPVs. Finally, the challenges and provided prospects are discussed for the further development of this type of NFAs.
Large Room‐Temperature Magnetoresistance in a High‐Spin Donor–Acceptor Conjugated Polymer
Authors: Tahir Hamas , Eedugurala Naresh , Hsu Sheng‐Ning , Mahalingavelar Paramasivam , Savoie Brett M. , Boudouris Bryan W. , Azoulay Jason D. 
Published: November 2023

AbstractOpen‐shell conjugated polymers (CPs) offer new opportunities for the development of emerging technologies that utilize the spin degree of freedom. Their light‐element composition, weak spin‐orbit coupling, synthetic modularity, high chemical stability, and solution‐processability offer attributes that are unavailable from other semiconducting materials. However, developing an understanding of how electronic structure correlates with emerging transport phenomena remains central to their application. Here, the first connections between molecular, electronic, and solid‐state transport in a high‐spin donor–acceptor CP, poly(4‐(4‐(3,5‐didodecylbenzylidene)‐4H‐cyclopenta[2,1‐b:3,4‐b’]dithiophen‐2‐yl)‐6,7‐dimethyl‐[1,2,5]‐thiadiazolo[3,4‐g]quinoxaline), are provided. At low temperatures (T < 180 K), a giant negative magnetoresistance (MR) is achieved in a thin‐film device with a value of −98% at 10 K, which surpasses the performance of all other organic materials. The thermal depopulation of the high‐spin manifold and negative MR decrease as temperature increases and at T > 180 K, the MR becomes positive with a relatively large MR of 13.5% at room temperature. Variable temperature electron paramagnetic resonance spectroscopy and magnetic susceptibility measurements demonstrate that modulation of both the sign and magnitude of the MR correlates with the electronic and spin structure of the CP. These results indicate that donor–acceptor CPs with open‐shell and high‐spin ground states offer new opportunities for emerging spin‐based applications.
Photocatalytic H2O2 Generation Reaction with a Benchmark Rate at Air‐Liquid‐Solid Joint Interfaces
Authors: Yan Shiwei , Li Yong , Yang Xinyue , Jia Xiaohua , Xu Jingsan , Song Haojie 
Published: November 2023

AbstractThe rapid charge recombination, low selectivity for two‐electron oxygen reduction reaction (ORR), and limited O2 diffusion rate hinder the practical applications of photocatalytic H2O2 generation. Herein, a triphase photocatalytic system in which the H2O2 generation occurs at the air‐liquid‐solid joint interfaces is developed, using polymeric carbon nitride (PCN). The introduction of pyrrole units and cyano group into PCN can promote the activation of oxygen molecules and facilitate the spatial separation of HOMO and LUMO orbits, hence improving the charge carrier separation efficiency and enhancing the formation of H2O2. Importantly, the gas‐liquid‐solid triphase interface system allows for the rapid transport of oxygen from the air to the reaction interface, overcoming the low solubility and slow diffusion of oxygen in the water in conventional liquid reaction systems. The triphase system shows a benchmark H2O2 generation rate over PCN‐based materials in pure water (2063.21 µmol g−1 h−1), which is an approximate tenfold enhancement as compared to powder photocatalyst (215.44 µmol g−1 h−1). Simulation and electrochemical tests reveal that the rapid oxygen diffusion rate of triphase interface can promote charge separation and provide more O2 to generate H2O2. This work provides a promising strategy for constructing an efficient and sustainable H2O2 production system.
Elucidating the Bulk Morphology of Cellulose‐Based Conducting Aerogels with X‐Ray Microtomography
Authors: Oikonomou Vasileios K. , Dreier Till , Sandéhn Alexandra , Mohammadi Mohsen , Christensen Jakob Lønborg , Tybrandt Klas , Dahl Anders Bjorholm , Dahl Vedrana Andersen , Bech Martin , Stavrinidou Eleni 
Published: November 2023

AbstractConducting cellulose composites are promising sustainable functional materials that have found application in energy devices, sensing and water purification. Herein, conducting aerogels are fabricated based on nanofibrillated cellulose and poly(3,4‐ethylenedioxythiophene) polystyrene sulfonate, using the ice templating technique, and their bulk morphology is characterized with X‐ray microtomography. The freezing method (−20 °C in a freezer vs liquid nitrogen) does not impact the mean porosity of the aerogels but the liquid‐N2 aerogels have smaller pores. The integration of carbon fibers as addressing electrodes prior to freezing results in increased mean porosity and pore size in the liquid‐N2 aerogels signifying that the carbon fibers alter the morphology of the aerogels when the freezing is fast. Spatially resolved porosity and pore size distributions also reveal that the liquid‐N2 aerogels are more inhomogeneous. Independent of the freezing method, the aerogels have similar electrochemical properties. For aerogels without carbon fibers, freezer‐aerogels have higher compression modulus and are less stable under cycling compression fatigue test. This can be explained by higher porosity with larger pores in the center of liquid‐N2 aerogels and thinner pore walls. This work demonstrates that micro‐CT is a powerful tool for characterizing the morphology of aerogels in a non‐destructive and spatially resolved manner.
Electrodeposition in Perovskite Solar Cells: A Critical Review, New Insights, and Promising Paths to Future Industrial Applications
Authors: Al‐Katrib Mirella , Perrin Lara , Flandin Lionel , Planes Emilie 
Published: November 2023

AbstractThe active layer quality significantly impacts perovskite solar cell performances. In competition with the common spin, the electrodeposition (ED) method has emerged as a cost‐effective, scalable, and environmentally friendly alternative for perovskite deposition. This article combines an up‐to‐date critical review with experimental results for the development of perovskite photovoltaics. The first review section offers a critical understanding of the current state of the art for the processing of perovskite using an ED step. With the comparison of various methods described in the literature, the pros and cons of the technique are reviewed to assess its applicability at the industrial scale. The second part presents experimental findings from the authors, resulting from a 5‐year experience in this area. Various important and specific topics are covered including the optimization of the ED parameters, the influence of the substrate, the material's selection, the architecture, and the impact on active surface properties. The comparison of the performance data from the literature and the new set of experimental data allows to pace the way for the future development and the integration of stable, affordable, and large‐scale photovoltaics cells.
Flexible a‐IGZO TFT‐Based Circuit for Active Addressing in Neural Stimulation Electrode Arrays
Authors: Rodriguez‐Lopez Ovidio , Rocha‐Flores Pedro E. , Maeng Jimin , Cogan Stuart F. , Pancrazio Joseph J. , Tamil Lakshman , Voit Walter E. , Gutierrez‐Heredia Gerardo 
Published: November 2023

AbstractNeural interfaces have undergone significant advancements in recent decades, aiming for flexible, compact, and high‐density electrode arrays with a large number of channels. However, the scalability of these devices is often hindered by the number of wires needed to separately connect each electrode to external electronics. To address this limitation, thin‐film transistor (TFT)‐based electronic circuits offer a promising solution by enabling active addressing of stimulation electrodes and potentially increasing the channel count with fewer interconnections. This paper presents the integration of a circuit comprising two amorphous indium–gallium–zinc‐oxide (a‐IGZO) TFTs and a titanium nitride (TiN) electrode on a flexible polymer platform. This circuit precisely controls the electrode's On/Off states and the delivery of current for nerve stimulation. Characterization studies involving frequency and electrochemical analysis demonstrate the TFT‐based circuit's capability to operate at high frequencies, deliver biphasic stimulation pulses to the electrode, and store sufficient charge for effective neural stimulation. Moreover, the a‐IGZO TFTs exhibit remarkable stability during repeated gate voltage sweeps with minimal changes in electrical performance. This circuit has the potential to be extended to active‐matrix devices that enable electrode arrays with a high number of channels and enhanced spatial resolution, which is crucial for selective neural stimulation.
Enantioselective Assembly of α, β‐Diamine Acid Derivatives via Three‐Component Reaction of α‐H Diazoacetates with Sulfonamides and Imines
Authors: Sha Hongkai , Xie Xiongda , Zhang Dan , Hu Wenhao , Kang Zhenghui 
Published: November 2023

AbstractAn asymmetric three‐component reaction of α‐H diazoacetate with sulfonamide and imine has been developed under the co‐catalyzation of Rh2(OAc)4 and a chiral phosphoric acid (CPA), which proceed through Mannich‐type interception of transient ammonium ylide. The reaction offers a convenient access to α, β‐diamine acid derivatives with two adjacent chiral centers in 59%‐74% yields with 91%‐99% ee and 92:8 to>95:5 dr. Moreover, the generated products could be easily converted to free chiral diamines and other useful chiral motifs.
Thienoacene‐Based Conjugated Porous Polymer/TiO2 Hybrids as Photocatalysts in Artificial Photosynthesis
Authors: López‐Calixto Carmen G. , Gomez‐Mendoza Miguel , Barawi Mariam , Collado Laura , Liras Marta , de la Peña O´Shea Víctor A. 
Published: November 2023

AbstractHerein, the design and synthesis of a couple of CPPs based on thienoacene units (named as IEP‐14 and IEP‐15, stand for IMDEA Energy Polymer numbers 14 and 15) are described, which show high BET surface areas, good photo(thermal) stabilities, and appropriate electronic alignment with TiO2 to prepare hybrids (named as IEP‐x@T‐10, X = 14 and 15, being 10 wt% of polymer loading). It is shown that the simultaneous UV–vis irradiation of both materials leads to better H2 production (ca. 925 and 827 µmol g−1 h−1 by IEP‐15@T‐10 and IEP‐14@T‐10, 12 and 11‐fold higher production than bare TiO2) than the solely irradiation at visible of the CPPs (ca. 124 and 90 µmol g−1 h−1 by IEP‐15@T‐10 and IEP‐14@T‐10 when TiO2 is photocatalytically inactive). The reason is attributed to the charge‐transfer mechanisms that occur between the counterparts of the hybrid material: in the first case it consists in a Z‐scheme charge transfer mechanism, while in the second one is a sensitization charge transfer mechanism. Both mechanisms are elucidated by advanced techniques. Furthermore, in a gas phase CO2 photoreduction test, IEP‐15@T‐10 shows sixfold higher CH4 evolution than TiO2, which result in a selectivity shift from CO to CH4 (i.e., >26% greater selectivity than bare TiO2).
The Mechanism of Fluorine Doping for the Enhanced Lithium Storage Behavior in Cation‐Disordered Cathode Oxide
Authors: Jiao Sichen , Sun Yujian , Wang Junyang , Shi Dekai , Li Yapei , Jiang Xiangkang , Wang Fangwei , Zhang Yuanpeng , Liu Jue , Wang Xuelong , Yu Xiqian , Li Hong , Chen Liquan , Huang Xuejie 
Published: November 2023

AbstractLi‐rich cation‐disordered rock‐salt (DRX) materials have emerged as promising candidates for high‐capacity oxide cathodes. Their fluorinated variants have shown improved cycling stability with effectively suppressed oxygen loss. However, a comprehensive understanding of how fluorination impacts the multiscale structure and lithium transportation in DRX remains elusive in experiments. Herein, the neutron total scattering technique in conjunction with the advanced reverse Monte Carlo (RMC) fitting method is employed to characterize the intricate structure of Li1.16Ti0.37Ni0.37Nb0.1O2 (LTNNO) and the fluorinated Li1.2Ti0.35Ni0.35Nb0.1O1.8F0.2 (LTNNOF). Through rigorous statistical analysis, the multiscale structural evolution upon fluorination is quantified from atomic (≤5 Å) to long‐range scale (≈100 Å). The local Li‐rich environments around F induce a modest 2.4% increment in the number of fast Li 0TM (transition metal) channels. Crucially, at a broader scale, the proportion of 0TM channels participating in percolation increases significantly from 2.9% in LTNNO to 8.7% in LTNNOF. Fluorination improves the capacity release mainly through merging isolated fast Li channels into the percolation network. This work experimentally unravels the multiscale mechanism of fluorination‐induced performance improvement in DRX materials and highlights the necessity of adopting an advanced RMC fitting method to obtain a full view of the complex structural features in developing high‐capacity DRX cathodes.
High dynamic separation performance of metal–organic frameworks forD2/H2: Independent or competitive adsorption?
Authors: Li Yu , Situ Yizhen , Guan Kexin , Guan Yafang , Huang Xiaoshan , Cai Chengzhi , Li Shuhua , Liu Zili , Liang Hong , Wu Yufang , Yang Qingyuan , Qiao Zhiwei 
Published: November 2023

AbstractMost traditional D2/H2separation techniques are energy‐intensive with low efficiency. Metal–organic frameworks (MOFs) provide a promising solution for D2/H2separation due to their excellent chemical and structural characteristics. Here, machine learning‐assisted high‐throughput computational screening was employed to identify the high‐performance MOFs for the dynamic D2/H2separation. Extensive data analysis reveals that there were two adsorption behaviors in the optimal MOFs, independent adsorption and competitive adsorption, and the independent adsorption was favorable for the preferential adsorption of D2. To quantify these two adsorption behaviors, we introduced and defined overlap degree (OD) and independence degree (ID), and developed a software for the rapid assessment of OD/ID. After batch simulation of the breakthrough curves of 2000 optimal MOFs, ~80% MOFs exhibited independent occupancy, confirming its contribution to good dynamic separation capabilities. This work provides a new idea for designing MOFs with independent adsorption behavior to improve the dynamic separation performance of hydrogen isotopes.
A Proposal for a Low‐Frequency Axion Search in the 1–2 μ$\umu$ eV Range and Below with the BabyIAXO Magnet
Authors: Ahyoune Saiyd , Álvarez Melcón Alejandro , Arguedas Cuendis Sergio , Calatroni Sergio , Cogollos Cristian , Devlin Jack , Díaz‐Morcillo Alejandro , Díez‐Ibáñez David , Döbrich Babette , Galindo Javier , Gallego Juan Daniel , García‐Barceló Jose María , Gimeno Benito , Golm Jessica , Gu Yikun , Herwig Louis , Garcia Irastorza Igor , Lozano‐Guerrero Antonio Jose , Malbrunot Chloé , Miralda‐Escudé Jordi , Monzó‐Cabrera Juan , Navarro Pablo , Navarro‐Madrid Jose Ramón , Redondo Javier , Reina‐Valero José , Schmieden Kristof , Schneemann Tim , Siodlaczek Marc , Ulmer Stefan , Wuensch Walter 
Published: November 2023

AbstractIn the near future BabyIAXO will be the most powerful axion helioscope, relying on a custom‐made magnet of two bores of 70 cm diameter and 10 m long, with a total available magnetic volume of more than 7 m3. In this document, it proposes and describe the implementation of low‐frequency axion haloscope setups suitable for operation inside the BabyIAXO magnet. The RADES proposal has a potential sensitivity to the axion‐photon coupling down to values corresponding to the KSVZ model, in the (currently unexplored) mass range between 1 and 2 eV, after a total effective exposure of 440 days. This mass range is covered by the use of four differently dimensioned 5‐meter‐long cavities, equipped with a tuning mechanism based on inner turning plates. A setup like the one proposed will also allow an exploration of the same mass range for hidden photons coupled to photons. An additional complementary apparatus is proposed using LC circuits and exploring the low energy range ( eV). The setup includes a cryostat and cooling system to cool down the BabyIAXO bore down to about 5 K, as well as an appropriate low‐noise signal amplification and detection chain.
Understanding the Synergy between Fe and Mo Sites in the Nitrate Reduction Reaction on a Bio‐Inspired Bimetallic MXene Electrocatalyst
Authors: Abbott Daniel F. , Xu Yuan‐Zi , Kuznetsov Denis A. , Kumar Priyank , Müller Christoph R. , Fedorov Alexey , Mougel Victor 
Published: November 2023

AbstractMo‐ and Fe‐containing enzymes catalyze the reduction of nitrate and nitrite ions in nature. Inspired by this activity, we study here the nitrate reduction reaction (NO3RR) catalyzed by an Fe‐substituted two‐dimensional molybdenum carbide of the MXene family, viz., Mo2CTx : Fe (Tx are oxo, hydroxy and fluoro surface termination groups). Mo2CTx : Fe contains isolated Fe sites in Mo positions of the host MXene (Mo2CTx) and features a Faradaic efficiency (FE) and an NH3 yield rate of 41 % and 3.2 μmol h−1 mg−1, respectively, for the reduction of NO3− to NH4+ in acidic media and 70 % and 12.9 μmol h−1 mg−1 in neutral media. Regardless of the media, Mo2CTx : Fe outperforms monometallic Mo2CTx owing to a more facile reductive defunctionalization of Tx groups, as evidenced by in situ X‐ray absorption spectroscopy (Mo K‐edge). After surface reduction, a Tx vacancy site binds a nitrate ion that subsequently fills the vacancy site with O* via oxygen transfer. Density function theory calculations provide further evidence that Fe sites promote the formation of surface O vacancies, which are identified as active sites and that function in NO3RR in close analogy to the prevailing mechanism of the natural Mo‐based nitrate reductase enzymes.
Alicyclic‐Amine‐Derived Imine‐BF3 Complexes: Easy‐to‐Make Building Blocks for the Synthesis of Valuable α‐Functionalized Azacycles
Authors: Dutta Subhradeep , Kim Jae Hyun , Bhatt Kamal , Rickertsen Dillon R. L. , Abboud Khalil A. , Ghiviriga Ion , Seidel Daniel 
Published: November 2023

AbstractA new strategy to access α‐functionalized alicyclic amines via their corresponding imine‐BF3 complexes is reported. Isolable imine‐BF3 complexes, readily prepared via dehydrohalogenation of N‐bromoamines in a base‐promoted/18‐crown‐6 catalyzed process followed by addition of boron trifluoride etherate, undergo reactions with a wide range of organometallic nucleophiles to afford α‐functionalized azacycles. Organozinc and organomagnesium nucleophiles add at ambient temperatures, obviating the need for cryogenic conditions. In situ preparation of imine‐BF3 complexes provides access to α‐functionalized morpholines and piperazines directly from their parent amines in a single operation. α‐Functionalized morpholines can be elaborated further, for instance by installing a second substituent in the α′‐position.
Comparing biofilm reactors inoculated with Shewanella for decolorization of Reactive Black 5 using different carrier materials
Authors: Zheng Yumin , Song Haihong , Chen Qianfei , Hou Yayi , Zhang Xinxin , Han Songlei 
Published: November 2023

AbstractThis study assessed the performance of biofilm reactors inoculated with azo dye degrading Shewanella for the decolorization of Reactive Black 5 (RB5), using three different carrier materials, namely almond shell biochar, moving bed biofilm reactor (MBBR), and polypropylene carrier (PPC). The reactors were fed with low‐nutrient artificial wastewater containing RB5, and all three carriers showed good RB5 decolorization performance, with varying efficiencies. Liquid Chromatography‐Mass Spectrometry analysis revealed distinct RB5 degradation pathways associated with each carrier, influenced by carrier materials and microbial communities. The MBBR carrier exhibited good stability due to its rough surface and microbial aggregates. Sequencing results highlighted differences in the microbial community structures among the carriers. Shewanella predominated the functional bacteria in the MBBR and PPC carriers, while the biochar carrier fostered highly efficient degrading microbial communities. The physicochemical properties of carrier materials significantly influenced the microbial community and RB5 degradation efficiency. These findings provide valuable insights for optimizing biofilm reactors for dye‐containing wastewater treatment.