bluuebunny/crossref_metadata_2025 huggingface dataset:
Pre‐Embedded Multisite Chiral Molecules Realize Bottom‐Up Multilayer Manipulation toward Stable and Efficient Perovskite Solar Cells
Authors: Zhou Qian , Liu Baibai , Chen Yu , Ma Danqing , Han Xiao , He Dongmei , Zhang Zhengfu , Yang Hua , Ding Liming , Feng Jing , Yi Jianhong , Chen Cong , Chen Jiangzhao
Published: January 2024

The defects from functional layers and interface, the agglomeration of SnO2 nanoparticles (NPs), and poor perovskite crystallization are the main barrier to further heightening the power conversion efficiency (PCE) and stability of regular perovskite solar cells. Here, a bottom‐up multilayer manipulation strategy by pre‐embedding multisite racemic DL‐cysteine hydrochloride monohydrate (DLCH) into the SnO2 electron transport layer (ETL) is reported. The positively and negatively charged defects from ETL, perovskite layer and their interface can be passivated through the synergistic effect of the ─SH, ─COOH, ─NH3+, and Cl− groups in DLCH. The synergy of multiple functional groups and multiple chemical bonds enables bottom‐up cross‐layer passivation, which minimizes bulk and interfacial nonradiative recombination losses. Furthermore, the multifunctional DLCH plays a role in inhibiting the agglomeration of SnO2 NPs, managing photons, relieving interfacial tensile stress, and manipulating perovskite crystallization. Benefiting from the above advantages, the DLCH‐incorporating device delivers a PCE of 24.01%, which is much higher than the 21.61% of the control device. Moreover, the DLCH‐modified devices demonstrate inviting thermal and ambient stabilities by maintaining 93% of the initial efficiency after aging at 65 °C for 1800 h and 95% of the original PCE after aging under a relative humidity of 20–25% for 2000 h.
Highly Ordered Eutectic Mesostructures via Template‐Directed Solidification within Thermally Engineered Templates
Authors: Kang Sung Bum , Huang Guanglong , Singhal Gaurav , Xie Dajie , Hsieh Daniel H. , Lee Youngmun , Kulkarni Ashish A. , Smith John W. , Chen Qian , Thornton Katsuyo , Sinha Sanjiv , Braun Paul V.
Published: January 2024

Template‐directed self‐assembly of solidifying eutectics results in emergence of unique microstructures due to diffusion constraints and thermal gradients imposed by the template. Here, the importance of selecting the template material based on its conductivity to control heat transfer between the template and the solidifying eutectic, and thus the thermal gradients near the solidification front, is demonstrated. Simulations elucidate the relationship between the thermal properties of the eutectic and template and the resultant microstructure. The overarching finding is that templates with low thermal conductivities are generally advantageous for forming highly organized microstructures. When electrochemically porosified silicon pillars (thermal conductivity < 0.3 Wm−1K−1) are used as the template into which an AgCl‐KCl eutectic is solidified, 99% of the unit cells in the solidified structure exhibit the same pattern. In contrast, when higher thermal conductivity crystalline silicon pillars (≈100 Wm−1K−1) are utilized, the expected pattern is only present in 50% of the unit cells. The thermally engineered template results in mesostructures with tunable optical properties and reflectances nearly identical to the simulated reflectances of perfect structures, indicating highly ordered patterns are formed over large areas. This work highlights the importance of controlling heat flows in template‐directed self‐assembly of eutectics.
Ultraclean Interface of Metal Chalcogenides with Metal through Confined Interfacial Chalcogenization
Authors: Yoo Min Seok , Byun Kyung‐Eun , Lee Hyangsook , Lee Min‐Hyun , Kwon Junyoung , Kim Sang Won , Jeong Unyong , Seol Minsu
Published: January 2024

Acquisition of defect‐free transition metal dichalcogenides (TMDs) channels with clean heterojunctions is a critical issue in the production of TMD‐based functional electronic devices. Conventional approaches have transferred TMD onto a target substrate, and then apply the typical device fabrication processes. Unfortunately, those processes cause physical and chemical defects in the TMD channels. Here, a novel synthetic process of TMD thin films, named confined interfacial chalcogenization (CIC) is proposed. In the proposed synthesis, a uniform TMDlayer is created at the Au/transition metal (TM) interface by diffusion of chalcogen through the upper Au layer and the reaction of chalcogen with the underlying TM. CIC allows for ultraclean heterojunctions with the metals, synthesis of various homo‐ and hetero‐structured TMDs, and in situ TMD channel formation in the last stage of device fabrication. The mechanism of TMD growth is revealed by the TM‐accelerated chalcogen diffusion, epitaxial growth of TMD on Au(111). We demonstrated a wafer‐scale TMD‐based vertical memristors which exhibit excellent statistical concordance in device performance enabled by the ultraclean heterojunctions and superior uniformity in thickness. CIC proposed in this study represents a breakthrough in in TMD‐based electronic device fabrication and marking a substantial step toward practical next‐generation integrated electronics.
Liquid Crystal Elastomer Lattices with Thermally Programmable Deformation via Multi‐Material 3D Printing
Authors: Kotikian Arda , Watkins Audrey A. , Bordiga Giovanni , Spielberg Andrew , Davidson Zoey S. , Bertoldi Katia , Lewis Jennifer A.
Published: January 2024

An integrated design, modeling, and multi‐material 3D printing platform for fabricating liquid crystal elastomer (LCE) lattices in both homogeneous and heterogeneous layouts with spatially programmable nematic director order and local composition is reported. Depending on their compositional topology, these lattices exhibit different reversible shape‐morphing transformations upon cycling above and below their respective nematic‐to‐isotropic transition temperatures. Further, it is shown that there is good agreement between their experimentally observed deformation response and model predictions for all LCE lattice designs evaluated. Lastly, an inverse design model is established and the ability to print LCE lattices with the predicted deformation behavior is demonstrated. This work opens new avenues for creating architected LCE lattices that may find potential application in energy‐dissipating structures, microfluidic pumping, mechanical logic, and soft robotics.
Biphasic GaIn Alloy Constructed Stable Percolation Network in Polymer Composites over Ultrabroad Temperature Region
Authors: Zhou Xinfeng , Liu Yue , Gao Zijie , Min Peng , Liu Ji , Yu Zhong‐Zhen , Nicolosi Valeria , Zhang Hao‐Bin
Published: January 2024

Flexible and adaptable polymer composites with high‐performance reliability over wide temperature range are imperative for various applications. However, the distinct filler‐matrix thermomechanical behaviors often cause severe structure damage and performance degradation upon large thermal shock. To address this issue, a general strategy is proposed to construct leakage‐free, self‐adaptive, stable percolation networks in polymer composites over wide temperature (77–473 K) with biphasic Ga35In65 alloy. The in situ micro‐CT technology, for the first time, reveals the conformable phase transitions of Ga35In65 alloys in the polymer matrix that help repair the disruptive conductive networks over large temperature variations. The cryo‐expanded Ga compensates the disruptive carbon networks at low temperatures, and flowable Ga and melted In at high temperatures conformably fill and repair the deboned interfaces and yielded crevices. As a proof‐of‐concept, this temperature‐resistant composite demonstrates superb electrical conductivity and electromagnetic interference shielding properties and stability even after a large temperature shock (ΔT = 396 K). Furthermore, the superiority of the construction of temperature self‐adaptive networks within the composite enables them for additive manufacturing of application‐oriented components. This work offers helpful inspiration for developing high‐performance polymer composites for extreme‐temperature applications.
Zeolitic Imidazolate‐Framework‐Engineered Heterointerface Catalysis for the Construction of Plant‐Wearable Sensors
Authors: Yan Xu , Ma Yuan , Lu Yang , Su Changshun , Liu Xiaomin , Li Hongxia , Lu Geyu , Sun Peng
Published: January 2024

Plant‐wearable sensors provide real‐time information that enables pesticide inputs to be finely tuned and play critical roles in precision agriculture. However, tracking pesticide information in living plants remains a formidable challenge owing to inadequate shape adaptabilities and low in‐field sensor sensitivities. In this study, plant‐wearable hydrogel discs are designed by embedding a dual‐shelled upconversion‐nanoparticles@zeolitic‐imidazolate‐framework@polydopamine (UCNPs@ZIF@PDA) composite in double‐network hydrogels to deliver on‐site pesticide‐residue information. Benefiting from the enzyme‐mimetic catalytic activity of ZIFs and enzyme triggered‐responsive property of PDA shell, the hydrogel discs are endowed with high sensing sensitivity toward 2,4‐dichlorophenoxyacetic acid pesticide at the nanogram per milliliter level via boosting fluorescence quenching efficiency. Notably, hydrogel discs mounted on tomato plants exhibit sufficient adaptability to profile dynamic pesticide degradation when used in conjunction with an ImageJ processing algorithm, which is practically applicable. Such hydrogel discs form a noninvasive and low‐cost toolkit for the on‐site acquisition of pesticide information, thereby contributing to the precise management of the health status of a plant and the judicious development of precision agriculture.
Highly Efficient Monolithic Perovskite/Perovskite/Silicon Triple‐Junction Solar Cells
Authors: Li Faming , Wu Dan , Shang Le , Xia Rui , Zhang Hengrui , Huang Zhengxin , Gong Jue , Mao Lin , Zhang Hao , Sun Yinqing , Yang Tian , Sun Xianggang , Feng Zhiqiang , Liu Mingzhen
Published: January 2024

Wide‐bandgap metal halide perovskites have demonstrated promise in multijunction photovoltaic (PV) cells. However, photoinduced phase segregation and the resultant low open‐circuit voltage (Voc) have greatly limited the PV performance of perovskite‐based multijunction devices. Here, a alloying strategy is reported to achieve uniform distribution of triple cations and halides in wide‐bandgap perovskites by doping Rb+ and Cl− with small ionic radii, which effectively suppresses halide phase segregation while promoting the homogenization of surface potential. Based on this strategy, a Voc of 1.33 V is obtained from single‐junction perovskite solar cells, and a VOC approaching 3.0 V and a power conversion efficiency of 25.0% (obtained from reverse scan direction, certified efficiency: 24.19%) on an 1.04 cm2 photoactive area can be achieved in a perovskite/perovskite/c‐Si triple‐junction tandem cell, where the certification efficiency is by far the greatest performance of perovskite‐based triple‐junction tandem solar cells. This work overcomes the performance deadlock of perovskite‐based triple‐junction tandem cells by setting a materials‐by‐design paradigm.
One‐Step Electrochemical Synthesis of Multiyolk–Shell Nanocoils for Exceptional Photocatalytic Performance
Authors: Moon Jun Hwan , Oh Eunsoo , Koo Thomas Myeongseok , Jeon Yoo Sang , Jang Young Jun , Fu Hong En , Ko Min Jun , Kim Young Keun
Published: January 2024

Multiyolk–shell (mYS) nanostructures have garnered significant interest in various photocatalysis applications such as water splitting and waste treatment. Nonetheless, the complexity and rigorous conditions for the synthesis have hindered their widespread implementation. This study presents a one‐step electrochemical strategy for synthesizing multiyolk–shell nanocoils (mYSNC), wherein multiple cores of noble metal nanoparticles, such as Au, are embedded within the hollow coil‐shaped FePO4 shell structures, mitigating the challenges posed by conventional methods. By capitalizing on the dissimilar dissolution rates of bimetallic alloy nanocoils in an electrochemically programmed solution, nanocoils of different shapes and materials, including two variations of mYSNCs are successfully fabricated. The resulting Au‐FePO4 mYSNCs exhibit exceptional photocatalytic performance for environmental remediation, demonstrating up to 99% degradation of methylene blue molecules within 50 min and 95% degradation of tetracycline within 100 min under ultraviolet–visible (UV‐vis) light source. This remarkable performance can be attributed to the abundant electrochemical active sites, internal voids facilitating efficient light harvesting with coil morphology, amplified localized surface plasmon resonance (LSPR) at the plasmonic nanoparticle‐semiconductor interface, and effective band engineering. The innovative approach utilizing bimetallic alloys demonstrates precise geometric control and design of intricate multicomponent hybrid composites, showcasing the potential for developing versatile hollow nanomaterials for catalytic applications.
Whole‐Cell Electrochemical Aptasensors for Cancer Diagnosis: Current Advances and Prospects
Authors: Putri Athika Darumas , Murti Bayu Tri , Manga Yankuba B. , Kanchi Suvardhan , Huang Yi‐June , Peng Chih‐Wei , Yang Po‐Kang , Hsieh Chien‐Ming
Published: January 2024

Cancer is one of the most life‐threatening diseases worldwide. Numerous diagnostic and therapeutic techniques, such as nanomaterials‐based cancer detection and imaging‐guided focal therapy, are successfully developed to achieve highly precise cancer theranostic strategies. However, due to unpredictive alterations occurring in cancer cell morphology, a lack of sensitivity and selectivity is a critical challenge among most biomarkers’ detection. To address this issue, instead of targeting proteins or biomarkers, the detection of cancer using whole cell‐based biosensors are ubiquitously discovered through a selective oligonucleotide, so‐called aptamer. Aptamer‐based whole‐cell detection is concurrently engaged with various nanomaterials, such as magnetic beads, gold (Au) nanoparticles, and graphene family to establish a better performance of the biosensor. In this research review, the recent strategies and prospects on whole‐cell cancer detection platform based on electrochemical aptasensors integrated with nanomaterials are thoroughly discussed and summarized. Finally, future challenges and prospects are also provided.
Programmable Electro‐Assembly of Collagen: Constructing Porous Janus Films with Customized Dual Signals for Immunomodulation and Tissue Regeneration in Periodontitis Treatment
Authors: Lei Miao , Wan Haoran , Song Jia , Lu Yanhui , Chang Ronghang , Wang Honglei , Zhou Hang , Zhang Xuehui , Liu Changsheng , Qu Xue
Published: January 2024

Currently available guided bone regeneration (GBR) films lack active immunomodulation and sufficient osteogenic ability‐ in the treatment of periodontitis, leading to unsatisfactory treatment outcomes. Challenges remain in developing simple, rapid, and programmable manufacturing methods for constructing bioactive GBR films with tailored biofunctional compositions and microstructures. Herein, the controlled electroassembly of collagen under the salt effect is reported, which enables the construction of porous films with precisely tunable porous structures (i.e., porosity and pore size). In particular, bioactive salt species such as the anti‐inflammatory drug diclofenac sodium (DS) can induce and customize porous structures while enabling the loading of bioactive salts and their gradual release. Sequential electro‐assembly under pre‐programmed salt conditions enables the manufacture of a Janus composite film with a dense and DS‐containing porous layer capable of multiple functions in periodontitis treatment, which provides mechanical support, guides fibrous tissue growth, and acts as a barrier preventing its penetration into bone defects. The DS‐containing porous layer delivers dual bio‐signals through its morphology and the released DS, inhibiting inflammation and promoting osteogenesis. Overall, this study demonstrates the potential of electrofabrication as a customized manufacturing platform for the programmable assembly of collagen for tailored functions to adapt to specific needs in regenerative medicine.
Construction of a 2D/2D Crystalline Porous Materials Based S‐Scheme Heterojunction for Efficient Photocatalytic H2 Production
Authors: Hu Haijun , Zhang Xinyu , Zhang Kailai , Ma Yali , Wang Haitang , Li Hui , Huang Hongwei , Sun Xiaodong , Ma Tianyi
Published: January 2024

Generally, the low electron–hole separation efficiency of covalent organic frameworks (COFs) prevents their catalytic performance from reaching satisfactory results. For this reason, the creation of heterojunctions is considered an effective strategy but usually suffers from dimensional mismatch of the integrated material, even at the expense of its redox capacity. To overcome these difficulties, a novel 2D/2D S‐scheme heterojunction between H2N–Cu–MOF (NCM) and TpPa–1–COF (TP1C) is successfully constructed for efficient photocatalytic H2 production. The matching dimensions of two crystalline porous materials enables the integrated materials with abundant surface reactive sites, strong interaction and optimized electronic structure. Moreover, the combination of two crystalline porous materials can also form a S–scheme heterojunction, which can not only promote the separation of electron–hole pair, but also preserve the redox ability, thus remarkably boosting the catalytic competence. Consequently, the rate of optimal 20% NCM/TP1C in photocatalytic H2 production reaches 4.19 mmol g−1 h−1, which is 46.5 times higher than that of bare NCM, and 22.1 folds over that of pure TP1C. This research offers an innovative perspective for the formation of S–scheme heterojunctions based on porous crystal materials for efficient solar energy utilization.
Bioinformatics procedure for investigating senolytic (anti‐aging) agents: A digital signal processing technique
Authors: Nwankwo Norbert , Okafor Ignatius
Published: January 2024

Objective

Cell growth involves cell division. This stops after reaching a certain limit. Some cells become inactive and unable to undergo apoptosis (programmed cell death). These cells accumulate at sites of tissue damage or disease, thus accelerating aging. They are called senescent cells. Therapeutic interventions that can either eliminate senescent cells (senolytics) or suppress their harmful effects (senomorphics) have been developed. Senescence (aging) is caused by the inter‐ and intramolecular interactions between the domains of forkhead (FHD) and transactivation (TAD), as well as C‐terminal region 3 (CR3) and DNA binding (DBD). On the other hand, anti‐senescent/senolytic (anti‐aging) activities are achieved by disrupting these interactions with CR3‐ and forkhead box protein O4 (FOXO4)‐based peptides, such as ES2 and DRI, respectively. In this study, we use a computerized procedure based on digital signal processing to systematically analyze the inter‐molecular interactions between senolytics and their targets.

Methods

Informational spectrum method (ISM) is engaged.

Results

We obtained the sequences of the peptides from the interacting proteins of CR3 and FOXO4 and evaluated their ability to disrupt the inter‐molecular interactions between FOXO4 and DRI and CR3 and BDB, which are responsible for senescence (aging). Our results show that the peptides have different degrees of senolytic (anti‐aging) activity, depending on their affinity for CR3 and BDB, or FOXO4 and DRI. We found that enhanced senescence 2 (ES2) has a higher affinity for CR3 and BDB than FOXO4 and DRI, and that the interaction between CR3 and BDB is crucial for aging. Therefore, ES2 and other CR3‐based peptides are more potent senolytics than FOXO4‐based peptides. Our findings are consistent with previous studies and reveal new insights into the mechanisms of senescence and senolytics. ES2 is considered the best senolytic candidate, as it is 3–7 times more effective than DRI. We verified that ES2 has a weaker interaction with FOXO4 than CR3. However, the performance of DRI has been noted to depend on its intramolecular interactions and stability. Hence, intramolecular analyses using the digital signal processing‐based technique has become very vital and will follow.

Conclusion

CR3‐based peptides are promising candidates for senolytic therapy. Senolytics are linear chains of amino acids that can target and eliminate senescent cells, which are cells that have stopped dividing and contribute to aging and age‐related diseases. By using this proposed, novel computerized technique that is based on digital signal processing, senolytics can be easily analyzed and optimized for their effectiveness and safety. This provides a more rational approach to enhancing our longevity and well‐being by offering interventions that can delay or reverse aging and insights that can advance the field of gerontology. This procedure also will compliment other approaches such as molecular stimulation, etc.
Dual‐Stream Fusion and Multi‐scale Analysis: Introducing the Synergistic Dual‐Stream Network (SDS‐Net) for Image Manipulation Segmentation
Authors: Song HuaQing , Lin BaiChuan , Xie LanChi
Published: January 2024

This article introduces the synergistic dual‐stream network (SDS‐Net), a novel neural network architecture that significantly enhances the detection of image manipulations. SDS‐Net employs a unique dual‐stream fusion strategy that processes both RGB image and the corresponding noise map. It innovatively combines features computation from the different blocks of dual backbones, and leverages a multi‐scale spatial pyramid pooling (MSPP) module to expand the receptive fields of shallow features. This approach not only enriches the feature representation, but also ensures the precise localization of manipulated regions. Extensive experiments conducted on various public datasets demonstrate the superiority of SDS‐Net over several state‐of‐the‐art methods.
A Double‐ligand Chelating Strategy to Iron Complex Anolytes with Ultrahigh Cyclability for Aqueous Iron Flow Batteries
Authors: Wang Shaocong , Ma Long , Niu Shiyang , Sun Shibo , Liu Yong , Cheng Yuanhui
Published: January 2024

Aqueous all‐iron flow batteries (AIFBs) are attractive for large‐scale and long‐term energy storage due to their extremely low cost and safety features. To accelerate commercial application, a long cyclable and reversible iron anolyte is expected to address the critical barriers, namely iron dendrite growth and hydrogen evolution reaction (HER). Herein, we report a robust iron complex with triethanolamine (TEA) and 2‐methylimidazole (MM) double ligands. By introducing two ligands into one iron center, the binding energy of the complex increases, making it more stable in the charge‐discharge reactions. The Fe(TEA)MM complex achieves reversible and stable redox between Fe3+ and Fe2+, without metallic iron growth and HER. AIFBs based on this anolyte perform a high energy efficiency of 80.5 % at 80 mA cm−2 and exhibit a record durability among reported AIFBs. The efficiency and capacity retain nearly 100 % after 1,400 cycles. The capital cost of this AIFB is $ 33.2 kWh−1 (e.g., 20 h duration), cheaper than Li‐ion battery and vanadium flow battery. This double‐ligand chelating strategy not only solves the current problems faced by AIFBs, but also provides an insight for further improving the cycling stability of other flow batteries.
Photoredox‐Catalyzed Generation of Tertiary Anions from Primary Amines via a Radical Polar Crossover
Authors: Marchese Austin D. , Dorsheimer Julia R. , Rovis Tomislav
Published: January 2024

A method for the generation of tertiary carbanions via a deaminative radical‐polar crossover is reported using redox active imines from α‐tertiary primary amines. A variety of benzylic amines and amino esters can be used in this approach, with the latter engaging in a novel “aza‐Reformatsky” reaction. Electronic trends correlate the stability of the resulting carbanion with reaction efficiency. The anions can be trapped with different electrophiles including aldehydes, ketones, imines, Michael acceptors, and H2O/D2O. Selective anion formation can be achieved in the presence of another equivalent or more acidic C−H bond in both an inter‐ and intramolecular fashion. Mechanistic studies suggest the intermediacy of a discrete carbanion intermediate.
Emerging two dimensional metastable‐phase oxides: insights and prospects in synthesis and catalysis
Authors: Su Jiaqi , Huang Xiaoqing , Shao Qi
Published: January 2024

Since the discovery of graphene, the development of new two‐dimensional (2D) materials has received considerable interest. Recently, as a newly emerging member of the 2D family, 2D metastable‐phase oxides that combine the unique advantages of metal oxides, 2D structures, and metastable‐phase materials have shown enormous potential in various catalytic reactions. In this review, the potential of various 2D materials to form a metastable‐phase is predicted. The advantages of 2D metastable‐phase oxides for advanced applications, reliable methods of synthesizing 2D metastable‐phase oxides, and the application of these oxides in different catalytic reactions are presented. Finally, the challenges associated with 2D metastable‐phase oxides and future perspectives are discussed.
Guest‐Shuttling in a Nanosized Metallobox
Authors: Ibáñez Susana , Salvà Paula , Dawe Louise N. , Peris Eduardo
Published: January 2024

An iridium‐conjoined long and narrow metallorectangle was obtained by combining a quinoxalinophenanthrophenazine‐connected Janus‐di‐imidazolylidene ligand and pyrazine. The size and shape of this assembly together with the fused polyaromatic nature of its panels provides it with properties that are uncommon for other metallosupramolecular assemblies. For example, this nanosized ‘slit‐like’ metallobox is able show very large binding affinities with planar organic molecules in such a way, that the cavity is asymmetrically occupied by the guest molecule. This unsymmetrical conformation leads to the existence of a large amplitude motion of these guests, which slide between the two sides of the cavity of the host, thus constituting rare examples of molecular shuttles.
A Sulfur‐Doped Copper Catalyst with Efficient Electrocatalytic Formate Generation during the Electrochemical Carbon Dioxide Reduction Reaction
Authors: Wang Yinuo , Xu Hongming , Liu Yushen , Jang Juhee , Qiu Xiaoyi , Delmo Ernest P. , Zhao Qinglan , Gao Ping , Shao Minhua
Published: January 2024

Catalysts involving post‐transition metals have shown almost invincible performance on generating formate in electrochemical CO2 reduction reaction (CO2RR). Conversely, Cu without post‐transition metals has struggled to achieve comparable activity. In this study, a sulfur (S)‐doped‐copper (Cu)‐based catalyst is developed, exhibiting excellent performance in formate generation with a maximum Faradaic efficiency of 92 % and a partial current density of 321 mA cm−2. Ex situ structural elucidations reveal the presence of abundant grain boundaries and high retention of S−S bonds from the covellite phase during CO2RR. Furthermore, thermodynamic calculations demonstrate that S−S bonds can moderate the binding energies with various intermediates, further improving the activity of the formate pathway. This work is significant in modifying a low‐cost catalyst (Cu) with a non‐metallic element (S) to achieve comparable performance to mainstream catalysts for formate generation in industrial grade.
Engineering Tunable Ratiometric Dual Emission in Single Emitter‐based Amorphous Systems
Authors: Sun Hao , He Menglu , Baryshnikov Glib V. , Wu Bin , Valiev Rashid R. , Shen Shen , Zhang Man , Xu Xiaoyan , Li Zhongyu , Liu Guofeng , Ågren Hans , Zhu Liangliang
Published: January 2024

Molecular emitters with multi‐emissive properties are in high demand in numerous fields, while these properties basically depend on specific molecular conformation and packing. For amorphous systems, special molecular arrangement is unnecessary, but it remains challenging to achieve such luminescent behaviors. Herein, we present a general strategy that takes advantage of molecular rigidity and S1‐T1 energy gap balance for emitter design, which enables fluorescence–phosphorescence dual‐emission properties in various solid forms, whether crystalline or amorphous. Subsequently, the amorphism of the emitters based polymethyl methacrylate films endowed an in situ regulation of the dual‐emissive characteristics. With the ratiometric regulation of phosphorescence by external stimuli and stable fluorescence as internal reference, highly controllable luminescent color tuning (yellow to blue including white emission) was achieved. There properties together with a persistent luminous behavior is of benefit for an irreplaceable set of optical information combination, featuring an ultrahigh‐security anti‐counterfeiting ability. Our research introduces a concept of eliminating the crystal‐form and molecular‐conformational dependence of complex luminescent properties through emitter molecular design. This has profound implications for the development of functional materials.
Toward Simultaneous Dense Zinc Deposition and Broken Side‐Reaction Loops in the Zn//V2O5 System
Authors: Wang Huirong , Zhou Anbin , Hu Zhengqiang , Hu Xin , Zhang Fengling , Song Zhihang , Huang Yongxin , Cui Yanhua , Cui Yixiu , Li Li , Wu Feng , Chen Renjie
Published: January 2024

The Zn//V2O5 system not only faces the incontrollable growth of zinc (Zn) dendrites, but also withstands the cross‐talk effect of by‐products produced from the cathode side to the Zn anode, inducing interelectrode talk and aggravating battery failure. To tackle these issues, we construct a rapid Zn2+‐conducting hydrogel electrolyte (R‐ZSO) to achieve Zn deposition modulation and side reaction inhibition in Zn//V2O5 full cells. The polymer matrix and BN exhibit a robust anchoring effect on SO42−, accelerating Zn2+ migration and enabling dense Zn deposition behavior. Therefore, the Zn//Zn symmetric cells based on the R‐ZSO electrolyte can operate stably for more than 1500 h, which is six times higher than that of cells employing the blank electrolyte. More importantly, the R‐ZSO hydrogel electrolyte effectively decouples the cross‐talk effects, thus breaking the infinite loop of side reactions. As a result, the Zn//V2O5 cells using this modified hydrogel electrolyte demonstrate stable operation over 1,000 cycles, with a capacity loss rate of only 0.028 % per cycle. Our study provides a promising gel chemistry, which offers a valuable guide for the construction of high‐performance and multifunctional aqueous Zn‐ion batteries.
Identification of Cu(111) as Superior Active Sites for Electrocatalytic NO Reduction to NH3 with High Single‐Pass Conversion Efficiency
Authors: Xiao Lei , Mou Shiyong , Dai Weidong , Yang Weiping , Cheng Qin , Liu Siyuan , Dong Fan
Published: January 2024

Opting for NO as an N source in electrocatalytic NH3 synthesis presents an intriguing approach to tackle energy and environmental challenges. However, blindly pursuing high NH3 synthesis rates and Faradaic efficiency (FE) while ignoring the NO conversion ratio could result in environmental problems. Herein, Cu nanosheets with exposed (111) surface is fabricated and exhibit a NO‐to‐NH3 yield rate of 371.89 μmol cm−2 h−1 (flow cell) and the highest FE of 93.19±1.99 % (H‐type cell). The NO conversion ratio is increased to the current highest value of 63.74 % combined with the development of the flow cell. Additionally, Crystal Orbital Hamilton Population (COHP) clearly reveals that the “σ‐π* acceptance‐donation” is the essence of the interaction between the Cu and NO as also supported by operando attenuated total reflection infrared spectroscopy (ATR‐IRAS) in observing the key intermediate of NO−. This work not only achieves a milestone NO conversion ratio for electrocatalytic NO‐to‐NH3, but also proposes a new descriptor that utilizes orbital hybridization between molecules and metal centers to accurately identify the real active sites of catalysts.
In situ Light‐Writable Orientation Control in Liquid Crystal Elastomer Film Enabled by Chalcones
Authors: Xu Yiyi , Zhang Xinfang , Song Zhenpeng , Chen Xiao , Huang Yinliang , Wang Jinyu , Li Bingxiang , Huang Shuai , Li Quan
Published: January 2024

Liquid crystal elastomers (LCEs) are stimulus‐responsive materials with intrinsic anisotropy. However, it is still challenging to in situ program the mesogen alignment to realize three‐dimensional (3D) deformations with high‐resolution patterned structures. This work presents a feasible strategy to program the anisotropy of LCEs by using chalcone mesogens that can undergo a photoinduced cycloaddition reaction under linear polarized light. It is shown that by controlling the polarization director and the irradiation region, patterned alignment distribution in a freestanding LCE film can be created, which leads to complex and reversible 3D shape‐morphing behaviors. The work demonstrates an in situ light‐writing method to achieve sophisticated topography changes in LCEs, which has potential applications in encryption, sensors, and beyond.
Design, preparation, physicochemical characterization, structural conformational, biological evaluation, and DNA interaction for some new benzimidazole complexes
Authors: Abu‐Dief Ahmed M. , El‐Khatib Rafat M. , El‐Dabea Tarek , Feizi‐Dehnayebi Mehran , Barnawi Ibrahim Omar , Alsehli Amal H. , Al‐Ghamdi Khalaf , El‐Remaily Mahmoud Abd El Aleem Ali Ali
Published: January 2024

New Cu (II), VO (II), Ag(I), and Pd (II)‐[BIP = 4,6‐dimethyl‐N‐(octahydro‐2H‐benzimidazol‐2‐ylidene)pyrimidin‐2‐amine] chelates have been synthesized by the reaction of BIP ligand resulting from the condensation of benzimidazole guanidine as well as acetylacetone with tested metal salts. The suggested structures of prepared compounds have been investigated spectroscopically through (FT‐IR, NMR, Mass spectra, and UV–Vis spectra), CHN analyses, conductivity, pH stability as well asmagnetic moment measurements. TGA studies have been also studied to govern the thermal behavior, stability, and decomposition of the metal chelates. Structural study of the tested chelates exposed their chemical transformation of ligand by chelation with the studied metals. The studies predicted a hexa‐coordinated geometry for the Cu and VO chelates, whereas tetra‐coordinated for the Ag and Pd chelates. DFT/B3LYP theoretical method was applied to obtain optimized geometry, molecular electrostatic potential (MEP) surface, and HOMO‐LUMO analysis for tested compounds. For estimation in the in vitro study, all the tested compounds have been screened for their biochemical features, including antioxidant, antimicrobial performances, and cytotoxicity. The antioxidant performance of prepared molecules has been studied by DPPH study and all the tested chelates displayed close antioxidant performance against the standard drugs. The cytotoxic analysis of tested compounds has been estimated against various cancer cell lines: (Hep‐G2, HCT‐116, and MCF‐7) using MTT analysis as well as calculated the cell viability for the corresponding human cell. The DNA binding capability for the tested compounds has been evaluated through absorption spectroscopic, viscosity estimation, as well as gel electrophoresis. The outcomes displayed a good binding tendency through the binding constant from 1.01 × 104to 1.99 × 104 M−1in the order BIPCu> BIPVO > BIPPd > BIPAg, respectively. Finally, docking simulation results indicated that the complexes were located in the intercalation site of DNA and confirmed experimental findings.
Study on the combination of the annular jet pump and static mixer to improve the fluid‐carrying capacity of gas wells
Authors: Liang Huizhen , Li Chengzhen , Ma Jian , Mu Lin
Published: January 2024

Aiming at the problem that the suction chamber of the gas‐driven jet pump has insufficient mixing of the power gas and the sucked fluid leading to efficiency reduction, this study proposes to effectively combine the static mixer with the annular jet pump and design a new type of annular jet pump and apply it to the gas wells to improve the fluid recovery capacity. Numerical simulations based on the gas–liquid two‐phase flow model are carried out for a conventional annular jet pump (CAJP) and a new annular jet pump (NAJP). The reliability of the simulation results is verified by gas–liquid two‐phase flow experiments, and the differences between the two in terms of velocity, pressure loss, and turbulent kinetic energy are analyzed. Meanwhile, the validity of NAJP is verified, and the effects of different structures such as static mixer torsion angle, suction chamber angle, and area ratio on the performance of NAJP are analyzed. The results show that NAJP enhances the degree of mixing between the sucked fluid and the power gas through the cyclonic effect created by the static mixer compared with CAJP. It results in a 10.6% year‐on‐year increase in the velocity of the sucked fluid, a 3% year‐on‐year increase in the pressure drop, and a 12.2% year‐on‐year increase in efficiency. NAJP can significantly improve the fluid‐carrying performance. With a mixer angle of 210°, a suction chamber angle of 21°, and an area ratio of 1.77, the NAJP achieves an efficiency of 39.7%, which is a year‐on‐year increase of 7.3% compared to the structure under the same conditions before optimization. This study lays a foundation for the determination of the optimal design scheme of the annular jet pump and at the same time can provide theoretical and technical support for researchers in related fields.
Structure‐guided design of potent JAK1‐selective inhibitors based on 4‐amino‐7H‐pyrrolo[2,3‐d]pyrimidine with anti‐inflammatory efficacy
Authors: Zhang Jiahao , Xing Shuming , Cui Jianming , Wei Xiujian , Cao Zhi , Shao Bin , Jiang Nan , Zhai Xin
Published: January 2024

In a continuous effort to develop Janus kinase 1 (JAK1)‐selective inhibitors, a novel series of 4‐amino‐7H‐pyrrolo[2,3‐d]pyrimidine derivatives bearing the piperidinyl fragment were designed and synthesized according to a combination strategy. Through enzymatic assessments, the superior compound 12a with an IC50 value of 12.6 nM against JAK1 was identified and a 10.7‐fold selectivity index over JAK2 was achieved. It was indicated that 12a displayed considerable effect in inhibiting the pro‐inflammatory NO generated from lipopolysaccharide (LPS)‐induced RAW264.7 macrophages, while on normal RAW264.7 cells, 12a exerted a weak cytotoxicity effect (IC50 = 143.3 μM). Furthermore, H&E stain assay demonstrated the conspicuous capacity of 12a to suppress CCl4‐induced hepatic fibrosis levels in a dose‐dependent manner in vivo. The binding model of 12a ideally reflects the excellent activity of JAK1 over the homologous kinase JAK2. Overall, 12a, a JAK1‐selective inhibitor, exhibited potential for liver fibrosis and inflammatory diseases.
A comprehensive stem cell laboratory module with blended learning for medical students at Tongji University
Authors: Xu Jie , Shao Zhihua , Jia Song , Sha Jihong , Li Jiao , Gao Furong , Shi Xiujuan , Wang Juan , Jin Caixia , Jiang Mei , Tian Haibin , Cao Jinfeng , Pu Hu , Xu Lei , Lu Lixia
Published: January 2024

The laboratory practice “Primary culture and directional differentiation of rat bone marrow mesenchymal stem cells (BMSCs)” is part of a required course for sophomore medical students at Tongji university, which has been conducted since 2012. Blended learning has been widely applied in medical courses. Based on a student‐centered teaching philosophy, we reconstructed a comprehensive stem cell laboratory module with blended learning in 2021, aiming to facilitate students in enhancing their understanding of the multi‐lineage differentiation potential of stem cells and improve their experimental skills, self‐directed learning ability, and innovative thinking. First, we constructed in‐depth online study resources, including videos demonstrating laboratory procedures, a PowerPoint slide deck, and published literature on student self‐learning before class. In class, students performed a primary culture of BMSCs, freely chose among adipogenic, osteogenic, or chondrogenic differentiation, and used cytochemical or immunofluorescence staining for identification. After class, the extracurricular part involved performing quantitative polymerase chain reaction to examine the expression of multi‐lineage differentiation marker genes, which was designed as an elective. After 2 years of practice, positive feedback was obtained from both students and faculty members who achieved, the learning goal as expected. The reconstructed stem cell laboratory module provides comprehensive practice opportunities for students. Students have a better understanding of BMSC at the molecular, cellular, and functional levels and have improved their experimental skills, which forms a basis for scientific research for medical students. Introducing blended learning into other medical laboratory practices thus seems valuable.
The value of an MRI‐based radiomics model in predicting the survival and prognosis of patients with extrahepatic cholangiocarcinoma
Authors: Wang Limin , Liu Jiong , Zeng Yanyan , Shu Jian
Published: January 2024

Objectives

The study aimed to establish radiomics models based on magnetic resonance imaging (MRI) multiparameter images to predict the survival and prognosis of patients with extrahepatic cholangiocarcinoma (ECC).

Methods

Seventy‐eight patients with ECC confirmed by pathology were collected retrospectively. The radiomics model_a/b/c were constructed based on the 1/2/3‐year survival of patients with ECC. The best texture features were selected according to postoperative survival time and ECC patient status to calculate the radiomics score (Rad‐score). A cutoff value was selected, and patients were divided into high‐risk and low‐risk groups.

Results

Model_a, model_b, and model_c were used to predict 1‐, 2‐, and 3‐year postoperative survival rates, respectively. The area under the curve values in the training and test groups were 1.000 and 0.933 for model_a, 0.909 and 0.907 for model_b, 1.000 and 0.975 for model_c, respectively. The survival prediction model based on the Rad‐score showed that the postoperative mortality risk differed significantly between risk groups (p < 0.0001).

Conclusions

The MRI radiomics model could be used to predict the survival and prognosis of patients with ECC.
Bone mineral density fall during aromatase inhibitor treatment may predict lower breast cancer recurrence
Authors: Martin Hilary , Redfern Andrew
Published: January 2024

Purpose

Aromatase inhibitors (AIs) are associated with reduction in bone mineral density (BMD). The use of bone strengthening agents zoledronic acid and denosumab are associated with improved breast cancer outcomes for post‐menopausal patients treated with AIs. This study investigates whether change in BMD with AI therapy is associated with breast cancer recurrence.

Methods

A cohort of patients treated at a single institution diagnosed with hormone receptor‐positive breast cancer with baseline BMD and subsequent BMD test while receiving adjuvant aromatase inhibitor therapy were studied. Demographic, treatment and outcome data was obtained. Simple and multiple linear regression analysis was performed to investigate predictors of annual percent BMD change at the LS and hip. Univariate and multivariate Cox proportional hazards modelling were undertaken to investigate predictors of breast cancer recurrence.

Results

353 patients eligible patients were identified. In multivariate analysis of lumbar spine BMD change, the difference between those in quartile 1, which showed the greatest reduction in BMD, and quartile 3, with substantially less reduction, was significant (HR = 3.02, 95% CI 1.15–7.90 p = 0.025). Hip BMD reduction was also not significantly associated with breast cancer recurrence. The two quartiles with the least reduction in hip BMD showing a non‐significant reduced risk of recurrence relative to the quartile with the greatest (p = 0.10).

Conclusions

The findings suggest an association may exist between lumbar spine BMD change and breast cancer recurrence for patients treated with adjuvant AI. Further research is required to determine whether BMD change can be utilised as a biomarker.
A study of machine learning models for rapid intraoperative diagnosis of thyroid nodules for clinical practice in China
Authors: Ma Yan , Zhang Xiuming , Yi Zhongliang , Ding Liya , Cai Bojun , Jiang Zhinong , Liu Wangwang , Zou Hong , Wang Xiaomei , Fu Guoxiang
Published: January 2024

Background

In China, rapid intraoperative diagnosis of frozen sections of thyroid nodules is used to guide surgery. However, the lack of subspecialty pathologists and delayed diagnoses are challenges in clinical treatment. This study aimed to develop novel diagnostic approaches to increase diagnostic effectiveness.

Methods

Artificial intelligence and machine learning techniques were used to automatically diagnose histopathological slides. AI‐based models were trained with annotations and selected as efficientnetV2‐b0 from multi‐set experiments.

Results

On 191 test slides, the proposed method predicted benign and malignant categories with a sensitivity of 72.65%, specificity of 100.0%, and AUC of 86.32%. For the subtype diagnosis, the best AUC was 99.46% for medullary thyroid cancer with an average of 237.6 s per slide.

Conclusions

Within our testing dataset, the proposed method accurately diagnosed the thyroid nodules during surgery.
Cost‐effectiveness analysis of continuing bevacizumab plus chemotherapy versus chemotherapy alone after first progression of metastatic colorectal cancer
Authors: Li Yulian , Hu Min , Zhang Zhe , Chu Mingming , Xu Rufu , Liu Lulu , Dong Wenxing , Yang Mengmeng , Zhang Rong
Published: January 2024

Background

Continuation of bevacizumab plus second‐line chemotherapy has significantly improved overall and progression‐free survival in patients with metastatic colorectal cancer (mCRC). However, the cost‐effectiveness of such high cost therapy is still uncertain in China; so this analysis was performed to evaluate the cost‐effectiveness of these treatment options from the Chinese health care system perspective.

Methods

A cost‐effectiveness analysis was conducted using data from the ML18147 trial (ClinicalTrials.gov identifier NCT00700102) by modeling a partitioned survival model. Main evaluation indicators were quality‐adjusted life years (QALYs) and incremental cost‐effectiveness ratio (ICER) with a willingness to pay (WTP) threshold of $38,201 per QALY. One‐way and probabilistic sensitivity analyses were conducted to assess the robustness and stability of the model. Subgroup and scenario analyses were also performed to make our study more relevant.

Results

Bevacizumab plus chemotherapy increased 0.12 QALYs and an incremental cost of $22,761.62 compared with chemotherapy, resulting in an ICER of $188,904.09 per QALY. The model was most sensitive to the utility of progression‐free survival and the cost of bevacizumab. Compared with chemotherapy, bevacizumab plus chemotherapy had a 0% cost‐effectiveness probability, and no cost‐effectiveness in subgroups at the WTP threshold of $38,201 per QALY. The scenario analysis found that bevacizumab biosimilar gained an ICER of $126,397.38 per QALY when assuming the cost of drugs was calculated at the most affordable price.

Conclusions

At the WTP threshold of $38,201 per QALY, continuation of bevacizumab plus chemotherapy is unlikely considered cost‐effective for patients after first progression of mCRC.