bluuebunny/crossref_metadata_2025_split huggingface dataset:
Unusual modifications of protein biomarkers expressed by plasmid, prophage, and bacterial host of pathogenic Escherichia coli identified using top‐down proteomic analysis
Authors: Fagerquist Clifton K. , Shi Yanlin , Park Jihyun 
Published: November 2023

RationalePathogenic bacteria often carry prophage (bacterial viruses) and plasmids (small circular pieces of DNA) that may harbor toxin, antibacterial, and antibiotic resistance genes. Proteomic characterization of pathogenic bacteria should include the identification of host proteins and proteins produced by prophage and plasmid genomes.MethodsProtein biomarkers of two strains of Shiga toxin–producing Escherichia coli (STEC) were identified using antibiotic induction, matrix‐assisted laser desorption/ionization tandem time‐of‐flight (MALDI‐TOF‐TOF) tandem mass spectrometry (MS/MS) with post‐source decay (PSD), top‐down proteomic (TDP) analysis, and plasmid sequencing. Alphafold2 was also used to compare predicted in silico structures of the identified proteins to prominent fragment ions generated using MS/MS‐PSD. Strain samples were also analyzed with and without chemical reduction treatment to detect the attachment of pendant groups bound by thioester or disulfide bonds.ResultsShiga toxin was detected and/or identified in both STEC strains. For the first time, we also identified the osmotically inducible protein (OsmY) whose sequence unexpectedly had two forms: a full and a truncated sequence. The truncated OsmY terminates in the middle of an α‐helix as determined by Alphafold2. A plasmid‐encoded colicin immunity protein was also identified with and without attachment of an unidentified cysteine‐bound pendant group (~307 Da). Plasmid sequencing confirmed top‐down analysis and the identification of a promoter upstream of the immunity gene that is activated by antibiotic induction, that is, SOS box.ConclusionsTDP analysis, coupled with other techniques (e.g., antibiotic induction, chemical reduction, plasmid sequencing, and in silico protein modeling), is a powerful tool to identify proteins (and their modifications), including prophage‐ and plasmid‐encoded proteins, produced by pathogenic microorganisms.
Conversion Mechanism of Organic Matter While Cleaning Oil‐Based Drilling Cuttings Using Surfactant‐Free Microemulsions
Authors: Li Jing , Yue Hong , Wen Ming , Zhao Liang , Jiang Guobin , Yu Jinlei , Wang Hongjuan , Meng Tian , Yin Xiaoyun , Chen Xinglong 
Published: November 2023

AbstractSurfactant‐free microemulsions (SFMEs) cleaning technology can effectively separate and recover petroleum pollutants from oil‐based drilling cuttings (OBDCs). The identification of the molecular composition of OBDCs is helpful to accurately grasp the conversion mechanism of organic matter. Therefore, the understanding of the mechanism of petroleum removal at the microscopic molecular level in the cleaning process needs to be further studied. The conversion mechanism of organic matter during the use of SFMEs to clean OBDCs was investigated by positive ion atmospheric pressure photoionization Fourier transform ion cyclotron resonance mass spectrometry (+APPI FT‐ICR MS). The results show that the SFMEs cleaning technology can separate and recover CH and CHO organic matter in OBDCs, but there is still a small amount of organic matter with high molecular weight and unsaturated degree in OBDCs that has not been separated. The majority of this organic matter is CH, accounting for 91 %, and it is mainly polycyclic aromatic hydrocarbons. A total of 255 kinds of organic matter in 110# industrial white oil were detected in the recovered oil after treatment, accounting for more than 99 % of the total, which has a certain recoverable value. This study can provide a theoretical reference for the efficient degradation of OBDCs.
Enhancing the Electrochemical Properties of LiNi0.8Co0.15Al0.05O2 with ZrO2 Surface Coating
Authors: Hu Jiawei , Zhang Yang , Zhou Xiang , Liu Jie 
Published: November 2023

AbstractNi‐rich transition metal oxides have high energy density and are promising cathode materials for lithium‐ion batteries. However, the capacity of Li‐ion batteries decays rapidly due to side reactions at the electrode‐electrolyte interface with electrolyte erosion of the material. Surface modification can be used to alleviate these conditions. Here, we report the cathode material modified by ZrO2 coating, which prevents the active material from being corroded by the electrolyte and thus can significantly inhibit the interfacial side reactions between the cathode and the electrolyte. Leveraging these advantages, ZrO2‐coated LiNi0.8Co0.15Al0.05O2 achieves 85.8 % capacity retention at 1 C rate after 100 cycles. This modification method is an important advance and is expected to be used in the research of high‐performance cathode materials.
Investigating the Chemical Reactivity of Kahalalides: A Promising Source of Therapeutic Peptides from Marine Natural Products Using Conceptual Density Functional Theory
Authors: Flores‐Holguín Norma , Frau Juan , Glossman‐Mitnik Daniel 
Published: November 2023

AbstractMarine organisms have been found to produce compounds that have the potential to serve as templates for novel therapeutics. Among these compounds, peptides are of particular interest due to their intermediate size between amino acids and proteins. Kahalalides are a family of structurally complex cyclic peptides with potent cytotoxic and antitumor activities, making them promising candidates for cancer therapy. In this study, we investigate the chemical reactivity of Kahalalides A–F using Conceptual Density Functional Theory to gain insight into their bioactivity from a molecular perspective. Our investigation includes characterizing and isolating the peptides, determining their local and global properties and predicting the active reaction sites. We also calculate Bioactivity Scores to predict their biological targets. Overall, this study contributes to the discovery of new therapeutic peptides from natural sources by providing insights into their chemical reactivity and potential biological targets.
Impact of Surface Ligand on the Biocompatibility of InP/ZnS Quantum Dots with Platelets
Authors: Gil Hélio M. , Booth Zoe , Price Thomas W. , Lee Jessica , Naylor‐Adamson Leigh , Avery Michelle , Muravitskaya Alina , Hondow Nicole , Allsup David , Schneider Jürgen E. , Naseem Khalid , Adawi Ali M. , Bouillard Jean‐Sebastien G. , Chamberlain Thomas W. , Calaminus Simon D. J. , Stasiuk Graeme J. 
Published: November 2023

AbstractInP/ZnS quantum dots (QDs) have received a large focus in recent years as a safer alternative to heavy metal‐based QDs. Given their intrinsic fluorescent imaging capabilities, these QDs can be potentially relevant for in vivo platelet imaging. The InP/ZnS QDs are synthesized and their biocompatibility investigated through the use of different phase transfer agents. Analysis of platelet function indicates that platelet‐QD interaction can occur at all concentrations and for all QD permutations tested. However, as the QD concentration increases, platelet aggregation is induced by QDs alone independent of natural platelet agonists. This study helps to define a range of concentrations and coatings (thioglycolic acid and penicillamine) that are biocompatible with platelet function. With this information, the platelet‐QD interaction can be identified using multiple methods. Fluorescent lifetime imaging microscopy (FLIM) and confocal studies have shown QDs localize on the surface of the platelet toward the center while showing evidence of energy transfer within the QD population. It is believed that these findings are an important stepping point for the development of fluorescent probes for platelet imaging.
Aerosol Jet Printing Conductive 3D Microstructures from Graphene Without Post‐Processing
Authors: Smith Brittany N. , Ballentine Peter , Doherty James L. , Wence Ryan , Hobbie Hansel Alex , Williams Nicholas X. , Franklin Aaron D. 
Published: November 2023

AbstractThree‐dimensional (3D) graphene microstructures have the potential to boost performance in high‐capacity batteries and ultrasensitive sensors. Numerous techniques have been developed to create such structures; however, the methods typically rely on structural supports, and/or lengthy post‐print processing, increasing cost and complexity. Additive manufacturing techniques, such as printing, show promise in overcoming these challenges. This study employs aerosol jet printing for creating 3D graphene microstructures using water as the only solvent and without any post‐print processing required. The graphene pillars exhibit conductivity immediately after printing, requiring no high‐temperature annealing. Furthermore, these pillars are successfully printed in freestanding configurations at angles below 45° relative to the substrate, showcasing their adaptability for tailored applications. When graphene pillars are added to humidity sensors, the additional surface area does not yield a corresponding increase in sensor performance. However, graphene trusses, which add a parallel conduction path to the sensing surface, are found to improve sensitivity nearly 2×, highlighting the advantages of a topologically suspended circuit construction when adding 3D microstructures to sensing electrodes. Overall, incorporating 3D graphene microstructures to sensor electrodes can provide added sensitivity, and aerosol jet printing is a viable path to realizing these conductive microstructures without any post‐print processing.
High Performance Thermoelectric Power of Bi0.5Sb1.5Te3Through Synergistic Cu2GeSe3and Se Incorporations
Authors: Pang Kaikai , Yuan Minhui , Zhang Qiang , Li Yanan , Zhang Yuyou , Zhou Wenjie , Wu Gang , Tan Xiaojian , Noudem Jacques G. , Cui Chen , Hu Haoyang , Wu Jiehua , Sun Peng , Liu Guo‐Qiang , Jiang Jun 
Published: November 2023

AbstractBi2Te3‐based alloys are the benchmark for commercial thermoelectric (TE) materials, the widespread demand for low‐grade waste heat recovery and solid‐state refrigeration makes it imperative to enhance the figure‐of‐merits. In this study, high‐performance Bi0.5Sb1.5Te3(BST) is realized by incorporating Cu2GeSe3and Se. Concretely, the diffusion of Cu and Ge atoms optimizes the hole concentration and raises the density‐of‐states effective mass (md*), compensating for the loss of “donor‐like effect” exacerbated by ball milling. The subsequent Se addition further increasesmd*, enabling a total 28% improvement of room‐temperature power factor (S2σ), reaching 43.6 µW cm−1 K−2compared to the matrix. Simultaneously, the lattice thermal conductivity is also significantly suppressed by multiscale scattering sources represented by Cu‐rich nanoparticles and dislocation arrays. The synergistic effects yield a peakZTof 1.41 at 350 K and an averageZTof 1.23 (300–500 K) in the Bi0.5Sb1.5Te2.94Se0.06+ 0.11 wt.% Cu2GeSe3sample. More importantly, the integrated 17‐pair TE module achieves a conversion efficiency of 6.4%, 80% higher than the commercial one at ΔT = 200 K. These results validate that the facile composition optimization of the BST/Cu2GeSe3/Se is a promising strategy to improve the application of BST‐based TE modules.
Regulating Li Nucleation and Growth Heterogeneities via Near‐Surface Lithium‐Ion Irrigation for Stable Anode‐Less Lithium Metal Batteries
Authors: Xie Chuyi , Zhao Chen , Jeong Heonjae , Liu Qiang , Li Tianyi , Xu Wenqian , Cheng Lei , Xu Gui‐Liang , Amine Khalil , Chen Guohua 
Published: November 2023

AbstractThe inhomogeneous nucleation and growth of Li dendrite combined with the spontaneous side reactions with the electrolytes dramatically challenge the stability and safety of Li metal anode (LMA). Despite tremendous endeavors, current success relies on the use of significant excess of Li to compensate the loss of active Li during cycling. Herein, a near‐surface Li+ irrigation strategy is developed to regulate the inhomogeneous Li deposition behavior and suppress the consequent side reactions under limited Li excess condition. The conformal polypyrrole (PPy) coating layer on Cu surface via oxidative chemical vapor deposition technique can induce the migration of Li+ to the interregional space between PPy and Cu, creating a near‐surface Li+‐rich region to smooth diffusion of ion flux and uniform the deposition. Moreover, as evidenced by multiscale characterizations including synchrotron high‐energy X‐ray diffraction scanning, a robust N‐rich solid‐electrolyte interface (SEI) is formed on the PPy skeleton to effectively suppress the undesired SEI formation/dissolution process. Strikingly, stable Li metal cycling performance under a high areal capacity of 10 mAh cm−2 at 2.0 mA cm−2 with merely 0.5 × Li excess is achieved. The findings not only resolve the long‐standing poor LMA stability/safety issues, but also deepen the mechanism understanding of Li deposition process.
Ultralow‐Overpotential Acidic Oxygen Evolution Reaction Over Bismuth Telluride–Carbon Nanotube Heterostructure with Organic Framework
Authors: Arbab Alvira Ayoub , Cho Sehyeon , Jung Euibeen , Han Hyun Soo , Park Sangwook , Lee Hyoungsoon 
Published: November 2023

AbstractThe state‐of‐the‐art iridium and ruthenium oxides‐based materials are best known for high efficiency and stability in acidic oxygen evolution reaction (OER). However, the development of economically feasible catalysts for water‐splitting technologies is challenging by the requirements of low overpotential, high stability, and resistance of catalysts to dissolution during the acidic oxygen evolution reaction . Herein, an organometallic core–shell heterostructure composed of a carbon nanotube core (CNT) and bismuth telluride (Bi2Te3) shell (denoted as nC–Bi2Te3) is designed and use it as a catalyst for the acidic OER. The proposed catalyst achieves an ultralow overpotential of 160 mV at 10 mA cm−2 (geometrical), thereby outperforming most of the state‐of‐the‐art precious‐metal‐based catalysts. The low Tafel slope of 30 mV dec−1 and charge transfer resistance (RCT) of 1.5 Ω demonstrate its excellent electrocatalytic activity. The morphological and chemical compositions of nC–Bi2Te3 enable the generation of ─OH functional group in the Bi─Te sections formed via a ligand support, which enhances the absorption capacity of H+ ions and increases the intrinsic catalytic activity. The presented insights regarding the material composition–structure relationship can help expand the application scope of high‐performance catalysts.
Chiral‐Achiral Cations Intercalation Induced Lead‐Free Chiral‐Polar Hybrid Perovskites Enable Self‐Powered X‐Ray and Ultraviolet–Visible–Near‐Infrared Photo Detection
Authors: Zhu Zeng‐Kui , Zhu Tingting , You Shihai , Yu Panpan , Wu Jianbo , Zeng Ying , Guan Qianwen , Li Zhou , Qu Chang , Zhong Haiqing , Li Lina , Luo Junhua 
Published: November 2023

AbstractLead halide hybrid perovskites have made great progress in direct X‐ray detection and broadband photodetection, but the existence of toxic Pb and the demand for external operating voltage have severely limited their further applications and operational stability improvements. Therefore, exploring “green” lead‐free hybrid perovskite that can both achieve X‐ray detection and broadband photodetection without external voltage is of great importance, but remains severely challenging. Herein, using centrosymmetric (BZA)3BiI6 (1, BZA = benzylamine) as a template, a pair of chiral‐polar lead‐free perovskites, (BZA)2(R/S‐PPA)BiI6 (2‐R/S, R/S‐PPA = (R/S)‐1‐Phenylpropylamine) are successfully obtained by introducing chiral aryl cations of (R/S)‐1‐Phenylpropylamine. Compared to 1, chiral‐polar 2‐R presents a significant irradiation‐responsive bulk photovoltaic effect (BPVE) with an open circuit photovoltage of 0.4 V, which enables it with self‐powered X‐ray, UV–vis‐NIR broadband photodetection. Specifically, 2‐R device exhibits an ultralow detection limit of 18.5 nGy s−1 and excellent operational stability. Furthermore, 2‐R as the first lead‐free perovskite achieves significant broad‐spectrum (377–940 nm) photodetection via light‐induced pyroelectric effect. This work sheds light on the rational crystal reconstruction engineering and design of “green” hybrid perovskite toward high‐demanded self‐powered radiation detection and broadband photodetection.
Structural Engineering of Co‐Metal–Organic Frameworks via Ce Incorporation for Improved Oxygen Evolution
Authors: Liao Yuanyuan , Xiao Yue , Li Zhiquan , Zhou Xiaoqing , Liu Jiahao , Guo Feng , Li Jing , Li Yongxiu 
Published: November 2023

AbstractThe rational design of metal–organic framework (MOF)‐based electrocatalysts plays a key role in achieving high‐efficiency oxygen evolution reaction (OER). Herein, a synergetic morphology and electronic structure engineering strategy are proposed to design a Co‐MOF nanoflower grown on carbon paper via rare‐earth cerium doping (CoCe‐MOF/CP). Compared with Co‐MOF/CP, the developed CoCe‐MOF/CP exhibited superior OER performance with a low overpotential of 267 mV at 10 mA cm−2 and outstanding long‐term stability over 100 h. Theoretical calculations show that the unique 4f valence electron structure of Ce induced charge redistribution of the Co‐MOF surface through the strong Co 3d‐O 2p‐Ce 4f orbital electronic coupling below the Fermi level. Ce‐doped plays a key role in the engineering of the electronic states of the Co sites to endow them with the optimal free energy landscape for enhanced OER catalytic activity. This work provides new insights into comprehending the RE‐enhanced mechanism of electrocatalysis and provides an effective strategy for the design of MOF‐based electrocatalysts.
Modulating the Distribution of Formamidinium Iodide by Ultrahigh Humidity Treatment Strategy for High‐Quality Sequential Vapor Deposited Perovskite
Authors: Lin Dongxu , Fang Jun , Yang Xiaoxin , Wang Xin , Li Sibo , Wang Daozeng , Xie Guanshui , Li Huan , Wang Xiao , Qiu Longbin 
Published: November 2023

AbstractThe quality of two‐step processed perovskites is significantly influenced by the distribution of organic amine salts. Especially, modulating the distribution of organic amine salts remains a grand challenge for sequential vapor‐deposited perovskites due to the blocking effect of bottom compact PbI2. Herein, an ultrahigh humidity treatment strategy is developed to facilitate the diffusion of formamidinium iodide (FAI) from the top surface to the buried bottom interface on the sequential vapor‐deposited bilayer structure. Both experimental and theoretical investigations elucidate the mechanism that moisture helps to i) create FAI diffusion channels by inducing a phase transition from α‐ to δ‐phase in the perovskite, and ii) enhance the diffusivity of FAI by forming hydrogen bonds. This ultrahigh humidity treatment strategy enables the formation of a desired homogeneous and high‐quality α‐phase after annealing. As a result, a champion efficiency of 22.0% is achieved and 97.5% of its initial performance is maintained after aging for 1050 h under ambient air with a relative humidity of up to 80%. This FAI diffusion strategy provides new insights into the reproducible, scalable, and high‐performance sequential vapor‐deposited perovskite solar cells.
Manipulating the Host−Guest Chemistry of Cucurbituril to Propel Highly Reversible Zinc Metal Anodes
Authors: Zhao Yiming , Wei Mengying , Tan Li‐Li , Luo Zhixuan , Peng Jiahui , Wei Chunguang , Kang Feiyu , Wang Jian‐Gan 
Published: November 2023

AbstractRechargeable aqueous zinc‐ion batteries are practically plagued by the short lifespan and low Coulombic efficiency (CE) of Zn anodes resulting from random dendrite deposition and parasitic reactions. Herein, the host−guest chemistry of cucurbituril additive with Zn2+ to achieve longstanding Zn anodes is manipulated. The macrocyclic molecule of cucurbit[5]uril (CB[5]) is delicately designed to reconstruct both the CB[5]‐adsorbed electric‐double layer (EDL) structure at the Zn interface and the hydrated sheath of Zn2+ ions. Especially benefiting from the desirable carbonyl rims and suitable hydrophobic cavities, the CB[5] has a strong host−guest interaction with Zn2+ ions, which exclusively permits rapid Zn2+ flux across the EDL interface but retards the H2O radicals and SO42−. Accordingly, such a unique particle redistributor warrants long‐lasting dendrite‐free deposition by homogenizing Zn nucleation/growth and significantly improved CE by inhibiting side reactions. The Zn anode can deliver superior reversibility in CB[5]‐containing electrolyte with a ninefold increase of cycle lifetime and an elevated CE of 99.7% under harsh test conditions (10 mA cm−2/10 mA h cm−2). The work opens a new avenue from the perspective of host−guest chemistry to propel the development of rechargeable Zn metal batteries and beyond.
Electrolyte Engineering Empowers Li||CFx Batteries to Achieve High Energy Density and Low Self‐Discharge at Harsh Conditions
Authors: Xiao Yukang , Chen Xunxin , Jian Junhua , Cheng Yong , Zou Yue , Su Yu , Wu Qilong , Tang Chao , Zhang Zhongru , Wang Ming‐Sheng , Zheng Jianming , Yang Yong 
Published: November 2023

AbstractGiven its exceptional theoretical energy density (over 2000 Wh kg−1), lithium||carbon fluoride (Li||CFx) battery has garnered global attention. N‐methylpyrrolidone (NMP)‐based electrolyte is regarded as one promising candidate for tremendously enhancing the energy density of Li||CFx battery, provided self‐discharge challenges can be resolved. This study successfully achieves a low self‐discharge (LSD) and desirable electrochemical performance in Li||CFx batteries at high temperatures by utilizing NMP as the solvent and incorporating additional ingredients, including vinylene carbonate additive, as well as the dual‐salt systems formed by LiBF4 with three different Li salts, namely lithium bis(oxalato)borate, lithium difluoro(oxalato)borate, and LiNO3. The experimental results unfold that the proposed methods not only minimize aluminum current collector corrosion, but also effectively passivate the Li metal anode. Among them, LiNO3 exhibits the most pronounced effect that achieves an energy density of ≈2400 Wh kg−1 at a current density of 10 mA g−1 at 30 °C, nearly 0% capacity‐fade rate after 300 h of storage at 60 °C, and the capability to maintain a stable open‐circuit voltage over 4000 h. This work provides a distinctive perspective on how to realize both high energy density and LSD rates at high temperature of Li||CFx battery.
Defect Compensation and Lattice Stabilization Enables High Voltage Output in Tin Halide Perovskite Solar Cells
Authors: Wang Shurong , Wu Cheng , Yao Huanhuan , Xie Lisha , Xiao Yu , Ding Liming , Hao Feng 
Published: November 2023

AbstractTin halide perovskite solar cells (PSCs) are regarded as the most promising lead‐free alternatives for photovoltaic applications. However, they still suffer from uncompetitive photovoltaic performance because of the facile Sn2+ oxidation and Sn‐related defects. Herein, a defect and carrier management strategy by using diaminopyridine (DP) and 4‐bromo‐2,6‐diaminopyridine (4BrDP) as multifunctional additives for tin halide perovskites is reported. Both DP and 4BrDP induced strong interaction with tin perovskites by coordinate bonding and N─H···I hydrogen bonding, which greatly suppresses the micro‐strain and Urbach energy of tin halide perovskite films. The strong hydrogen bonding inhibits the formation of I3− and related defect density. Meanwhile, the electron‐donor species of halogen bond in 4BrDP provides higher reactivity of 2 and 6 sites, which indicates stronger passivation ability with tin halide perovskites. These advances enable a champion power conversion efficiency (PCE) of 13.40% in 4BrDP‐processed devices with remarkable improvement in both open‐circuit voltage (Voc) of 881 mV and fill factor (FF) of 71.26%. The 4BrDP devices retain 91% and 82% of the pristine PCE after 2000 h storage in N2 atmosphere and 1000 h under 85 °C, respectively. Therefore, this work provides new insight into molecular design for high‐performance and stable lead‐free optoelectronics.