bluuebunny/crossref_metadata_2025_split huggingface dataset:
Boosting Electrochemical Reduction of CO2 to Formate over Oxygen Vacancy Stabilized Copper–Tin Dual Single Atoms Catalysts
Authors: Wang Haihua , Wen Ning , Wang Yuqing , Jiao Xiuling , Xia Yuguo , Chen Dairong 
Published: June 2023

AbstractDesigning reasonable atomic structures is essential in modulating the selectivity of the valuable products produced in the electrochemical CO2 reduction. Herein, a CuSn diatomic sites electrocatalyst stabilized by double oxygen vacancies on CeO2‐x is constructed, which exhibits superior electrochemical selectivity toward formate, achieving a 90.0% Faradaic efficiency at formate partial current density of 216.8 mA cm−2 with the applied bias of −1.2 V versus REH. The experimental characterizations and theoretical calculations highlight the significance of the synergistic effect of Cu and Sn diatoms on reducing the activation energy and promoting the formation of intermediate *OCHO, which accounts for its high selectivity toward formate. Meanwhile, the oxygen vacancies on the CeO2‐x also play a pivotal role in manipulating the electrochemical performance and stability, which underlines the importance of regulating the electronic metal‐support interaction between CuSn diatoms and CeO2‐x. This work demonstrates an effective method to design efficient electrochemical CO2 reduction catalysts by modulating the surface structures of single‐atoms anchored support.
Photogenerated Defect‐Transit Dual S‐Scheme Charge Separation for Highly Efficient Hydrogen Production
Authors: Luan Xue , Yu Ziqi , Zi Jiangzhi , Gao Fangfang , Lian Zichao 
Published: June 2023

AbstractThe rational design of a step‐scheme (S‐scheme) heterojunctions in hybrid semiconductors by avoiding unwanted charge transport paths is considered as an attractive way to achieve high photocatalytic activity in hydrogen evolution reaction (HER). Here, a dual S‐scheme heterojunction formed in the lychee‐shaped W18O49/CdWO4/CdS nanostructures is proposed for improving the photocatalytic performance in HER under visible light irradiation. The remarkable activity in photocatalytic HER of W18O49/CdWO4/CdS is attributed to the unique structure and effective charge separation by the photoinduced defect‐transit dual S‐scheme mechanism and strong internal electric field. The measurements of X‐ray photoelectron spectroscopy (XPS), femtosecond transient absorption (fs‐TA) spectroscopy, and electron paramagnetic resonance (EPR) further confirm the photoinduced carrier transfer pathways following the dual S‐scheme mechanism. This research can provide a new strategy for designing the dual S‐scheme heterojunctions to improve photocatalytic performance through the defect band structure engineering.
Interface Engineering of Copper Nanocluster Assemblies with White‐Light Emission
Authors: Wang Zhong‐Xia , Gao Hang , Li Xiao‐Qiong , Jia Yi‐Lei , Wang Ting , Cheng Qiu‐Yue , Kang Bin , Chen Hong‐Yuan , Xu Jing‐Juan 
Published: June 2023

AbstractConstruction of white‐light emitters is of great importance in practical applications but is challenging for metal nanoclusters. Herein, arginine (Arg)‐mediated copper nanoclusters (Cu NCs) assemblies with white‐light emission (WLE) are reported for the first time. The multidentate ligand, Arg, not only effectively tailors the high stability and locally‐excited emission (LES) of aqueous phase Cu NCs, but also bridges 1‐naphthalenol methylcarbamate (NMC) to generate a blue emitter via through‐space interactions (TSIs), resulting in a stable mixed light. Density functional theory calculation and mass spectrum further confirm that Arg can allow for the formation of strong hydrogen‐bonds with the ligand 2,4‐diaminotoluene of Cu NCs, and formation of TSIs‐based complexes with NMC. More importantly, pure white‐light emission (WLE) with Commission Internationale de L’Eclairagecoordination (0.30, 0.31) is observed by regulating the ratio between Arg and the interfacial ligand of NMC. The findings not only provide a new perspective for the construction of WLE emitters via interface modification chemistry but also open a window to gain insight into the mechanism of interface engineering.
Mucosa‐Mimetic Materials for the Study of Intestinal Homeostasis and Disease
Authors: Donahue Rebecca , Sahoo Jugal Kishore , Rudolph Sara , Chen Ying , Kaplan David L. 
Published: June 2023

AbstractMucus is a viscoelastic hydrogel that lines and protects the epithelial surfaces of the body that houses commensal microbiota and functions in host defense against pathogen invasion. As a first‐line physical and biochemical barrier, intestinal mucus is involved in immune surveillance and spatial organization of the microbiome, while dysfunction of the gut mucus barrier is implicated in several diseases. Mucus can be collected from a variety of mammalian sources for study, however, established methods are challenging in terms of scale and efficiency, as well as with regard to rheological similarity to native human mucus. Therefore, there is a need for mucus‐mimetic hydrogels that more accurately reflect the physical and chemical profile of the in vivo human epithelial environment to enable the investigation of the role of mucus in human disease and interactions with the intestinal microbiome. This review will evaluate the material properties of synthetic mucus mimics to date designed to address the above need, with a focus toward an improved understanding of the biochemical and immunological functions of these biopolymers related to utility for research and therapeutic applications.
Vectorial On‐Surface Synthesis of Polar 2D Polymer Crystals
Authors: Kojima Takahiro , Patel Karan , Nobusue Shunpei , Mahmoud Ahmed , Xie Cong , Nakae Takahiro , Kawai Shigeki , Fukami Kazuhiro , Sakaguchi Hiroshi 
Published: June 2023

AbstractThe asymmetric introduction of functional groups into polymers is promising due to its potential to provide novel electronic and magnetic properties. Though traditional on‐surface bottom‐up synthesis has succeeded in creating various types of polymers, it struggles at realizing asymmetry due to the difficulty of stereoregular polymerization and the tendency for overall polarity cancellation during agglomeration. Here, enabled by the low halogen‐contaminated metal surfaces provided by two‐zone chemical vapor deposition, “compass” precursors possessing three independent bonding, edge, and dipole vectors undergo isotactic polymerization via the vectorial self‐assembly of chiral precursor diradicals without the need for chiral catalysts required in conventional in‐solution polymerization. The isotactic polymers exhibit polar 2D crystalline structures due to the hetero‐edge CH–π interaction between the standing phenyl and butoxy group surpassing the homo‐edge interactions of π–π and CHCH. The developed vectorial on‐surface synthetic technique not only paves the way to the realization of stereoregular control but also unlocks unprecedented crystal engineering.
H‐Bonded Supramolecular Crystals‐Coated Solid‐Phase Microextraction enables the Matrix Interference‐Free Detection of the COVID‐19 Antiviral Drugs
Authors: Wang Shaohan , Shi Yueru , Yu Jiaxing , Peng Xiaoru , Tong Linjing , Li Nan , Ouyang Gangfeng , Zhu Fang 
Published: June 2023

AbstractSince the outbreak of COVID‐19, many antiviral drugs have been used to treat infected patients. Excessive drug concentrations may not only damage patients' organs, but also lead to increased mortality. The lack of data makes it difficult for them to be treated with these drugs under proper and safe dosage. However, due to the complexity of fluid matrixand structures of the antiviral drugs, it is still difficult to detect the drugs in biofluids. Herein, solid‐phase microextraction (SPME) is applied for the detection of biological matrix, which has the advantages of simplicity, efficiency and environmental protection. With abundant hydrogen bond sites and appropriate molecular volume, biocompatible graded‐pore HOF10x series materials are selected as the fiber coating for exploration. Consequently, HOF101 could achieve high enrichment effect of drugs due to the commensurate mesopores and hydrogen bond non‐covalent interaction. Moreover, the excellent extraction capacity of the HOF101 fiber is verified to be consistent in various interfering conditions. The obtained limits of detections (LODs) are 0.24–0.66 ng L−1, and the recoveries of the biofluids in three concentration levels ranged from 80.30% to 120.1%. It shows the low LODs and satisfactory recoveries of this analytical method, which is expected to be applied in medical systems for drug monitoring.
Correlating the Nonlinear Roughening and Optical Properties of Anatase Thin Films—A Fractal Geometric Approach
Authors: Das Abhijeet , Jaiswal Jyoti , Borah Chandra Kamal , Ruti Itum , Matos Robert S. , Pinto Erveton P. , Yadav R. P. , Ţălu Ştefan , Kumar Sanjeev 
Published: June 2023

AbstractThe anatase phase of TiO2 is highly suitable for photocatalytic application consequently, prerequisite an unpretentious scale‐independent understanding of its roughening‐facilitated surface topography dynamics. Herein, the nonlinear roughening in anatase thin films and its correlation with the nonlinear trend of optical properties in the framework of fractal geometry are investigated. The self‐affine nature of analyzed surfaces is confirmed from the autocorrelation function. The dynamic scaling exponents indicate the existence of Kardar–Parisi–Zhang scaling in surface growth. In addition, the trend of generalized Hurst exponent and mass exponent indicates insignificant multifractal characteristics in the analyzed surfaces. Moreover, fractal analysis explains and aids to description of roughening trend from stereometric and Minkowski functionals analysis. Furthermore, the significance of fractal dimension for probing the surface roughening is validated from the principal component analysis. Consequently, variation in optical bandgap and linear refractive index are investigated in regards to the fractal dimension and root mean‐squared surface slope and regression equations are proposed for tuning of bandgap.
N4‐Acetylcytidine Drives Glycolysis Addiction in Gastric Cancer via NAT10/SEPT9/HIF‐1α Positive Feedback Loop
Authors: Yang Qingbin , Lei Xuetao , He Jiayong , Peng Yanmei , Zhang Yihao , Ling Ruoyu , Wu Chaorui , Zhang Guofan , Zheng Boyang , Chen Xinhua , Zou Boya , Fu Ziyi , Zhao Liying , Liu Hao , Hu Yanfeng , Yu Jiang , Li Fengping , Ye Gengtai , Li Guoxin 
Published: June 2023

AbstractAnti‐angiogenic therapy has long been considered a promising strategy for solid cancers. Intrinsic resistance to hypoxia is a major cause for the failure of anti‐angiogenic therapy, but the underlying mechanism remains unclear. Here, it is revealed that N4‐acetylcytidine (ac4C), a newly identified mRNA modification, enhances hypoxia tolerance in gastric cancer (GC) cells by promoting glycolysis addiction. Specifically, acetyltransferase NAT10 transcription is regulated by HIF‐1α, a key transcription factor of the cellular response to hypoxia. Further, acRIP‐sequencing, Ribosome profiling sequencing, RNA‐sequencing, and functional studies confirm that NAT10 in turn activates the HIF‐1 pathway and subsequent glucose metabolism reprogramming by mediating SEPT9 mRNA ac4C modification. The formation of the NAT10/SEPT9/HIF‐1α positive feedback loop leads to excessive activation of the HIF‐1 pathway and induces glycolysis addiction. Combined anti‐angiogenesis and ac4C inhibition attenuate hypoxia tolerance and inhibit tumor progression in vivo. This study highlights the critical roles of ac4C in the regulation of glycolysis addiction and proposes a promising strategy to overcome resistance to anti‐angiogenic therapy by combining apatinib with ac4C inhibition.
Transient Photocurrent Response in a Perovskite Single Crystal‐Based Photodetector: A Case Study on the Role of Electrode Spacing and Bias
Authors: Mahapatra Apurba , Anilkumar Vishnu , Nawrocki Jan , Pandey Siddhi Vinayak , Chavan Rohit D. , Yadav Pankaj , Prochowicz Daniel 
Published: June 2023

AbstractTransient photocurrent is a widely applied characterization technique to probe the charge‐carrier photogeneration and extraction dynamics in perovskite optoelectronic devices. Despite the large number of studies on the properties of perovskite single‐crystals (SCs) photodetectors (PDs), the underlying mechanism that governs the spectral line shape of transient photocurrent is not fully understood. Here, methylammonium lead bromide (MAPbBr3)SC based PDs are used to study the effect of different electrode spacing and bias on the transient photocurrent response under blue and green light irradiation. The observed differences in the spectral line shape of the transient photocurrent are explained using three‐step carrier transport model, which reveals the occurrence of carrier trapping and a recombination process in MAPbBr3 SC. The findings are further corroborated by intensity‐dependent photocurrent and impedance spectroscopy analysis of the resulting PDs. This work provides a basic insight into the origin of the different behavior of transient photocurrent response under variable electrode distance, bias, and irradiance light, which is expected to help to further understand and optimize the performance of perovskite based PDs.
In Situ Spectroscopic Probing of Oxygen Crossover Effects on Solid Electrolyte Interphase in Aprotic Lithium‐Oxygen Batteries
Authors: Zhao Zhiwei , Pang Long , Wu Yuyue , Chen Yazhou , Peng Zhangquan 
Published: June 2023

AbstractThe solid electrolyte interphase (SEI) on lithium metal anodes (LMA) plays a critical role in affording a long lifespan required for aprotic lithium‐oxygen (Li–O2) batteries. Nevertheless, the crossover of oxygen from the cathode to the anode, an inevitable phenomenon for most of the current Li–O2 batteries, and its effects on the formation and operation of SEI on LMA remain less explored. In this work, a mechanistic study of the SEI formation at a model Cu/dimethyl sulfoxide (DMSO) interface in the presence of oxygen is presented. Direct spectroscopic evidence coupled with theoretical calculation reveals that oxygen can alter the SEI formation pathway and result in distinct SEI properties. Specifically, oxygen can inhibit the fission of the C–S bond of DMSO solvent and therefore reduce the formation of unstable SEI components (e.g., C≡C species) and volatile products (e.g., C2H6 and H2). Thus, the SEI formed under oxygen is more uniform and of less voids, and enables improved electrochemical performance of LMA. This work presents new insights into the oxygen crossover effects on SEI chemistry and is beneficial for designing better LMA/electrolyte interface for future Li–O2 batteries.
Tailoring crystal facet microenvironments for simultaneous electrochemical ozone and hydrogen peroxide production
Authors: Wang Xiaosa , Li Jiayuan , Ding Lei , Shi Huaijie , Liu Jia , Yang Xinying , Li Min , Zhong Xing , Yao Zihao , Wang Jianguo 
Published: June 2023

AbstractDeveloping a bifunctional electrocatalyst that can effectively produce O3 and H2O2 is significant for the electrochemical synthesis of O3 and H2O2 for the synergistic oxidative degradation of organic pollutants. In this study, SnO with various exposed facets was synthesized by tailoring the crystal facet microenvironment for oxygen intermediates adsorption for electrochemical ozone production (EOP) and two‐electron oxygen reduction reaction (2e− ORR). The Faraday efficiency of SnO‐1 with a high (110) facet ratio for O3 was 22.0%, while SnO‐4 with a high (002) facet ratio achieved a selectivity of 93.6% for H2O2. The theoretical calculation indicates that their excellent performances originated from the strong adsorption of the (110) facet on O* and O2* and the suitable adsorption and desorption strength of the (002) facet on OOH*, respectively. This study provides an attractive strategy for the development of a bifunctional electrocatalyst for advanced electrochemical oxidation by tailoring the crystal facet microenvironment.
Highly efficient electrocatalytic oxidation of sterol by synergistic effect of aminoxyl radicals and SeNi5P4
Authors: He Jiahui , Li Suiqin , Li Chun , Li Kai , Xu Yinjie , Wang Mengxin , Zhao Shuying , Zhang Jiefeng , Zhong Xing , Li Xiaonian , Zhang Zhengbin , Wang Jianguo 
Published: June 2023

AbstractThe exploration of efficient and environmentally friendly oxidation method is highly desirable to overcome the critical problems of poor selectivity and heavy metal contamination for the fine chemicals industry. Herein, a self‐supported three‐dimensional (3D) SeNi5P4 nanosheet electrocatalyst was rationally designed and fabricated. Benefiting from the synergistic effect of aminoxyl radical and mesoporous SeNi5P4/graphite felt (GF), an excellent performance of ≥98% selectivity and 33.12 kg (m−3 h−1) space–time yield was obtained for sterol intermediate oxidation with the enhanced mass transfer effect of the continuous flow system. The doping of anionic selenium and phosphorus modulated the electronic structure of SeNi5P4, and the oxyhydroxides generated by surface reconstruction accelerated the turnover of 2,2,6,6‐tetramethyl‐1‐piperidine N‐oxyl (TEMPO), thereby enhancing the intrinsic electrocatalytic activity. A scale‐up experiment was conducted with stacked‐flow electrolyzer demonstrated the application potential. This work provided an efficient synergistic electrocatalytic strategy to facilitate rapid electron and mass transfer for electrochemical alcohol oxidation and highlighted the potential for practical electrosynthesis applications.
Efficient treatment of salty organic wastewater by α‐MnO2‐N/C synergistic catalytic ozonation: Effect and mechanism
Authors: Tu Yuming , Shao Gaoyan , Liu Feng , Li Qunsheng , Zhou Zhiyong , Ren Zhongqi 
Published: June 2023

AbstractA novel and efficient α‐MnO2‐N/C@active carbon (AC) catalyst was proposed and synthesized through a surface modification method based on imprinting process. Uniformly dispersed α‐MnO2 and N/C sites were constructed simultaneously and the competitive adsorption of metal precursors with nonmetal precursors was avoided. Conformational relationship of α‐MnO2‐N/C@AC revealed that α‐MnO2 and graphite N were the main active sites, cleverly forming synergistic catalytic effect, which results in a good degradation effect for two actual printing and dyeing wastewater. The removal rate of chemical oxygen demand (COD) could reach 78% and 58% within 60 min, respectively, and it maintained stable after 20 repetitions without leaching of metal ions. Mechanistic investigation demonstrated that N/C sites rapidly adsorbed ozone to generate ·O2− and synergistically catalyzed with adjacent α‐MnO2 sites to further produce ·OH, significantly facilitating the generation of ·OH. This work provides a promising strategy to synthesize novel and efficient catalysts for ozone catalytic oxidation process.
Clinical characteristics analysis of sinonasal diffuse large B‐cell lymphoma and extranodal NK/T‐cell lymphoma
Authors: Jang Hye‐Bin , Lee Dong Hoon , Song Ga‐Young , Yang Deok‐Hwan , Lim Sang Chul 
Published: June 2023

Keypoints
Extranodal NK/T‐cell lymphoma (ENKL) was the most common sinonasal lymphoma at our hospital.
ENKL occurs at a younger age, and is more prevalent in the nasal cavity.
ENKL had a lower Ann Arbor stage, and a better prognosis than diffuse large B‐cell lymphoma (DLBLC).
Molecular‐Orbital Delocalization Enhances Charge Transfer in π‐Conjugated Organic Semiconductors
Authors: Guo Shuang , Park Yeonju , Park Eungyeong , Jin Sila , Chen Lei , Jung Young Mee 
Published: June 2023

Abstractπ‐Conjugated organic semiconductors are promising materials for surface‐enhanced Raman scattering (SERS)‐active substrates based on the tunability of electronic structures and molecular orbitals. Herein, we investigate the effect of the temperature‐mediated resonance‐structure transitions of poly(3,4‐ethylenedioxythiophene) (PEDOT) in poly(3,4‐ethylenedioxythiophene)‐poly(styrenesulfonate) (PEDOT : PSS) films on the interactions between substrate and probe molecules, thereby affecting the SERS activity. Absorption spectroscopy and density functional theory calculations show that this effect occurs mainly due to delocalization of the electron distribution in molecular orbitals, effectively promoting the charge transfer between the semiconductor and probe molecules. In this work, we investigate for the first time the effect of electron delocalization in molecular orbitals on SERS activity, which will provide new design ideas for the development of highly sensitive SERS substrates.
Boosting Alkaline Hydrogen Evolution Reaction through Water Structure Manipulation
Authors: Jiao Yan , Zheng Yao 
Published: June 2023

AbstractIn the past, the design of efficient electrocatalyst materials for alkaline hydrogen evolution reaction (HER) was mostly focused on tuning the adsorption properties of reaction intermediates. A recent breakthrough shows that the performance can be improved by manipulating water structure at the electrode‐electrolyte interface using atomically localized electric fields. The new approach was realized by using IrRu dizygotic single‐atom sites and led to a significantly accelerated water dissociation and an overall improved alkaline HER performance. Supported by extensive data from advanced modeling, characterization, and electrochemical measurements, the work delivers an intricate examination of the interaction between water molecules and the catalyst surface, thereby enriching our understanding of water dissociation kinetics and offering new insights to boost overall alkaline HER efficiency.
Biosynthesis of a tri‐metallic nanoalloy for magnetic and biomedical applications
Authors: Lurthu Pushparaj T. , Fantin Irudaya Raj E. , Francy Irudaya Rani E. , Appadurai M. 
Published: June 2023

The tri‐metallic magnetic nanoalloy synthesized via the eco‐friendly procedure discussed here contains cobalt (Co), nickel (Ni), and zirconium (Zr) metals in a 3:1:1 M ratio (Co3O4.NiO.ZrO2 nanoalloy). Two different plant extracts which are rich in biologically active compounds from Spermacoce hispida and Vernonia cinereum were combined to get a multispecies nanoalloy with magnetic properties and medicinal values. The Fourier transform infrared, X‐ray diffraction, and transmission and scanning electron microscopes analyses confirmed the spherical shape of the bioinspired Co3O4.NiO.ZrO2 nanoalloy. The average size of our nanoalloy was 32 nm, but the individual nanoparticles are between 21 and 73 nm in size. A vibrating sample magnetometer study of the magnetic characteristics of the nanoalloy reveals strong saturation magnetization (12.42 emu/g), low retentivity (Mr), and low coercivity (Hc) (282.36 Oe). The higher saturation magnetization in nanoalloy is attributed to their larger particle size, a high degree of crystalline structure, and slight external spinning deformation. The low coercive field (Hc) value reveals the unique soft nature of our nanoalloy. The disc diffusion study confirms that a 6.3 μg/mL solution of the nanoalloy kills almost 96% of the harmful bacteria like Bacillus subtilis (29 mm), Bacillus cereus (26 mm), and Escherichia coli (21 mm). It shows a moderate effect of 85% killing factor against Staphylococcus albus (17 mm), Pseudomonas aeruginosa (13 mm), and Klebsiella pneumoniae (15 mm) bacteria.