bluuebunny/crossref_metadata_2025_split huggingface dataset:
Heterogeneous Catalysis for Carbon Dioxide Mediated Hydrogen Storage Technology Based on Formic Acid
Authors: Liu Mingxu , Xu Yuankang , Meng Yu , Wang Lijiao , Wang Hang , Huang Yichao , Onishi Naoya , Wang Lin , Fan Zhuangjun , Himeda Yuichiro 
Published: June 2022

AbstractIn the context of global carbon dioxide increasing drastically, renewable energy is crucial maintain the economic growth of the world. Hydrogen has attracted considerable attention as a clean fuel, but the large‐scale storage and controllable release of H2 is still urgently needed, yet largely not yet accomplished. Through the reactions of CO2 hydrogenation to formic acid (FA) and FA dehydrogenation to hydrogen, a “carbon neutral” sustainable hydrogen storage system can be constructed. With advantages of excellent recyclability and facile separation for heterogeneous catalysis, developing efficient heterogeneous catalysts for hydrogen storage based on FA is the primary focus of this review, mainly involving metal catalysts from nanoscale to single‐atom scale. Firstly, the effects of metal size on the catalytic activities are highlighted in detail. Additionally, special attention is paid to the relevant structure–activity relationships of various supported catalysts and the mechanistic insights, which can provide a theoretical foundation for rational catalyst design. This review brings new and systemic insights into innovative and efficient heterogeneous catalysts design and applications for the ultimate FA‐based sustainable hydrogen storage system with a closed carbon loop.
A versatile AIE fluorogen with selective reactivity to primary amines for monitoring amination, protein labeling, and mitochondrial staining
Authors: He Xinyuan , Xie Huilin , Hu Lianrui , Liu Pengchao , Xu Changhuo , He Wei , Du Wutong , Zhang Siwei , Xing Hao , Liu Xinyue , Park Hojeong , Cheung Tsz Shing , Li Min‐Hui , Kwok Ryan T. K. , Lam Jacky W. Y. , Lu Jian , Tang Ben Zhong 
Published: June 2022

AbstractSpecific bioconjugation for native primary amines is highly valuable for both chemistry and biomedical research. Despite all the efforts, scientists lack a proper strategy to achieve high selectivity for primary amines, not to mention the requirement of fast response in real applications. Herein, we report a chromone‐based aggregation‐induced emission (AIE) fluorogen called CMVMN as a self‐reporting bioconjugation reagent for selective primary amine identification, and its applications for monitoring bioprocesses of amination and protein labeling. CMVMN is AIE‐active and capable of solid‐state sensing. Thus, its electrospun films are manufactured for visualization of amine diffusion and leakage process. CMVMN also shows good biocompatibility and potential mitochondria‐staining ability, which provides new insight for organelle‐staining probe design. Combined with its facile synthesis and good reversibility, CMVMN would not only show wide potential applications in biology, but also offer new possibilities for molecular engineering.
Characteristics of suicide among farmers and ranchers: Using the CDC NVDRS 2003–2018
Authors: Miller Cristina D. M. , Rudolphi Josie M. 
Published: June 2022

AbstractBackgroundSuicide is among the top 10 causes of premature death in the United States. This study provides details on farmer and rancher suicide decedents, including demographic information, mental health status, history of suicidal thoughts and attempts, and circumstances associated with death.MethodsData for this study were obtained from the Centers for Disease Control and Prevention's National Violent Death Reporting System Restricted Access Database for the years 2003–2018. Descriptive statistics and adjusted odds ratios are presented for farm and nonfarm populations in addition to farm populations by age groups and sex.ResultsThis study found that almost half of the farmer suicide decedents were over 65 years old. Firearms were the most widely used method for farmers and ranchers regardless of age and sex. Young farmers and ranchers that died by suicide were more likely to have had relationship problems and older farmers and ranchers that died by suicides were more likely to have had a physical health problem. Male farmer and rancher suicide decedents were more likely to die by firearm than females, and female farmer and rancher suicide decedents were likely to have resided in a small metropolitan area, however, due to small numbers and suppression in the data, most sex comparisons were not able to be presented.ConclusionsWhile no clear risk factor for suicide among farmers and ranchers emerged, results underscore the complex nature of suicide and the need for multifaceted, culturally competent interventions and campaigns that address suicide risk and prevention at the individual and community levels.
Relaxation of the Plant Cell Wall Barrier via Zwitterionic Liquid Pretreatment for Micelle‐Complex‐Mediated DNA Delivery to Specific Plant Organelles
Authors: Miyamoto Takaaki , Tsuchiya Kousuke , Toyooka Kiminori , Goto Yumi , Tateishi Ayaka , Numata Keiji 
Published: June 2022

AbstractTargeted delivery of genes to specific plant organelles is a key challenge for fundamental plant science, plant bioengineering, and agronomic applications. Nanoscale carriers have attracted interest as a promising tool for organelle‐targeted DNA delivery in plants. However, nanocarrier‐mediated DNA delivery in plants is severely hampered by the barrier of the plant cell wall, resulting in insufficient delivery efficiency. Herein, we propose a unique strategy that synergistically combines a cell wall‐loosening zwitterionic liquid (ZIL) with a peptide‐displaying micelle complex for organelle‐specific DNA delivery in plants. We demonstrated that ZIL pretreatment can enhance cell wall permeability without cytotoxicity, allowing micelle complexes to translocate across the cell wall and carry DNA cargo into specific plant organelles, such as nuclei and chloroplasts, with significantly augmented efficiency. Our work offers a novel concept to overcome the plant cell wall barrier for nanocarrier‐mediated cargo delivery to specific organelles in living plants.
Site‐Selective Functionalization of Carboranes at the Electron‐Rich Boron Vertex: Photocatalytic B−C Coupling via a Carboranyl Cage Radical
Authors: Chen Meng , Xu Jingkai , Zhao Deshi , Sun Fangxiang , Tian Songlin , Tu Deshuang , Lu Changsheng , Yan Hong 
Published: June 2022

AbstractFunctionalization of carboranes in a vertex‐specific manner is a perennial challenge. Here, we report a photocatalytic B−C coupling for the selective functionalization of carboranes at the boron site which is most distal to carbon. This reaction was achieved by the photo‐induced decarboxylation of carborane carboxylic acids to generate boron vertex‐centered carboranyl radicals. Theoretical calculations also demonstrate that the reaction more easily occurs at the boron site bearing higher electron density owing to the lower energy barrier for a single‐electron transfer to generate a carboranyl radical. By using this strategy, a number of functionalized carboranes could be accessed through alkylation, alkenylation, and heteroarylation under mild conditions. Moreover, both a highly efficient blue emitter with a solid‐state luminous efficiency of 42 % and a drug candidate for boron neutron capture therapy (BNCT) containing targeting and fluorine units were obtained.
Microplastics and their Additives in the Indoor Environment
Authors: Salthammer Tunga 
Published: June 2022

AbstractAnalyses of air and house dust have shown that pollution of the indoor environment with microplastics could pose a fundamental hygienic problem. Indoor microplastics can result from abrasion, microplastic beads are frequently added to household products and microplastic granules can be found in artificial turf for sports activities and in synthetic admixtures in equestrian hall litter. In this context, the question arose as to what extent particulate emissions of thermoplastic materials from 3D printing should be at least partially classified as microplastics or nanoplastics. The discussion about textiles as a possible source of indoor microplastics has also been intensified. This Minireview gives an overview of the current exposure of residents to microplastics. Trends can be identified from the results and preventive measures can be derived if necessary. It is recommended that microplastics and their additives be given greater consideration in indoor environmental surveys in the future.
Origin of Red‐Shifted Phosphorescence from Triphenylamines: Triplet Excimer or Impurity?
Authors: Cheng Aoyuan , Jiang Yifan , Su Hao , Zhang Baicheng , Jiang Jun , Wang Tao , Luo Yi , Zhang Guoqing 
Published: June 2022

AbstractTriphenylamine (TPA) was reported to exhibit temperature‐dependent dual phosphorescence, where the red‐shifted band was assigned as the excimeric phosphorescence with an energy shift of >3000 cm−1(J. Phys. Chem.1991,95, 7189). Here we show that purified TPA (purity: >99.97 %) shows a single phosphorescence band with a small energy shift of <200 cm−1under the same experimental conditions. The new experimental results, along with theoretical calculations, suggest that the previously reported triplet excimer of TPA is probably not valid and is most likely due to an unidentified impurity. As‐received TPA samples, however, do exhibit temperature‐dependent dual phosphorescence bands, and the wavelength, relative intensity, and temperature dependence of the lower‐energy phosphorescence band vary significantly depending on dopant structures. It was found that dopant phosphorescence could still become dominant even in dilute third‐party solutions of the host at low temperature.
Aufgabenspezifische Janus‐Materialien in der heterogenen Katalyse
Authors: Vafaeezadeh Majid , Thiel Werner R. 
Published: June 2022

AbstractJanus‐Materialien sind anisotrope Nano‐ und Mikroarchitekturen, die zwei verschiedene Seiten mit unterschiedlichen oder entgegengesetzten physikochemischen Eigenschaften aufweisen. Parallel zur Entwicklung neuer Methoden zur Herstellung dieser Materialien wurden entscheidende Fortschritte in Bezug auf Anwendungen erzielt, z. B. in der Biologie, der Katalyse, der Pharmazie und neuerdings auch in der Batterietechnologie. Dieser Kurzaufsatz stellt die jüngsten und wichtigsten Erfolge bei der Anwendung aufgabenspezifisch funktionalisierter Janus‐Nanomaterialien im Bereich der heterogenen Katalyse für unterschiedliche chemische Transformationen vor. Er umfasst Reduktionreaktionen, oxidative Entschwefelung und Farbstoffabbau, asymmetrische Katalyse, Biomassetransformationen, Kaskadenreaktionen, Oxidationsreaktionen, übergangsmetallkatalysierte Kreuzkupplungsreaktionen, elektro‐ und photokatalytische Reaktionen sowie Gasphasenreaktionen. Zum Abschluss folgt ein Ausblick auf mögliche zukünftige Anwendungen.
Counter Electrode Reactions—Important Stumbling Blocks on the Way to a Working Electro‐organic Synthesis
Authors: Klein Martin , Waldvogel Siegfried R. 
Published: June 2022

AbstractOver the past two decades, electro‐organic synthesis has gained significant interest, both in technical and academic research as well as in terms of applications. The omission of stoichiometric oxidizers or reducing agents enables a more sustainable route for redox reactions in organic chemistry. Even if it is well‐known that every electrochemical oxidation is only viable with an associated reduction reaction and vice versa, the relevance of the counter reaction is often less addressed. In this Review, the importance of the corresponding counter reaction in electro‐organic synthesis is highlighted and how it can affect the performance and selectivity of the electrolytic conversion. A selection of common strategies and unique concepts to tackle this issue are surveyed to provide a guide to select appropriate counter reactions for electro‐organic synthesis.
Water‐Soluble Melanin–Protein–Fe/Cu Conjugates Derived from Norepinephrine as Reliable Models for Neuromelanin of Human Brain Locus Coeruleus
Authors: Capucciati Andrea , Monzani Enrico , Sturini Michela , Nicolis Stefania , Zucca Fabio A. , Bubacco Luigi , Bortolus Marco , Zecca Luigi , Casella Luigi 
Published: June 2022

AbstractWater‐soluble melanin‐protein‐Fe/Cu conjugates derived from norepinephrine and fibrillar β‐lactoglobulin are reliable models for neuromelanin (NM) of human brain locus coeruleus. Both iron and copper promote catecholamine oxidation and exhibit strong tendency to remain coupled in oligonuclear aggregates. The Fe‐Cu clusters are EPR silent and affect the 1H NMR spectra of the conjugates through a specific sequence of signals. Derivatives containing only Fe or Cu exhibit different NMR patterns. The EPR spectra show weak signals of paramagnetic FeIII in conjugates containing Fe or mixed Fe‐Cu sites due to small amounts of mononuclear centers. The latter derivatives exhibit EPR signals for isolated CuII centers. These features parallel the EPR behavior of NM from locus coeruleus. The spectral data indicate that FeIII is bound to the melanic fraction, whereas CuII is bound on the protein fibrils, suggesting that the Fe‐Cu clusters occur at the interface between the two components of the synthetic NMs.
1,5‐Allyl Shift by a Sequential Achmatowicz/Oxonia‐Cope/Retro‐Achmatowicz Rearrangement
Authors: Zhang Xiayan , Tong Yi , Li Gang , Zhao Hao , Chen Guanye , Yao Hongliang , Tong Rongbiao 
Published: June 2022

Abstract1,3‐Allyl and 1,2‐allyl shifts through [3,3]‐ and [2,3]‐sigmatropic rearrangements are well‐established and widely used in organic synthesis. In contrast, 1,5‐allyl shift through related [3,5]‐sigmatropic rearrangement is unknown because [3,5]‐sigmatropic rearrangement is thermally Woodward–Hoffmann forbidden. Herein, we report an unexpected discovery of a formal 1,5‐allyl shift of allyl furfuryl alcohol through a 2‐step sequential rearrangement. Mechanistically, this formal 1,5‐allyl shift is achieved through a sequential ring expansion/contraction rearrangement: 1) Achmatowicz rearrangement (ring expansion), and 2) cascade oxonia‐Cope rearrangement/retro‐Achmatowicz rearrangement (ring contraction). This new 1,5‐allyl shift method is demonstrated with >20 examples and expected to find applications in organic synthesis and materials chemistry.
Controlling the Valence‐Electron Arrangement of Nickel Active Centers for Efficient Hydrogen Oxidation Electrocatalysis
Authors: Zhao Xu , Li Xiangyang , An Lulu , Zheng Lirong , Yang Jinlong , Wang Deli 
Published: June 2022

AbstractThe valence‐electron arrangement of heterogeneous catalysts can significantly affect the binding behavior of absorbates. However, it remains a challenge to understand the role of the valence‐electron arrangement in electrocatalysis, which limits its utilization as a tool to design efficient electrocatalysts. Here, we describe experiments in which the valence‐electron arrangement of Ni active centers for hydrogen oxidation is controlled precisely by using Ni‐vacancy‐enriched Ni3N as a platform. These Ni vacancies can promote the valence‐electron delocalization of OH‐adsorption centers to enhance the Ni ds–O 2p valence‐electron‐orbital interaction with elevated OH adsorption. Meanwhile, the deficit of valence‐electrons of H‐adsorption centers at Ni vacancies can lower Ni ds–H 1s interaction with weakened H binding. Relative to Ni3N poor in vacancies, the Ni‐vacancy‐enriched Ni3N showed a mass activity enhanced by 15‐fold. This strategy paves a rational way to design efficient catalysts by finely tuning the valence‐electron arrangement.
Total Synthesis and Prediction of Ulodione Natural Products Guided by DFT Calculations**
Authors: Bestwick Jacob S. , Jones David J. , Jones Helen E. , Kalomenopoulos Panagiotis G. , Szabla Rafal , Lawrence Andrew L. 
Published: June 2022

AbstractA biomimetic synthetic strategy has resulted in a two‐step total synthesis of (±)‐ulodione A and the prediction of two potential natural products, (±)‐ulodiones C and D. This work was guided by computational investigations into the selectivity of a proposed biosynthetic Diels–Alder dimerization, which was then utilized in the chemical synthesis. This work highlights how biosynthetic considerations can both guide the design of efficient synthetic strategies and lead to the anticipation of new natural products.
Selective Oxidative Coupling of Methane to Ethylene in a Solid Oxide Electrolyser Based on Porous Single‐Crystalline CeO2 Monoliths
Authors: Ye Lingting , Shang Zhibo , Xie Kui 
Published: June 2022

AbstractCatalytic conversion of CH4 to C2H4 plays an important role in the light olefin industry. Here, we report the electrochemical conversion of CH4 to C2H4/C2H6 at the anode with the electrolysis of CO2 to CO at the cathode in a solid oxide electrolyser. We constructed well‐defined interfaces that function as three‐phase boundaries by exsolving single‐crystalline Ni nanoparticles in porous single‐crystalline CeO2 monoliths. We engineered the chemical states and flux of active oxygen species for the oxidation of CH4 at the anode by controlling voltage and temperature. We show the unprecedented C2 selectivity (C2H4 and C2H6) of ≥99.5 % at a CH4 conversion of ≈7 %. The electrolyser exhibits excellent durability without performance degradation being observed in a continuous operation of 100 hours. Our work enables a novel path for the selective conversion of CH4/CO2 into useful chemicals, and the technique of building well‐defined interfaces may find potential applications in other fields.
Delineating the Bonghwang earth castle and Royal Palace of Geumgwan Gaya Kingdom using multiple geophysical techniques
Authors: Jeon Hang‐Tak , Hamm Se‐Yeong , Lee Hyoun‐Jae , Park Samgyu , Kim Sang‐Hyun 
Published: June 2022

AbstractGeophysical techniques such as electrical resistivity, ground penetrating radar (GPR), gravity, magnetic, and seismic surveys are useful for prospecting archaeological remains. In this study, we delineated the domain and underground structure of the Bonghwang earth castle and the Royal Palace of the Geumgwan Gaya Kingdom, using multiple geophysical surveys (magnetic, electromagnetic, GPR, and electrical resistivity). Based on the results, the Bonghwang earth castle was extended from a small hill branching from the northern end of the Bonghwangdae hill with a width of 20 m to the hill on the southeast end with a width of slightly over 40 m. The Royal Palace inside the Bonghwang earth castle was further explored using magnetic and GPR surveys. As a result low magnetic values are surrounded radially by high magnetic values at multiple independent locations in an irregular shape in the centre of the Royal Palace. In contrast, the high anomaly zone near the centre of the Royal Palace had a rectangular or ellipsoidal shape, necessitating a clear need for archaeological investigation and excavation in the future.
Considerations for new manganese analytical techniques for drinking water quality management
Authors: Pei Yu , Prepas‐Strobeck Natasha S. , Payne Sarah Jane , She Zhe 
Published: June 2022

AbstractManganese (Mn) is a contaminant of emerging concern in drinking water, as recent epidemiologic evidence suggests an association between Mn exposure in drinking water and negative neurodevelopmental effects. The nature of Mn events in distribution systems can be sporadic and difficult to predict, with conventional laboratory methods being limited in their ability to provide the flexible on‐line Mn monitoring. Emerging methods such as colorimetric and electrochemical methods offer advantages for monitoring as they have potential to be less expensive, rapid, and readily deployed in the field. These emerging methods, however, face hurdles to adaptation and acceptance including demonstration of sufficient accuracy, precision, sensitivity and yet‐to‐be resolved issues with interfering agents. These hurdles are not insurmountable, and investment is warranted in these novel methods to address pressing needs by the water industry to protect human health. This review paper highlights the opportunities and advantages of advancing field‐testing techniques for Mn management.
Luminescent inorganic mixed borate phosphors materials for lighting
Authors: Tawalare Pritee Kishor 
Published: June 2022

AbstractThe need of new materials with desirable optical properties has become important in recent years. In particular, a need has emerged for compounds having better luminescence properties in various practical applications. The introduction of rare earth ions as activators improves the luminescence properties of the compounds considerably. Boron is one of the most abundant elements in nature. It readily combines with almost all other elements. In combination with oxygen; it forms borates comprised of various anions such as BO33−, B2O54−, etc. Apart from these simple borates, several complex compositions exist involving mixed anions as well as double metal borates, due to the three‐fold, or four‐fold coordination of borate atoms. Borates intrinsically possesses characteristics that are advantageous for optical materials, which include a wide transparency range, large electronic band gap, good thermal and chemical stability, low preparative temperature, optical stability with good nonlinear characteristics, and an exceptionally high optical damage threshold. The unique crystal structure of borates determines their enhanced ultraviolet light transparency, good nonlinearity, and relatively high resistance against laser‐induced damage. Some of these complex borates have interesting luminescence properties that are covered in this review. These include double borates containing rare earths RM3(BO3)4, pentaborates LaMgB5O10, M3R2(BO3)4, where M is an alkaline earth, mixed anion borates such as aluminoborate SrAl2B2O7, silicate‐borates such as pekovite, SrB2Si2O8, haloborates, M2B5O9X, where M is an alkaline earth and X is a halogen, phosphate borates, and MBPO5, where M is an alkaline earth. Phosphors based on these compositions find use in various applications such as fluorescence lamps, colour TVs, plasma display panels, high‐intensity discharge lamps based on xenon, optically pumped solid‐state lasers, eye‐safe lasers, and X‐ray imaging.