bluuebunny/crossref_metadata_2025 huggingface dataset:
Prevalence of Helicobacter Pylori Gastritis among Patients with Symptomatic Cholelithiasis
Authors: Memon Amir Iqbal , Naz Samina , Memon Riaz Ahmed , Bhatti Aisha Masroor , Nayab . , Ali Mansoor
Published: April 2022

Background: H. Pylori gastritis is considered to be the causative factor for gallstone disease. Though this infection is reported to be the leading factor contributing to the pathogenesis of gastro-duodenal ulcers, and gastric cancer. Its infestation of the gallbladder and causing chronic cholecystitis and cholelithiasis are still debatable.

Methodology: This study was descriptive cross-sectional in nature, performed on 110 patients (chosen via non-probability, consecutive sampling), presented at Surgical OPD with symptomatic cholelithiasis. All the participants underwend for diagnostic endoscopy and a biopsy was taken for confirmation of h.Pylori gastritis. Those who had positive H. Pylori test, were treated by eradication therapy first and then submitted for the laparoscopic cholecystectomy and those who were negative submitted for the laparoscopic cholecystectomy. The study lasted 1 year from February 2021 to February 2022.

Results: Among the subjects, 72.7% (n=80) were female, 32.5% were under 40 years old while male gender composed of 17.3% of the sample population. 3/4th of the population hailed from the rural setting. 70.1% (n=78) of the patients had positive H. Pylori test on histopathology.

Upon the findings of diagnostic endoscopy, severe and moderate gastritis was found to be in 25.6% and 74.4% of the participants with positive helicobector gastritis, respectively. A significant association was found out between familial history of gall stones and helicobector pylori gastritis (p=0.02).

Conclusion: A high prevalence of H. Pylori infection is among patients with symptomatic cholelithiasis, which also crossponds to the endoscopic findings. The association between the familial history of gall stones and helicobetor gastritis merits to be explore further to establish the casuality of the relationship.
Ocean temperature and density dependence as key drivers of the population dynamics of an intertidal crab at the Brazilian oceanic islands
Authors: Macedo Thais P. , Zhao Qing , Costa Natasha V. , Freire Andrea S.
Published: April 2022

Understanding how climatic and density‐dependent processes affect demography is crucial for predicting population responses to climate change. For marine invertebrates with complex life cycle such as decapod crustaceans, increasing temperatures might affect survival and development of early pelagic stages, whereas high density can increase competition and thus reduce growth and fecundity of older life stages. In this study, we investigate the effects of warm ocean events, body size and density on the population dynamics of the intertidal Sally lightfoot crab (Grapsus grapsus) at the Brazilian oceanic islands. Firstly, we assessed the trends of marine heatwaves (MHW) and positive temperature anomalies (ΔSST+) at the equatorial St Peter and St Paul (SPSP) Archipelago and Rocas Atoll and the subtropical Trindade Island. We then jointly analyzed short‐term count, capture‐recapture and fecundity data, and long‐term population monitoring data (2003–2019) using an integrated population model. Warm ocean events have become more frequent and intense only at the equatorial islands. Increasing MHW frequency positively influenced recruitment in the high‐density SPSP population, while MHW intensity and ΔSST+ frequency had negative impacts. Conversely, no climatic effects were observed for the low‐density Rocas population, which has the largest crabs. Despite a lack of warming in Trindade, this subtropical population with intermediate density and body size was negatively affected by ΔSST+. Our findings revealed population‐specific responses to climate change when accounting for local life history and ecology. Thus, environmental and density‐dependent effects should be broadly considered in future conservation studies regarding ocean warming impacts on marine invertebrate populations.
Transient Out‐of‐Equilibrium Nucleic Acid‐Based Dissipative Networks and Their Applications
Authors: Li Zhenzhen , Wang Jianbang , Willner Itamar
Published: April 2022

Dynamic, dissipative reactions play important roles in biological processes, and emulating such biological processes by artificial circuits and networks is a challenging topic in the area of Systems Chemistry. The present article summarizes efforts to apply the information encoded in the base sequence of nucleic acids to assemble transient, dissipative DNA‐based networks mimicking natural processes. The design principles of the transient nucleic acid‐based systems are introduced. Triggered reaction moduli lead to a transient intermediary constituent recovered to the parent moduli by enzymes, DNAzyme, or light as control units are described. Transient DNA‐based circuitries of enhanced complexities revealing temporal gated or cascaded transformations are demonstrated. Different applications of dynamically triggered transient circuits are introduced, including the temporal aggregation and deaggregation of plasmonic nanoparticles or semiconductor quantum dots and the control over their optical properties, the transient release and uptake of loads by aptamer scaffolds, and the transient reconfiguration of constitutional dynamic networks and the control over emergent catalytic functions. The future perspectives of dissipative nucleic acid‐based networks and their potential future applications are discussed.
Bifunctional Fusion Membrane‐Based Hydrogel Enhances Antitumor Potency of Autologous Cancer Vaccines by Activating Dendritic Cells
Authors: Ke Yaohua , Zhu Junmeng , Chu Yanhong , Cen Lanqi , Fu Yao , Fan Xiangshan , Shao Jingyi , Li Rutian , Yu Lixia , Liu Baorui , Liu Qin
Published: April 2022

Autologous tumor cell vaccine is an individualized tumor treatment strategy to elicit tumor‐specific immune responses. However, it is difficult to exert efficacy in “cold” tumors, which lack tumor‐infiltrating T cells and are not sensitive to immunotherapy. Here, a dendritic cells (DCs) activation hydrogel is constructed based on bifunctional fusion membrane nanoparticles (FM‐NPs) composed of autologous tumor cell membranes and Mycobacterium phlei membrane extracts. The FM‐NPs not only provide tumor antigens but also can activate DCs. Afterward, the FM‐NPs are loaded in an injectable alginate hydrogel together with granulocyte‐macrophage colony‐stimulating factor (GM‐CSF). GM‐CSF releases rapidly and recruits DCs to hydrogel, while FM‐NPs retain in hydrogel to continuously interconnected with DCs, enriching mature DCs loaded with tumor antigens. In the 4T1 mouse breast tumor model, this hydrogel promotes the maturation of DCs in tumor‐draining lymph nodes and induces sufficient effector memory T cells that migrate to the tumor microenvironment. This successfully converts the “cold” tumors to “hot”, thus exerting a significant antitumor effect synergized with the PD‐1 antibody. It is also verified the inhibitory effect of FM‐NPs using human gastric cancer organoids. Altogether, these findings demonstrate the application potential for the bifunctional fusion membrane‐based hydrogel as an autologous tumor vaccine by activating DCs.
Direct Plasma‐Enhanced‐Chemical‐Vapor‐Deposition Syntheses of Vertically Oriented Graphene Films on Functional Insulating Substrates for Wide‐Range Applications
Authors: Zhou Fan , Shan Junjie , Cui Lingzhi , Qi Yue , Hu Jingyi , Zhang Yanfeng , Liu Zhongfan
Published: April 2022

Graphene has inspired wide‐range research interests and practical applications due to its intriguing materials properties and versatile application prospects. Specifically, vertically oriented graphene (VG) constructed by vertically aligned nanosheets emerges as a unique material type, usually achieved through a plasma‐enhanced chemical vapor deposition (PECVD) route. The VG films possess abundant exposed active edges, large surface areas, relatively high electrical conductivity, and excellent thermal property in both in‐plane and out‐of‐plane directions. Direct synthesizing of such VG films on various functional substrates enables their transfer‐free integrations and direct applications in thermal management, sensing, energy storage and conversion, etc. In this review article, it is planned to showcase the recent advances in direct PECVD growth of VG films on some novel functional insulating substrates (e.g., glass, functional ceramics), mainly in terms of improving the electrical conductivity, enhancing the interfacial adhesion, and graphene growth orientation modulation. Meanwhile, the applications of the PECVD‐derived products in various new fields will also be discussed, such as photothermal conversion, switchable windows, light attenuation in photography, transparent heating, and thermal management for high‐power devices. Finally, current challenges and future opportunities will also be presented regarding controllable syntheses of high‐quality VG films and practical application explorations in different fields.
Reinforced Layered Double Hydroxide Oxygen‐Evolution Electrocatalysts: A Polyoxometallic Acid Wet‐Etching Approach and Synergistic Mechanism
Authors: Cai Zhengyang , Wang Ping , Zhang Jiajia , Chen Aiying , Zhang Jiangwei , Yan Ya , Wang Xianying
Published: April 2022

Nickel–iron‐based layered double hydroxides (NiFe LDHs) have attracted tremendous research and industrial interests for oxygen evolution reaction (OER) electrocatalysis. However, methodologies on simultaneous regulation of performance‐influencing factors remain scarce and their real synergistic effects are not clear enough. Herein, a versatile polyoxometallic acids (POMs) etching approach is reported to ingeniously reconstruct NiFe LDH, including 3D morphological nanotailoring, Fe3+ and α‐Ni(OH)2 active species reconfiguration, creation of multiple Ni, Fe, and O vacancies, and intercalation of POM polyanionic clusters. The experimental and theoretical data collaboratively unveil that control of the key performance‐influencing factors and their multiple synergistic mechanisms dominantly contribute to the step‐like OER performance enhancement. The reinforced electrocatalyst is further produced with low cost and high performance up to Ф180 mm in diameter, showing its feasibility and advancement of the promising configuration of NiFe LDH‐PMo12(+) II Ni@NiFe LDH(−) for alkaline anion‐exchange‐membrane electrode stack cells. Furthermore, to mathematically evaluate the evolution, a novel empirical formula is proposed for quantitative identification of structure–activity correlations, which offers an opportunity for first and fast reliability on materials screening.
Structural Reconstruction of Catalysts in Electroreduction Reaction: Identifying, Understanding, and Manipulating
Authors: Wang Wenbin , Duan Junyuan , Liu Youwen , Zhai Tianyou
Published: April 2022

Electroreduction transformation of small molecules (CO2, N2, and H2O) into chemical feedstocks offers a promising approach to eliminate carbon emissions and harness renewable energy. Most cathodic catalysts often undergo structural transformation under operating electroreduction conditions. These structural reconstructions are reflected in changes in their catalytic activity. In‐depth understanding of the change of active sites and influence parameters of reconstruction behaviors is an essential precondition for the design of highly efficient catalysts. Despite the previous achievements, comprehensive insight toward the structural evolution mechanism in cathodic catalysts, compared to anode ones, under reaction conditions is still lacking. Herein, an overview of structural reconstruction for cathodic catalysts in terms of fundamental mechanisms, reconstruction process, advanced characterizations, and influencing parameters is provided. On this basis, the typical strategies for manipulating the structural reconfiguration of catalysts are also explicitly discussed from the catalyst structure and working environment. By delivering the mechanism, strategies, insights, and techniques, this review will provide a comprehensive understanding of the structural reconstruction of cathodic catalysts in electroreduction reactions and future guidelines for their rational development.
Boosting Electrochemical Styrene Transformation via Tandem Water Oxidation over a Single‐Atom Cr1/CoSe2 Catalyst
Authors: Dang Kun , Dong Hongliang , Wang Ligang , Jiang Mai , Jiang Sen , Sun Wenming , Wang Dingsheng , Tian Yang
Published: April 2022

Electrocatalytic oxidation of organics using water as the oxygen source is a prospective but challenging method to produce high‐value‐added chemicals; especially, the competitive oxygen evolution reaction (OER) limits its efficiency. Herein, a tandem catalysis strategy based on a single‐atom catalyst with Cr atoms atomically dispersed at a CoSe2 support (Cr1/CoSe2) is presented. Thereinto, Co and Cr sites are endowed with a specific function to activate water and styrene respectively, and the competition between the OER and styrene oxidation is turned into mutual benefits via cooperated active sites. Under a potential of 1.6 VAg/AgCl, excellent selectivity of 95% to benzaldehyde and a high conversion rate of styrene at 88% without any exogenous oxidizing reagent are achieved. Isotopic tracing, isotope‐labeled in situ Raman spectra, and detailed theoretical calculation further reveal the tandem mechanism, showing that the transfer of *OOH intermediates from the Co to the Cr sites serves as a bridge to link the oxidation of water and styrene. This work develops a new strategy for the co‐oxidation of multi‐species based on tandem catalysis, providing novel insights for the design of single‐atom catalysts.
Universal Dynamic Liquid Interface for Healing Perovskite Solar Cells
Authors: Guo Qiyao , Duan Jialong , Zhang Junshuai , Zhang Qiaoyu , Duan Yanyan , Yang Xiya , He Benlin , Zhao Yuanyuan , Tang Qunwei
Published: April 2022

Healing charge‐selective contact interfaces in perovskite solar cells (PSCs) highly determines the power conversion efficiency (PCE) and stability. However, the state‐of‐the‐art strategies are often static by one‐off formation of a functional interlayer, which delivers fixed interfacial properties during the subsequent operation. As a result, defects formed in‐service will gradually deteriorate the photovoltaic performances. Herein, a dynamic healing interface (DHI) is presented by incorporating a low‐melting‐point small molecule onto perovskite film surface for highly efficient and stable PSCs. Arising from the reduced non‐radiative recombination, the DHI boosts the PCE to 12.05% for an all‐inorganic CsPbIBr2 solar cell and 14.14% for a CsPbI2Br cell, as well as 23.37% for an FA0.92MA0.08PbI3 (FA = formamidinium, MA = methylammonium) cell. The solid‐to‐liquid phase conversion of DHI at elevated temperature causes a longitudinal infiltration into the bulk perovskite film to maximize the charge extraction, passivate defects at grain boundaries, and suppress ion migration. Furthermore, the stability is remarkably enhanced under air, heat, and persistent light‐irradiation conditions, paving a universal strategy for advanced perovskite‐based optoelectronics.
Monitoring Wound Healing with Topically Applied Optical NanoFlare mRNA Nanosensors
Authors: Hwang Jangsun , Seo Youngmin , Jeong Daun , Ning Xiaoyu , Wiraja Christian , Yang Lixia , Tan Chew Teng , Lee Jinhyuck , Kim Yesol , Kim Ji Won , Kim Dai Hyun , Choi Jonghoon , Lim Chin Yan , Pu Kanyi , Jang Woo Young , Xu Chenjie
Published: April 2022

An effective wound management strategy needs accurate assessment of wound status throughout the whole healing process. This can be achieved by examining molecular biomarkers including proteins, DNAs, and RNAs. However, existing methods for quantifying these biomarkers such as immunohistochemistry and quantitative polymerase chain reaction are usually laborious, resource‐intensive, and disruptive. This article reports the development and utilization of mRNA nanosensors (i.e., NanoFlare) that are topically applied on cutaneous wounds to reveal the healing status through targeted and semi‐quantitative examination of the mRNA biomarkers in skin cells. In 2D and 3D in vitro models, the efficacy and efficiency of these nanosensors are demonstrated in revealing the dynamic changes of mRNA biomarkers for different stages of wound development. In mouse models, this platform permits the tracking and identification of wound healing stages and a normal and diabetic wound healing process by wound healing index in real time.
DNA Walkers for Biosensing Development
Authors: Song Lu , Zhuge Ying , Zuo Xiaolei , Li Min , Wang Fang
Published: April 2022

The ability to design nanostructures with arbitrary shapes and controllable motions has made DNA nanomaterials used widely to construct diverse nanomachines with various structures and functions. The DNA nanostructures exhibit excellent properties, including programmability, stability, biocompatibility, and can be modified with different functional groups. Among these nanoscale architectures, DNA walker is one of the most popular nanodevices with ingenious design and flexible function. In the past several years, DNA walkers have made amazing progress ranging from structural design to biological applications including constructing biosensors for the detection of cancer‐associated biomarkers. In this review, the key driving forces of DNA walkers are first summarized. Then, the DNA walkers with different numbers of legs are introduced. Furthermore, the biosensing applications of DNA walkers including the detection‐ of nucleic acids, proteins, ions, and bacteria are summarized. Finally, the new frontiers and opportunities for developing DNA walker‐based biosensors are discussed.
Thermally Conductive AlN‐Network Shield for Separators to Achieve Dendrite‐Free Plating and Fast Li‐Ion Transport toward Durable and High‐Rate Lithium‐Metal Anodes
Authors: Guo Yue , Wu Qiang , Liu Liwei , Li Guochang , Yang Lijun , Wang Xizhang , Ma Yanwen , Hu Zheng
Published: April 2022

Lithium‐metal anodes suffer from inadequate rate and cycling performances for practical application mainly due to the harmful dendrite growth, especially at high currents. Herein a facile construction of the porous and robust network with thermally conductive AlN nanowires onto the commercial polypropylene separator by convenient vacuum filtration is reported. The so‐constructed AlN‐network shield provides a uniform thermal distribution to realize homogeneous Li deposition, super electrolyte‐philic channels to enhance Li‐ion transport, and also a physical barrier to resist dendrite piercing as the last fence. Consequently, the symmetric Li|Li cell presents an ultralong lifetime over 8000 h (20 mA cm−2, 3 mAh cm−2) and over 1000 h even at an unprecedented high rate (80 mA cm−2, 80 mAh cm−2), which is far surpassing the corresponding performances reported to date. The corresponding Li|LiFePO4 cell delivers a high specific capacity of 84.3 mAh g−1 at 10 C. This study demonstrates an efficient approach with great application potential toward durable and high‐power Li–metal batteries and even beyond.
A Comprehensive Understanding of the Aging Effects of Extreme Fast Charging on High Ni NMC Cathode
Authors: Tanim Tanvir R. , Yang Zhenzhen , Finegan Donal P. , Chinnam Parameswara R. , Lin Yulin , Weddle Peter J. , Bloom Ira , Colclasure Andrew M. , Dufek Eric J. , Wen Jianguo , Tsai Yifen , Evans Michael C. , Smith Kandler , Allen Jeffery M. , Dickerson Charles C. , Quinn Alexander H. , Dunlop Alison R. , Trask Stephen E. , Jansen Andrew N.
Published: April 2022

As the battery industry shifts toward high Ni content cathodes, such as LiNi0.8Mn0.1Co0.1O2 [NMC811], a complete understanding of the degradation mechanisms of NMC811 under extreme fast charging (XFC) (XFC, ≤10–15 min charging) conditions is needed. Such comprehensive understanding would identify the most critical materials gaps that need to be addressed for enabling XFC long‐life cells for electric vehicles. This study maps out the key aging mechanisms for NMC811 cycled at different XFC conditions (between 1C and 9C) for up to 1000 cycles. To acquire a fundamental understanding of utilization and degradation, cells are evaluated using a range of electrochemical techniques, and multimodal and multiscale microscopy techniques to quantify chemical, structural, and crystallographic degradation as a function of cycling conditions for the NMC cathode. When comparing NMC811 to NMC532, it is observed that NMC811 has a greater subsurface crystallographic degradation and displays a similar magnitude of subparticle cracking. However, the NMC811 maintains superior performance despite those advanced degradations. The superior cycle life performance is attributed to the NMC811 particles having radially oriented grains and improved transport properties. NMC811 shows between 4.6× and 3.15× reduction in capacity fade than NMC532 for charging rates between 4C (e.g., 15‐min charging) and 6C (10‐min charging).
A Polymerized‐Ionic‐Liquid‐Based Polymer Electrolyte with High Oxidative Stability for 4 and 5 V Class Solid‐State Lithium Metal Batteries
Authors: Fu Chengyin , Homann Gerrit , Grissa Rabeb , Rentsch Daniel , Zhao Wengao , Gouveia Tom , Falgayrat Anaïs , Lin Rongying , Fantini Sébastien , Battaglia Corsin
Published: April 2022

Polymer solid electrolytes for solid‐state batteries typically suffer from low ionic conductivity and low oxidative stability. Herein, a polymer electrolyte based on a polymerized ionic liquid and an ionic liquid plasticizer offering simultaneously a high room‐temperature ionic conductivity of 0.8 mS cm−1 and a high oxidative stability >5.0 V versus Li+/Li, is reported. The electrolyte is compatible with lithium metal and non‐flammable upon direct flame exposure. In symmetric lithium metal cells, the electrolyte enables stable lithium plating and stripping at 0.1 mA cm−2 with a capacity of 1 mAh cm−2 per half cycle for over 1700 h at 25 °C. Cells with a lithium metal anode cycled against a state‐of‐the‐art high‐energy uncoated layered LiNi0.8Mn0.1Co0.1O2 cathode achieve an initial capacity of 162 mA h g−1 and a capacity retention of 72% after 600 cycles to an upper cut‐off voltage of 4.4 V at 25 °C. Cells with a high‐voltage spinel LiMn1.5Ni0.5O4 cathode reach an initial capacity of 132 mAh g−1 and a capacity retention of 76% after 300 cycles to an upper cut‐off voltage of 5 V at 25 °C, confirming the high oxidative stability and technological potential of this electrolyte for high‐voltage solid‐state lithium metal batteries.
Atomic‐Level Platinum Filling into Ni‐Vacancies of Dual‐Deficient NiO for Boosting Electrocatalytic Hydrogen Evolution
Authors: Yan Yaotian , Lin Jinghuang , Xu Tianxiong , Liu Baishen , Huang Keke , Qiao Liang , Liu Shude , Cao Jian , Jun Seong Chan , Yamauchi Yusuke , Qi Junlei
Published: April 2022

Developing low‐cost and high‐efficiency catalysts for sustainable hydrogen production through electrocatalytic hydrogen evolution reaction (HER) is crucial yet remains challenging. Here, a strategy is proposed to fill Ni‐vacancy (Niv) sites of dual‐deficient NiO (D‐NiO‐Pt) deliberately created by Ar plasma with homogeneously distributed Pt atoms driven by oxygen vacancies (Ov). The incorporated Pt atoms filling the Niv reduce the formation energy to increase crystal stability, and subsequently combine with additional Ov to tune the electronic structure of the surrounding Ni sites. Thus, a more ideal hydrogen adsorption free energy (ΔGH*) closer to 0 of Ni sites and Pt sites can be achieved. As a result, the D‐NiO‐Pt electrode achieves superior mass activity of ≈1600 mA mg−1 (normalized by platinum) and nearly negligible loss of activity during long‐term operation, which is much better than as‐prepared Pt‐containing NiO catalysts without plasma treatment. A low overpotential of 20 mV is required for the D‐NiO‐Pt at 10 mA cm−2 in alkaline HER, outperforming that of the commercial Pt/C. In addition, the universal access to the other Ni‐based compounds including nickel phosphide (Ni2P), nickel sulfide (Ni0.96S), and nickel selenide (NiSe2) is also demonstrated by employing a vacancy‐driven Pt filling mechanism.
Indigo: A Natural Molecular Passivator for Efficient Perovskite Solar Cells
Authors: Guo Junjun , Sun Jianguo , Hu Long , Fang Shiwen , Ling Xufeng , Zhang Xuliang , Wang Yao , Huang Hehe , Han Chenxu , Cazorla Claudio , Yang Yingguo , Chu Dewei , Wu Tom , Yuan Jianyu , Ma Wanli
Published: April 2022

Organic–inorganic hybrid lead halide perovskite solar cells have made unprecedented progress in improving photovoltaic efficiency during the past decade, while still facing critical stability challenges. Herein, the natural organic dye Indigo is explored for the first time to be an efficient molecular passivator that assists in the preparation of high‐quality hybrid perovskite film with reduced defects and enhanced stability. The Indigo molecule with both carbonyl and amino groups can provide bifunctional chemical passivation for defects. In‐depth theoretical and experimental studies show that the Indigo molecules firmly binds to the perovskite surfaces, enhancing the crystallization of perovskite films with improved morphology. Consequently, the Indigo‐passivated perovskite film exhibits increased grain size with better uniformity, reduced grain boundaries, lowered defect density, and retarded ion migration, boosting the device efficiency up to 23.22%, and ≈21% for large‐area device (1 cm2). Furthermore, the Indigo passivation can enhance device stability in terms of both humidity and thermal stress. These results provide not only new insights into the multipassivation role of natural organic dyes but also a simple and low‐cost strategy to prepare high‐quality hybrid perovskite films for optoelectronic applications based on Indigo derivatives.
Simultaneous Incorporation of V and Mn Element into Polyanionic NASICON for High Energy‐Density and Long‐Lifespan Zn‐Ion Storage
Authors: Wu Zeyi , Ye Fei , Liu Qiang , Pang Ruilvjing , Liu Yang , Jiang Le , Tang Zilong , Hu Linfeng
Published: April 2022

Aqueous Zn‐ion battery (AZIB) has attracted huge attention due to its distinct advantages such as abundant zinc sources, low development cost, high security, and environmental friendliness compared to traditional commercialized batteries. Developing novel cathode materials with high energy density and long lifespan is very important for the practical application of AZIB in the coming years. Herein, V and Mn elements are simultaneously incorporated into the NASICON host to make use of the electrochemical redox reaction in both V and Mn transition metal elements for aqueous Zn‐ion storage. A significant increase in both capacity and working voltage has been observed after Mn doping into Na3V2(PO4)3 to form Na4VMn(PO4)3. Taking advantage of the merits of both high capacity and high voltage, the Na4VMn(PO4)3@Graphene cathode delivers an optimal energy density of 309.7 Wh kg−1 with very stable cycle performance (89.1% capacity retention after 3000 cycles at 5.0 A g−1). A two‐step electron transfer mechanism between V4+/V3+ and Mn3+/Mn2+ redox couple in Na4VMn(PO4)3 has been revealed during the electrochemical process for Zn‐ion storage.
Aggregation‐induced emission luminogens for organic light‐emitting diodes with a single‐component emitting layer
Authors: Hwang Jinhyo , Nagaraju Peethani , Cho Min Ju , Choi Dong Hoon
Published: April 2022

Organic light‐emitting diodes (OLEDs) have garnered increasing attention as a promising candidate for application in next‐generation displays and solid‐state lighting devices. The doping technique commonly used to fabricate light‐emitting layers (EMLs) of OLEDs disperses the emitting material in a host matrix to mitigate aggregation‐induced quenching (ACQ). Alternatively, owing to their high efficiency and ease of manufacture, nondoped OLEDs have been developed as a substitute for doped OLEDs. When fabricating nondoped OLEDs, it is essential to suppress the ACQ effect in the EML and efficiently utilize the generated excitons for radiative decay. Since the discovery of aggregation‐induced emission (AIE) by Tang et al., significant work has been done to improve the stability and efficiency of nondoped OLEDs based on fluorescent AIE luminogens (AIEgens). Fluorescent AIEgens, synthesized using various molecular frameworks, such as silole, tetra/triphenylethylene, tetraphenylpyrazine, and tetraphenylbenzene, exhibit high photoluminescence quantum yields in the solid state. Therefore, many studies have reported that fluorescent AIEgen‐based OLEDs have excellent external quantum efficiency and exhibit emission at various wavelengths, including deep‐blue/blue/green emission. With the development of fluorescent AIEgens, delayed fluorescent AIEgens with efficient triplet utilization through reverse intersystem crossing and AIE properties have been adopted as ideal emitters and used in nondoped OLEDs. This review systematically discusses and summarizes recent reports on the development of AIEgens for nondoped OLEDs by grouping them into fluorescent and delayed fluorescent AIEgens. The purpose of this review is to provide deep insights into the design of novel AIEgens for high‐performance nondoped OLEDs.
Factors linked to participant attrition in a longitudinal occupational health surveillance program
Authors: Hubbell Zachariah , Howard Sara , Golden Ashley , Stange Bill , Cragle Donna , Dally Miranda , McInerney John , Newman Lee S.
Published: April 2022

Background

For occupational medical screening programs focused on long‐term health surveillance, participant attrition is a significant barrier to success. We investigate demographic, medical history, and clinical data from National Supplemental Screening Program (NSSP) examinees for association with likelihood of return for a second exam (rescreening).

Methods

A total of 15,733 individuals completed at least one NSSP exam before December 31, 2016; of those, 4832 also completed a second exam on or before December 31, 2019. Stepwise logistic regression models were used to identify variables associated with whether a participant was rescreened in the NSSP.

Results

Individuals were less likely to return for rescreening if they had a history of any cancer; cardiovascular problems; diabetes or kidney disease; or if they used insulin. Age at time of first exam and job site category significantly influenced likelihood of return. Workers categorized as “guests” were more likely to return. Participants were less likely to return if they had an abnormal urinalysis, abnormal pulmonary function, pneumoconiosis, aortic atherosclerosis, or hearing loss at their initial exam. Participants who received a chest X‐ray at their initial screening were more likely to return.

Conclusions

The presence of health problems is strongly linked to screening program attrition. Participants who are older at the time of their initial screening exam are less likely to return. The discovery of several strong demographic, medical, and job associations reveals the importance for medical screening programs to understand and address factors that influence participant retention and, consequently, the effectiveness of long‐term health surveillance activities.
Stereodefined Skipped Dienes through Iridium‐Catalyzed Formal Addition of Tertiary Allylic C−H Bonds to Alkynes
Authors: Wang Zi‐Xuan , Gao Peng‐Chao , Lin En‐Ze , Li Bi‐Jie
Published: April 2022

Preparation of skipped dienes with a quaternary carbon center at the C‐3 position remains a synthetic challenge. We report here an iridium‐catalyzed formal addition of tertiary sp3 C−H bond to alkyne for the facile preparation of skipped dienes. The tertiary allylic C−H bond is cleaved regioselectively, at the site of which a new C−C bond is formed. Enantioselective construction of acyclic quaternary carbon stereocenters is also demonstrated.
Reticular Synthesis of Hydrogen‐Bonded Organic Frameworks and Their Derivatives via Mechanochemistry
Authors: Qin Wei‐Kang , Si Duan‐Hui , Yin Qi , Gao Xiang‐Yu , Huang Qian‐Qian , Feng Ya‐Nan , Xie Lei , Zhang Shuo , Huang Xin‐Song , Liu Tian‐Fu , Cao Rong
Published: April 2022

Rational synthesis of hydrogen‐bonded organic frameworks (HOFs) with predicted structure has been a long‐term challenge. Herein, by using the efficient, simple, low‐cost, and scalable mechanosynthesis, we demonstrate that reticular chemistry is applicable to HOF assemblies based on building blocks with different geometry, connectivity, and functionality. The obtained crystalline HOFs show uniform nano‐sized morphology, which is challenging or unachievable for conventional solution‐based methods. Furthermore, the one‐pot mechanosynthesis generated a series of Pd@HOF composites with noticeably different CO oxidation activities. In situ DRIFTS studies indicate that the most efficient composite, counterintuitively, shows the weakest CO affinity to Pd sites while the strongest CO affinity to HOF matrix, revealing the vital role of porous matrix to the catalytic performance. This work paves a new avenue for rational synthesis of HOF and HOF‐based composites for broad application potential.
Gas‐Phase Mechanism of O.−/Ni2+‐Mediated Methane Conversion to Formaldehyde
Authors: Li Ya‐Ke , Müller Fabian , Schöllkopf Wieland , Asmis Knut R. , Sauer Joachim
Published: April 2022

The gas‐phase reaction of NiAl2O4+ with CH4 is studied by mass spectrometry in combination with vibrational action spectroscopy and density functional theory (DFT). Two product ions, NiAl2O4H+ and NiAl2O3H2+, are identified in the mass spectra. The DFT calculations predict that the global minimum‐energy isomer of NiAl2O4+ contains Ni in the +II oxidation state and features a terminal Al−O.− oxygen radical site. They show that methane can react along two competing pathways leading to formation of either a methyl radical (CH3⋅) or formaldehyde (CH2O). Both reactions are initiated by hydrogen atom transfer from methane to the terminal O.− site, followed by either CH3⋅ loss or CH3⋅ migration to an O2− site next to the Ni2+ center. The CH3⋅ attaches as CH3+ to O2− and its unpaired electron is transferred to the Ni‐center reducing it to Ni+. The proposed mechanism is experimentally confirmed by vibrational spectroscopy of the reactant and two different product ions.
In‐Sequence High‐Specificity Dual‐Reporter Unlocking of Fluorescent Probe Enables the Precise Identification of Atherosclerotic Plaques
Authors: Ye Zhuo , Ji Moxuan , Wu Kefeng , Yang Jie , Liu An‐An , Sun Wei , Ding Dan , Liu Dingbin
Published: April 2022

The formation of atherosclerotic plaques is the root cause of various cardiovascular diseases (CVDs). Effective CVD interventions thus call for precise identification of the plaques to aid clinical assessment, diagnosis, and treatment of such diseases. In this study, we introduce a dual‐target sequentially activated fluorescence reporting system, termed in‐sequence high‐specificity dual‐reporter unlocking (iSHERLOCK), to precisely identify the atherosclerotic plaques in vivo and ex vivo. ISHERLOCK was achieved by creating a three‐in‐one fluorescent probe that permits highly specific and sensitive detection of lipid droplets and hypochlorous acid via “off‐on” and ratiometric readouts, respectively. Based on this format, the upregulated lipid accumulation and oxidative stress—the two hallmarks of atherosclerosis (AS)—were specifically measured in the atherosclerotic plaques, breaking through the barrier of precise tissue biopsy of AS and thus aiding effective CVD stewardship.
ESA's Cometary Mission Rosetta—Re‐Characterization of the COSAC Mass Spectrometry Results
Authors: Leseigneur Guillaume , Bredehöft Jan Hendrik , Gautier Thomas , Giri Chaitanya , Krüger Harald , MacDermott Alexandra J. , Meierhenrich Uwe J. , Caro Guillermo M. Muñoz , Raulin François , Steele Andrew , Steininger Harald , Szopa Cyril , Thiemann Wolfram , Ulamec Stephan , Goesmann Fred
Published: April 2022

The most pristine material of the Solar System is assumed to be preserved in comets in the form of dust and ice as refractory matter. ESA's mission Rosetta and its lander Philae had been developed to investigate the nucleus of comet 67P/Churyumov–Gerasimenko in situ. Twenty‐five minutes after the initial touchdown of Philae on the surface of comet 67P in November 2014, a mass spectrum was recorded by the time‐of‐flight mass spectrometer COSAC onboard Philae. The new characterization of this mass spectrum through non‐negative least squares fitting and Monte Carlo simulations reveals the chemical composition of comet 67P. A suite of 12 organic molecules, 9 of which also found in the original analysis of this data, exhibit high statistical probability to be present in the grains sampled from the cometary nucleus. These volatile molecules are among the most abundant in the comet's chemical composition and represent an inventory of the first raw materials present in the early Solar System.
Multifunctional benzoin derivatives based macrophotoinitiators: Synthesis, inorganic fillers modification, and fabrication of composite materials
Authors: Ohar Halyna , Tokareva Maria , Nagursky Oleg , Mosnáček Jaroslav , Tokarev Viktor
Published: April 2022

Photopolymer composites are the materials with wide application potential in paints and varnishes, diverse lithographic processes, electronics, medicine, and so forth. Here a new approach to the synthesis of macrophotoinitiators (MPIs) were developed and their effective application for curing polymer composites after immobilization on the surface of diverse mineral fillers was demonstrated. The MPIs were synthesized by reaction of benzoin or 3‐hydroxy‐1,2‐diphenyl‐2‐(propan‐2‐yloxy)propan‐1‐one as a photodissociating species with a copolymer of maleic anhydride with methyl methacrylate as carrier. Chemical structure of MPIs and the content of the tethered photoinitiating moieties were determined using 1NMR‐, IR‐, and UV‐spectroscopies. Photolysis of MPIs was investigated in details using a spot‐light curing system. It was demonstrated that MPIs are effective surface modifiers of mineral fillers, such as titanium dioxide, zinc oxide, and nanohydroxyapatite; and behave as effective photoinitiators. The benefits of using the fillers surface‐modified by MPIs in photo‐curable polymer composites were discussed.
Sodium alginate‐cl‐poly (N,N‐dimethyl acryl amide‐co‐2‐acrylamino‐2‐methyl‐1‐propane sulphonic acid)/titanium dioxide nanocomposite hydrogel: An efficient dye‐removing agent
Authors: Samanta Santu Kumar , Mandal Barun , Tripathy Tridib
Published: April 2022

Sodium alginate (SAG) crosslinked poly (N,N‐dimethyl Acrylamide‐co‐2 acrylamino‐2‐methyl‐1‐propane sulfonic acid)/Titanium dioxide [SAG‐cl‐poly(N,N‐DMA‐co‐AMPS)/TiO2] nanocomposite hydrogel (NCHG) was prepared by in situ crosslinked free radical polymerization technique using SAG, a mixture of DMA and AMPS and titanium isopropoxide in presence of methylene‐bis‐acrylamide as a cross linking agent. Different characterization techniques are used to characterize NCHG. Water swelling behavior of NCHG together with swelling kinetics is evaluated. Maximum swelling (35% at 30 min) is observed at pH 8. NCHG is used for the removal of one cationic dye methylene blue (MB) and one anionic dye carmosine‐A (CR‐A) from their aqueous solution. Adsorption dynamics, kinetics and isotherms are evaluated. Maximum dye adsorption occurs at pH 8 and 2, at time 50 min for both the cases, at temperature 60°C, 40°C for MB and CR‐A respectively. Pseudo‐second order kinetics and Langmuir isotherm model are followed for all the two cases with Qmax 403.22 mg.g−1, 106.26 mg.g−1 and the R2 value 0.9987 and 0.9950 for MB and CR‐A respectively. Evaluation of thermodynamic parameters of the adsorption indicates that the adsorption is spontaneous in nature for the two dyes.
Healing the divide: From black‐and‐white to a new color
Authors: Smolar Andrew I. , Eichen Ann
Published: April 2022

In this study, the authors identify and describe factors that have contributed to an acrimonious political divide in the United States. Informed by a developmental perspective, the authors first establish the universal motive for group belonging. Next, they describe how group forces have organized citizens into hostile groups built around these variables: expansion of technology, global warming, rising immigration, cultish leader/follower dynamics, religion, national attitudes toward the pandemic, and characteristics of the national leader. The authors propose several solutions to the current divide, including the elevation of the school to the pinnacle of the civic public square.
Protection effectiveness and sea urchin predation risk: The role of roving predators beyond the boundaries of a marine protected area in the Western Mediterranean Sea
Authors: Farina Simone , Ceccherelli Giulia , Piazzi Luigi , Grech Daniele , Panzalis Pieraugusto , Navone Augusto Giuseppe , Guala Ivan
Published: April 2022

Effective marine protected areas (MPAs) increase top predator density. Accordingly, a large abundance of predatory fish potentially increases predation risk for sea urchins inside an MPA.

Intensity of predation was investigated for the sea urchin Paracentrotus lividus at a Mediterranean MPA. Predation rates were estimated for three levels of protection (full, partial, and absent) and two habitats (rocky reefs and Posidonia oceanica meadows). The natural density of sea urchins was correlated with predator biomass (fish sparids Diplodus spp. and Sparus aurata and the gastropod Hexaplex trunculus), and predation risk was evaluated through a tethering experiment.

Significantly higher fish predation was found on the rocky reefs of the fully and non‐protected areas than in the partially protected area. These findings are consistent with the sparid biomass estimated in the fully and partially protected areas. However, a discrepancy between high predation risk and low sparid biomass was detected outside of the MPA's northern boundary, where marine farms (fish and mussels) are present. Benthic predator biomass also increased significantly across the northern boundary, but its predation activity was negligible.

The low predatory fish biomass and low sea urchin density suggest a top‐down control by roving predatory fish on the rocky reefs of the non‐protected area, in proximity to the fish farms. Similarly, a significant gradient of benthic predator biomass and low sea urchin density suggest potential predation interactions inside the P. oceanica meadows across the northern MPA boundary near the mussel farms.

This study highlights deviations from the expected trophic interactions outside the MPA that could be caused by aquaculture activities. Our understanding of the potential synergies between the MPAs and the nearby human activities needs to be broadened to improve the effectiveness of both ecosystem conservation and resource management.
Tuning the Stereoselectivity of an Intramolecular Aldol Reaction by Precisely Modifying a Metal‐Organic Framework Catalyst
Authors: Cornelio Joel , Telfer Shane G.
Published: April 2022

We report the catalysis of an enantioselective, intramolecular aldol reaction accelerated by an organocatalyst embedded in a series of multicomponent metal‐organic frameworks. By precisely programming the pore microenvironment around the site of catalysis, we show how important features of an intramolecular aldol reaction can be tuned, such as the substrate consumption, enantioselectivity, and degree of dehydration of the products. This tunability arises from non‐covalent interactions between the reaction participants and modulator groups that occupy positions in the framework remote from the catalytic site. Further, the catalytic moiety can be switched form one framework linker to another. Deliberately building up microenvironments that can influence the outcome of reaction processes in this way is not possible in conventional homogenous catalysts but is reminiscent of enzymes.
Heterogeneity of social cognitive performance in autism and schizophrenia
Authors: Hajdúk Michal , Pinkham Amy E. , Penn David L. , Harvey Philip D. , Sasson Noah J.
Published: April 2022

Autistic adults and those with schizophrenia (SCZ) demonstrate similar levels of reduced social cognitive performance at the group level, but it is unclear whether these patterns are relatively consistent or highly variable within and between the two conditions. Seventy‐two adults with SCZ (52 male, Mage = 28.2 years) and 94 with diagnoses on the autism spectrum (83 male, Mage = 24.2 years) without intellectual disability completed a comprehensive social cognitive battery. Latent profile analysis identified four homogeneous subgroups that were compared on their diagnosis, independent living skills, neurocognition, and symptomatology. Two groups showed normative performance across most social cognitive tasks but were differentiated by one having significantly higher hostility and blaming biases. Autistic participants were more likely to demonstrate fully normative performance (46.8%) than participants with SCZ, whereas normative performance in SCZ was more likely to co‐occur with increased hostility and blaming biases (36.1%). Approximately 43% of participants in the full sample were classified into the remaining two groups showing low or very low performance. These participants tended to perform worse on neurocognitive tests and have lower IQ and fewer independent living skills. The prevalence of low performance on social cognitive tasks was comparable across clinical groups. However, nearly half of autistic participants demonstrated normative social cognitive performance, challenging assumptions that reduced social cognitive performance is inherent to the condition. Subgrouping also revealed a meaningful distinction between the clinical groups: participants with SCZ were more likely to demonstrate hostility biases than autistic participants, even when social cognitive performance was otherwise in the typical range.

Lay Summary

Social cognition refers to the perception and interpretation of social information. Previous research has shown that both autistic people and those with schizophrenia demonstrate reduced performance on traditional social cognitive tasks, which we replicate here at the group level. However, we also found that almost half of autistic participants performed in the normal range. Over a third of participants with schizophrenia did as well, but for them this performance was accompanied by a hostility bias not commonly found in the autistic sample. Taken together, findings challenge assumptions that difficulties in social cognition are a uniform characteristic of these clinical conditions in those without intellectual disability.