bluuebunny/crossref_metadata_2025 huggingface dataset:
Nitric Oxide‐Assisted Photodynamic Therapy for Enhanced Penetration and Hypoxic Bacterial Biofilm Elimination
Authors: Lv Xinyi , Jiang Jingai , Ren Jie , Li Hui , Yang Dongliang , Song Xuejiao , Hu Yanling , Wang Wenjun , Dong Xiaochen
Published: July 2023

The presence of a biofilm matrix barrier and hypoxic microenvironment within the biofilm significantly impedes the efficacy of photodynamic therapy for bacterial biofilm infections. Herein, a phototherapeutic nanoagent with type‐I photodynamic behavior and nitric oxide (NO) release performance is reported for overcoming biofilm‐associated infectious diseases. Sodium nitroprusside (SNP), a NO donor, is loaded onto amino‐modified mesoporous silica nanoparticles (MSN) to form MSN@SNP NPs. The resulting nanoparticles are further modified with a porphyrin‐based metal–organic framework (Ti‐TCPP MOF) to obtain MSN@MOF/SNP NPs (MMS NPs) for phototherapeutic applications. In the hypoxia biofilm microenvironment, the MMS NPs release NO to enhance the biofilm permeability and induce the generation of hydroxyl radical (•OH) and superoxide anion radical (O2•−) via Type‐I photodynamic pathway under laser irradiation. Subsequently, the biofilm‐associated infections are effectively eliminated through reactive oxygen species (ROS) and NO gas synergistic therapy. In addition, NO also stimulates collagen deposition and promotes angiogenesis in vivo. Therefore, the MMS NPs efficiently treat biofilm‐related infections, providing an alternative approach to combat biofilm‐associated infectious diseases.
Metal–Organic Frameworks and Their Composites for Chronic Wound Healing: From Bench to Bedside
Authors: Xiong Yuan , Feng Qian , Lu Li , Qiu Xingan , Knoedler Samuel , Panayi Adriana Christine , Jiang Dongsheng , Rinkevich Yuval , Lin Ze , Mi Bobin , Liu Guohui , Zhao Yanli
Published: August 2023

Chronic wounds are characterized by delayed and dysregulated healing processes. As such, they have emerged as an increasingly significant threat. The associated morbidity and socioeconomic toll are clinically and financially challenging, necessitating novel approaches in the management of chronic wounds. Metal–organic frameworks (MOFs) are an innovative type of porous coordination polymers, with low toxicity and high eco‐friendliness. Documented anti‐bacterial effects and pro‐angiogenic activity predestine these nanomaterials as promising systems for the treatment of chronic wounds. In this context, the therapeutic applicability and efficacy of MOFs remain to be elucidated. It is, therefore, reviewed the structural–functional properties of MOFs and their composite materials and discusses how their multifunctionality and customizability can be leveraged as a clinical therapy for chronic wounds.
Introducing a Phenyl End Group in the Inner Side Chains of A‐DA'D‐A Acceptors Enables High‐Efficiency Organic Solar Cells Processed with Nonhalogenated Solvent
Authors: Wu Xiangxi , Jiang Xin , Li Xiaojun , Zhang Jinyuan , Ding Kan , Zhuo Hongmei , Guo Jing , Li Jing , Meng Lei , Ade Harald , Li Yongfang
Published: July 2023

Power conversion efficiency (PCE) of organic solar cells (OSCs) processed by nonhalogenated solvents is unsatisfactory due to the unfavorable morphology. Herein, two new small molecule acceptors (SMAs) Y6‐Ph and L8‐Ph are synthesized by introducing a phenyl end group in the inner side chains of the SMAs of Y6 and L8‐BO, respectively, for overcoming the excessive aggregation of SMAs in the long‐time film forming processed by nonhalogenated solvents. First, the effect of the film forming time on the aggregation property and photovoltaic performance of Y6, L8‐BO, Y6‐Ph, and L8‐Ph is studied by using the commonly used solvents: chloroform (CF) (rapid film forming process) and chlorobenzene (CB) (slow film forming process). It is found that Y6‐ and L8‐BO‐based OSCs exhibit a dramatic drop in PCE from CF‐ to CB‐processed devices owing to the large phase separation, while the Y6‐Ph and L8‐Ph based OSCs show obviously increased PCEs Furthermore, L8‐Ph‐based OSCs processed by nonhalogenated solvent o‐xylene (o‐XY) achieved a high PCE of 18.40% with an FF of 80.11%. The results indicate that introducing a phenyl end group in the inner side chains is an effective strategy to modulate the morphology and improve the photovoltaic performance of the OSCs processed by nonhalogenated solvents.
Exceptional Microscale Plasticity in Amorphous Aluminum Oxide at Room Temperature
Authors: Frankberg Erkka J. , Lambai Aloshious , Zhang Jiahui , Kalikka Janne , Khakalo Sergei , Paladino Boris , Cabrioli Mattia , Mathews Nidhin G. , Salminen Turkka , Hokka Mikko , Akola Jaakko , Kuronen Antti , Levänen Erkki , Di Fonzo Fabio , Mohanty Gaurav
Published: July 2023

Oxide glasses are an elementary group of materials in modern society, but brittleness limits their wider usability at room temperature. As an exception to the rule, amorphous aluminum oxide (a‐Al2O3) is a rare diatomic glassy material exhibiting significant nanoscale plasticity at room temperature. Here, it is shown experimentally that the room temperature plasticity of a‐Al2O3 extends to the microscale and high strain rates using in situ micropillar compression. All tested a‐Al2O3 micropillars deform without fracture at up to 50% strain via a combined mechanism of viscous creep and shear band slip propagation. Large‐scale molecular dynamics simulations align with the main experimental observations and verify the plasticity mechanism at the atomic scale. The experimental strain rates reach magnitudes typical for impact loading scenarios, such as hammer forging, with strain rates up to the order of 1 000 s−1, and the total a‐Al2O3 sample volume exhibiting significant low‐temperature plasticity without fracture is expanded by 5 orders of magnitude from previous observations. The discovery is consistent with the theoretical prediction that the plasticity observed in a‐Al2O3 can extend to macroscopic bulk scale and suggests that amorphous oxides show significant potential to be used as light, high‐strength, and damage‐tolerant engineering materials.
Tuning Ligands Ratio Allows for Controlling Gold Nanocluster Conformation and Activating a Nonantimicrobial Thiol Fragrance for Effective Treatment of MRSA‐Induced Keratitis
Authors: Pang Zeyang , Ren Ning , Wu Yujie , Qi Jie , Hu Fupin , Guo Yuan , Xie Yangzhouyun , Zhou Dejian , Jiang Xingyu
Published: July 2023

Bacterial keratitis is a serious ocular disease that affects millions of people worldwide each year, among which ≈25% are caused by Staphylococcus aureus. With the spread of bacterial resistance, refractory keratitis caused by methicillin‐resistant S. aureus (MRSA) affects ≈120 000–190 000 people annually and is a significant cause of infectious blindness. Atomically precise gold nanoclusters (GNCs) recently emerged as promising antibacterial agents; although how the GNC structure and capping ligands control the antibacterial properties remains largely unexplored. In this study, by adjusting the ratio of a “bulky” thiol fragrance to a linear zwitterionic ligand, the GNC conformation is transformed from Au25(SR)18 to Au23(SR)16 species, simultaneously converting both inactive thiol ligands into potent antibacterial nanomaterials. Surprisingly, mixed‐ligand capped Au23(SR)16 GNCs exhibit superior antibacterial potency compared to their monoligand counterparts. The optimal GNC is highly potent against MRSA, showing >1024‐fold lower minimum inhibitory concentration than the corresponding free ligands. Moreover, it displays excellent potency in treating MRSA‐induced keratitis in mice with greatly accelerated corneal recovery (by approximately ninefold). Thus, this study establishes a feasible method to synthesize antibacterial GNCs by adjusting the ligand ratio to control GNC conformation and active non‐antibacterial ligands, thereby greatly increasing the repertoires for combating multidrug‐resistant bacterial infections.
Synthesis of 2H/fcc‐Heterophase AuCu Nanostructures for Highly Efficient Electrochemical CO2 Reduction at Industrial Current Densities
Authors: Zhou Xichen , Zhang An , Chen Bo , Zhu Shangqian , Cui Yu , Bai Licheng , Yu Jinli , Ge Yiyao , Yun Qinbai , Li Lujiang , Huang Biao , Liao Lingwen , Fu Jiaju , Wa Qingbo , Wang Gang , Huang Zhiqi , Zheng Long , Ren Yi , Li Siyuan , Liu Guangyao , Zhai Li , Li Zijian , Liu Jiawei , Chen Ye , Ma Lu , Ling Chongyi , Wang Jinlan , Fan Zhanxi , Du Yonghua , Shao Minhua , Zhang Hua
Published: July 2023

Structural engineering of nanomaterials offers a promising way for developing high‐performance catalysts toward catalysis. However, the delicate modulation of thermodynamically unfavorable nanostructures with unconventional phases still remains a challenge. Here, the synthesis of hierarchical AuCu nanostructures is reported with hexagonal close‐packed (2H‐type)/face‐centered cubic (fcc) heterophase, high‐index facets, planar defects (e.g., stacking faults, twin boundaries, and grain boundaries), and tunable Cu content. The obtained 2H/fcc Au99Cu1 hierarchical nanosheets exhibit excellent performance for the electrocatalytic CO2 reduction to produce CO, outperforming the 2H/fcc Au91Cu9 and fcc Au99Cu1. The experimental results, especially those obtained by in‐situ differential electrochemical mass spectroscopy and attenuated total reflection Fourier‐transform infrared spectroscopy, suggest that the enhanced catalytic performance of 2H/fcc Au99Cu1 arises from the unconventional 2H/fcc heterophase, high‐index facets, planar defects, and appropriate alloying of Cu. Impressively, the 2H/fcc Au99Cu1 shows CO Faradaic efficiencies of 96.6% and 92.6% at industrial current densities of 300 and 500 mA cm−2, respectively, as well as good durability, placing it among the best CO2 reduction electrocatalysts for CO production. The atomically structural regulation based on phase engineering of nanomaterials (PEN) provides an avenue for the rational design and preparation of high‐performance electrocatalysts for various catalytic applications.
Managing Interfacial Charged Defects with Multiple Active Sited Macrocyclic Valinomycin for Efficient and Stable Inverted Perovskite Solar Cells
Authors: He Zhangwei , Li Minghua , Jia Haoran , Yu Runnan , Zhang Yuling , Wang Ruyue , Dong Yiman , Liu Xiangyang , Xu Donghui , Tan Zhan'ao
Published: July 2023

The unavoidably positively and negatively charged defects at the interface between perovskite and electron transport layer (ETL) often lead to severe surface recombination and unfavorable energy level alignment in inverted perovskite solar cells (PerSCs). Inserting interlayers at this interface is an effective approach to eliminate charged defects. Herein, the macrocyclic molecule valinomycin (VM) with multiple active sites of ─C═O, ─NH, and ─O─ is employed as an interlayer at the perovskite/ETL contact to simultaneously eliminate positively and negatively charged defects. Combined with a series of theoretical calculations and experimental analyzes, it is demonstrated that the ─C═O and ─O─ groups in VM can immobilize the uncoordinated Pb2+ to manage the positively charged defect and the formation of N─H···I hydrogen bonding can recompense the formamidine vacancies to eliminate the negatively charged defect. In addition, the VM interlayer induces a favorable downshift band bending at the perovskite/ETL interface, facilitating charge separation and boosting charge transfer. Thanks to the reduced charged defects and favorable energy level alignment, the fabricated inverted PerSC delivers an outstanding power conversion efficiency of 24.06% with excellent long‐term ambient and thermal stability. This work demonstrates that managing charged defects via multiple functional groups and simultaneously regulating energy level alignment is a reliable strategy to boost the performance of PerSCs.
Antibubbles Enable Tunable Payload Release with Low‐Intensity Ultrasound
Authors: Moreno‐Gomez Nicolas , Athanassiadis Athanasios G. , Poortinga Albert T. , Fischer Peer
Published: July 2023

The benefits of ultrasound are its ease‐of‐use and its ability to precisely deliver energy in opaque and complex media. However, most materials responsive to ultrasound show a weak response, requiring the use of high powers, which are associated with undesirable streaming, cavitation, or temperature rise. These effects hinder response control and may even cause damage to the medium where the ultrasound is applied. Moreover, materials that are currently in use rely on all‐or‐nothing effects, limiting the ability to fine‐tune the response of the material on the fly. For these reasons, there is a need for materials that can respond to low intensity ultrasound with programmable responses. Here it is demonstrated that antibubbles are a low‐intensity‐ultrasound‐responsive material system that can controllably release a payload using acoustic pressures in the kilopascal range. Varying their size and composition tunes the release pressure, and the response can be switched between a single release and stepwise release across multiple ultrasound pulses. Observations using confocal and high‐speed microscopy reveal different ways that can lead to release. These findings lay the groundwork to design antibubbles that controllably respond to low‐intensity ultrasound, opening a wide range of applications ranging from ultrasound‐responsive material systems to carriers for targeted delivery.
Chirality Versus Symmetry: Electron's Spin Selectivity in Nonpolar Chiral Lead–Bromide Perovskites
Authors: Abhervé Alexandre , Mercier Nicolas , Kumar Anil , Das Tapan Kumar , Even Jacky , Katan Claudine , Kepenekian Mikaël
Published: August 2023

In the last decade, chirality‐induced spin selectivity (CISS), the spin‐selective electron transport through chiral molecules, has been described in a large range of materials, from insulators to superconductors. Because more experimental studies are desired for the theoretical understanding of the CISS effect, chiral metal‐halide semiconductors may contribute to the field thanks to their chiroptical and spintronic properties. In this regard, this work uses new chiral organic cations S‐HP1A and R‐HP1A (HP1A = 2‐hydroxy‐propyl‐1‐ammonium) to prepare 2D chiral halide perovskites (HPs) which crystallize in the enantiomorphic space groups P43212 and P41212, respectively. The fourfold symmetry induces antiferroelectricity along the stacking axis which, combined to incomplete Rashba‐like splitting in each individual 2D polar layer, results in rare spin textures in the band structure. As revealed by magnetic conductive‐probe atomic force microscopy (AFM) measurements, these materials show CISS effect with partial spin polarization (SP; ±40–45%). This incomplete effect is efficient enough to drive a chiro‐spintronic device as demonstrated by the fabrication of spin valve devices with magnetoresistance (MR) responses up to 250 K. Therefore, these stable lead–bromide HP materials not only represent interesting candidates for spintronic applications but also reveal the importance of polar symmetry‐breaking topology for spin selectivity.
Microvasculature‐on‐a‐Post Chip That Recapitulates Prothrombotic Vascular Geometries and 3D Flow Disturbance
Authors: Zhang Yingqi , Aye San‐Seint‐Seint , Cheng Vivian , Nasser Arian , Hong Tianbo , Vatankhah Parham , Jiang Fengtao , Zhao Yunduo Charles , Moldovan Laura , Sun Allan , Dupuy Alexander , Wang Yao , Li Zhiyong , Ang Timothy , Passam Freda , Yong Ken‐Tye , Ju Lining Arnold
Published: July 2023

Stenosis, characterized by partial vessel narrowing, alters blood hemodynamics and can lead to unpredictable thrombosis. Existing models struggle to accurately represent the complex vascular geometries and hemodynamics involved in such conditions. To address this challenge, a microvasculature‐on‐a‐post chip is developed to mimic partially stenotic vascular geometries and thrombogenicity, featuring isolated 3D micropost structures with variable sizes that recreate disturbed flow profiles. To emulate the diseased vessel wall, the post microfluidics are vascularized with a confluent layer of endothelial cells. Subsequently, human blood is perfused through the endothelialized post microfluidics, observing the temporal and spatial thrombotic response governed by Virchow's triad, including vessel wall injury, hemodynamic disturbance, and hypercoagulability. The innovative model offers valuable insights into stenosis‐induced thrombosis and endothelial behavior, paving the way for improved assessment of thrombotic risks associated with stenotic vessels. This advanced microfluidic platform also offers new approaches for evaluation of prothrombotic phenotypes and cardiovascular risk assessment in the future.
Carbon‐Based Electrochemical‐Free Chlorine Sensors
Authors: Siddiqui Junaid , Taheri Mahtab , Nami Mohammad , Deen Imran A. , Packirisamy Muthukumaran , Deen M. Jamal
Published: July 2023

Sodium hypochlorite is a widely used additive in water used to disinfect and remove any disease‐causing bacteria that can be found in sources of water, and is used to wash contaminants from meats, fruits, and vegetables. Many free chlorine sensors exist which monitor free chlorine levels such as the use of colorimetric or electrochemical methods, ensuring that the free chlorine is within safe and regulated levels. However colorimetric sensing methods are irreversible and often use toxic compounds, and electrochemical sensors, although reversible, are made with materials which are not suitable to be used near drinking water or food products. By developing sensors which are made using alternative materials and methods, the sensors can be used in and around drinking water and food products. This review article discusses various electrochemical‐free chlorine sensors made with various carbon‐based materials and methods resulting in sensors that are biodegradable, relatively inert, and resilient in the presence of harsh chemicals, making them safe to use near and around food and still maintain competitive performance parameters. This review article showcases some of the recent progress, the importance, preconditions, and the various future needs and potentials of carbon‐based electrochemical‐free chlorine sensors.
Phonon Polaritons: A New Paradigm for Light‐Controllable Heat Sources
Authors: Yang Bei , Pan Deng , Dai Qing
Published: July 2023

Photothermal applications, such as therapy, imaging, and catalysis, necessitate heat sources capable of generating high temperatures under mid‐infrared (mid‐IR) illumination. However, commonly used metal nanostructures suffer from low efficiency due to their high carrier concentrations, resulting in shallow surface heating and optical range restrictions. To overcome these limitations, this work proposes a novel approach employing materials that support phonon polaritons (PhPs) as a promising paradigm for light‐controllable heat sources. The theoretical demonstration reveals that hexagonal boron nitride (hBN) nanorods can produce up to 46 times more heat compared to plasmonic gold counterparts under resonant monochromatic light. This superior heating capability stems from the unique properties of PhPs, which enable stronger field confinement and deeper penetration within the nanostructure, leading to higher efficiency by circumventing the electrostatic shielding effect associated with plasmonic heating. Furthermore, this work demonstrates that the heating performance of hBN antennas can be optimized by manipulating their size, geometry, and material loss. Notably, the use of isotopically pure hBN can triple the heat power. These findings highlight the tremendous potential of hBN antennas as light‐controllable heat sources, opening up new possibilities for IR photothermal applications by harnessing materials that support PhPs.
Organoid‐Based Human Stomach Micro‐Physiological System to Recapitulate the Dynamic Mucosal Defense Mechanism
Authors: Jeong Hye‐Jin , Park Ji‐Hyeon , Kang Joo H. , Sabaté del Río Jonathan , Kong Seong‐Ho , Park Tae‐Eun
Published: August 2023

Several stomach diseases are attributed to the dysregulation of physiological function of gastric mucosal barrier by pathogens. Gastric organoids are a promising tool to develop treatment strategies for gastric infections. However, their functional features of in vivo gastric mucosal barrier and host–microbe interactions are limited due to the lack of physiological stimuli. Herein, a human stomach micro‐physiological system (hsMPS) with physiologically relevant gastric mucosal defense system is described based on the combination of organoid and MPS technology. A fluid flow enhanced epithelial‐mesenchymal interaction in the hsMPS enables functional maturation of gastric epithelial cells, which allows for the recreation of mesh‐like mucus layer containing high level of mucus protective peptides and well‐developed epithelial junctional complexes. Furthermore, gastroprotection mechanisms against Helicobacter pylori (H. pylori) are successfully demonstrated in this system. Therefore, hsMPS represents a new in vitro tool for research where gastric mucosal defense mechanism is pivotal for developing therapeutic strategies.
Design of Antioxidant Nanoparticle, which Selectively Locates and Scavenges Reactive Oxygen Species in the Gastrointestinal Tract, Increasing The Running Time of Mice
Authors: Toriumi Takuto , Ohmori Hajime , Nagasaki Yukio
Published: August 2023

Excess reactive oxygen species (ROS) produced during strong or unfamiliar exercise cause exercise‐induced gastrointestinal syndrome (EIGS), leading to poor health and decreased exercise performance. The application of conventional antioxidants can neither ameliorate EIGS nor improve exercise performance because of their rapid elimination and severe side effects on the mitochondria. Hence, a self‐assembling nanoparticle‐type antioxidant (RNPO) that is selectively located in the gastrointestinal (GI) tract for an extended time after oral administration is developed. Interestingly, orally administered RNPO significantly enhances the running time until exhaustion in mice with increasing dosage, whereas conventional antioxidants (TEMPOL) tends to reduce the running time with increasing dosage. The running (control) and TEMPOL groups show severe damage in the GI tract and increased plasma lipopolysaccharide (LPS) levels after 80 min of running, resulting in fewer red blood cells (RBCs) and severe damage to the skeletal muscles and liver. However, the RNPO group is protected against GI tract damage and elevation of plasma LPS levels, similar to the nonrunning (sedentary) group, which prevents damage to the whole body, unlike in the control and TEMPOL groups. Based on these results, it is concluded that continuous scavenging of excessive intestinal ROS protects against gut damage and further improves exercise performance.
Identification and expression analysis of WRKY superfamily genes under lychee downy blight stress in lychee
Authors: Liu Hailun , Jiang Yonghua , Wen Yingjie , Tan Zhaolong , Shi Fachao , Chen Jiezhen , Cai Changhe , Yan Qian , Ou Liangxi
Published: August 2023

WRKY proteins comprise a large family of transcription factors that play important roles in plant growth, development, and responses to stress, but little information is available about these genes in lychee (Litchi chinensis Sonn.). Despite being a popular fruit worldwide, lychee is highly vulnerable to lychee downy blight (LDB; caused by Peronophythora litchii), a major disease affecting lychee. Based on lychee whole‐genome data, a total of 50 LcWRKY genes were identified across 15 chromosomes. According to a conserved domain and phylogenetic analysis, these 50 LcWRKYs were classified into three distinct subfamilies. Gene structure analysis revealed the presence of 2–11 exons in the LcWRKYs. Cis‐acting regulatory element analysis identified many stress‐response elements in LcWRKY promoters. Moreover, a comprehensive 2‐year investigation involving the screening of a lychee natural population led to the identification of Guiwei and Yurong1 as displaying stable susceptibility and resistance against LDB, respectively. Furthermore, expression patterns indicated that LcWRKY13, LcWRKY17, and LcWRKY34 were significantly upregulated in response to LDB induction, while LDB suppressed the expression of LcWRKY11. These findings suggest that these four genes may play a crucial role in lychee resistance to LDB. The present study has provided a foundation for future investigations of LcWRKY gene function in lychee.
A polydisperse model for thixotropic elasto‐viscoplastic suspensions of aggregating particles using population balances
Authors: Jariwala Soham , Song Rong , Hipp Julie B. , Diemer R. Bertrum , Wagner Norman J. , Beris Antony N.
Published: July 2023

An improved population balance‐based rheological constitutive framework for polydisperse aggregating suspensions is derived by incorporating detailed models for orthokinetic and perikinetic aggregation and shear breakage processes. The framework accounts for critical properties such as dynamic arrest, viscoelasticity, kinematic hardening, thixotropy, and yield stress to generate a full range of thixotropic elasto‐viscoplastic (TEVP) response. Additionally, the model is thermodynamically consistent because the dynamics and timescales are completely determined by internal structural and kinetic variables. The model connects the rheological response to the structural descriptors such as the size distribution of agglomerates, mean sizes, fractal dimension, and agglomerate volume fraction. Predictions are compared against a wide range of shear rheology measurements data for model thixotropic suspensions of fumed silica and carbon black, including large amplitude oscillatory shear (LAOS), as well as ultra‐small angle neutron scattering under steady shear (Rheo‐uSANS).
Artificial intelligence and the work–health interface: A research agenda for a technologically transforming world of work
Authors: Jetha Arif , Bakhtari Hela , Rosella Laura C. , Gignac Monique A. M. , Biswas Aviroop , Shahidi Faraz V. , Smith Brendan T. , Smith Maxwell J. , Mustard Cameron , Khan Naimul , Arrandale Victoria H. , Loewen Peter J. , Zuberi Daniyal , Dennerlein Jack T. , Bonaccio Silvia , Wu Nicole , Irvin Emma , Smith Peter M.
Published: August 2023

The labor market is undergoing a rapid artificial intelligence (AI) revolution. There is currently limited empirical scholarship that focuses on how AI adoption affects employment opportunities and work environments in ways that shape worker health, safety, well‐being and equity. In this article, we present an agenda to guide research examining the implications of AI on the intersection between work and health. To build the agenda, a full day meeting was organized and attended by 50 participants including researchers from diverse disciplines and applied stakeholders. Facilitated meeting discussions aimed to set research priorities related to workplace AI applications and its impact on the health of workers, including critical research questions, methodological approaches, data needs, and resource requirements. Discussions also aimed to identify groups of workers and working contexts that may benefit from AI adoption as well as those that may be disadvantaged by AI. Discussions were synthesized into four research agenda areas: (1) examining the impact of stronger AI on human workers; (2) advancing responsible and healthy AI; (3) informing AI policy for worker health, safety, well‐being, and equitable employment; and (4) understanding and addressing worker and employer knowledge needs regarding AI applications. The agenda provides a roadmap for researchers to build a critical evidence base on the impact of AI on workers and workplaces, and will ensure that worker health, safety, well‐being, and equity are at the forefront of workplace AI system design and adoption.
Applications of artificial intelligence in clinical laboratory genomics
Authors: Aradhya Swaroop , Facio Flavia M. , Metz Hillery , Manders Toby , Colavin Alexandre , Kobayashi Yuya , Nykamp Keith , Johnson Britt , Nussbaum Robert L.
Published: July 2023

The transition from analog to digital technologies in clinical laboratory genomics is ushering in an era of “big data” in ways that will exceed human capacity to rapidly and reproducibly analyze those data using conventional approaches. Accurately evaluating complex molecular data to facilitate timely diagnosis and management of genomic disorders will require supportive artificial intelligence methods. These are already being introduced into clinical laboratory genomics to identify variants in DNA sequencing data, predict the effects of DNA variants on protein structure and function to inform clinical interpretation of pathogenicity, link phenotype ontologies to genetic variants identified through exome or genome sequencing to help clinicians reach diagnostic answers faster, correlate genomic data with tumor staging and treatment approaches, utilize natural language processing to identify critical published medical literature during analysis of genomic data, and use interactive chatbots to identify individuals who qualify for genetic testing or to provide pre‐test and post‐test education. With careful and ethical development and validation of artificial intelligence for clinical laboratory genomics, these advances are expected to significantly enhance the abilities of geneticists to translate complex data into clearly synthesized information for clinicians to use in managing the care of their patients at scale.
Transition‐Metal‐Free Synthesis of N‐Heterocyclic Compounds via Multi‐Component Reactions
Authors: Boruah Dhruba Jyoti , Borkotoky Lodsna , Newar Uma Devi , Maurya Ram Awatar , Yuvaraj Panneerselvam
Published: July 2023

Multicomponent reactions (MCRs) have emerged as powerful tools in synthetic chemistry for the efficient synthesis of diverse molecular scaffolds, particularly nitrogen‐containing heterocycles. Despite their numerous advantages, the use of transition metal catalysts or additives in MCRs can present limitations due to cost, toxicity, and environmental concerns. In recent years, there has been a growing interest in transition metal‐free MCRs for the synthesis of N‐heterocyclic compounds. This review provides a comprehensive and concise overview of the recent advancements in transition metal‐free MCRs for the synthesis of valuable N‐heterocycles over the past five years. The review is systematically organized, categorizing the discussed MCRs based on the size of the heterocyclic ring and the number of nitrogen atoms. Only MCRs that result in the formation of heterocyclic rings containing at least one nitrogen atom are included, while the derivatization of N‐heterocycles using transition metal‐free MCRs falls outside the scope of this review. By highlighting the recent developments in this field, this review aims to showcase the potential and significance of transition metal‐free MCRs as sustainable and efficient strategies for accessing N‐heterocyclic compounds. The elimination of transition metals not only simplifies the reaction conditions but also contributes to greener and more environmentally friendly synthetic approaches. This review serves as a valuable resource for researchers interested in the design and application of transition metal‐free MCRs in the synthesis of nitrogen‐containing heterocycles.
The various meanings and uses of bone “remodeling” in biological anthropology: A review
Authors: Wei Xuan , Cooper David M. L.
Published: July 2023

Objectives

In modern bone biology, the term “remodeling” generally refers to internal bone turnover that creates secondary osteons. However, it is also widely used by skeletal biologists, including biological anthropologists as a catch‐all term to refer to different skeletal changes. In this review, we investigated how “remodeling” is used across topics on skeletal biology in biological anthropology to demonstrate potential problems with such pervasive use of a generalized term.

Methods

Using PubMed and Google Scholar, we selected and reviewed 205 articles that use the term remodeling to describe skeletal processes and have anthropological implications. Nine edited volumes were also reviewed as examples of collaborative work by different experts to demonstrate the diverse and extensive use of the term remodeling.

Results

Four general meanings of bone “remodeling” were identified, namely, internal turnover, functional adaptation, fracture repair, and growth remodeling. Additionally, remodeling is also used to refer to a broad array of pathological skeletal changes.

Discussion

Although we initially identified four general meanings of bone remodeling, they are not mutually exclusive and often occur in combination. The term “remodeling” has become an extensively used catch‐all term to refer to different processes and outcomes of skeletal changes, which inevitably lead to misunderstanding and a loss of information. Such ambiguity and confusion are potentially problematic as the field of biological anthropology becomes increasingly multidisciplinary. Therefore, we advocate for precise, context‐specific definitions and explanations of bone remodeling as it continues to be used across disciplines within and beyond biological anthropology.
Molecular Engineering of Cation Solvation Structure for Highly Selective Carbon Dioxide Electroreduction
Authors: Ni Wenpeng , Guan Yongji , Chen Houjun , Zhang Yan , Wang Shuangyin , Zhang Shiguo
Published: July 2023

Balancing the activation of H2O is crucial for highly selective CO2 electroreduction (CO2RR), as the protonation steps of CO2RR require fast H2O dissociation kinetics, while suppressing hydrogen evolution (HER) demands slow H2O reduction. We herein proposed one molecular engineering strategy to regulate the H2O activation using aprotic organic small molecules with high Gutmann donor number as a solvation shell regulator. These organic molecules occupy the first solvation shell of K+ and accumulate in the electrical double layer, decreasing the H2O density at the interface and the relative content of proton suppliers (free and coordinated H2O), suppressing the HER. The adsorbed H2O was stabilized via the second sphere effect and its dissociation was promoted by weakening the O−H bond, which accelerates the subsequent *CO2 protonation kinetics and reduces the energy barrier. In the model electrolyte containing 5 M dimethyl sulfoxide (DMSO) as an additive (KCl‐DMSO‐5), the highest CO selectivity over Ag foil increased to 99.2 %, with FECO higher than 90.0 % within −0.75 to −1.15 V (vs. RHE). This molecular engineering strategy for cation solvation shell can be extended to other metal electrodes, such as Zn and Sn, and organic molecules like N,N‐dimethylformamide.
Nano‐Impact Electrochemistry Reveals Kinetics Information of Metal‐Ion Battery Materials with Multiple Redox Centers
Authors: Xu Wei , Zheng Jia‐Jia , Li Yu‐An , Gao Xingfa , Ji Xiaobo , Zhou Yi‐Ge
Published: July 2023

Prussian blue (PB) has emerged as a promising cathode material in aqueous batteries. It possesses two distinct redox centers, and the potassium ions (K+) are unevenly distributed throughout the compound, adding complexity to the interpretation of the K+ insertion/de‐insertion kinetic mechanism. Traditional ensemble‐averaged measurements are limited in uncovering the precise kinetic information of the PB particles, as the results are influenced by the construction of the porous composite electrode and the redox behavior from different particles. In this study, the electrochemical processes of individual PB particles were investigated using nano‐impact electrochemistry. By varying the potentials, different types of transient current signals were obtained that revealed the kinetic mechanism of each oxidation/reduction reaction in combination with theoretical simulation. Additionally, a partially contradictory conclusion between single‐particle analysis and the ensemble‐averaged measurement was discussed. These findings contribute to a better understanding of the electrochemical processes of cathode materials with multiple redox centers, which facilitates the development of effective strategies to optimize these materials.
Coupling Titanium and Chromium Catalysis in a Reaction Network for the Reprogramming of [BH4]− as Electron Transfer and Hydrogen Atom Transfer Reagent for Radical Chemistry
Authors: Heinz Michael , Weiss Gregor , Shizgal Grigoriy , Panfilova Anastasia , Gansäuer Andreas
Published: July 2023

We describe a unique catalytic system with an efficient coupling of Ti‐ and Cr‐catalysis in a reaction network that allows the use of [BH4]− as stoichiometric hydrogen atom and electron donor in catalytic radical chemistry. The key feature is a relay hydrogen atom transfer from [BH4]− to Cr generating the active catalysts under mild conditions. This enables epoxide reductions, regiodivergent epoxide opening and radical cyclizations that are not possible with cooperative catalysis with radicals or by epoxide reductions via Meinwald rearrangement and ensuing carbonyl reduction. No typical SN2‐type reactivity of [BH4]− salts is observed.
Fragment‐Screening und schnelle mikromolare Detektion mit einem Benchtop‐NMR‐Spektrometer ermöglicht durch photoinduzierte Hyperpolarisation
Authors: Stadler Gabriela R. , Segawa Takuya F. , Bütikofer Matthias , Decker Venita , Loss Sandra , Czarniecki Barbara , Torres Felix , Riek Roland
Published: August 2023

Fragmentbasiertes Wirkstoffdesign ist eine gut etablierte Strategie für rationales Arzneimitteldesign, wobei die Kernspinresonanzspektroskopie (NMR) auf Hochfeldspektrometern als Referenzmethode für das Screening und die Hit‐Validierung dient. Hochfeld‐NMR‐Spektrometer sind jedoch nicht nur teuer, sondern erfordern auch eine spezielle Wartung, einen speziellen Raum und sind auf die Kühlung mit flüssigem Helium angewiesen, was angesichts der wiederkehrenden weltweiten Heliumknappheit kritisch geworden ist. Wir schlagen eine Alternative zum Hochfeld‐NMR‐Screening vor, indem wir den kürzlich entwickelten Ansatz des Fragment‐Screenings durch photoinduzierte hyperpolarisierte NMR auf einem kryogenfreien 80‐MHz‐Benchtop‐NMR‐Spektrometer anwenden, der Signalverstärkungen von bis zu drei Größenordnungen ermöglicht. Es wird gezeigt, dass es möglich ist, mit einem Benchtop‐NMR‐Spektrometer bei niedrigen mikromolaren Konzentrationen sowohl von Proteinen als auch von Liganden neue Hits zu entdecken und die Entwicklung von Medikamenten einzuleiten. Der vorgestellte Ansatz arbeitet mit höherer Geschwindigkeit als moderne Hochfeld‐NMR‐Ansätze und weist eine Nachweisgrenze im nanomolaren Bereich auf. Die photoinduzierte Hyperpolarisation ist bekanntlich kostengünstig und einfach zu implementieren, was der Philosophie von Benchtop‐NMR‐Spektrometern sehr entgegenkommt. Diese Ergebnisse ebnen den Weg für den Einsatz von Benchtop‐NMRunter nahezu physiologischen Bedingungen für die Entwicklung von Arzneimitteln und weitere Life‐Science‐Anwendungen.
Lichtinduzierte, metallfreie Erzeugung von Cyanocarbenen aus Alkinyltriazenen für die Synthese von Nitrilderivaten
Authors: Michel Elena , Grieser Fabian F. , Mackenroth Alexandra V. , Schukin Michael , Krämer Petra , Tahir Shaista , Rominger Frank , Rudolph Matthias , Hashmi A. Stephen K.
Published: July 2023

Die Chemie der Alkinyltriazene ist ein aufstrebendes Gebiet für organische Chemiker, und insbesondere säureinduzierte nukleophile Funktionalisierungen, entweder direkt oder nach einer vorherigen Reaktion mit aromatischen Triazenen unter Ausschluss von Stickstoff, ebneten den Weg für erfolgreiche Strategien. Im Gegensatz dazu ist das chemische Verhalten von Alkinyltriazenen bei einer Bestrahlung mit Licht noch unbekannt. Wir stellen hier die erste Photoaktivierung von Alkinyltriazenen vor, die ein ungewöhnliches Reaktivitätsmuster auslöst, bei dem die N1−N2‐Bindung der Triazeneinheit gespalten wird, was zu einem einzigartigen Zugang zu Cyanocarbenen aus einem leicht verfügbaren, stabilen und unempfindlichen Vorläufer führt. Dies ermöglicht den Zugang zu verschiedenen Nitrilverbindungen ohne die Verwendung eines toxischen Cyanierungsmittels, indem das Reaktivitätsmuster von Carbenen ausgenutzt wird. Durch Variation der Reaktionsbedingungen und Lichtquellen können verschiedene Substitutionsmuster selektiv und in guter Ausbeute unter milden und metallfreien Bedingungen erhalten werden, wodurch die Alkinyltriazen‐Einheit als photozugängliches Methylennitril‐Synthon eingeführt wird. Mit diesem Synthon werden Unterklassen wie α‐Alkoxynitrile, α‐Aminonitrile und α‐Cyanohydrazone leicht verfügbar. Diese weisen synthetisch wertvolle Substitutionsmuster für die Synthese von Arzneimitteln, Zwischenprodukten für die Totalsynthese und die Aminosäuresynthese auf.
Tribochemically Controlled Atom Transfer Radical Polymerization Enabled by Contact Electrification
Authors: Wang Chen , Zhao Ruoqing , Fan Wenru , Li Lei , Feng Haoyang , Li Zexuan , Yan Ci , Shao Xiaoyang , Matyjaszewski Krzysztof , Wang Zhenhua
Published: July 2023

Traditional mechanochemically controlled reversible‐deactivation radical polymerization (RDRP) utilizes ultrasound or ball milling to regenerate activators, which induce side reactions because of the high‐energy and high‐frequency stimuli. Here, we propose a facile approach for tribochemically controlled atom transfer radical polymerization (tribo‐ATRP) that relies on contact‐electro‐catalysis (CEC) between titanium oxide (TiO2) particles and CuBr2/tris(2‐pyridylmethylamine (TPMA), without any high‐energy input. Under the friction induced by stirring, the TiO2 particles are electrified, continuously reducing CuBr2/TPMA into CuBr/TPMA, thereby conversing alkyl halides into active radicals to start ATRP. In addition, the effect of friction on the reaction was elucidated by theoretical simulation. The results indicated that increasing the frequency could reduce the energy barrier for the electron transfer from TiO2 particles to CuBr2/TPMA. In this study, the design of tribo‐ATRP was successfully achieved, enabling CEC (ca. 10 Hz) access to a variety of polymers with predetermined molecular weights, low dispersity, and high chain‐end fidelity.
NH4+ Charge Carrier Coordinated H‐Bonded Organic Small Molecule for Fast and Superstable Rechargeable Zinc Batteries
Authors: Song Ziyang , Miao Ling , Lv Yaokang , Gan Lihua , Liu Mingxian
Published: July 2023

Organic small molecules as high‐capacity cathodes for Zn‐organic batteries have inspired numerous interests, but are trapped by their easy‐dissolution in electrolytes. Here we knit ultrastable lock‐and‐key hydrogen‐bonding networks between 2, 7‐dinitropyrene‐4, 5, 9, 10‐tetraone (DNPT) and NH4+ charge carrier. DNPT with octuple‐active carbonyl/nitro centers (H‐bond acceptor) are redox‐exclusively accessible for flexible tetrahedral NH4+ ions (H‐bond donator) but exclude larger and rigid Zn2+, due to a lower activation energy (0.14 vs. 0.31 eV). NH4+ coordinated H‐bonding chemistry conquers the stability barrier of DNPT in electrolyte, and gives fast diffusion kinetics of non‐metallic charge carrier. A stable two‐step 4e− NH4+ coordination with DNPT cathode harvests a high capacity (320 mAh g−1), a high‐rate capability (50 A g−1) and an ultralong life (60,000 cycles). This finding points to a new paradigm for H‐bond stabilized organic small molecules to design advanced zinc batteries.
Thiophene‐Containing Covalent Organic Frameworks for Overall Photocatalytic H2O2 Synthesis in Water and Seawater
Authors: Yue Jie‐Yu , Song Li‐Ping , Fan Yan‐Fei , Pan Zi‐Xian , Yang Peng , Ma Yu , Xu Qing , Tang Bo
Published: August 2023

H2O2 is a significant chemical widely utilized in the environmental and industrial fields, with growing global demand. Without sacrificial agents, simultaneous photocatalyzed H2O2 synthesis through the oxygen reduction reaction (ORR) and water oxidation reaction (WOR) dual channels from seawater is green and sustainable but still challenging. Herein, two novel thiophene‐containing covalent organic frameworks (TD‐COF and TT‐COF) were first constructed and served as catalysts for H2O2 synthesis via indirect 2e− ORR and direct 2e− WOR channels. The photocatalytic H2O2 production performance can be regulated by adjusting the N‐heterocycle modules (pyridine and triazine) in COFs. Notably, with no sacrificial agents, just using air and water as raw materials, TD‐COF exhibited high H2O2 production yields of 4060 μmol h−1 g−1 and 3364 μmol h−1 g−1 in deionized water and natural seawater, respectively. Further computational mechanism studies revealed that the thiophene was the primary photoreduction unit for ORR, while the benzene ring (linked to the thiophene by the imine bond) was the central photooxidation unit for WOR. The current work exploits thiophene‐containing COFs for overall photocatalytic H2O2 synthesis via ORR and WOR dual channels and provides fresh insight into creating innovative catalysts for photocatalyzing H2O2 synthesis.
Progress and Perspectives on the Development of Pouch‐Type Lithium Metal Batteries
Authors: Jie Yulin , Tang Chao , Xu Yaolin , Guo Youzhang , Li Wanxia , Chen Yawei , Jia Haojun , Zhang Jing , Yang Ming , Cao Ruiguo , Lu Yuhao , Cho Jaephil , Jiao Shuhong
Published: July 2023

Lithium (Li) metal batteries (LMBs) are the “holy grail” in the energy storage field due to their high energy density (theoretically >500 Wh kg−1). Recently, tremendous efforts have been made to promote the research & development (R&D) of pouch‐type LMBs toward practical application. This article aims to provide a comprehensive and in‐depth review of recent progress on pouch‐type LMBs from full cell aspect, and to offer insights to guide its future development. It will review pouch‐type LMBs using both liquid and solid‐state electrolytes, and cover topics related to both Li and cathode (including LiNixCoyMn1‐x‐yO2, S and O2) as both electrodes impact the battery performance. The key performance criteria of pouch‐type LMBs and their relationship in between are introduced first, then the major challenges facing the development of pouch‐type LMBs are discussed in detail, especially those severely aggravated in pouch cells compared with coin cells. Subsequently, the recent progress on mechanistic understandings of the degradation of pouch‐type LMBs is summarized, followed with the practical strategies that have been utilized to address these issues and to improve the key performance criteria of pouch‐type LMBs. In the end, it provides perspectives on advancing the R&Ds of pouch‐type LMBs towards their application in practice.
Effective Activation of Strong C−Cl Bonds for Highly Selective Photosynthesis of Bibenzyl via Homo‐Coupling
Authors: Yang Qingning , Li Xiyi , Chen Lu , Han Xiaoyu , Wang Feng Ryan , Tang Junwang
Published: July 2023

Carbon‐carbon (C−C) coupling of organic halides has been successfully achieved in homogeneous catalysis, while the limitation, e.g., the dependence on rare noble metals, complexity of the metal‐ligand catalylst and the poor catalyst stability and recyclability, needs to be tackled for a green process. The past few years have witnessed heterogeneous photocatalysis as a green and novel method for organic synthesis processes. However, the study on C−C coupling of chloride substrates is rare due to the extremely high bond energy of C−Cl bond (327 kJ mol−1). Here, we report a robust heterogeneous photocatalyst (Cu/ZnO) to drive the homo‐coupling of benzyl chloride with high efficiency, which achieves an unprecedented high selectivity of bibenzyl (93 %) and yield rate of 92 % at room temperature. Moreover, this photocatalytic process has been validated for C−C coupling of 10 benzylic chlorides all with high yields. In addition, the excellent stability has been observed for 8 cycles of reactions. With detailed characterization and DFT calculation, the high selectivity is attributed to the enhanced adsorption of reactants, stabilization of intermediates (benzyl radicals) for the selective coupling by the Cu loading and the moderate oxidation ability of the ZnO support, besides the promoted charge separation and transfer by Cu species.