bluuebunny/crossref_metadata_2025_split huggingface dataset:
General Access to Clavine Alkaloids via a Rhodium(I)‐Catalyzed Diastereoselective Hayashi‐Miyaura Reaction
Authors: Leoni Giovanni , Bartoccini Francesca , Piersanti Giovanni 
Published: January 2024

AbstractWe report the development of the diastereoselective rhodium(I)‐catalyzed intramolecular conjugate addition (Hayashi‐Miyaura reaction) of robust and easily handled 4‐pinacolboronic ester D‐tryptophan derivatives tethering an activated alkene as the acceptor. This methodology provides, access to the functionalized chiral tricyclic core of the ergoline skeleton diastereoselectivity and allows further modification for the cyclization of the fused fourth ring present in several clavine alkaloids.
Alginate‐Coated Silicone Implants with Antisolvent‐Crystallized Paclitaxel to Prevent Breast Cancer Recurrence and Reduce Fibrosis
Authors: Myung Noehyun , Hwang Seoyoung , Ha Won , Kang Hyun‐Wook 
Published: January 2024

AbstractBreast cancer patients undergoing mastectomy receive silicone‐implant‐based breast reconstruction to mitigate the psychological distress of breast loss, typically in conjunction with adjuvant therapy. However, significant problems remain, such as systemic toxicity from chemotherapy and fibrosis that causes capsular contracture. Here, the development of a silicone implant coated with an alginate gel containing antisolvent‐crystallized paclitaxel (acPTX) is reported. By antisolvent crystallization, the compact formulation of acPTX ensures slow release for long‐term breast cancer recurrence prevention. The mixture of acPTX and the biodegradable alginate gel, which reduces fibrosis, is uniformly coated onto the silicone implant using 3D printed implant‐specific molds based on the shape obtained from 3D scanning. In a breast cancer recurrence mouse model, silicone implants coated with acPTX gel show a long‐term preventive effect compared to gel‐coated implants with commercially available PTX. Furthermore, animal studies using C57BL/6 mice show that alginate‐gel‐coated implants significantly reduce capsule thickness, collagen density, and the number of fibrosis‐related cells around the implant compared to silicone implants. The developed acPTX‐gel‐coated implant presents a promising approach for breast reconstruction in mastectomized breast cancer patients. It provides a novel platform for developing implants with long‐term drug release properties.
Liquid Metal Composites‐Enabled Real‐Time Hand Gesture Recognizer with Superior Recognition Speed and Accuracy
Authors: Chen Yi , Tao Zhe , Chang Ruizhe , Cao Yudong , Yun Guolin , Li Weihua , Zhang Shiwu , Sun Shuaishuai 
Published: January 2024

AbstractProsthetic hands play a vital role in restoring forearm functionality for patients who have suffered hand loss or deformity. The hand gesture intention recognition system serves as a critical component within the prosthetic hand system. However, accurately and swiftly identifying hand gesture intentions remains a challenge in existing approaches. Here, a real‐time motion intention recognition system utilizing liquid metal composite sensor bracelets is proposed. The sensor bracelet detects pressure signals generated by forearm muscle movements to recognize hand gesture intent. Leveraging the remarkable pressure sensitivity of liquid metal composites and the efficient classifier based on the optimized recognition algorithm, this system achieves an average offline and real‐time recognition accuracy of 98.2% and 92.04%, respectively, with an average recognition speed of 0.364 s. Thus, this wearable system shows advantages in superior recognition speed and accuracy. Furthermore, this system finds applications in master‐slave control of prosthetic hands in unmanned scenarios, such as electrically powered operations, space exploration, and telemedicine. The proposed system promises significant advances in next‐generation intent‐controlled prosthetic hands and robots.
When Machine Learning Meets 2D Materials: A Review
Authors: Lu Bin , Xia Yuze , Ren Yuqian , Xie Miaomiao , Zhou Liguo , Vinai Giovanni , Morton Simon A. , Wee Andrew T. S. , van der Wiel Wilfred G. , Zhang Wen , Wong Ping Kwan Johnny 
Published: January 2024

AbstractThe availability of an ever‐expanding portfolio of 2D materials with rich internal degrees of freedom (spin, excitonic, valley, sublattice, and layer pseudospin) together with the unique ability to tailor heterostructures made layer by layer in a precisely chosen stacking sequence and relative crystallographic alignments, offers an unprecedented platform for realizing materials by design. However, the breadth of multi‐dimensional parameter space and massive data sets involved is emblematic of complex, resource‐intensive experimentation, which not only challenges the current state of the art but also renders exhaustive sampling untenable. To this end, machine learning, a very powerful data‐driven approach and subset of artificial intelligence, is a potential game‐changer, enabling a cheaper – yet more efficient – alternative to traditional computational strategies. It is also a new paradigm for autonomous experimentation for accelerated discovery and machine‐assisted design of functional 2D materials and heterostructures. Here, the study reviews the recent progress and challenges of such endeavors, and highlight various emerging opportunities in this frontier research area.
Spatiotemporally Precise Optical Manipulation of Intracellular Molecular Activities
Authors: Dong Bin , Mahapatra Shivam , Clark Matthew G. , Carlsen Mark S. , Mohn Karsten J. , Ma Seohee , Brasseale Kent A. , Crim Grace , Zhang Chi 
Published: January 2024

AbstractControlling chemical processes in live cells is a challenging task. The spatial heterogeneity of biochemical reactions in cells is often overlooked by conventional means of incubating cells with desired chemicals. A comprehensive understanding of spatially diverse biochemical processes requires precise control over molecular activities at the subcellular level. Herein, a closed‐loop optoelectronic control system is developed that allows the manipulation of biomolecular activities in live cells at high spatiotemporal precision. Chemical‐selective fluorescence signals are utilized to command lasers that trigger specific chemical processes or control the activation of photoswitchable inhibitors at desired targets. This technology is fully compatible with laser scanning confocal fluorescence microscopes. The authors demonstrate selective interactions of a 405 nm laser with targeted organelles and simultaneous monitoring of cell responses by fluorescent protein signals. Notably, blue laser interaction with the endoplasmic reticulum leads to a more pronounced reduction in cytosolic green fluorescent protein signals in comparison to that with nuclei and lipid droplets. Moreover, when combined with a photoswitchable inhibitor, microtubule polymerization is selectively inhibited within the subcellular compartments. This technology enables subcellular spatiotemporal optical manipulation over chemical processes and drug activities, exclusively at desired targets, while minimizing undesired effects on non‐targeted locations.
Using Cu‐Based Metal–Organic Framework as a Comprehensive and Powerful Antioxidant Nanozyme for Efficient Osteoarthritis Treatment
Authors: Yu Bo , Sun Wei , Lin Juntao , Fan Chaoyu , Wang Chengxinqiao , Zhang Zhisen , Wang Yupeng , Tang Yonghua , Lin Youhui , Zhou Dongfang 
Published: January 2024

AbstractDeveloping nanozymes with effective reactive oxygen species (ROS) scavenging ability is a promising approach for osteoarthritis (OA) treatment. Nonetheless, numerous nanozymes lie in their relatively low antioxidant activity. In certain circumstances, some of these nanozymes may even instigate ROS production to cause side effects. To address these challenges, a copper‐based metal–organic framework (Cu MOF) nanozyme is designed and applied for OA treatment. Cu MOF exhibits comprehensive and powerful activities (i.e., SOD‐like, CAT‐like, and •OH scavenging activities) while negligible pro‐oxidant activities (POD‐ and OXD‐like activities). Collectively, Cu MOF nanozyme is more effective at scavenging various types of ROS than other Cu‐based antioxidants, such as commercial CuO and Cu single‐atom nanozyme. Density functional theory calculations also confirm the origin of its outstanding enzyme‐like activities. In vitro and in vivo results demonstrate that Cu MOF nanozyme exhibits an excellent ability to decrease intracellular ROS levels and relieve hypoxic microenvironment of synovial macrophages. As a result, Cu MOF nanozyme can modulate the polarization of macrophages from pro‐inflammatory M1 to anti‐inflammatory M2 subtype, and inhibit the degradation of cartilage matrix for efficient OA treatment. The excellent biocompatibility and protective properties of Cu MOF nanozyme make it a valuable asset in treating ROS‐related ailments beyond OA.
Innate Immune Training Initiates Efferocytosis to Protect against Lung Injury
Authors: Kang Yoon‐Young , Kim Dong‐Young , Lee Sang‐Yong , Kim Hee‐Joong , Kim Taehawn , Cho Jeong A. , Lee Taewon , Choi Eun Young 
Published: January 2024

AbstractInnate immune training involves myelopoiesis, dynamic gene modulation, and functional reprogramming of myeloid cells in response to secondary heterologous challenges. The present study evaluates whether systemic innate immune training can protect tissues from local injury. Systemic pretreatment of mice with β‐glucan, a trained immunity agonist, reduces the mortality rate of mice with bleomycin‐induced lung injury and fibrosis, as well as decreasing collagen deposition in the lungs. β‐Glucan pretreatment induces neutrophil accumulation in the lungs and enhances efferocytosis. Training of mice with β‐glucan results in histone modification in both alveolar macrophages (AMs) and neighboring lung epithelial cells. Training also increases the production of RvD1 and soluble mediators by AMs and efferocytes. Efferocytosis increases trained immunity in AMs by stimulating RvD1 release, thus inducing SIRT1 expression in neighboring lung epithelial cells. Elevated epithelial SIRT1 expression is associated with decreased epithelial cell apoptosis after lung injury, attenuating tissue damage. Further, neutrophil depletion dampens the effects of β‐glucan on macrophage accumulation, epigenetic modification in lung macrophages, epithelial SIRT1 expression, and injury‐mediated fibrosis in the lung. These findings provide mechanistic insights into innate immune training and clues to the potential ability of centrally trained immunity to protect peripheral organs against injury‐mediated disorders.
Strong Photon‐Magnon Coupling Using a Lithographically Defined Organic Ferrimagnet
Authors: Xu Qin , Cheung Hil Fung Harry , Cormode Donley S. , Puel Tharnier O. , Pal Srishti , Yusuf Huma , Chilcote Michael , Flatté Michael E. , Johnston‐Halperin Ezekiel , Fuchs Gregory D. 
Published: January 2024

AbstractA cavity‐magnonic system composed of a superconducting microwave resonator coupled to a magnon mode hosted by the organic‐based ferrimagnet vanadium tetracyanoethylene (V[TCNE]x) is demonstrated. This work is motivated by the challenge of scalably integrating a low‐damping magnetic system with planar superconducting circuits. V[TCNE]xhas ultra‐low intrinsic damping, can be grown at low processing temperatures on arbitrary substrates, and can be patterned via electron beam lithography. The devices operate in the strong coupling regime, with a cooperativity exceeding 1000 for coupling between the Kittel mode and the resonator mode at T≈0.4 K, suitable for scalable quantum circuit integration. Higher‐order magnon modes are also observed with much narrower linewidths than the Kittel mode. This work paves the way for high‐cooperativity hybrid quantum devices in which magnonic circuits can be designed and fabricated as easily as electrical wires.
Insight of Synthesis of Single Crystal Ni‐Rich LiNi1−x−yCoxMnyO2 Cathodes
Authors: Wu Yingqiang , Wu Hanfeng , Deng Jiushuai , Han Zhiding , Xiao Xiang , Wang Li , Chen Zonghai , Deng Yida , He Xiangming 
Published: January 2024

AbstractSingle‐crystal Ni‐rich LiNi1−x−yCoxMnyO2 (NCM) cathodes have garnered widespread attention in the lithium‐ion battery community due to their unique advantages in mechanical performance and their ability to minimize interfacial electrochemical side reactions. The synthesis of single‐crystal materials with monodisperse and appropriate size, minimal lattice defects, and highly ordered structures is the key for high‐performance batteries. However, achieving this goal poses challenges due to the lack of in‐depth understanding regarding specific experimental parameters and the solid reaction mechanism during the synthesis process. In this review, the aim is to provide an in‐depth analysis of the critical process parameters involved in the synthesis and their impact on crystal morphology, structure, and electrochemical performance. Consequently, the first section focuses on the effect of the precursor morphology, lithium salt, atmosphere, and sintering procedure. In the second section, the study delves into an in‐depth discussion of the solid reaction and crystal growth mechanism. Lastly, it is concluded by highlighting the prospects and challenges associated with the synthesis and application of single‐crystal Ni‐rich NCM cathodes.
A 3 µm‐Ultrathin Hybrid Electrolyte Membrane with Integrative Architecture for All‐Solid‐State Lithium Metal Batteries
Authors: Liu Kexin , Cheng Hui , Wang Zhuyi , Zhao Yin , Lv Yingying , Shi Liyi , Cai Xuesong , Cheng Zhongling , Zhang Haijiao , Yuan Shuai 
Published: January 2024

AbstractUltrathin all‐solid‐state electrolytes with an excellent Li+ transport behavior are highly desirable for developing high‐energy‐density solid‐state lithium metal batteries. However, how to balance the electrochemical performance and their mechanical properties remains a huge challenge. Herein, an ultrathin solid electrolyte membrane with a thickness of only 3 µm and a weight of 11.7 g m−2 is well constructed by integrating individual functionalized organic with inorganic modules. Impressively, the optimized hybrid electrolyte membrane shows a set of merits including a high room‐temperature ionic conductivity of 1.77 × 10−4 S cm−1, large Li+ transference number of 0.65, and strong mechanical strength (strength of 29 MPa, elongation of 95%), as well as negligible thermal shrink at 180 °C. The analysis results reveal that the lithium sulfonate‐functionalized mesoporous silica nanoparticles in the membrane play a crucial role in the selective transport of Li+ through anion trapping and cation exchange. The pouch full cell is further assembled with a high‐voltage NCM cathode and thin lithium anode, which exhibits excellent long‐term cycling stability, outstanding rate performance at room temperature, and high safety against abused conditions. The current work provides an innovative strategy for achieving lithium metal batteries with ultrathin all‐solid‐state electrolytes.
Factors Influencing Gas Evolution from High‐Nickel Layered Oxide Cathodes in Lithium‐Based Batteries
Authors: Sim Richard , Manthiram Arumugam 
Published: January 2024

AbstractGas evolution from high‐nickel layered oxide cathodes (>90% Ni) remains a major issue for their practical application. Gaseous species, such as CO2, O2, and CO, that are evolved at high states of charge (SOC) worsen the overall safety of batteries, as pressure build‐up within the cell may lead to cell rupture. Since these gasses are produced during cathode degradation, tracking the formation of gasses is also important in diagnosing cathode failure. Online electrochemical mass spectrometry (OEMS) is a powerful in situ technique to study gas evolution from the cathode during high‐voltage charge. However, the differences in the OEMS experimental setups between different groups make it challenging to compare results between groups. In this perspective, the various factors that influence gas evolution based on the OEMS results collected in this group are presented. The focus is on the conditions that lead to gas release, with a particular emphasis on reactive oxygen formation and subsequent chemical reactions with the electrolyte. Promising strategies, such as electrolytes, compositional tuning, and surface coatings that are effective at suppressing gas evolution from the cathode are highlighted. Critical insights into mitigating cathode degradation and gas evolution are provided to guide the development of safer, high‐energy batteries.
Decoding Polymeric Additive‐Driven Self‐Healing Processes in Perovskite Solar Cells from Chemical and Physical Bonding Perspectives
Authors: Nam Jeong‐Seok , Choi Jin‐Myung , Lee Jang Woo , Han Jiye , Jeon Il , Kim Hyung Do 
Published: January 2024

AbstractThis review addresses the self‐healing effects in perovskite solar cells (PSCs), emphasizing the significance of chemical and physical bonding as core mechanisms. Polymeric additives play a vital role in inducing self‐healing phenomena along with the intrinsic properties of perovskite materials, both of which are discussed herein. As a relatively underexplored area, the self‐healing effect induced by polymeric additives in PSCs is reviewed from a chemical perspective. The chemical bonds involved in self‐healing include isocyanate, disulfide, and carboxylic acid groups. The physical bonds related to self‐healing effects are primarily hydrogen bonding and chelation. Self‐healing in flexible perovskite devices extends their lifespan and improves their mechanical robustness against environmental and mechanical stressors. This discussion delves into the initiation methods for self‐healing, the conditions required, and the recovery‐rate profiles. This review not only catalogs various approaches to self‐healing, but also considers the fundamental limitations and potential of this phenomenon in PSCs. In addition, insights and an outlook on self‐healing in perovskite‐based optoelectronics are provided, offering guidance for future research and applications.
The current multidisciplinary management of rectal cancer
Authors: Bhutiani Neal , Peacock Oliver , Uppal Abhineet , You Y. Nancy , Bednarski Brian K. , Skibber John M. , Messick Craig , White Michael G. , Chang George J. , Konishi Tsuyoshi 
Published: January 2024

AbstractMultidisciplinary management of rectal cancer has rapidly evolved over the last several years. This review describes recent data surrounding total neoadjuvant therapy, organ preservation, and management of lateral pelvic lymph nodes. It then presents our treatment algorithm for management of rectal cancer at The University of Texas MD Anderson Cancer Center in the context of this and other existing literature. As part of this discussion, the review describes how we tailor management based upon both patient and tumor‐related factors in an effort to optimize patient outcomes.
Leveraging Expertise in Thermal Catalysis to Understand Plasma Catalysis
Authors: Lefferts Leon 
Published: January 2024

AbstractBest practices in testing heterogeneous catalysts are translated to plasma‐catalytic experiments. Independent determination of plasma‐catalytic and plasma‐chemical contributions is essential. Non‐porous catalyst particles are preferred because active sites inside sub‐micron pores cannot contribute. Temperature variation is needed to determine kinetics, despite the complexity of thermal effects in plasma. Rigorous checks on catalyst deactivation and mass balance are needed. Plasma enhanced reversed reactions should be minimized by keeping conversion low and far from thermodynamic equilibrium, preventing underestimation of the rate of forward reaction. In contrast, plasma‐catalytic studies often aim at conversions surpassing thermodynamic equilibrium, not obtaining any information on kinetics. Calculation of catalyst activity per active sites (turn‐over‐frequency) requires also appropriate characterization to determine the number of active sites. The relationship between kinetics and thermodynamics for plasma‐catalysis is discussed using endothermic decomposition of CO2 and exothermic synthesis of ammonia from N2 and H2 as examples. Assuming Langmuir–Hinshelwood and Eley‐Rideal mechanisms, the effect of excitation of reactant molecules on activation barriers and surface coverages are discussed, influencing reaction rates. The consequences of reversed reactions are considered. Plasma‐catalysis with catalysts applied for thermal catalysis at much higher temperature should be avoided, as adsorbed species are bonded too strongly resulting in low rates.
Water‐Degradable Oxygen‐Rich Polymers with AB/ABB Units from Fast and Selective Copolymerization
Authors: Zhang Xun , Xia Yanni , Sun Yue , Zhang Chengjian , Zhang Xinghong 
Published: January 2024

AbstractResearchers have been chasing plastics that can automatically and fully degrade into valuable products under natural conditions. Here, we develop a series of water‐degradable polymers from the first reported fast and selective cationic copolymerization of formaldehyde (B) with cyclic anhydrides (A). In addition to readily accessible monomers, the method is performed at industrially relevant temperatures (~100 °C), takes tens or even minutes, and uses common acid as the catalyst. Interestingly, such polymers possess tunable AB/ABB‐type repeating units, which are considered to be thermodynamic and kinetic products, respectively, resulting in low carbon content ([O] : [C] up to 1 : 1). Notably, the polymers can completely degrade to valuable diacids within 150 days in water at ambient temperature owing to the incorporation of carboxyl terminals and acid‐responsive acetal units. By washing with aqueous sodium carbonate, the polymers are relatively stable over several months.
Enhanced Directed Evolution in Mammalian Cells Yields a Hyperefficient Pyrrolysyl tRNA for Noncanonical Amino Acid Mutagenesis
Authors: Jewel Delilah , Kelemen Rachel E. , Huang Rachel L. , Zhu Zeyu , Sundaresh Bharathi , Malley Kaitlin , Pham Quan , Loynd Conor , Huang Zeyi , van Opijnen Tim , Chatterjee Abhishek 
Published: January 2024

AbstractHeterologous tRNAs used for noncanonical amino acid (ncAA) mutagenesis in mammalian cells typically show poor activity. We recently introduced a virus‐assisted directed evolution strategy (VADER) that can enrich improved tRNA mutants from naïve libraries in mammalian cells. However, VADER was limited to processing only a few thousand mutants; the inability to screen a larger sequence space precluded the identification of highly active variants with distal synergistic mutations. Here, we report VADER2.0, which can process significantly larger mutant libraries. It also employs a novel library design, which maintains base‐pairing between distant residues in the stem regions, allowing us to pack a higher density of functional mutants within a fixed sequence space. VADER2.0 enabled simultaneous engineering of the entire acceptor stem of M. mazei pyrrolysyl tRNA (tRNAPyl), leading to a remarkably improved variant, which facilitates more efficient incorporation of a wider range of ncAAs, and enables facile development of viral vectors and stable cell‐lines for ncAA mutagenesis.