bluuebunny/crossref_metadata_2025_split huggingface dataset:
Nonmetallic Se/N Co‐Doped Amorphous Carbon Anode Collaborates to Realize Ultra‐High Capacity and Fast Potassium Storage for Potassium Dual‐Ion Batteries
Authors: Guan Shuhua , Zhou Jiwei , Sun Shuling , Peng Qiaoling , Guo Xiuli , Liu Botian , Zhou Xiaolong , Tang Yongbing 
Published: January 2024

AbstractHeteroatom doping in carbon‐based anode materials is crucial to improve their capacity and promoting the practical application of low‐cost potassium‐ion batteries (KIBs). Herein, the selenium/nitrogen co‐doped amorphous carbon nanocluster (SeN‐ACN) anodes exhibit an ultra‐high reversible capacity of 621 mAh g−1 at 0.75 C (225 mA g−1) and a capacity retention of 93% after 2000 cycles at 5 C, which represent a remarkable achievement in potassium storage in nonmetallic doped carbon materials. This is attributed to the synergistic effects of Se/N co‐doping and their anchoring effects on potassium ions. As a proof of concept, a potassium‐based dual‐ion battery (K‐DIB), which consists of a SeN‐ACN anode and low‐cost graphite cathode, demonstrates a high reversible capacity of 118 mAh g−1 at 150 mA g−1 with a high cut‐off voltage of 5.2 V. Moreover, it presents excellent long‐term cycling performance, with 70% capacity retention after 500 cycles, among the best reported results of K‐DIBs.
Orthogonally Sequential Activation of Self‐Powered DNAzymes Cascade for Reliable Monitoring of mRNA in Living Cells
Authors: Zhang Fuqiang , Yang Nan , Zhou Fu , Qiao Ruonan , Wan Yifei , Liu Rong , Yang Suwan , Gu Mingzheng , Xu Huae , Dong Xiaochen , Wang Guangfeng 
Published: January 2024

AbstractRatiometric imaging of tumor‐related mRNA is significant, yet spatiotemporally resolved regulation on the ratiometric signals to avoid non‐specific activation in the living cells remains challenging. Herein, orthogonally sequential activation of concatenated DNAzyme circuits is, first, developed for Spatio Temporally regulated Amplified and Ratiometric (STAR) imaging of TK1 mRNA inside living cells with enhanced reliability and accuracy. By virtue of the synthesized CuO/MnO2 nanosheets, orthogonally regulated self‐powered DNAzyme circuits are operated precisely in living cells, sequentially activating two‐layered DNAzyme cleavage reactions to achieve the two ratiometric signal readouts successively for reliable monitoring of low‐abundance mRNA in living cells. It is found that the ratiometric signals can only be derived from mRNA over‐expressed tumor cells, also irrespective of probes’ delivery concentration. The presented approach could provide new insight into orthogonally regulated ratiometric systems for reliable imaging of specific biomarkers in living cells, benefiting disease precision diagnostics.
Resistive Memory Devices at the Thinnest Limit: Progress and Challenges
Authors: Li Xiao‐Dong , Chen Nian‐Ke , Wang Bai‐Qian , Niu Meng , Xu Ming , Miao Xiangshui , Li Xian‐Bin 
Published: January 2024

AbstractThe Si‐based integrated circuits industry has been developing for more than half a century, by focusing on the scaling‐down of transistor. However, the miniaturization of transistors will soon reach its physical limits, thereby requiring novel material and device technologies. Resistive memory is a promising candidate for in‐memory computing and energy‐efficient synaptic devices that can satisfy the computational demands of the future applications. However, poor cycle‐to‐cycle and device‐to‐device uniformities hinder its mass production. 2D materials, as a new type of semiconductor, is successfully employed in various micro/nanoelectronic devices and have the potential to drive future innovation in resistive memory technology. This review evaluates the potential of using the thinnest advanced materials, that is, monolayer 2D materials, for memristor or memtransistor applications, including resistive switching behavior and atomic mechanism, high‐frequency device performances, and in‐memory computing/neuromorphic computing applications. The scaling‐down advantages of promising monolayer 2D materials including graphene, transition metal dichalcogenides, and hexagonal boron nitride are presented. Finally, the technical challenges of these atomic devices for practical applications are elaborately discussed. The study of monolayer‐2D‐material‐based resistive memory is expected to play a positive role in the exploration of beyond‐Si electronic technologies.
Self‐Heating Multistage Microneedle Patch for Topical Therapy of Skin Cancer
Authors: Shao Jundong , Li Xingxing , Li Yashi , Lin Jing , Huang Peng 
Published: January 2024

AbstractTopical therapy is a favored route for treating skin cancers, but remain many challenges, such as low delivery efficiency, limited tumor tissue penetration, and unsatisfactory blood circulation. Here, a self‐heating microneedle (MN) patch with multilevel structures, including a dissolvable base for rapid drug release, a degradable tip for sustained drug release, and a self‐heating substrate is described. The thermally enhanced drug release performance is validated through both in vitro and in vivo experiments. High tumor therapeutic efficacy can be achieved due to the rapid release of 5‐fluorouracil, while the sustained release of thymoquinone endows the MN patch with long‐term tumor inhibition ability. It is further demonstrated the feasibility of such an MN patch for in vivo topical therapy of cutaneous squamous cell carcinoma with high efficacy, low side effects, and long‐term inhibition of recurrence. This self‐heating MN patch holds great promise for potential clinical applications, especially for the treatment of skin cancers.
Surface Engineered Single‐atom Systems for Energy Conversion
Authors: Yu Yutang , Zhu Zijian , Huang Hongwei 
Published: January 2024

AbstractSingle‐atom catalysts (SACs) are demonstrated to show exceptional reactivity and selectivity in catalytic reactions by effectively utilizing metal species, making them a favorable choice among the different active materials for energy conversion. However, SACs are still in the early stages of energy conversion, and problems like agglomeration and low energy conversion efficiency are hampering their practical applications. Substantial research focus on support modifications, which are vital for SAC reactivity and stability due to the intimate relationship between metal atoms and support. In this review, a category of supports and a variety of surface engineering strategies employed in SA systems are summarized, including surface site engineering (heteroatom doping, vacancy introducing, surface groups grafting, and coordination tunning) and surface structure engineering (size/morphology control, cocatalyst deposition, facet engineering, and crystallinity control). Also, the merits of support surface engineering in single‐atom systems are systematically introduced. Highlights are the comprehensive summary and discussions on the utilization of surface‐engineered SACs in diversified energy conversion applications including photocatalysis, electrocatalysis, thermocatalysis, and energy conversion devices. At the end of this review, the potential and obstacles of using surface‐engineered SACs in the field of energy conversion are discussed. This review aims to guide the rational design and manipulation of SACs for target‐specific applications by capitalizing on the characteristic benefits of support surface engineering.
Designable Photo‐Responsive Micron‐Scale Ultrathin Peptoid Nanobelts for Enhanced Performance on Hydrogen Evolution Reaction
Authors: Wu Pengchao , Sui Pengliang , Peng Guiping , Sun Zichao , Liu Fan , Yao Wenqian , Jin Haibao , Lin Shaoliang 
Published: January 2024

AbstractThe development of high‐reactive single‐atom catalysts (SACs) based on long‐range‐ordered ultrathin organic nanomaterials (UTONMs) (i.e., below 3 nm) provides a significant tactic for the advancement in hydrogen evolution reactions (HER) but remains challenging. Herein, photo‐responsive ultrathin peptoid nanobelts (UTPNBs) with a thickness of ≈2.2 nm and micron‐scaled length are generated using the self‐assembly of azobenzene‐containing amphiphilic ternary alternating peptoids. The pendants hydrophobic conjugate stacking mechanism reveals the formation of 1D ultralong UTPNBs, whose thickness is dictated by the length of side groups that are linked to peptoid backbones. The photo‐responsive feature is demonstrated by a reversible morphological transformation from UTPNBs to nanospheres (21.5 nm) upon alternative irradiation with UV and visible lights. Furthermore, the electrocatalyst performance of these aggregates co‐decorated with nitrogen‐rich ligand of terpyridine (TE) and uniformly‐distributed atomic platinum (Pt) is evaluated toward HER, with a photo‐controllable electrocatalyst activity that highly depended on both the presence of Pt element and structural characteristic of substrates. The Pt‐based SACs using TE‐modified UTPNBs as support exhibit a favorable electrocatalytic capacity with an overpotential of ≈28 mV at a current density of 10 mA cm−2. This work presents a promising strategy to fabricate stimuli‐responsive UTONMs‐based catalysts with controllable HER catalytic performance.
Tertiary‐Amine Controlled (3+3) or (4+2) Annulations of β′‐Acetoxy Allenoates with N‐Sulfonyl Ketimines: An Entry to m‐Teraryl and Fused Dihydropyridines
Authors: Qureshi Asif Ali , Kumar A. Sanjeeva , Kumara Swamy K. C. 
Published: January 2024

AbstractLewis base dependent (3+3) and (4+2) annulations of β′‐acetoxy allenoates with N‐sulfonyl ketimines offer m‐teraryl and fused dihydropyridines with varying substituents depending on the tertiary amine as well as subtle changes in the reaction conditions. The triazabicyclodecene (TBD)‐catalyzed (3+3) annulation involves 1,2‐elimination followed by 6‐endo‐dig cyclization as key steps in delivering fused 1,4‐hydropyridines. The same reactants under DMAP catalysis offer m‐teraryl via Mannich coupling, rather than 1,2‐elimination followed by C−N bond cleavage/aromatization. Key intermediates have been identified by HRMS studies.
Akt activator SC79 stimulates antibacterial nitric oxide generation in human nasal epithelial cells in vitro
Authors: Lee Robert J. , Adappa Nithin D. , Palmer James N. 
Published: January 2024

AbstractBackgroundThe role of Akt in nasal immunity is unstudied. Akt phosphorylates and activates endothelial nitric oxide synthase (eNOS) expressed in epithelial ciliated cells. Nitric oxide (NO) production by ciliated cells can have antibacterial and antiviral effects. Increasing nasal NO may be a useful antipathogen strategy in chronic rhinosinusitis (CRS). We previously showed that small‐molecule Akt activator SC79 induces nasal cell NO production and suppresses IL‐8 via the transcription factor Nrf‐2. We hypothesized that SC79 NO production may additionally have antibacterial effects.MethodsNO production was measured using fluorescent dye DAF‐FM. We tested effects of SC79 during co‐culture ofPseudomonas aeruginosawith primary nasal epithelial cells, using CFU counting and live–dead staining to quantify bacterial killing. Pharmacology determined the mechanism of SC79‐induced NO production and tested dependence on Akt.ResultsSC79 induced dose‐dependent, Akt‐dependent NO production in nasal epithelial cells. The NO production required eNOS and Akt. The NO released into the airway surface liquid killedP. aeruginosa. No toxicity (LDH release) or inflammatory effects (IL8 transcription) were observed over 24 h.ConclusionsTogether, these data suggest multiple immune pathways are stimulated by SC79, with antipathogen effects. This in vitro pilot study suggests that a small‐molecule Akt activator may have clinical utility in CRS or respiratory other infection settings, warranting future in vivo studies.
Bidirectional Regulation of Intracellular Enzyme Activity Using Light‐Driven Nano‐Inhibitors
Authors: Zhao Yu , Huang Qingqing , Li Qiushi , Chen Zihan , Liu Yang 
Published: January 2024

AbstractPhotochemical regulation provides precise control over enzyme activities with high spatiotemporal resolution. A promising approach involves anchoring “photoswitches” at enzyme active sites to modulate substrate recognition. However, current methods often require genetic mutations and irreversible enzyme modifications for the site‐specific anchoring of “photoswitches”, potentially compromising the enzyme activities. Herein, we present a pioneering reversible nano‐inhibitor based on molecular imprinting technique for bidirectional regulation of intracellular enzyme activity. The nano‐inhibitor employs a molecularly imprinted polymer nanoparticle as its body and azobenzene‐modified inhibitors (“photoswitches”) as the arms. By using a target enzyme as the molecular template, the nano‐inhibitor acquires oriented binding sites on its surface, resulting in a high affinity for the target enzyme and non‐covalently firm anchoring of the azobenzene‐modified inhibitor to the enzyme active site. Harnessing the reversible isomerization of azobenzene units upon exposure to ultraviolet and visible light, the nano‐inhibitor achieves bidirectional enzyme activity regulation by precisely docking and undocking inhibitor at the active site. Notably, this innovative approach enables the facile in situ regulation of intracellular endogenous enzymes, such as carbonic anhydrase. Our results represent a practical and versatile tool for precise enzyme activity regulation in complex intracellular environments.
A Giant Heterometallic Polyoxometalate Nanocluster for Enhanced Brain‐Targeted Glioma Therapy
Authors: Song Nizi , Lu Mengya , Liu Jiancai , Lin Ming , Shangguan Ping , Wang Jiefei , Shi Bingyang , Zhao Junwei 
Published: January 2024

AbstractGiant heterometallic polyoxometalate (POM) clusters with precise atom structures, flexibly adjustable and abundant active sites are promising for constructing functional nanodrugs. However, current POM drugs are almost vacant in orthotopic brain tumor therapy due to the inability to effectively penetrate the blood–brain barrier (BBB) and low drug activity. Here, we designed the largest (3.0 nm × 6.0 nm) transition‐metal–lanthanide co‐encapsulated POM cluster {[Ce10Ag6(DMEA)(H2O)27W22O70][B‐α‐TeW9O33]9}288− featuring 238 metal centers via synergistic coordination between two geometry‐unrestricted Ce3+ and Ag+ linkers with tungsten‐oxo cluster fragments. This POM was combined with brain‐targeted peptide to prepare a brain‐targeted nanodrug that could efficiently traverse BBB and target glioma cells. The Ag+ active centers in the nanodrug specifically activate reactive oxygen species to regulate the apoptosis pathway of glioma cells with a low half‐maximal inhibitory concentration (5.66 μM). As the first brain‐targeted POM drug, it efficiently prolongs the survival of orthotopic glioma‐bearing mice.
Patient‐derived Immunocompetent Tumor Organoids: A Platform for Chemotherapy Evaluation in the Context of T‐cell Recognition**
Authors: Zhao Zihan , Zhang Shuren , Jiang Ning , Zhu Wenjie , Song Dongfan , Liu Siyang , Yu Wenhao , Bai Yuhao , Zhang Yulin , Wang Xiaoyu , Zhong Xuanmeng , Guo Hongqian , Guo Zijian , Yang Rong , Li Jie P. 
Published: January 2024

AbstractMost of the anticancer compounds synthesized by chemists are primarily evaluated for their direct cytotoxic effects at the cellular level, often overlooking the critical role of the immune system. In this study, we developed a patient‐derived, T‐cell‐retaining tumor organoid model that allows us to evaluate the anticancer efficacy of chemical drugs under the synergistic paradigm of antigen‐specific T‐cell‐dependent killing, which may reveal the missed drug hits in the simple cytotoxic assay. We evaluated clinically approved platinum (Pt) drugs and a custom library of twenty‐eight PtIV compounds. We observed low direct cytotoxicity of Pt drugs, but variable synergistic effects in combination with immune checkpoint inhibitors (ICIs). In contrast, the majority of PtIV compounds exhibited potent tumor‐killing capabilities. Interestingly, several PtIV compounds went beyond direct tumor killing and showed significant immunosynergistic effects with ICIs, outstanding at sub‐micromolar concentrations. Among these, Pt‐19, PtIV compounds with cinnamate axial ligands, emerged as the most therapeutically potent, demonstrating pronounced immunosynergistic effects by promoting the release of cytotoxic cytokines, activating immune‐related pathways and enhancing T cell receptor (TCR) clonal expansion. Overall, this initiative marks the first use of patient‐derived immunocompetent tumor organoids to explore and study chemotherapy, advancing their path toward more effective small molecule drug discovery.
N‐Heterocycle‐Editing to Access Fused‐BN‐Heterocycles via Ring‐Opening/C−H Borylation/Reductive C−B Bond Formation
Authors: Zhang Xu , Su Wanlan , Guo Huosheng , Fang Pengyuan , Yang Kai , Song Qiuling 
Published: January 2024

AbstractSkeletal editing of N‐heterocycles has recently received considerable attention, and the introduction of boron atom into heterocycles often results in positive property changes. However, direct enlargement of N‐heterocycles through boron atom insertion is rarely reported in the literature. Here, we report a N‐heterocyclic editing reaction through the combination boron atom insertion and C−H borylation, accessing the fused‐BN‐heterocycles. The synthetic potential of this chemistry was demonstrated by substrate scope and late‐stage diversification of products.
Confining Bismuth‐Halide Perovskite in Mesochannels of Silica Nanomembranes for Exceptional Photocatalytic Abatement of Air Pollutants
Authors: Yang Jingling , Liu Bin , Zeng Lixi , Du Bibai , Zhou Yingtang , Tao Hengcong , Yun Yang , Zhu Mingshan 
Published: January 2024

AbstractSpatially confined photocatalysis has emerged as a viable strategy for the intensification of various redox reactions, but the influence of confined structure on reaction behavior is always overlooked in gas‐solid reactions. Herein, we report a nanomembrane with confining Cs3Bi2Br9 nanocrystals inside vertical channels of porous insulated silica thin sheets (CBB@SBA(⊥)) for photocatalytic nitric oxide (NO) abatement. The ordered one‐dimensional (1D) pore channels with mere 70 nm channel length provide a highly accessible confined space for catalytic reactions. A record‐breaking NO conversion efficiency of 98.2 % under a weight hourly space velocity (WHSV) of 3.0×106 mL g−1 h−1, as well as exceptionally high stability over 14 h and durability over a wide humidity range (RH=15–90 %) was realized over SBA(⊥) confined Cs3Bi2Br9, well beyond its nonconfined analogue and the Cs3Bi2Br9 confine in Santa Barbara Amorphous (SBA‐15). Mechanism studies suggested that the insulated pore channels of SBA(⊥) in CBB@SBA(⊥) endow concentrated electron field and enhanced mass transfer that render high exposure of reactive species and lower reaction barrier needs for ⋅O2− formation and NO oxidation, as well as prevents structural degradation of Cs3Bi2Br9. This work expands an innovative strategy for designing efficient photocatalysts for air pollution remediation.
Learning functional human anatomy with a new interactive three‐dimensional digital tool
Authors: Gallot Mélanie , di Rienzo Franck , Binay Marion , Collet Christian , Hoyek Nady 
Published: January 2024

AbstractHuman anatomy requires understanding spatial relationships among anatomical structures and is often perceived as difficult to learn by students. To overcome this concern, several digital tools exist with some strengths and limitations among which the lack of interactivity especially for complex functional anatomy learning. In this way, a new interactive three‐dimensional tool called Antepulsio was designed. Antepulsio was assessed by comparing three groups of first year kinesiology students to test whether it is likely to favor functional anatomy learning during three training sessions spread over a week. The experiment was conducted during a real academic course. Laterality judgment, 3D spatial abilities and working memory abilities from all participants were previously collected to create three homogeneous groups: the active group (n = 17, 17.76 ± 0.56 years) interacted with Antepulsio, the passive group (n = 18, 17.89 ± 0.83 years) watched videos of Antepulsio while the control group (n = 15, 18.07 ± 0.80 years) performed a neutral activity unrelated to anatomy. Anatomy knowledge was also assessed during pretest, posttest, and retention test (8 weeks after the posttest). The most significant outcome of this study revealed that in case of better working visual memory, the active group outperformed the passive group between pretest and retention test (p < 0.01). In other words, Antepulsio tool is efficient only for students with high visuospatial working memory. These selective benefits of Antepulsio are discussed in terms of cognitive load, training duration and the necessary period of familiarization with the tool.
Bi‐ and tridentate coordination behaviour of a novel bis(phosphinimino)methanide ligand
Authors: Burgert Bastian B. , Sun Xiaofei , Hauser Adrian , Wingering Perrine M. R. , Breher Frank , Roesky Peter W. 
Published: January 2024

AbstractHerein, we report the synthesis of a novel ferrocenyl‐functionalized bis(phosphinimino)methane ligand (CH2(PPh2NFc)2). Deprotonation of CH2(PPh2NFc)2 with KN(SiMe3)2 gave the dimeric species [K{CH(PPh2NFc)2}]2, which was further reacted with ECl2 (E=Ge, Sn) to yield the tetrylene compounds [{CH(PPh2NFc)2}ECl]. The ligand and the resulting tetrylenes were examined for their electrochemical properties with the aid of cyclic voltammetry. Furthermore, the reaction of the tetrylenes [{CH(PPh2NFc)2}ECl] with [AuC6F5(tht)] resulted in the bimetallic complexes [{(AuC6F5)CH(PPh2NFc)2}ECl] with an unusual Au coordination on the ligand backbone.
Efficiency and safety of hepatic arterial infusion chemotherapy (HAIC) combined with anti‐PD1 therapy versus HAIC monotherapy for advanced hepatocellular carcinoma: A multicenter propensity score matching analysis
Authors: Li Yangyang , Liu Wendao , Chen Junwei , Chen Yongxin , Guo Jiandong , Pang Huajin , Zhang Wentao , An Chao , Li Chengzhi 
Published: January 2024

AbstractPurposeTo investigate the clinical efficacy and safety of combination therapy of hepatic arterial infusion chemotherapy (HAIC) and anti‐programmed cell death protein‐1 (PD‐1) therapy in the treatment of advanced hepatocellular carcinoma (HCC).MethodsIn this retrospective clinical research, from March 2018 to December 2019, 1158 HCC patients categorized as BCLC stage C were reviewed for eligibility. We utilized propensity score matching (PSM) to mitigate initial disparities between the groups. The evaluation of the best tumor response was conducted in accordance with mRECIST 1.1 criteria. The difference in survival outcomes including overall survival (OS), progression‐free survival (PFS), and objective response rate (ORR) between groups were compared.ResultsFollowing the eligibility review, 453 patients underwent a combined treatment of HAIC with PD1 inhibitors (HAIC‐PD1 group), while 221 patients received HAIC monotherapy (HAIC group) met the inclusion criteria and were finally enrolled in this study. In the entire cohort, the HAIC‐PD1 group exhibited significantly prolonged overall survival (median overall survival: 40.4 months vs. 9.7 months, p < 0.001) and progression‐free survival (median progression‐free survival: 22.1 months vs. 5.8 months, p < 0.001). By propensity score, patients were matched according to baseline differences, resulting in all 442 patients in group HAIC‐PD1 (n = 221) and group HAIC (n = 221). After PSM adjustment, as well, the survival of the HAIC‐PD1 group was still distinctly longer than the HAIC group (median overall survival time, 40.4 months vs 9.7 months, p < 0.001; median progression‐free survival, 22.1 months vs 5.7 months, p < 0.001). Univariate and multivariable analysis demonstrated that AFP level, metastasis, and therapeutic schedule were independent predictive factors for overall survival.ConclusionThe combination therapy of HAIC and PD1 inhibitors successfully extended OS to advanced HCC patients and could be a better choice than HAIC monotherapy.