bluuebunny/crossref_metadata_2025 huggingface dataset:
Mental Health Impairment and Outpatient Mental Health Care of US Children and Adolescents
Authors: Olfson Mark , McClellan Chandler , Zuvekas Samuel H. , Wall Melanie , Blanco Carlos
Published: March 2024

Importance

Despite a federal declaration of a national child and adolescent mental health crisis in 2021, little is known about recent national trends in mental health impairment and outpatient mental health treatment of US children and adolescents.

Objective

To characterize trends in mental health impairment and outpatient mental health care among US children and adolescents from 2019 to 2021 across demographic groups and levels of impairment.

Design, Setting, and Participants

Survey study with a repeated cross-sectional analysis of mental health impairment and outpatient mental health care use among youth (ages 6-17 years) within the 2019 and 2021 Medical Expenditure Panel Surveys, nationally representative surveys of US households. Race and ethnicity were parent reported separately from 15 racial categories and 8 ethnic categories that were aggregated into Black, non-Hispanic; Hispanic; Other, non-Hispanic; and White, non-Hispanic.

Exposure

Time period from 2019 to 2021.

Main Outcomes and Measures

Age- and sex-adjusted differences between 2019 and 2021 in mental health impairment measured with the Columbia Impairment Scale (a score ≥16 indicates severe; 1-15, less severe; and 0, no impairment) and age-, sex-, and Columbia Impairment Scale strata–adjusted differences in the use of any outpatient mental health care in 2019 and 2021.

Results

The analysis involved 8331 participants, including 4031 girls and 4300 boys; among them, 1248 were Black and 3385 were White. The overall mean (SE) age was 11.6 (3.4) years. The percentage of children and adolescents with severe mental health impairment was 9.7% in 2019 and 9.4% in 2021 (adjusted difference, −0.3%; 95% CI, −1.9% to 1.2%). Between 2019 and 2021, there was also no significant difference in the percentage of children and adolescents with less severe impairment and no impairment. The overall annual percentages of children with any outpatient mental health care showed little change: 11.9% in 2019 and 13.0% in 2021 (adjusted difference, 1.3%; 95% CI, −0.4% to 3.0%); however, this masked widening differences by race. Outpatient mental health care decreased for Black youth from 9.2% in 2019 to 4.0% in 2021 (adjusted difference, −4.3%; 95% CI, −7.3% to −1.4%) and increased for White youth from 15.1% to 18.4% (adjusted difference, 3.0%; 95% CI, 0.0% to 6.0%).

Conclusions and Relevance

Between 2019 and 2021, there was little change in the overall percentage of US children and adolescents with severe mental health impairment. During this period, however, there was a significant increase in the gap separating outpatient mental health care of Black and White youth.
Recrystallization Behavior of Ti–6.5Al–3.5Mo–1.5Zr–0.3Si Alloy under Electroshocking Treatment
Authors: Zhou Jian , Sun Hongxin , Wen Yan , Li Jiashun , Wang Liqiang , Zhang Lai‐Chang , Xie Lechun
Published: March 2024

In this work, a novel electroshocking treatment (EST) method is employed to modify the microstructure of Ti–6.5Al–3.5Mo–1.5Zr–0.3Si alloy. The microstructural morphology and texture distribution after EST are characterized and analyzed to study the recrystallization behavior of the titanium alloy. After EST with 0.04 s, secondary αs phase transforms into β phase. After EST with 0.06 s, surrounding the αp phase, a significant amount of needlelike martensitic phase (αM) precipitates. Electron backscatter diffraction results reveal that EST reduces intragranular orientation gradients, resulting in a convergence of each point orientations within individual grains. Under longer EST time, grain boundaries display greater irregularity. After EST with 0.05 s, partial recrystallization takes place, and with an increase of EST time to 0.06 s, all deformed grains undergo complete recrystallization, forming defect‐free recrystallized grains. A substantial enhancement in texture intensity for both α and β phases, exhibiting prominent preferred orientations, and the increase in hardness values is contributed to the precipitation of αM phase. The stress analyses indicate that EST can optimize the distribution of residual stress and offer a potential solution for improving fatigue performance. In all results, it is shown that EST is an effective approach for manipulating the microstructure and optimizing the residual stress distribution of titanium alloys.
Domain Dynamics and Resistive Switching in Ferroelectric Al1–xScxN Thin Film Capacitors
Authors: Lu Haidong , Schönweger Georg , Petraru Adrian , Kohlstedt Hermann , Fichtner Simon , Gruverman Alexei
Published: March 2024

In this paper, using a combination of pulse testing measurements and piezoresponse force microscopy (PFM), an investigation of the polarization reversal behavior and the accompanying resistive switching in the Al0.72Sc0.28N thin film capacitors is reported. The obtained results reveal a transition from the nucleation‐limited switching (NLS) in the low field range toward the more uniform switching described by the Kolmogorov–Avrami–Ishibashi (KAI) model in the high field range. It is found that the Al0.72Sc0.28N capacitors exhibit an unusually steep change in the switching time– it decreases by five orders of magnitude with a moderate increase of the applied field. This feature is caused by a significantly higher activation field value (≈126 MV cm−1) in comparison with the conventional perovskite ferroelectrics. PFM visualization of the field‐induced domain dynamics has allowed the evaluation of the nucleation rate and domain wall velocity. Furthermore, capacitors in the polydomain state generated by partial switching of polarization exhibit a significant (up to two orders of magnitude) increase in the steady‐state conductance. This effect is likely caused by the injection of strongly inclined conducting 180° domain walls. Resistance tunability offers additional functionalities to the Al1‐xScxN devices where conductive domain walls are used as active elements.
Natural Glycyrrhizic Acid‐Tailored Nanoparticles toward the Enhancement of Pesticide Bioavailability
Authors: Wei Kailun , Li Zilu , Zheng Zhiran , Gao Yuxia , Huang Qiliang , Li Min‐Hui , Hu Jun
Published: March 2024

Pesticide spraying serves as a prevalent segment in crop production for substantial economic and ecological benefits. Nevertheless, the existing pesticide formulations are often plagued by droplets rebounding during the spraying process, and the controlled‐release, photolysis protection, and non‐targeted bio‐friendliness are not inadequately considered. Herein, by combining spinosad (SSD, a model pesticide) with glycyrrhizic acid (GL) as an attractive building block, a supramolecular co‐assembly strategy is employed to elaborate pesticide formulations (GL‐SSD) simultaneously featuring high deposition, controlled‐release, and environmental friendliness. The resulting spherical GL‐SSD nanoparticles (NPs) have an average diameter of 207 nm and show an improved 5.2‐fold photostability compared with commercial spinosad suspension (SSD SC). Upon impacting on hydrophobic surfaces of polytetrafluoroethylene film and cabbage leaf, the droplets of GL‐SSD NPs exhibit superior affinity to the micro/nano structure of the surface. Consequently, the droplet rebounding is inhibited effectively, ensuring high deposition efficiency of droplets on surfaces. In addition, the release of SSD from GL‐SSD NPs can be controlled by pH variation. Indoor toxicity and pot experiments demonstrate that GL‐SSD NPs possess good control efficacy against Plutella xylostella. The work offers an alternative approach for the development of multi‐functional and sustainable pesticide formulations with promising potentials in actual agriculture production.
V‐Doping Strategy Induces the Construction of the Functionally Complementary Ru2P/V‐RuP4 Heterostructures to Achieve Amperometric Current Density for HER
Authors: Liu Jie , Ren Jinhong , Du Yunmei , Chen Xiao , Wang Mengmeng , Liu Yanru , Wang Lei
Published: March 2024

It is a great challenge to induce the formation of the RuP4 phase and realize the construction of a metal‐rich phase/phosphorus‐rich phase‐ruthenium phosphide heterostructure by directional regulation of the proportion of P and metal atoms. The ultra‐high conductivity of Ru2P and the excellent ability of V‐doped RuP4 to absorb/desorb H* are confirmed by density functional theory (DFT) calculations, which laid a theoretical foundation for the construction of a unique Ru2P/V‐RuP4 structure to accelerate HER reaction kinetics. This work innovatively uses the V‐doping strategy to induce the formation of RuP4 phase with high intrinsic activity, and finally construct V‐RuxPy nanosheets with rich Ru/Ru2P/V‐RuP4 heterostructures. Thanks to the rich Ru/Ru2P/V‐RuP4 heterostructure and the optimization of V dopants, the V‐RuxPy catalyst only needs 180 mV to obtain an industrial‐grade current density of 1 A cm−2. In summary, this work provides a new idea for the design and performance optimization of ruthenium‐based catalysts.
A Scanning Microwave Impedance Microscopy Study of α‐In2Se3 Ferroelectric Semiconductor
Authors: Wang Lin , Chen Han , Chen Mingfeng , Long Yinfeng , Liu Kai , Loh Kian Ping
Published: March 2024

Van der Waals ferroelectric semiconductors, which encompass both ferroelectricity and semiconductivity, have garnered intensive research interests for developing novel non‐volatile functional devices. Previous studies focus on ferroelectricity characterization and device demonstration, with little attention paid to the fundamental electronic properties of these materials and their functional structures, which are essential for both device design and optimization. In this study, scanning microwave impedance microscopy (sMIM) is utilized to investigate the ferroelectric semiconductor of α‐phase indium selenide (α‐In2Se3) and its synaptic field effect transistors. α‐In2Se3 nanoflakes of varying thicknesses are visualized through capacitive signal detection, whose responses are consistent with finite element simulations manifesting dependence on both flake thickness and its semiconductor property. sMIM spectroscopy performed on α‐In2Se3‐based metal‐oxide‐semiconductor (MOS) structures reveals typical MOS capacitance‐voltage characteristics, with additional hysteresis arising from the ferroelectric switching of α‐In2Se3. The local conductance state changes of synaptic α‐In2Se3 ferroelectric semiconductor transistors (FeSFET) in response to gate voltage stimuli are effectively detected by in situ sMIM, in good agreement with electrical device transport properties. This work deepens the understanding of ferroelectric semiconductor physics toward their practical device application.
Self‐Limited Formation of Nanoporous Nickel Heterostructure Catalyst for Electrochemical Hydrogen Production
Authors: Qiao Lin , Xi Cong , Li Chao , Zhang Kaiyue , Li Qi , Han Jiuhui , Ding Yi
Published: March 2024

Nickel has risen as a viable and cost‐effective substitute to noble metal catalysts in electrochemical hydrogen production, yet developing air‐stable and highly efficient nanostructured nickel‐based catalysts remains a significant challenge. Here a facile method for creating nanoporous Ni/NiO heterostructure catalysts for electrocatalytic hydrogen production is reported. The protocol employs chemical dealloying to establish a 3D bicontinuous nanoporous structure, followed by a controlled oxidation process to in situ generate uniform NiO surface layers atop the metallic nickel matrix in a self‐limiting manner. This approach not only yields highly active nickel‐based catalysts through a simple and controlled procedure but also effectively mitigates the auto‐ignition issue inherent in nanosized Ni, thereby enhancing air stability. By leveraging the synergistic interaction between Ni‐NiO co‐catalysis and improved access to intensified active sites, the electrocatalysts exhibit superior performance in the hydrogen evolution reaction, markedly outperforming noble Pt/C catalysts, and high stability in alkaline environments. The exploration of self‐limiting oxidation in nanostructured transition metals opens new avenues for developing advanced metal/oxide heterostructure catalysts for diverse energy applications.
Synthetic Colonic Mucus Enables the Development of Modular Microbiome Organoids
Authors: Miller Michael A. , Medina Scott
Published: March 2024

The human colon is home to trillions of microorganisms that modulate gastrointestinal physiology. The understanding of how this gut ecosystem impacts human health, although evolving, is slowed by the lack of accessible tools suitable to studying complex host‐mucus‐microbe interactions. Here, a synthetic gel‐like material capable of recapitulating the varied structural, mechanical, and biochemical profiles of native human colonic mucus is reported to develop compositionally simple microbiome screening platforms with utility in microbiology and drug discovery. The viscous fibrillar material is realized through templated assembly of a fluorine‐rich amino acid at liquid‐liquid interphases. The fluorine‐assisted mucus surrogate (FAMS) can be decorated with mucins to serve as a habitat for microbial colonization and integrated with human colorectal cells to generate artificial mucosae, referred to as a microbiome organoid. Notably, FAMS are made with inexpensive and commercially available materials and can be generated using simple protocols and standard laboratory hardware. As a result, this platform can be broadly incorporated into various laboratory settings to advance probiotic research and inform in vivo approaches. If implemented into high throughput screening approaches, FAMS may represent a valuable tool to study compound metabolism and gut permeability, with an exemplary demonstration of this utility presented here.
Nonhalogenated Solvent Processable and High‐Density Photopatternable Polymer Semiconductors Enabled by Incorporating Hydroxyl Groups in the Side Chains
Authors: Gao Chenying , Li Cheng , Yang Yiming , Jiang Ziling , Xue Xiang , Chenchai Kaiyuan , Liao Junchao , Shangguan Zhichun , Wu Changchun , Zhang Xisha , Jia Di , Zhang Fengjiao , Liu Guoming , Zhang Guanxin , Zhang Deqing
Published: March 2024

Polymer semiconductors hold tremendous potential for applications in flexible devices, which is however hindered by the fact that they are usually processed by halogenated solvents rather than environmentally more friendly solvents. An effective strategy to boost the solubility of high‐performance polymer semiconductors in nonhalogenated solvents such as tetrahydrofuran (THF) by appending hydroxyl groups in the side chains is herein presented. The results show that hydroxyl groups, which can be easily incorporated into the side chains, can significantly improve the solubility of typical p‐ and n‐types as well as ambipolar polymer semiconductors in THF. Meanwhile, the thin films of these polymer semiconductors from the respective THF solutions show high charge mobilities. With THF as the processing and developing solvents these polymer semiconductors with hydroxyl groups in the side chains can be well photopatterned in the presence of the photo‐crosslinker, and the charge mobilities of the patterned thin films are mostly maintained by comparing with those of the respective pristine thin films. Notably, THF is successfully utilized as the processing and developing solvent to achieve high‐density photopatterning with ≈82 000 device arrays cm−2 for polymer semiconductors in which hydroxyl groups are appended in the side chains.
Salt‐Assisted Vapor–Liquid–Solid Growth of 1D van der Waals Materials
Authors: Pham Thang , Reidy Kate , Thomsen Joachim D. , Wang Baoming , Deshmukh Nishant , Filler Michael A. , Ross Frances M.
Published: March 2024

The method of salt‐assisted vapor–liquid–solid (VLS) growth is introduced to synthesize 1D nanostructures of trichalcogenide van der Waals (vdW) materials, exemplified by niobium trisulfide (NbS3). The method uses a unique catalyst consisting of an alloy of Au and an alkali metal halide (NaCl) to enable rapid and directional growth. High yields of two types of NbS3 1D nanostructures, nanowires and nanoribbons, each with sub‐ten nanometer diameter, tens of micrometers length, and distinct 1D morphology and growth orientation are demonstrated. Strategies to control the location, size, and morphology of growth, and extend the growth method to synthesize other transition metal trichalcogenides, NbSe3 and TiS3, as nanowires are demonstrated. Finally, the role of the Au–NaCl alloy catalyst in guiding VLS synthesis is described and the growth mechanism based on the relationships measured between structure (growth orientation, morphology, and dimensions) and growth conditions (catalyst volume and growth time) is discussed. These results introduce opportunities to expand the library of emerging 1D vdW materials to make use of their unique properties through controlled growth at nanoscale dimensions.
Anchoring Active Li Metal in Oriented Channel by In Situ Formed Nucleation Sites Enabling Durable Lithium‐Metal Batteries
Authors: Peng Huai‐Yu , Xu Yan‐Song , Wei Xu‐Yang , Li Yun‐Nuo , Liang Xiongyi , Wang Jun , Tan Shuang‐Jie , Guo Yu‐Guo , Cao Fei‐Fei
Published: March 2024

Lithium metal is the ultimate anode material for pursuing the increased energy density of rechargeable batteries. However, fatal dendrites growth and huge volume change seriously hinder the practical application of lithium metal batteries (LMBs). In this work, a lithium host that preinstalled CoSe nanoparticles on vertical carbon vascular tissues (VCVT/CoSe) is designed and fabricated to resolve these issues, which provides sufficient Li plating space with a robust framework, enabling dendrite‐free Li deposition. Their inherent N sites coupled with the in situ formed lithiophilic Co sites loaded at the interface of VCVT not only anchor the initial Li nucleation seeds but also accelerate the Li+ transport kinetics. Meanwhile, the Li2Se originated from the CoSe conversion contributes to constructing a stable solid‐electrolyte interphase with high ionic conductivity. This optimized Li/VCVT/CoSe composite anode exhibits a prominent long‐term cycling stability over 3000 h with a high areal capacity of 10 mAh cm−2. When paired with a commercial nickel‐rich LiNi0.83Co0.12Mn0.05O2 cathode, the full‐cell presents substantially enhanced cycling performance with 81.7% capacity retention after 300 cycles at 0.2 C. Thus, this work reveals the critical role of guiding Li deposition behavior to maintain homogeneous Li morphology and pave the way to stable LMBs.
Manipulating Hetero‐Nanowire Films for Flexible and Multifunctional Thermoelectric Devices
Authors: Chen Cheng , Xu Feng‐Qi , Wu Yabei , Li Xin‐Lin , Xu Jie‐Long , Zhao Bin , He Zhen , Yang Jiong , Zhang Wenqing , Liu Jian‐Wei
Published: March 2024

Flexible thermoelectric devices hold significant promise in wearable electronics owing to their capacity for green energy generation, temperature sensing, and comfortable wear. However, the simultaneous achievement of excellent multifunctional sensing and power generation poses a challenge in these devices. Here, ordered tellurium‐based hetero‐nanowire films are designed for flexible and multifunctional thermoelectric devices by optimizing the Seebeck coefficient and power factor. The obtained devices can efficiently detect both object and environment temperature, thermal conductivity, heat proximity, and airflow. In addition, combining the thermoelectric units with radiative cooling materials exhibits remarkable thermal management capabilities, preventing device overheating and avoiding degradation in power generation. Impressively, this multifunctional electronics exhibits excellent resistance in extreme low earth orbit environments. The fabrication of such thermoelectric devices provides innovative insights into multimodal sensing and energy harvesting.
Spatiotemporal‐Controlled NIR‐II Immune Agonist Sensitizes Cancer Immunotherapy
Authors: Guo Shuai , Tang Dongsheng , Zhang Mengjie , Yang Haiyin , Zhang Tian , Hu Bo , Xu Chun , Weng Yuhua , Shang Kun , Huang Yuanyu
Published: March 2024

The integration of nanomedicine and immunotherapy has presented a promising opportunity for the treatment of cancer and diverse diseases. However, achieving spatiotemporal controllable immunotherapy with excellent efficacy and safety performances remains a significant challenge. This study develops a biodegradable near‐infrared II (NIR‐II) photothermal response polymer nanoparticle (PTEQ) system. This platform exhibits intrinsic immunostimulatory properties while concurrently delivering siRNA for Programmed Death‐Ligand 1 (siPD‐L1), leveraging enhanced immune responses and immune checkpoint blockade for safe and effective cancer therapy. In the CT26 tumor‐bearing mouse model, PTEQ, as an immune stimulant, significantly boosts the infiltration of CD4+ and CD8+ T cells within the tumor microenvironment (TME). The PTEQ/siPD‐L1+laser group not only initiates NIR‐II photothermal therapy but also promotes the activation and infiltration of T cells, M1 macrophage polarization, and maturation of dendritic cells in the TME, resulting in the complete elimination of tumors in 7/10 cases, achieving a 100% survival rate. In another in vivo vaccine experiment, all tumors on the right side are completely eliminated in the PTEQ/siPD‐L1+laser group, reaching a 100% tumor eradication rate. These findings underscore the potential of this strategy to overcome the current immunotherapeutic limitations and achieve immune therapy normalization.
Dendronized Polymer‐Derived Nanomedicines for Mitochondrial Dynamics Regulation and Immune Modulation
Authors: Hou Xingyu , Pan Dayi , Zhong Dan , Gong Qiyong , Luo Kui
Published: March 2024

The effects of dendron side chains in polymeric conjugates on tumor penetration and antigen presentation are systematically examined. Three polymer‐gemcitabine (Gem) conjugates (pG0‐Gem, pG1‐Gem, pG2‐Gem) are designed and prepared. The pG2‐Gem conjugate uniquely binds to the mitochondria of tumor cells, thus regulating mitochondrial dynamics. The interaction between the pG2‐Gem conjugate and the mitochondria promotes great penetration and accumulation of the conjugate at the tumor site, resulting in pronounced antitumor effects in an animal model. Such encouraging therapeutic effects can be ascribed to immune modulation since MHC‐1 antigen presentation is significantly enhanced due to mitochondrial fusion and mitochondrial metabolism alteration after pG2‐Gem treatment. Crucially, the drug‐free dendronized polymer, pG2, is identified to regulate mitochondrial dynamics, and the regulation is independent of the conjugated Gem. Furthermore, the combination of pG2‐Gem with anti‐PD‐1 antibody results in a remarkable tumor clearance rate of 87.5% and a prolonged survival rate of over 150 days, demonstrating the potential of dendronized polymers as an innovative nanoplatform for metabolic modulation and synergistic tumor immunotherapy.
Spatiotemporal Reaction Dynamics Control in Two‐Photon Polymerization for Enhancing Writing Characteristics
Authors: Mao Aofei , Fess Sarah , Kraiem Nada , Li Peizi , Wu Zhipeng , Zhu Qiuchi , Huang Xi , Fan Peixun , Cui Bai , Silvain Jean‐Francois , Hu Suxing , Anthamatten Mitchell , Regan Sean P. , Harding David , Lu Yongfeng
Published: March 2024

Since 2001, 3D microfabrication based on two‐photon polymerization (TPP) has drawn extensive attention and interest in biology, optics, photonics, material science, and high‐energy physics. The in‐volume fabrication capability due to the threshold behavior of two‐photon absorption enables TPP higher flexibility compared with other nanofabrication techniques. However, as determined by the in‐volume fabrication feature as well as various reaction dynamics, the writing characteristics of TPP, such as throughput, accuracy, surface quality, and fabrication capability, are still limited. Herein, a comprehensive study is performed on the spatiotemporal behavior of reaction dynamics during TPP fabrication, mainly focusing on spatiotemporal characteristics of radical diffusion, photothermal effect, microscale mechanics, and voxel stacking process. Based on the study, a nonsequential fabrication method is established to simultaneously improve key writing characteristics of TPP and realize sharp features, high speeds, large overhang structure, and smooth surfaces. The method established in this work can be applied to improve the performance of functional devices for various fields.
Mesenchymal Stem Cells‐Involved Strategies for Rheumatoid Arthritis Therapy
Authors: Li Chaoyang , Sun Yifu , Xu Weiguo , Chang Fei , Wang Yinan , Ding Jianxun
Published: March 2024

Rheumatoid arthritis (RA) is a systemic autoimmune disease characterized by chronic inflammation of the joints and bone destruction. Because of systemic administration and poor targeting, traditional anti‐rheumatic drugs have unsatisfactory treatment efficacy and strong side effects, including myelosuppression, liver or kidney function damage, and malignant tumors. Consequently, mesenchymal stem cells (MSCs)‐involved therapy is proposed for RA therapy as a benefit of their immunosuppressive and tissue‐repairing effects. This review summarizes the progress of MSCs‐involved RA therapy through suppressing inflammation and promoting tissue regeneration and predicts their potential clinical application.
Gastrointestinal Dysmotility Predisposes to Colitis through Regulation of Gut Microbial Composition and Linoleic Acid Metabolism
Authors: Zhang Youhua , Song Feifei , Yang Muqing , Chen Chunqiu , Cui Jiaqu , Xing Mengyu , Dai Yuna , Li Man , Cao Yuan , Lu Ling , Zhu Huiyuan , Liu Ying , Ma Chunlian , Wei Qing , Qin Huanlong , Li Jiyu
Published: March 2024

Disrupted gastrointestinal (GI) motility is highly prevalent in patients with inflammatory bowel disease (IBD), but its potential causative role remains unknown. Herein, the role and the mechanism of impaired GI motility in colitis pathogenesis are investigated. Increased colonic mucosal inflammation is found in patients with chronic constipation (CC). Mice with GI dysmotility induced by genetic mutation or chemical insult exhibit increased susceptibility to colitis, dependent on the gut microbiota. GI dysmotility markedly decreases the abundance of Lactobacillus animlalis and increases the abundance of Akkermansia muciniphila. The reduction in L. animlalis, leads to the accumulation of linoleic acid due to compromised conversion to conjugated linoleic acid. The accumulation of linoleic acid inhibits Treg cell differentiation and increases colitis susceptibility via inducing macrophage infiltration and proinflammatory cytokine expression in macrophage. Lactobacillus and A. muciniphila abnormalities are also observed in CC and IBD patients, and mice receiving fecal microbiota from CC patients displayed an increased susceptibility to colitis. These findings suggest that GI dysmotility predisposes host to colitis development by modulating the composition of microbiota and facilitating linoleic acid accumulation. Targeted modulation of microbiota and linoleic acid metabolism may be promising to protect patients with motility disorder from intestinal inflammation.
A Multifunctional Therapeutic Strategy Using P7C3 as A Countermeasure Against Bone Loss and Fragility in An Ovariectomized Rat Model of Postmenopausal Osteoporosis
Authors: Wei Fei , Hughes Megan , Omer Mahmoud , Ngo Christopher , Pugazhendhi Abinaya Sindu , Kolanthai Elayaraja , Aceto Matthew , Ghattas Yasmine , Razavi Mehdi , Kean Thomas J , Seal Sudipta , Coathup Melanie
Published: March 2024

By 2060, an estimated one in four Americans will be elderly. Consequently, the prevalence of osteoporosis and fragility fractures will also increase. Presently, no available intervention definitively prevents or manages osteoporosis. This study explores whether Pool 7 Compound 3 (P7C3) reduces progressive bone loss and fragility following the onset of ovariectomy (OVX)‐induced osteoporosis. Results confirm OVX‐induced weakened, osteoporotic bone together with a significant gain in adipogenic body weight. Treatment with P7C3 significantly reduced osteoclastic activity, bone marrow adiposity, whole‐body weight gain, and preserved bone area, architecture, and mechanical strength. Analyses reveal significantly upregulated platelet derived growth factor‐BB and leukemia inhibitory factor, with downregulation of interleukin‐1 R6, and receptor activator of nuclear factor kappa‐B (RANK). Together, proteomic data suggest the targeting of several key regulators of inflammation, bone, and adipose turnover, via transforming growth factor‐beta/SMAD, and Wingless‐related integration site/be‐catenin signaling pathways. To the best of the knowledge, this is first evidence of an intervention that drives against bone loss via RANK. Metatranscriptomic analyses of the gut microbiota show P7C3 increased Porphyromonadaceae bacterium, Candidatus Melainabacteria, and Ruminococcaceae bacterium abundance, potentially contributing to the favorable inflammatory, and adipo‐osteogenic metabolic regulation observed. The results reveal an undiscovered, and multifunctional therapeutic strategy to prevent the pathological progression of OVX‐induced bone loss.
NHC‐Au‐Catalyzed Isomerization of Propargylic B(MIDA)s to Allenes and Double Isomerization of Alkynes to 1,3‐Dienes
Authors: Liu Li‐Cai , Lin Shuang , Xu Kangwei , Qian Jiasheng , Wu Ruibo , Li Qingjiang , Wang Honggen
Published: March 2024

The synthesis of allenyl boronates is an important yet challenging topic in organic synthesis. Reported herein is an NHC‐gold‐catalyzed 1,3‐H shift toward allenyl boronates synthesis from simple propargylic B(MIDA)s. Mechanistic studies suggest dual roles of the boryl moiety in the reaction: to activate the substrate for isomerization and at the same time, to prevent the allene product from further isomerization. These effects should be a result of α‐anion stabilization and α‐cation destabilization conferred by the B(MIDA) moiety, respectively. The NHC‐Au catalyst, which is commercially available, is also found to be reactive in alkyne‐to‐1,3‐diene isomerization reactions in an atom‐economic and base‐free manner.
Photo‐Induced Charge State Dynamics of the Neutral and Negatively Charged Silicon Vacancy Centers in Room‐Temperature Diamond
Authors: Garcia‐Arellano G. , López‐Morales G. I. , Manson N. B. , Flick J. , Wood A. A. , Meriles C. A.
Published: March 2024

The silicon vacancy (SiV) center in diamond is drawing much attention due to its optical and spin properties, attractive for quantum information processing and sensing. Comparatively little is known, however, about the dynamics governing SiV charge state interconversion mainly due to challenges associated with generating, stabilizing, and characterizing all possible charge states, particularly at room temperature. Here, multi‐color confocal microscopy and density functional theory are used to examine photo‐induced SiV recombination — from neutral, to single‐, to double‐negatively charged — over a broad spectral window in chemical‐vapor‐deposition (CVD) diamond under ambient conditions. For the SiV0 to SiV‐ transition, a linear growth of the photo‐recombination rate with laser power at all observed wavelengths is found, a hallmark of single photon dynamics. Laser excitation of SiV‒, on the other hand, yields only fractional recombination into SiV2‒, a finding that is interpreted in terms of a photo‐activated electron tunneling process from proximal nitrogen atoms.
Easy but Efficient: Facile Approach to Molecule with Theoretically Justified Donor–Acceptor Structure for Effective Photothermal Conversion and Intravenous Photothermal Therapy
Authors: Zhong Yuan‐Hui , Huang Gui‐Feng , Zhao Sheng‐Yi , Chung Lai‐Hon , Zhang Hua‐Tang , Zheng Jin‐Hong , Yan Yi‐Lang , Ni Wen‐Xiu , He Jun
Published: March 2024

To accelerate the pace in the field of photothermal therapy (PTT), it is urged to develop easily accessible photothermal agents (PTAs) showing high photothermal conversion efficiency (PCE). As a proof‐of‐concept, hereby a conventional strategy is presented to prepare donor–acceptor (D–A) structured PTAs through cycloaddition‐retroelectrocyclization (CA–RE) reaction, and the resultant PTAs give high PCE upon near‐infrared (NIR) irradiation. By joint experimental‐theoretical study, these PTAs exhibit prominent D–A structure with strong intramolecular charge transfer (ICT) characteristics and significantly twisting between D and A units which account for the high PCEs. Among them, the DMA‐TCNQ exhibits the strongest absorption in NIR range as well as the highest PCE of 91.3% upon irradiation by 760‐nm LED lamp (1.2 W cm−2). In vitro and in vivo experimental results revealed that DMA‐TCNQ exhibits low dark toxicity and high phototoxicity after IR irradiation along with nude mice tumor inhibition up to 81.0% through intravenous therapy. The findings demonstrate CA–RE reaction as a convenient approach to obtain twisted D–A structured PTAs for effective PTT and probably promote the progress of cancer therapies.
Interface Modulation for the Heterointegration of Diamond on Si
Authors: Li Xing , Wan Li , Lin Chaonan , Huang Wen‐Tao , Zhou Jing , Zhu Jie , Yang Xun , Yang Xigui , Zhang Zhenfeng , Zhu Yandi , Ren Xiaoyan , Jin Ziliang , Dong Lin , Cheng Shaobo , Li Shunfang , Shan Chongxin
Published: March 2024

Along with the increasing integration density and decreased feature size of current semiconductor technology, heterointegration of the Si‐based devices with diamond has acted as a promising strategy to relieve the existing heat dissipation problem. As one of the heterointegration methods, the microwave plasma chemical vapor deposition (MPCVD) method is utilized to synthesize large‐scale diamond films on a Si substrate, while distinct structures appear at the Si‐diamond interface. Investigation of the formation mechanisms and modulation strategies of the interface is crucial to optimize the heat dissipation behaviors. By taking advantage of electron microscopy, the formation of the epitaxial β‐SiC interlayer is found to be caused by the interaction between the anisotropically sputtered Si and the deposited amorphous carbon. Compared with the randomly oriented β‐SiC interlayer, larger diamond grain sizes can be obtained on the epitaxial β‐SiC interlayer under the same synthesis condition. Moreover, due to the competitive interfacial reactions, the epitaxial β‐SiC interlayer thickness can be reduced by increasing the CH4/H2 ratio (from 3% to 10%), while further increase in the ratio (to 20%) can lead to the broken of the epitaxial relationship. The above findings are expected to provide interfacial design strategies for multiple large‐scale diamond applications.
Nucleation of Huntingtin Aggregation Proceeds via Conformational Conversion of Pre‐Formed, Sparsely‐Populated Tetramers
Authors: Torricella Francesco , Tugarinov Vitali , Clore G. Marius
Published: March 2024

Pathogenic huntingtin exon‐1 protein (httex1), characterized by an expanded polyglutamine tract located between the N‐terminal amphiphilic region and a C‐terminal polyproline‐rich domain, forms fibrils that accumulate in neuronal inclusion bodies, and is associated with a fatal, autosomal dominant neurodegenerative condition known as Huntington's disease. Here a complete kinetic model is described for aggregation/fibril formation of a httex1 construct with a 35‐residue polyglutamine repeat, httex1Q35. Using exchange NMR spectroscopy, it is previously shown that the reversible formation of a sparsely‐populated tetramer of the N‐terminal amphiphilic domain of httex1Q35, comprising a D2 symmetric four‐helix bundle, occurs on the microsecond time‐scale and is a prerequisite for subsequent nucleation and fibril formation on a time scale that is many orders of magnitude slower (hours). Here a unified kinetic model of httex1Q35 aggregation is developed in which fast, reversible tetramerization is directly linked to slow irreversible fibril formation via conversion of pre‐equilibrated tetrameric species to “active”, chain elongation‐capable nuclei by conformational re‐arrangement with a finite, monomer‐independent rate. The unified model permits global quantitative analysis of reversible tetramerization and irreversible fibril formation from a time series of 1H‐15N correlation spectra recorded during the course of httex1Q35 aggregation.
Innovative Arylimidazole‐Fused Phytovirucides via Carbene‐Catalyzed [3+4] Cycloaddition: Locking Viral Cell‐To‐Cell Movement by Out‐Competing Virus Capsid‐Host Interactions
Authors: Wei Chunle , Zhao Chunni , Li Jiao , Li Chunyi , Song Baoan , Song Runjiang
Published: March 2024

The control of potato virus Y (PVY) induced crop failure is a challengeable issue in agricultural chemistry. Although many anti‐PVY agents are designed to focus on the functionally important coat protein (CP) of virus, how these drugs act on CP to inactivate viral pathogenicity, remains largely unknown. Herein, a PVY CP inhibitor ‐3j (S) is disclosed, which is accessed by developing unusually efficient (up to 99% yield) and chemo‐selective (> 99:1 er in most cases) carbene‐catalyzed [3+4] cycloaddition reactions. Compound ‐3j bears a unique arylimidazole‐fused diazepine skeleton and shows chirality‐preferred performance against PVY. In addition, ‐3j (S) as a mediator allows ARG191 (R191) of CP to be identified as a key amino acid site responsible for intercellular movement of virions. R191 is further demonstrated to be critical for the interaction between PVY CP and the plant functional protein NtCPIP, enabling virions to cross plasmodesmata. This key step can be significantly inhibited through bonding with the ‐3j (S) to further impair pathogenic behaviors involving systemic infection and particle assembly. The study reveals the in‐depth mechanism of action of antiviral agents targeting PVY CP, and contributes to new drug structures and synthetic strategies for PVY management.
Nanowire Array Breath Acetone Sensor for Diabetes Monitoring
Authors: Wei Shiyu , Li Zhe , Murugappan Krishnan , Li Ziyuan , Lysevych Mykhaylo , Vora Kaushal , Tan Hark Hoe , Jagadish Chennupati , Karawdeniya Buddini I , Nolan Christopher J , Tricoli Antonio , Fu Lan
Published: March 2024

Diabetic ketoacidosis (DKA) is a life‐threatening acute complication of diabetes characterized by the accumulation of ketone bodies in the blood. Breath acetone, a ketone, directly correlates with blood ketones. Therefore, monitoring breath acetone can significantly enhance the safety and efficacy of diabetes care. In this work, the design and fabrication of an InP/Pt/chitosan nanowire array‐based chemiresistive acetone sensor is reported. By incorporation of chitosan as a surface‐functional layer and a Pt Schottky contact for efficient charge transfer processes and photovoltaic effect, self‐powered, highly selective acetone sensing is achieved. The sensor has exhibited an ultra‐wide acetone detection range from sub‐ppb to >100 000 ppm level at room temperature, covering those in the exhaled breath from healthy individuals (300–800 ppb) to people at high risk of DKA (>75 ppm). The nanowire sensor has also been successfully integrated into a handheld breath testing prototype, the Ketowhistle, which can successfully detect different ranges of acetone concentrations in simulated breath samples. The Ketowhistle demonstrates the immediate potential for non‐invasive ketone monitoring for people living with diabetes, in particular for DKA prevention.
Injectable Hydrogel Delivery System with High Drug Loading for Prolonging Local Anesthesia
Authors: Li Yongchun , Chen You , Xue Yifan , Jin Jinlong , Xu Yixin , Zeng Weian , Liu Jie , Xie Jingdun
Published: March 2024

Peripheral nerve block is performed for precise pain control and lesser side effects after surgery by reducing opioid consumption. Injectable hydrogel delivery systems with high biosafety and moisture content have good clinical application prospects for local anesthetic delivery. However, how to achieve high drug loading and long‐term controlled release of water‐soluble narcotic drugs remains a big challenge. In this study, heterogeneous microspheres and an injectable gel‐matrix composite drug delivery system are designed in two steps. First, heterogeneous hydrogel microspheres loaded with ropivacaine (HMS‐ROP) are prepared using a microfluidic chip and in situ alkalization. An injectable self‐healing hydrogel matrix (Gel) is then prepared from modified carboxymethylcellulose (CMC‐ADH) and oxidized hyaluronic acid (OHA). A local anesthetic delivery system, Gel/HMS‐ROP/dexmedetomidine (DEX), with long‐term retention and drug release in vivo is prepared by combining HMS‐ROP and Gel/DEX. The drug loading of HMS‐ROP reached 41.1%, with a drug release time of over 160 h in vitro, and sensory and motor blockade times in vivo of 48 and 36 h, respectively. In summary, the sequential release and synergistic analgesic effects of the two anesthetics are realized using core‐shell microspheres, DEX, and an injectable gel, providing a promising strategy for long‐acting postoperative pain management.
3D Printing of Anisotropic Piezoresistive Pressure Sensors for Directional Force Perception
Authors: Liu Jingfeng , Zhang Xuan , Liu Jintao , Liu Xingang , Zhang Chuhong
Published: March 2024

Anisotropic pressure sensors are gaining increasing attention for next‐generation wearable electronics and intelligent infrastructure owing to their sensitivity in identifying different directional forces. 3D printing technologies have unparalleled advantages in the design of anisotropic pressure sensors with customized 3D structures for realizing tunable anisotropy. 3D printing has demonstrated few successes in utilizing piezoelectric nanocomposites for anisotropic recognition. However, 3D‐printed anisotropic piezoresistive pressure sensors (PPSs) remain unexplored despite their convenience in saving the poling process. This study pioneers the development of an aqueous printable ink containing waterborne polyurethane elastomer. An anisotropic PPS featuring tailorable flexibility in macroscopic 3D structures and microscopic pore morphologies is created by adopting direct ink writing 3D printing technology. Consequently, the desired directional force perception is achieved by programming the printing schemes. Notably, the printed PPS demonstrated excellent deformability, with a relative sensitivity of 1.22 (kPa*wt. %)−1 over a substantial pressure range (2.8 to 8.1 kPa), approximately fivefold than that of a state‐of‐the‐art carbon‐based PPS. This study underscores the versatility of 3D printing in customizing highly sensitive anisotropic pressure sensors for advanced sensing applications that are difficult to achieve using conventional measures.
Lineage‐Specific CYP80 Expansion and Benzylisoquinoline Alkaloid Diversity in Early‐Diverging Eudicots
Authors: An Zhoujie , Gao Ranran , Chen Shanshan , Tian Ya , Li Qi , Tian Lixia , Zhang Wanran , Kong Lingzhe , Zheng Baojiang , Hao Lijun , Xin Tianyi , Yao Hui , Wang Yu , Song Wei , Hua Xin , Liu Chengwei , Song Jingyuan , Fan Huahao , Sun Wei , Chen Shilin , Xu Zhichao
Published: March 2024

Menispermaceae species, as early‐diverging eudicots, can synthesize valuable benzylisoquinoline alkaloids (BIAs) like bisbenzylisoquinoline alkaloids (bisBIAs) and sinomenines with a wide range of structural diversity. However, the evolutionary mechanisms responsible for their chemo‐diversity are not well understood. Here, a chromosome‐level genome assembly of Menispermum dauricum is presented and demonstrated the occurrence of two whole genome duplication (WGD) events that are shared by Ranunculales and specific to Menispermum, providing a model for understanding chromosomal evolution in early‐diverging eudicots. The biosynthetic pathway for diverse BIAs in M. dauricum is reconstructed by analyzing the transcriptome and metabolome. Additionally, five catalytic enzymes – one norcoclaurine synthase (NCS) and four cytochrome P450 monooxygenases (CYP450s) – from M. dauricum are responsible for the formation of the skeleton, hydroxylated modification, and C‐O/C‐C phenol coupling of BIAs. Notably, a novel leaf‐specific MdCYP80G10 enzyme that catalyzes C2′‐C4a phenol coupling of (S)‐reticuline into sinoacutine, the enantiomer of morphinan compounds, with predictable stereospecificity is discovered. Moreover, it is found that Menispermum‐specific CYP80 gene expansion, as well as tissue‐specific expression, has driven BIA diversity in Menispermaceae as compared to other Ranunculales species. This study sheds light on WGD occurrences in early‐diverging eudicots and the evolution of diverse BIA biosynthesis.
Room Temperature Ionic Liquid Capping Layer for High Efficiency FAPbI3 Perovskite Solar Cells with Long‐Term Stability
Authors: Lou Qiang , Xu Xinxin , Lv Xueqing , Xu Zhengjie , Sun Tian , Qiu Liwen , Dai Tingting , Zhou Erjun , Li Guijun , Chen Tong , Lin Yen‐Hung , Zhou Hang
Published: March 2024

Ionic liquid salts (ILs) are generally recognized as additives in perovskite precursor solutions to enhance the efficiency and stability of solar cells. However, the success of ILs incorporation as additives is highly dependent on the precursor formulation and perovskite crystallization process, posing challenges for industrial‐scale implementation. In this study, a room‐temperature spin‐coated IL, n‐butylamine acetate (BAAc), is identified as an ideal passivation agent for formamidinium lead iodide (FAPbI3) films. Compared with other passivation methods, the room‐temperature BAAc capping layer (BAAc RT) demonstrates more uniform and thorough passivation of surface defects in the FAPbI3 perovskite. Additionally, it provides better energy level alignment for hole extraction. As a result, the champion n–i–p perovskite solar cell with a BAAc capping layer exhibits a power conversion efficiency (PCE) of 24.76%, with an open‐circuit voltage (Voc) of 1.19 V, and a Voc loss of ≈330 mV. The PCE of the perovskite mini‐module with BAAc RT reaches 20.47%, showcasing the effectiveness and viability of this method for manufacturing large‐area perovskite solar cells. Moreover, the BAAc passivation layer also improves the long‐term stability of unencapsulated FAPbI3 perovskite solar cells, enabling a T80 lifetime of  3500 h when stored at 35% relative humidity at room temperature in an air atmosphere.
Revealing the Hole and Electron Transport Dynamics in the Working Devices for Efficient Semitransparent Perovskite Solar Cells
Authors: Jiang Chaofan , Qin Tingxiao , Tan Liguo , Li Hang , Zhou Junjie , Li Minghao , Dang Zhi‐Min , Ding Liming , Xiong Qihua , Yi Chenyi
Published: March 2024

The performance and stability of perovskite solar cells (PSCs) are dominated by the electron and hole transport dynamics, which are highly desired to be characterized in the working devices. Nevertheless, for the opaque PSCs, the hole transport layer (HTL) in n–i–p devices or the electron transport layer (ETL) in p–i–n devices are typically buried beneath the metal electrode, which makes it difficult to simultaneously characterize the charge transport dynamics from both sides of the working devices. In this work, for the first time, the charge transport dynamics of the working devices from both the front and rear side of semitransparent PSCs (ST‐PSCs) is characterized via femtosecond transient reflection spectroscopy (FS‐TRS). A significant enhancement of the hole transport and negligible change of the electron transport is observed when the perovskite/HTL interface is treated by 2‐chloro‐phenethylammonium iodide (2‐Cl‐PEAI). A champion power conversion efficiency (PCE) of 23.3% (certified 22.3%) is achieved, which is the highest certified PCE for ST‐PSCs up to date. The ST‐PSCs maintained more than 90% of its initial efficiency after 2000 h of maximum power point tracking (MPPT). Additionally, the ST‐PSCs are implemented in 4‐terminal (4‐T) perovskite/passivated emitter rear silicon cell (PERC), reaching a simulated output power of 30.8 mW cm−2.