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Ni/PiNe Heterogeneous Catalyst from Biomass Waste: Low-Loading, Ligand-Free Suzuki-Miyaura Cross-Coupling. 从生物质废弃物中提取的 Ni/PiNe 异构催化剂:低负载、无配体的 Suzukii-Miyaura 交叉偶联。
IF 7.5 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-19 DOI: 10.1002/cssc.202402011
Luigi Vaccaro, Federica Valentini, Shaomin Chen, Giulia Brufani, Yanlong Gu

An efficient Ni-based heterogeneous catalyst from pine needles urban waste valorization was designed and developed with a resource recycling strategy. The Ni/PiNe catalyst was fully characterized and tested in the Suzuki-Miyaura coupling under microwave irradiation. Although Ni is a promising candidate for replacing Pd-based catalytic systems, it generally requires a high catalyst amount and the exploitation of ligands and additives to enhance the reaction rate. On the contrary, with our new Ni/PiNe, 30 different products were efficiently synthesized with an isolated yield of up to 93%, using a very low catalyst amount and in the absence of ligands. Furthermore, the Ni/PiNe catalyst also showed good durability for consecutive cycles and an impressive TON value (1140). In addition to the catalytic efficiency in short reaction time and to the stability and durability under MW irradiation, the Ni/PiNe allowed for further optimization, achieving a low E-factor value (14.0), thus highlighting the potential in further reducing the waste and costs associated to the process.

采用资源循环利用策略,从松针中设计并开发了一种高效的镍基异相催化剂。对 Ni/PiNe 催化剂进行了全面表征,并在微波辐照下进行了铃木-宫浦偶联测试。虽然镍是替代钯基催化体系的理想候选催化剂,但通常需要较高的催化剂用量,并需要利用配体和添加剂来提高反应速率。相反,使用我们的新型 Ni/PiNe 催化剂,只需极低的催化剂用量,在不使用配体的情况下,就能高效合成 30 种不同的产品,分离产率高达 93%。此外,Ni/PiNe 催化剂还显示出良好的连续循环耐久性和令人印象深刻的吨值 (1140)。除了在短反应时间内的催化效率以及在兆瓦级辐照下的稳定性和耐久性之外,Ni/PiNe 催化剂还可以进一步优化,实现较低的 E 因子值(14.0),从而凸显了进一步减少废物和降低相关工艺成本的潜力。
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引用次数: 0
American Society of Clinical Oncology guideline update on palliative care for patients with cancer: Addressing the reality gap. 美国临床肿瘤学会癌症患者姑息治疗指南更新:解决现实差距。
IF 6.1 2区 医学 Q1 ONCOLOGY Pub Date : 2024-11-19 DOI: 10.1002/cncr.35656
Fionnuala Crowley, Cardinale B Smith, Robert M Arnold, Debora Afezolli
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引用次数: 0
Sustained Endocytosis Inhibition via Locally-Injected Drug-Eluting Hydrogel Improves ADCC-Mediated Antibody Therapy in Colorectal Cancer. 通过局部注射药物洗脱水凝胶持续抑制内吞作用可改善结直肠癌的 ADCC 媒介抗体疗法
IF 14.3 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-19 DOI: 10.1002/advs.202407239
Chong Wu, Xiaoting Liu, Rong Liu, Shiyao Song, Zi-Fan Zheng, Yilin Zeng, Yong Mei, Jing-Yang Zhang, Qijia Duan, Run Lin, Jin-Zhi Du, Weiling He

The epidermal growth factor receptor (EGFR) is a validated therapeutic target for RAS/RAF wild-type colorectal cancer (CRC). However, monoclonal antibody-based anti-EGFR therapies such as cetuximab have limited effectiveness. Herein, it is identified that EGFR internalization is associated with poor treatment response and prognosis in patients with CRC, based on a retrospective analysis of patients treated with cetuximab. It is further demonstrated that the endocytosis inhibitor prochlorperazine (PCZ) can move EGFR, which is hidden inside the cell, to the cell surface to improve therapeutic antibody binding. Thus, a thermosensitive hydrogel co-loaded with cetuximab and PCZ (Gel@Cmab/PCZ) is constructed for sustained inhibition of endocytosis and effective cetuximab delivery. Peritumoral injection of Gel@Cmab/PCZ shows strong antitumor efficacy in subcutaneous and orthotopic CRC tumor models and completely abrogated liver metastasis when combined with chemotherapy. In a humanized patient-derived xenograft model, a single injection of Gel@Cmab/PCZ with one-third of the conventional cetuximab dose achieved 91% tumor growth inhibition, which promoted NK cell infiltration into tumor tissues and their antibody-dependent cell-mediated cytotoxicity effect. This study represents a novel strategy to boost the monoclonal antibody-mediated anti-tumor response in CRC.

表皮生长因子受体(EGFR)是 RAS/RAF 野生型结直肠癌(CRC)的有效治疗靶点。然而,基于单克隆抗体的抗表皮生长因子受体疗法(如西妥昔单抗)疗效有限。本文通过对接受西妥昔单抗治疗的患者进行回顾性分析,发现表皮生长因子受体内化与 CRC 患者治疗反应差和预后不良有关。研究进一步证明,内吞抑制剂丙氯苯嗪(PCZ)可将隐藏在细胞内的表皮生长因子受体移至细胞表面,从而改善治疗性抗体的结合。因此,我们构建了一种共同负载西妥昔单抗和丙氯苯嗪的热敏水凝胶(Gel@Cmab/PCZ),用于持续抑制内吞并有效递送西妥昔单抗。Gel@Cmab/PCZ 的瘤周注射在皮下和正位 CRC 肿瘤模型中显示出很强的抗肿瘤疗效,在与化疗联合使用时可完全抑制肝转移。在人源化患者异种移植模型中,单次注射西妥昔单抗三分之一剂量的 Gel@Cmab/PCZ 可使肿瘤生长抑制率达到 91%,这促进了 NK 细胞向肿瘤组织的浸润及其抗体依赖性细胞介导的细胞毒性效应。这项研究代表了一种增强单克隆抗体介导的 CRC 抗肿瘤反应的新策略。
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引用次数: 0
Inverse Vulcanization of Aziridines: Enhancing Polysulfides for Superior Mechanical Strength and Adhesive Performance. 氮丙啶的反硫化:提高聚硫化物的机械强度和粘合性能。
IF 16.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-19 DOI: 10.1002/anie.202418764
Nikos Hadjichristidis, Jieai Fan, Changzheng Ju, Songjie Fan, Xia Li, Zhen Zhang

This study introduces a novel approach to inverse vulcanization by utilizing a commercially available triaziridine crosslinker as an alternative to conventional olefin-based crosslinkers. The model reactions reveal a self-catalyzed ring-opening of "unactivated" aziridine with elemental sulfur, forming oligosulfide-functionalized diamines. The triaziridine-derived polysulfides exhibit impressive mechanical properties, achieving a maximum stress of ~8.3 MPa and an elongation at break of ~107%. The incorporation of silicon dioxide (20 wt%) enhances the composite's rigidity, yielding a Young's modulus of ~0.94 GPa. Furthermore, these polysulfides display excellent adhesion strength on various substrates, such as aluminum (~7.0 MPa), walnut (~9.6 MPa), and steel (~11.0 MPa), with substantial retention of adhesion strength (~3.3 MPa on steel) at -196 °C. The straightforward synthetic process, combined with the accessibility of the triaziridine crosslinker, emphasizes the potential for further innovations in sulfur polymer chemistry.

本研究介绍了一种新型反向硫化方法,即利用市售的三氮脒交联剂替代传统的烯烃基交联剂。模型反应揭示了 "未活化 "氮丙啶与元素硫的自催化开环反应,形成低聚硫功能化二胺。三氮丙啶衍生的多硫化物表现出令人印象深刻的机械性能,最大应力约为 8.3 兆帕,断裂伸长率约为 107%。二氧化硅(20 wt%)的加入增强了复合材料的刚性,使杨氏模量达到约 0.94 GPa。此外,这些聚硫化物在铝材(约 7.0 兆帕)、胡桃木(约 9.6 兆帕)和钢材(约 11.0 兆帕)等各种基材上显示出优异的粘附强度,在 -196 °C 时仍能保持相当高的粘附强度(在钢材上约为 3.3 兆帕)。简单的合成工艺,加上三氮丙啶交联剂的易得性,都彰显了硫聚合物化学进一步创新的潜力。
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引用次数: 0
Self-Assembled Eutectogel with Cell Permeation and Multiple Anti-Inflammatory Abilities for Treating Chronic Periodontitis. 用于治疗慢性牙周炎的具有细胞渗透和多重抗炎能力的自组装共聚凝胶
IF 27.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-19 DOI: 10.1002/adma.202412866
Ziying Cheng, Mengyan Kang, Xu Peng, Li Ren, Jing Xie, Quan Yuan, Xinyuan Xu, Jianshu Li

Eutectogels represent an attractive option for various industrial applications that use deep eutectic solvents (DESs) as effective liquid active ingredients and offer remarkable stability, cost-effectiveness, and environmental friendliness. However, the biological applications of these compounds are limited. DESs are highly structurally tunable and exhibit remarkable biofunctionality and biocompatibility, conferring substantial benefits in the treatment of diseases. In this study, choline-chloride and mannose are used to fabricate ChCl/M DES, followed by introduction of lysozyme fibers and gallic acid for self-assembly into injectable eutectogels through hydrogen bonding and hydrophilic/hydrophobic interaction interactions. The eutectogels demonstrate almost 100% bactericidal activities against three strains and significant immune-regulation. This is supported by a decrease in the proportion of CD86-expressing cells from 64.02% to 18.17% and an increase in CD206-expressing cells from 2.53% to 29.96% through flow cytometry experiments. The eutectogels effectively inhibit alveolar bone loss and alleviated local inflammation in a rat model of chronic periodontitis owing to the promotion of gallic acid in the cell membrane by the ChCl/M DES. Hence, self-assembled eutectogels exhibit the potential to enhance the efficacy if treatments/therapies against inflammatory diseases by facilitating bacterial control, reactive oxygen species scavenging, and the regulation of macrophages by promoting cell permeation of small-molecule drugs.

在各种工业应用中,使用深共晶溶剂(DES)作为有效液体活性成分的共晶凝胶是一种极具吸引力的选择,它具有显著的稳定性、成本效益和环境友好性。然而,这些化合物的生物应用却很有限。DESs 在结构上具有很高的可调性,并表现出显著的生物功能性和生物兼容性,在治疗疾病方面具有很大的优势。本研究利用氯化胆碱和甘露糖制造氯化胆碱/M DES,然后引入溶菌酶纤维和没食子酸,通过氢键和亲水/疏水相互作用自组装成可注射的共凝胶。这种共聚凝胶对三种菌株的杀菌活性几乎达到 100%,并具有显著的免疫调节作用。通过流式细胞术实验,CD86 表达细胞的比例从 64.02% 降至 18.17%,CD206 表达细胞的比例从 2.53% 增至 29.96%,这都证明了这一点。在慢性牙周炎大鼠模型中,由于 ChCl/M DES 促进了细胞膜中没食子酸的生成,自组装共聚凝胶有效地抑制了牙槽骨流失,并缓解了局部炎症。因此,自组装共晶凝胶具有通过促进小分子药物的细胞渗透来控制细菌、清除活性氧和调节巨噬细胞的潜力,从而提高治疗炎症疾病的疗效。
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引用次数: 0
Rates of discordant CD20 status by flow cytometry and immunohistochemistry in B-ALL. 流式细胞术和免疫组化法检测 B-ALL 中 CD20 状态不一致的比率。
IF 5.1 2区 医学 Q1 HEMATOLOGY Pub Date : 2024-11-19 DOI: 10.1111/bjh.19909
Samuel Grigg, Melissa Ng Liet Hing, Kah Lok Chan, Surender Juneja, David Westerman
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引用次数: 0
Anabolic Sensitivity in Healthy, Lean, Older Men Is Associated With Higher Expression of Amino Acid Sensors and mTORC1 Activators Compared to Young. 与年轻人相比,健康、瘦弱的老年男性的合成代谢敏感性与氨基酸传感器和 mTORC1 激活剂的高表达有关。
IF 8.9 1区 医学 Pub Date : 2024-11-19 DOI: 10.1002/jcsm.13613
Oscar Horwath, Marcus Moberg, Nathan Hodson, Sebastian Edman, Mats Johansson, Eva Andersson, Gerrit van Hall, Olav Rooyackers, Andrew Philp, William Apró

Background: Sarcopenia is thought to be underlined by age-associated anabolic resistance and dysregulation of intracellular signalling pathways. However, it is unclear whether these phenomena are driven by ageing per se or other confounding factors.

Methods: Lean and healthy young (n = 10, 22 ± 3 years, BMI; 23.4 ± 0.8 kg/m2) and old men (n = 10, 70 ± 3 years, BMI; 22.7 ± 1.3 kg/m2) performed unilateral resistance exercise followed by intake of essential amino acids (EAA). Muscle biopsies were collected from the rested and the exercised leg before, immediately after and 60 and 180 min after EAA intake. Muscle samples were analysed for amino acid concentrations, muscle protein synthesis (MPS) and associated anabolic signalling.

Results: Following exercise, peak plasma levels of EAA and leucine were similar between groups, but the area under the curve was ~11% and ~28% lower in Young (p < 0.01). Absolute levels of muscle EAA and leucine peaked 60 min after exercise, with ~15 and ~21% higher concentrations in the exercising leg (p < 0.01) but with no difference between groups. MPS increased in both the resting (~0.035%·h-1 to 0.056%·h-1, p < 0.05) and exercising leg (~0.035%·h-1 to 0.083%·h-1, p < 0.05) with no difference between groups. Phosphorylation of S6K1Thr389 increased to a similar extent in the exercising leg in both groups but was 2.8-fold higher in the resting leg of Old at the 60 min timepoint (p < 0.001). Phosphorylation of 4E-BP1Ser65 increased following EAA intake and exercise, but differences between legs were statistically different only at 180 min (p < 0.001). However, phosphorylation of this site was on average 78% greater across all timepoints in Old (p < 0.01). Phosphorylation of eEF2Thr56 was reduced (~66% and 39%) in the exercising leg at both timepoints after EAA intake and exercise, with no group differences (p < 0.05). However, phosphorylation at this site was reduced by ~27% also in the resting leg at 60 min, an effect that was only seen in Old (p < 0.01). Total levels of Rheb (~45%), LAT1 (~31%) and Rag B (~31%) were higher in Old (p < 0.001).

Conclusion: Lean and healthy old men do not manifest AR as evidenced by potent increases in MPS and mTORC1 signalling following EAA intake and exercise. Maintained anabolic sensitivity with age appears to be a function of a compensatory increase in basal levels of proteins involved in anabolic signalling. Therefore, our results suggest that age per se does not appear to cause AR in human skeletal muscle.

背景:人们认为,与年龄相关的合成代谢阻力和细胞内信号通路失调是 "肌肉疏松症 "的主要原因。然而,目前还不清楚这些现象是由衰老本身还是其他干扰因素引起的:方法:健康瘦弱的年轻男性(n = 10,22 ± 3 岁,体重指数;23.4 ± 0.8 kg/m2)和老年男性(n = 10,70 ± 3 岁,体重指数;22.7 ± 1.3 kg/m2)进行单侧阻力运动,然后摄入必需氨基酸(EAA)。在摄入 EAA 前、摄入 EAA 后、摄入 EAA 后 60 分钟和 180 分钟,分别从休息和运动的腿部采集肌肉活检样本。对肌肉样本的氨基酸浓度、肌肉蛋白质合成(MPS)和相关合成代谢信号进行分析:运动后,各组间 EAA 和亮氨酸的血浆峰值水平相似,但 Young 组的曲线下面积分别低 11% 和 28%(P-1 至 0.056%-h-1,P-1 至 0.083%-h-1,P Thr389 在两组运动腿中的增加程度相似,但在静止腿中高 2.8 倍)。在摄入 EAA 和运动后,运动腿的 p Thr56 在两个时间点都降低了(约 66% 和 39%),没有组间差异(p 结论:摄入 EAA 和运动后,MPS 和 mTORC1 信号的强效增加证明,健康瘦弱的老年男性不会表现出 AR。随着年龄的增长,合成代谢敏感性的维持似乎是参与合成代谢信号传导的蛋白质基础水平补偿性增加的结果。因此,我们的研究结果表明,年龄本身似乎不会导致人体骨骼肌的合成代谢敏感性。
{"title":"Anabolic Sensitivity in Healthy, Lean, Older Men Is Associated With Higher Expression of Amino Acid Sensors and mTORC1 Activators Compared to Young.","authors":"Oscar Horwath, Marcus Moberg, Nathan Hodson, Sebastian Edman, Mats Johansson, Eva Andersson, Gerrit van Hall, Olav Rooyackers, Andrew Philp, William Apró","doi":"10.1002/jcsm.13613","DOIUrl":"https://doi.org/10.1002/jcsm.13613","url":null,"abstract":"<p><strong>Background: </strong>Sarcopenia is thought to be underlined by age-associated anabolic resistance and dysregulation of intracellular signalling pathways. However, it is unclear whether these phenomena are driven by ageing per se or other confounding factors.</p><p><strong>Methods: </strong>Lean and healthy young (n = 10, 22 ± 3 years, BMI; 23.4 ± 0.8 kg/m<sup>2</sup>) and old men (n = 10, 70 ± 3 years, BMI; 22.7 ± 1.3 kg/m<sup>2</sup>) performed unilateral resistance exercise followed by intake of essential amino acids (EAA). Muscle biopsies were collected from the rested and the exercised leg before, immediately after and 60 and 180 min after EAA intake. Muscle samples were analysed for amino acid concentrations, muscle protein synthesis (MPS) and associated anabolic signalling.</p><p><strong>Results: </strong>Following exercise, peak plasma levels of EAA and leucine were similar between groups, but the area under the curve was ~11% and ~28% lower in Young (p < 0.01). Absolute levels of muscle EAA and leucine peaked 60 min after exercise, with ~15 and ~21% higher concentrations in the exercising leg (p < 0.01) but with no difference between groups. MPS increased in both the resting (~0.035%·h<sup>-1</sup> to 0.056%·h<sup>-1</sup>, p < 0.05) and exercising leg (~0.035%·h<sup>-1</sup> to 0.083%·h<sup>-1</sup>, p < 0.05) with no difference between groups. Phosphorylation of S6K1<sup>Thr389</sup> increased to a similar extent in the exercising leg in both groups but was 2.8-fold higher in the resting leg of Old at the 60 min timepoint (p < 0.001). Phosphorylation of 4E-BP1<sup>Ser65</sup> increased following EAA intake and exercise, but differences between legs were statistically different only at 180 min (p < 0.001). However, phosphorylation of this site was on average 78% greater across all timepoints in Old (p < 0.01). Phosphorylation of eEF2<sup>Thr56</sup> was reduced (~66% and 39%) in the exercising leg at both timepoints after EAA intake and exercise, with no group differences (p < 0.05). However, phosphorylation at this site was reduced by ~27% also in the resting leg at 60 min, an effect that was only seen in Old (p < 0.01). Total levels of Rheb (~45%), LAT1 (~31%) and Rag B (~31%) were higher in Old (p < 0.001).</p><p><strong>Conclusion: </strong>Lean and healthy old men do not manifest AR as evidenced by potent increases in MPS and mTORC1 signalling following EAA intake and exercise. Maintained anabolic sensitivity with age appears to be a function of a compensatory increase in basal levels of proteins involved in anabolic signalling. Therefore, our results suggest that age per se does not appear to cause AR in human skeletal muscle.</p>","PeriodicalId":186,"journal":{"name":"Journal of Cachexia, Sarcopenia and Muscle","volume":" ","pages":""},"PeriodicalIF":8.9,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142666553","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A Fully Integrated Orthodontic Aligner With Force Sensing Ability for Machine Learning-Assisted Diagnosis. 用于机器学习辅助诊断的具有力传感功能的全集成正畸矫治器。
IF 14.3 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-19 DOI: 10.1002/advs.202411187
Hao Feng, Wenhao Song, Ruyi Li, Linxin Yang, Xiaoxuan Chen, Jiajun Guo, Xuan Liao, Lei Ni, Zhou Zhu, Junyu Chen, Xibo Pei, Yijun Li, Jian Wang

Currently, the diagnosis of malocclusion is a highly demanding process involving complicated examinations of the dental occlusion, which increases the demand for innovative tools for occlusal data monitoring. Nevertheless, continuous wireless monitoring within the oral cavity is challenging due to limitations in sampling and device size. In this study, by embedding high-performance piezoelectric sensors into the occlusal surfaces using flexible printed circuits, a fully integrated, flexible, and self-contained transparent aligner is developed. This aligner exhibits excellent sensitivity for occlusal force detection, with a broad detection threshold and continuous pressure monitoring ability at eight distinct sites. Integrated with machine learning algorithm, this fully integrated aligner can also identify and track adverse oral habits that can cause/exacerbate malocclusion, such as lip biting, thumb sucking, and teeth grinding. This system achieved 95% accuracy in determining malocclusion types by analyzing occlusal data from over 1400 malocclusion models. This fully-integrated sensing system, with wireless monitoring and machine learning processing, marks a significant advancement in the development of intraoral wearable sensors. Moreover, it can also facilitate remote orthodontic monitoring and evaluation, offering a new avenue for effective orthodontic care.

目前,错颌畸形的诊断是一项要求很高的工作,需要对牙齿咬合进行复杂的检查,这就增加了对咬合数据监测创新工具的需求。然而,由于采样和设备尺寸的限制,在口腔内进行连续无线监测具有挑战性。在这项研究中,通过使用柔性印刷电路将高性能压电传感器嵌入咬合表面,开发出了一种完全集成、灵活且独立的透明矫治器。该对准器在咬合力检测方面表现出极佳的灵敏度,具有较宽的检测阈值和对八个不同部位的持续压力监测能力。与机器学习算法相结合,这种完全集成的矫治器还能识别和跟踪可能导致/加剧错颌畸形的不良口腔习惯,如咬嘴唇、吸吮拇指和磨牙。该系统通过分析来自 1400 多个错颌畸形模型的咬合数据,在确定错颌畸形类型方面达到了 95% 的准确率。这种完全集成的传感系统具有无线监测和机器学习处理功能,标志着口内可穿戴传感器的发展取得了重大进展。此外,它还能促进远程正畸监测和评估,为有效的正畸护理提供了一条新途径。
{"title":"A Fully Integrated Orthodontic Aligner With Force Sensing Ability for Machine Learning-Assisted Diagnosis.","authors":"Hao Feng, Wenhao Song, Ruyi Li, Linxin Yang, Xiaoxuan Chen, Jiajun Guo, Xuan Liao, Lei Ni, Zhou Zhu, Junyu Chen, Xibo Pei, Yijun Li, Jian Wang","doi":"10.1002/advs.202411187","DOIUrl":"https://doi.org/10.1002/advs.202411187","url":null,"abstract":"<p><p>Currently, the diagnosis of malocclusion is a highly demanding process involving complicated examinations of the dental occlusion, which increases the demand for innovative tools for occlusal data monitoring. Nevertheless, continuous wireless monitoring within the oral cavity is challenging due to limitations in sampling and device size. In this study, by embedding high-performance piezoelectric sensors into the occlusal surfaces using flexible printed circuits, a fully integrated, flexible, and self-contained transparent aligner is developed. This aligner exhibits excellent sensitivity for occlusal force detection, with a broad detection threshold and continuous pressure monitoring ability at eight distinct sites. Integrated with machine learning algorithm, this fully integrated aligner can also identify and track adverse oral habits that can cause/exacerbate malocclusion, such as lip biting, thumb sucking, and teeth grinding. This system achieved 95% accuracy in determining malocclusion types by analyzing occlusal data from over 1400 malocclusion models. This fully-integrated sensing system, with wireless monitoring and machine learning processing, marks a significant advancement in the development of intraoral wearable sensors. Moreover, it can also facilitate remote orthodontic monitoring and evaluation, offering a new avenue for effective orthodontic care.</p>","PeriodicalId":117,"journal":{"name":"Advanced Science","volume":" ","pages":"e2411187"},"PeriodicalIF":14.3,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142666871","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
In-situ reduced Cu3N nanocrystals enable high-efficiency ammonia synthesis and zinc-nitrate batteries. 原位还原 Cu3N 纳米晶体实现了高效氨合成和硝酸锌电池。
IF 3.9 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-19 DOI: 10.1002/chem.202404129
Shanshan Chen, Zhiwei Wang, Quan Zhang, Shiming Qiu, Yifan Liu, Guangzhi Hu, Jun Luo, Xijun Liu

Nitrate reduction reaction (NO3RR) involves an 8-electron transfer process and competes with the hydrogen evolution reaction process, resulting in lower yields and Faraday efficiency (FE) in the process of NH3 synthesis. Especially, Cu-based catalysts (Cu0 and Cu+) have been investigated in the field of NO3RR due to the energy levels of d-orbital and the least unoccupied molecular orbital (LUMO) π* of nitrate's orbital. Based on the above, we synthesized a Cu-based compound containing Cu3N (Cu+) through a simple one-step pyrolysis method, applied it to electrocatalytic NO3RR, and tested the performance of the Zn-NO3- battery. Through various characterization analyses, Cu-based catalysts (Cu+) are the key active sites in reduction reactions, making Cu3N a potential catalyst for ammonia synthesis. The research results indicate the application of Cu3N catalyst in NO3RR shows the best NH3 yield of 173.7 μmol h-1 cm-2, with FENH3 reaching 91.0% at -0.3 V vs. RHE, which is much higher than that of Cu catalyst without N. In addition, the Zn-NO3- battery based on Cu3N electrode also exhibits an NH3 yield of 39.8 μmol h-1 cm-2, 63.0% FENH3, and a power density of 2.7 mW cm-2, as well as stable cycling charge-discharge stability for 5 hours.

硝酸还原反应(NO3RR)涉及一个 8 电子转移过程,并与氢进化反应过程竞争,导致 NH3 合成过程中的产率和法拉第效率(FE)降低。特别是铜基催化剂(Cu0 和 Cu+),由于其硝酸盐轨道的 d 轨道能级和最小未占分子轨道(LUMO)π*能级,在 NO3RR 领域得到了研究。在此基础上,我们通过简单的一步热解法合成了含 Cu3N (Cu+) 的铜基化合物,并将其应用于电催化 NO3RR,测试了 Zn-NO3- 电池的性能。通过各种表征分析,铜基催化剂(Cu+)是还原反应中的关键活性位点,使 Cu3N 成为合成氨的潜在催化剂。研究结果表明,Cu3N 催化剂在 NO3RR 中的应用显示出最佳的 NH3 产率,达到 173.7 μmol h-1 cm-2,在 -0.3 V 对 RHE 时 FENH3 达到 91.0%,远高于不含 N 的 Cu 催化剂。此外,基于 Cu3N 电极的 Zn-NO3- 电池还表现出 39.8 μmol h-1 cm-2 的 NH3 产率、63.0% 的 FENH3 和 2.7 mW cm-2 的功率密度,以及 5 小时稳定的循环充放电稳定性。
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引用次数: 0
Enhanced photocatalytic synthesis of urea from co-reduction of N2 and CO2 on Z-schematic SrTiO3-FeS-CoWO4 heterostructure. 在 Z 型 SrTiO3-FeS-CoWO4 异质结构上增强 N2 和 CO2 共同还原尿素的光催化合成。
IF 16.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-19 DOI: 10.1002/anie.202419628
Muhammad Irfan Ahmad, Yanming Liu, Yaqi Wang, Peike Cao, Hongtao Yu, Houfen Li, Shuo Chen, Xie Quan

The photocatalytic co-reduction of CO2 and N2 is a sustainable method for urea synthesis under mild conditions. However, high-yield synthesis of urea is a challenge due to the sluggish kinetics of the C-N coupling reaction. Herein, we have successfully engineered a Z-scheme photocatalyst, SrTiO3-FeS-CoWO4, for boosting photocatalytic urea synthesis via enhancing the initial CO2 and N2 adsorption step and reducing the energy barrier for the C-N coupling reaction. A high urea yield of 8054.2 μg·gcat-1·h-1 was achieved on SrTiO3-FeS-CoWO4, which was significantly higher than the state-of-the-art. The SrTiO3-FeS-CoWO4 Z-scheme photocatalyst, with accelerated charge transfer by FeS, not only had dual active sites for the chemical adsorption and activation of CO2 and N2, but also retained the high conduction band (-1.50 eV) and accelerated supply of electrons and protons, which are responsible for its good photoreduction activity and significantly reduced energy barrier for the rate-determining step of C-N coupling reaction.

CO2 和 N2 的光催化共还原反应是在温和条件下合成尿素的一种可持续方法。然而,由于 C-N 偶联反应的动力学缓慢,高产合成尿素是一项挑战。在此,我们成功地设计了一种 Z 型光催化剂 SrTiO3-FeS-CoWO4 ,通过增强 CO2 和 N2 的初始吸附步骤并降低 C-N 偶联反应的能量障碍,促进光催化尿素合成。SrTiO3-FeS-CoWO4 的尿素产率高达 8054.2 μg-gcat-1-h-1,明显高于最先进的水平。由 FeS 加速电荷转移的 SrTiO3-FeS-CoWO4 Z 型光催化剂不仅具有化学吸附和活化 CO2 和 N2 的双重活性位点,而且保留了高导带(-1.50 eV)和电子与质子的加速供应,这是其具有良好光导活性和显著降低 C-N 偶联反应决定速率步骤能垒的原因。
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引用次数: 0
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