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Carbon dioxide photoreduction using a photocatalyst with prolonged charge-separated states and excess electron reservoirs 利用具有长时间电荷分离态和过剩电子库的光催化剂进行二氧化碳光还原
IF 8.9 2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-05 DOI: 10.1016/j.xcrp.2024.102194
Lang Pei, Zhenggang Luo, Jiasong Zhong, Xusheng Wang, Peng Zhou, Shicheng Yan, Zhigang Zou

A persistent challenge in operating S-scheme photocatalysts involves maintaining complete neutralization of low-energy electrons and holes between reducing and oxidizing photocatalysts. To address this, we propose a charge replenishment-assisted S-scheme mechanism that combines a compatible host catalyst with a luminescence phosphor semiconductor capable of long-term storage of photogenerated electrons. Stored electrons can replenish the host photocatalyst, depleting the low-oxidizing holes, thus prolonging the charge-separated state. The concept is demonstrated in a core-shell-structured SrGa2O4:Cu2+/g-C3N4 (SGO/CN) photocatalyst, where stored electrons with a lifetime of up to several hours can continuously consume holes in the CN. The well-defined core-shell structure, abundant interfacial Sr-N bonds, and staggered band alignment between SGO and CN are crucial for this S-scheme interfacial charge transfer, which contributes to the enhanced CO2-to-CO transformation activity and selectivity. This S-scheme heterojunction, incorporating a charge-storing material as an excess electron reservoir, offers a promising template for designing efficient photocatalytic systems.

在运行 S 型光催化剂过程中,一个长期存在的难题是如何在还原型光催化剂和氧化型光催化剂之间保持低能电子和空穴的完全中和。为了解决这个问题,我们提出了一种电荷补充辅助 S-scheme机制,它将兼容的主催化剂与能够长期储存光生电子的发光荧光粉半导体相结合。储存的电子可以补充主光催化剂,消耗低氧空穴,从而延长电荷分离状态。这一概念在核壳结构的 SrGa2O4:Cu2+/g-C3N4 (SGO/CN) 光催化剂中得到了验证,在这种光催化剂中,寿命长达数小时的存储电子可持续消耗 CN 中的空穴。定义明确的核壳结构、丰富的界面 Sr-N 键以及 SGO 和 CN 之间的交错能带排列对这种 S 型界面电荷转移至关重要,这有助于提高 CO2 到 CO 的转化活性和选择性。这种 S 型异质结结合了电荷存储材料作为过剩电子库,为设计高效光催化系统提供了一个很有前景的模板。
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引用次数: 0
Magnetically powered cancer cell microrobots for surgery-free generation of targeted tumor mouse models 磁动力癌细胞微型机器人,用于免手术生成靶向肿瘤小鼠模型
IF 8.9 2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-04 DOI: 10.1016/j.xcrp.2024.102182
Zehao Wu, Heng Sun, Zichen Xu, Kai Feng, Josh Haipeng Lei, Chu-Xia Deng, Qingsong Xu

In precision therapy, patient-derived cancer cells are inoculated into the same organ from which they are derived to simulate the microenvironment of the original tumor. However, due to the high technical difficulty and low success rate of the required surgical operation, appropriate animal models are lacking, which restricts its application. Here, we report a surgery-free method for creating a desired tumor mouse model using cancer cell microrobots guided by rotating gradient magnetic fields. The uptake of magnetic particles produces cancer cell microrobots. The external magnetic field enables the microrobots to hover around the target localization, enhancing their ability to penetrate the vascular endothelium. In vivo tests in mice demonstrate the capability of creating a desired tumor mass in a particular body location. This work provides a promising method to generate a targeted tumor mouse model without using conventional surgery operations for further precision medicine treatment study of cancer.

在精准治疗中,将患者来源的癌细胞接种到其来源的同一器官,以模拟原始肿瘤的微环境。然而,由于所需的外科手术技术难度高、成功率低,目前缺乏合适的动物模型,限制了其应用。在此,我们报告了一种利用旋转梯度磁场引导的癌细胞微型机器人创建所需肿瘤小鼠模型的免手术方法。磁性微粒的吸收产生了癌细胞微机器人。外部磁场可使微机器人在目标定位周围盘旋,增强其穿透血管内皮的能力。在小鼠体内进行的测试表明,这项技术能够在特定身体部位产生所需的肿瘤块。这项工作为在不使用传统外科手术的情况下生成靶向肿瘤小鼠模型提供了一种很有前景的方法,可用于进一步的癌症精准医学治疗研究。
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引用次数: 0
Tuning pH-dependent cytotoxicity in cancer cells by peripheral fluorine substitution on pseudopeptidic cages 通过伪肽笼上的外围氟替代物调节癌细胞的 pH 依赖性细胞毒性
IF 8.9 2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-03 DOI: 10.1016/j.xcrp.2024.102152
Lucía Tapia, Yolanda Pérez, Israel Carreira-Barral, Jordi Bujons, Michael Bolte, Carmen Bedia, Jordi Solà, Roberto Quesada, Ignacio Alfonso

The acidic microenvironment of solid tumors is a potential source of selectivity in the anti-cancer activity of ionophores, which requires delicate control of their biophysical properties. In this context, we have systematically studied fluorine substitutions in the aromatic side chains of HCl-binding pseudopeptidic cages. Interconnected factors like chloride binding, protonation, lipophilicity, and conformation and diffusiveness of the cages can impact their ability to transport HCl through the aqueous-lipid interphase, as demonstrated by robust experimental (X-ray, nuclear magnetic resonance [NMR], fluorescence) and theoretical results. The fine-tuning of these properties allows the modulation of their pH-dependent cytotoxicity against cancer cells, from essentially non-cytotoxic at pH 7.5 (like the extracellular surroundings of healthy tissues) to highly toxic in slightly acidic microenvironments (like those around solid tumors). Thus, a distal fluorine substitution produces a big impact on the physicochemical and biological properties of the cages, improving their selectivity as potential therapeutic ionophores.

实体瘤的酸性微环境是离子源抗癌活性选择性的潜在来源,这需要对其生物物理特性进行精细控制。在此背景下,我们系统地研究了盐酸结合伪肽笼芳香侧链中的氟取代。正如可靠的实验(X 射线、核磁共振 [NMR]、荧光)和理论结果所证明的那样,笼子的氯化物结合、质子化、亲油性、构象和扩散性等相互关联的因素会影响它们通过水-脂质间质转运 HCl 的能力。通过对这些特性进行微调,可以调节它们对癌细胞的 pH 值依赖性细胞毒性,从 pH 值为 7.5 时的无毒性(如健康组织的细胞外环境)到微酸性微环境中的高毒性(如实体瘤周围环境)。因此,远端氟取代对笼子的物理化学和生物特性产生了很大影响,提高了它们作为潜在治疗离子源的选择性。
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引用次数: 0
A pure radiant cooling device for “air conditioning” without conditioning air 无需调节空气即可实现 "空调 "的纯辐射冷却装置
IF 8.9 2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-03 DOI: 10.1016/j.xcrp.2024.102191
Xinyao Zheng, Yuekuan Zhou, Jinbo Li, Siyi Li

Ever since the birth of the first air conditioner (Carrier air conditioner) in 1902, over one hundred years ago, it has been accompanied by several technical problems, e.g., (1) low energy efficiency in large open spaces, (2) spread of pollutants, airborne pandemic transmission (e.g., severe acute respiratory syndrome [SARS], COVID-19) through air-conditioning systems, and (3) low comfort caused by fan noise and blowing sounds. Here, we report a personalized pure radiant cooling device that decouples the fresh air supply from space cooling to achieve air conditioning without conditioning the air. Condensation-free radiant cooling with a radiant cooling capacity of 152 W/m2 is achieved with a polyethylene (PE) film-covered super-cold infrared-emissive surface. By optimizing the design and operation parameters, the device saves up to 50.4% of cooling energy in a typical summer building environment. Our concept opens up the possibility of pandemic-free personalized thermal management with high energy efficiency and thermal comfort.

自 1902 年第一台空调(开利空调)诞生以来,一百多年来,空调一直伴随着一些技术问题,例如:(1)大型开放空间能效低;(2)污染物通过空调系统传播,空气传播流行病(如严重急性呼吸系统综合征 [SARS]、COVID-19);(3)风扇噪音和吹风声导致舒适度低。在此,我们报告了一种个性化的纯辐射冷却装置,它将新风供应与空间冷却分离开来,在不调节空气的情况下实现空气调节。通过聚乙烯(PE)薄膜覆盖的超冷红外辐射表面实现了无结露辐射制冷,辐射制冷量为 152 W/m2。通过优化设计和运行参数,该设备在典型的夏季建筑环境中可节省高达 50.4% 的冷却能源。我们的概念为实现无大流行病的个性化热管理、高能效和热舒适性提供了可能。
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引用次数: 0
Disordered regions of inhibitor-bound α-synuclein suppress seed-induced fibril nucleation in cells 抑制剂结合的α-突触核蛋白的无序区可抑制细胞中种子诱导的纤维核形成
IF 8.9 2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-02 DOI: 10.1016/j.xcrp.2024.102180
Celina M. Schulz, Emil D. Agerschou, Luis Gardon, Miriam Alexander, Matthias Stoldt, Henrike Heise, Gültekin Tamgüney, Wolfgang Hoyer

Inhibitors of amyloid fibril formation can act in diverse ways and aid in elucidating the mechanisms of protein aggregation. The engineered binding protein β-wrapin AS69 binds monomers of Parkinson-disease-associated α-synuclein (αS), yet achieves inhibition at substoichiometric concentration. The substoichiometric activity was not attributed to the binding protein per se, but to its 1:1 complex with αS, in which AS69 sequesters αS residues 30–60 into a globular protein fold, whereas other αS parts remain intrinsically disordered regions (IDRs). Here, we investigate AS69-αS fusion constructs that form the AS69:αS complex by intramolecular folding and expose different IDRs. We find that not only the globular part of the complex but also αS IDRs are critical for substoichiometric inhibition, which is achieved by interference with primary and secondary fibril nucleation. The effects in vitro are reproduced in cellular seeding assays, indicating that secondary nucleation drives seeding in aggregate biosensing.

淀粉样纤维形成抑制剂的作用方式多种多样,有助于阐明蛋白质的聚集机制。经过改造的结合蛋白β-wrapin AS69能与帕金森病相关的α-突触核蛋白(αS)的单体结合,但在亚几何浓度下也能实现抑制作用。亚几何浓度的活性并不是由于结合蛋白本身,而是由于它与αS的1:1复合物,其中AS69将αS残基30-60封存在一个球状蛋白质折叠中,而αS的其他部分则保持在本征无序区(IDR)。在这里,我们研究了通过分子内折叠形成 AS69:αS 复合物并暴露出不同 IDR 的 AS69-αS 融合构建体。我们发现,不仅是复合物的球状部分,αS IDR 也是亚计量抑制的关键,这种抑制是通过干扰原生和次生纤维成核实现的。体外效应在细胞播种试验中得以重现,这表明在聚合体生物传感过程中,次生成核驱动了播种。
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引用次数: 0
Energy harvesting from algae using large-scale flat-tube solid oxide fuel cells 利用大型扁管固体氧化物燃料电池从水藻中获取能量
IF 8.9 2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-31 DOI: 10.1016/j.xcrp.2024.102214
Junkang Sang, Yuqing Li, Jun Yang, Tao Wu, Luo Xiang, Yongming Zhao, Wanbing Guan, Jingxiang Xu, Maorong Chai, Subhash C. Singhal
No Abstract
无摘要
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引用次数: 0
Energy-efficient and cost-effective ammonia electrolysis for converting ammonia to green hydrogen 将氨转化为绿色氢气的高能效、低成本氨电解技术
IF 8.9 2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-29 DOI: 10.1016/j.xcrp.2024.102171
Kui Zhang, Yangkai Han, Yun Zhao, Tao Wei, Jinchen Fu, Zhiwei Ren, Xiaozhi Xu, Li Zhou, Zhigang Shao

Ammonia (NH3), touted as a promising hydrogen carrier, has received increasing attention. However, the technoeconomic prospects of comprehensive conversion of hydrogen to ammonia and ammonia to hydrogen (H2-NH3-H2) are unclear, and the approach to ammonia-to-hydrogen conversion has not yet reached the full commercialization stage. In this work, we perform a technoeconomic analysis of a H2-NH3-H2 conversion system, including synthesis, storage and transportation, and ammonia-to-hydrogen conversion, where we particularly compared thermal ammonia cracking with ammonia electrolysis. We find that ammonia electrolysis has a significant economic advantage thanks to its low energy consumption and capital cost. With this as motivation, we develop an energy-efficient and durable ammonia electrolyzer with an energy consumption of 0.84 kWh Nm−3 H2 and a continuous operation for 317 h at 100 mA cm−2. In addition, we also innovate a tandem cell to produce hydrogen without any electric power supply by coupling fuel-cell and electrolysis technologies.

氨(NH3)被誉为一种前景广阔的氢载体,受到越来越多的关注。然而,氢-氨和氨-氢(H2-NH3-H2)综合转换的技术经济前景尚不明确,氨-氢转换的方法尚未达到完全商业化阶段。在这项工作中,我们对 H2-NH3-H2 转换系统进行了技术经济分析,包括合成、储存和运输以及氨制氢转换,其中我们特别对热氨裂解和氨电解进行了比较。我们发现,由于氨电解能耗低、成本低,因此具有显著的经济优势。在此基础上,我们开发了一种节能耐用的氨电解槽,能耗为 0.84 kWh Nm-3 H2,在 100 mA cm-2 的条件下可连续运行 317 h。此外,我们还创新了一种串联电池,通过将燃料电池和电解技术相结合,在没有任何电力供应的情况下生产氢气。
{"title":"Energy-efficient and cost-effective ammonia electrolysis for converting ammonia to green hydrogen","authors":"Kui Zhang, Yangkai Han, Yun Zhao, Tao Wei, Jinchen Fu, Zhiwei Ren, Xiaozhi Xu, Li Zhou, Zhigang Shao","doi":"10.1016/j.xcrp.2024.102171","DOIUrl":"https://doi.org/10.1016/j.xcrp.2024.102171","url":null,"abstract":"<p>Ammonia (NH<sub>3</sub>), touted as a promising hydrogen carrier, has received increasing attention. However, the technoeconomic prospects of comprehensive conversion of hydrogen to ammonia and ammonia to hydrogen (H<sub>2</sub>-NH<sub>3</sub>-H<sub>2</sub>) are unclear, and the approach to ammonia-to-hydrogen conversion has not yet reached the full commercialization stage. In this work, we perform a technoeconomic analysis of a H<sub>2</sub>-NH<sub>3</sub>-H<sub>2</sub> conversion system, including synthesis, storage and transportation, and ammonia-to-hydrogen conversion, where we particularly compared thermal ammonia cracking with ammonia electrolysis. We find that ammonia electrolysis has a significant economic advantage thanks to its low energy consumption and capital cost. With this as motivation, we develop an energy-efficient and durable ammonia electrolyzer with an energy consumption of 0.84 kWh Nm<sup>−3</sup> H<sub>2</sub> and a continuous operation for 317 h at 100 mA cm<sup>−2</sup>. In addition, we also innovate a tandem cell to produce hydrogen without any electric power supply by coupling fuel-cell and electrolysis technologies.</p>","PeriodicalId":9703,"journal":{"name":"Cell Reports Physical Science","volume":"7 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2024-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142226025","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Bioluminescence and photoacoustic dual-modality imaging of apoptosis using a duramycin-immobilized gold nanorod probe 使用杜拉霉素固定金纳米棒探针对细胞凋亡进行生物发光和光声双模式成像
IF 8.9 2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-29 DOI: 10.1016/j.xcrp.2024.102177
Jingyu Zhang, Bin Guo, Yiyi Jiang, Xiaorui Shi, Chong Hu, Zihao Jiao, Fu Wang

Phosphatidylethanolamine (PE) translocation is considered a hallmark event of cellular apoptosis. The development of non-invasive multi-modality probes targeting PE for apoptosis detection holds great promise. Here, we develop a dual-modality imaging probe, duramycin-Fluc-AuNRs (DFA), for detecting apoptosis in tumor cells. DFA is created by linking duramycin peptide and firefly luciferase (Fluc) recombinant protein to gold nanorods (AuNRs). Duramycin exhibits high affinity for PE, while Fluc produces a robust bioluminescence signal, and AuNRs enhance imaging resolution through photoacoustic conversion. The DFA probe demonstrates low toxicity in both cells and mice, showcasing its potential for in vivo applications. In A549 and 4T1 cell lines, the bioluminescence signal of the DFA probe increases with the degree of doxorubicin (Dox)-induced apoptosis. At the mouse level, mice with Dox-triggered apoptosis exhibit higher bioluminescence and photoacoustic imaging signals. Thus, this dual-modality bioluminescence/photoacoustic imaging platform holds significant potential for detecting cellular apoptosis and providing high-performance imaging information.

磷脂酰乙醇胺(PE)转位被认为是细胞凋亡的标志性事件。开发以 PE 为靶点的非侵入性多模态探针用于细胞凋亡检测前景广阔。在此,我们开发了一种用于检测肿瘤细胞凋亡的双模态成像探针--杜拉霉素-Fluc-AuNRs(DFA)。DFA 是通过将杜拉霉素肽和萤火虫荧光素酶(Fluc)重组蛋白与金纳米棒(AuNRs)连接而制成的。杜拉霉素对 PE 具有高亲和力,而萤火虫荧光素酶能产生强大的生物发光信号,AuNRs 则通过光声转换提高成像分辨率。DFA 探针在细胞和小鼠体内均表现出低毒性,展示了其体内应用的潜力。在 A549 和 4T1 细胞系中,DFA 探针的生物发光信号随着多柔比星(Dox)诱导的细胞凋亡程度而增加。在小鼠水平上,Dox 诱导凋亡的小鼠表现出更高的生物发光和光声成像信号。因此,这种双模式生物发光/光声成像平台在检测细胞凋亡和提供高性能成像信息方面具有巨大潜力。
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引用次数: 0
Wettability gradient of photoresponsive electrospun yarns for harp-based fog water harvesting 用于竖琴式雾水收集的光致伸缩电纺纱的润湿梯度
IF 8.9 2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-29 DOI: 10.1016/j.xcrp.2024.102176
Gregory Parisi, Piotr K. Szewczyk, Shankar Narayan, Urszula Stachewicz

Fog water harvesting offers a solution to water scarcity. Here, we introduce a method to enhance fog water harvesting systems utilizing electrospun yarns featuring a wettability gradient. These yarns, made from polyvinylidene fluoride (PVDF) and titanium dioxide (TiO2), gain photoinduced hydrophilicity under UV light due to TiO2 photocatalytic properties, allowing dynamic shifts from hydrophobic to hydrophilic states. Experiments show that an alternating PVDF-TiO2 harp with a wettability gradient surpasses purely hydrophobic or hydrophilic versions in fog collection. The strategic mix of hydrophobic and hydrophilic sections enhances droplet movement and water capture, achieving a 16% increase in collection rate up to 400 mg cm−2 h−1. This approach introduces a novel method for creating wettability gradients in electrospun yarns via UV irradiation and represents a significant advancement in adaptable fog water harvesting systems.

雾水收集为水资源短缺提供了一种解决方案。在此,我们介绍一种利用具有润湿梯度的电纺纱来增强雾水收集系统的方法。这些纱线由聚偏二氟乙烯(PVDF)和二氧化钛(TiO2)制成,由于二氧化钛的光催化特性,这些纱线在紫外线照射下可获得光诱导亲水性,从而实现从疏水状态到亲水状态的动态转变。实验表明,具有润湿梯度的 PVDF-TiO2 交替竖琴在雾气收集方面优于纯疏水性或亲水性竖琴。疏水和亲水部分的策略性混合增强了水滴的移动和水捕获,使收集率提高了 16%,最高可达 400 毫克厘米-2 小时-1。这种方法介绍了一种通过紫外线照射在电纺纱中产生润湿性梯度的新方法,是适应性雾水收集系统的一大进步。
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引用次数: 0
Intrinsically conductive polymer reinforced hydrogel with synergistic strength, toughness, and sensitivity for flexible motion-monitoring sensors 具有协同强度、韧性和灵敏度的本征导电聚合物增强水凝胶,可用于柔性运动监测传感器
IF 8.9 2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-29 DOI: 10.1016/j.xcrp.2024.102178
Mengke Zhao, Ting Wu, Xiaofa Wang, Long Liang, Hailong Lu, Zhanghong Xie, Tongqi Yuan, Guigan Fang

Conductive hydrogels with remarkable flexibility and sensitivity have attracted substantial attention as a potential material for the construction philosophy of wearable electronics. Nevertheless, the development of high-performance hydrogels continues to be a significant challenge due to the inherent trade-off between conductivity and deformation adaptability. Here, a novel strategy is demonstrated for the preparation of intrinsically conductive reticulated polymer-based hydrogels (allylated hydroxyethyl cellulose-PEDOT:PSS/PAM hydrogel [AHEC-PP/PAM]) with mechanical robustness and perceptual sensitivity. The conductive reticulated component, AHEC-PP, is obtained by an ingenious polymerization involving AHEC and EDOT and demonstrates favorable dispersion and stability, with the treatment of H2SO4 and the charge regulation of PSS. The AHEC-PP/PAM hydrogel has a tensile strength of 0.69 MPa, a fracture strain of 1,273%, a broad sensing range, and a high gauge factor of 7.86. The synergistic performance enables integration into smart wearable electronic devices for the detection of motion signals, electronic skin, and advanced human-machine interaction.

导电水凝胶具有出色的柔韧性和灵敏度,作为可穿戴电子设备构造理念的潜在材料,已经引起了广泛关注。然而,由于导电性和变形适应性之间的固有权衡,开发高性能水凝胶仍然是一项重大挑战。本文展示了一种新策略,用于制备具有机械坚固性和感知灵敏性的内在导电网状聚合物水凝胶(烯丙基羟乙基纤维素-PEDOT:PSS/PAM 水凝胶 [AHEC-PP/PAM])。导电网状成分 AHEC-PP 是通过 AHEC 和 EDOT 的巧妙聚合反应获得的,经 H2SO4 处理和 PSS 的电荷调节,具有良好的分散性和稳定性。AHEC-PP/PAM 水凝胶的拉伸强度为 0.69 兆帕,断裂应变为 1,273%,传感范围广,测量系数高达 7.86。这种协同性能可以集成到智能可穿戴电子设备中,用于检测运动信号、电子皮肤和高级人机交互。
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引用次数: 0
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Cell Reports Physical Science
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