Room temperature

室温
  • 文章类型: Journal Article
    提出了一种先进的扫描探针显微镜系统,该系统具有人工智能(AI-SPM),旨在用于自动驱动原子级测量。该系统熟练识别和操作原子位置,具有很高的精度,自主执行任务,如光谱数据采集和原子调整。AI-SPM的一个突出特点是能够检测和适应表面缺陷,必要时瞄准或避免他们。它还旨在克服典型的挑战,如位置漂移和尖端顶点原子变化由于热效应,确保准确,特定位置的表面分析。在室温的苛刻条件下的测试证明了系统的鲁棒性,成功导航热漂移和尖端波动。在Si(111)-(7×7)表面的这些测试中,AI-SPM自主识别出无缺陷区域,并在不同的吸附原子位点进行了大量的电流-电压谱测量,同时自动补偿热漂移和监测探头健康。这些实验产生了广泛的数据集,这些数据集对可靠的材料表征至关重要,并展示了AI-SPM显着改善数据采集的潜力。将AI集成到SPM技术中代表了朝着更有效的方向迈出的一步,精确可靠的原子级表面分析,革命性的材料表征方法。
    An advanced scanning probe microscopy system enhanced with artificial intelligence (AI-SPM) designed for self-driving atomic-scale measurements is presented. This system expertly identifies and manipulates atomic positions with high precision, autonomously performing tasks such as spectroscopic data acquisition and atomic adjustment. An outstanding feature of AI-SPM is its ability to detect and adapt to surface defects, targeting or avoiding them as necessary. It is also designed to overcome typical challenges such as positional drift and tip apex atomic variations due to the thermal effects, ensuring accurate, site-specific surface analysis. The tests under the demanding conditions of room temperature have demonstrated the robustness of the system, successfully navigating thermal drift and tip fluctuations. During these tests on the Si(111)-(7 × 7) surface, AI-SPM autonomously identified defect-free regions and performed a large number of current-voltage spectroscopy measurements at different adatom sites, while autonomously compensating for thermal drift and monitoring probe health. These experiments produce extensive data sets that are critical for reliable materials characterization and demonstrate the potential of AI-SPM to significantly improve data acquisition. The integration of AI into SPM technologies represents a step toward more effective, precise and reliable atomic-level surface analysis, revolutionizing materials characterization methods.
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  • 文章类型: Journal Article
    电子自旋量子位正在成为量子计算和信息存储领域的重要研究方向。然而,量子退相干严重阻碍了这一领域的发展。到目前为止,很少的量子比特表现出长的相位记忆时间(Tm),甚至更少的量子比特可以达到室温。一些报道表明,自由基的连贯时间通常较长,所以自由基可能是量子位的首选自旋载体。这里,我们证明了基于2,4,6-三(4-吡啶基)-1,3,5-三嗪的光生自由基(1a)的量子位性质(tpt,1).更重要的是,光生自由基是一种自旋自稀释络合物,在量子比特的研究中,为了克服量子比特的退相干,通常采用稀释的方法来减少环境对量子比特的干扰。令人惊讶的是,激进的tpt在20K以上具有稳定的Tm=1.1μs,甚至保持在室温。此外,通过真空蒸发制备的tpt膜在低温下显着增加了T1和Tm。
    Electron spin qubits are becoming an important research direction in the field of quantum computing and information storage. However, the quantum decoherence has seriously hindered the development of this field. So far, few qubits exhibit long phase memory time (Tm), and even fewer qubits that can reach room temperature. Some reports show that the coherence times of radicals are generally long, so radicals may be the preferred spin carriers for qubits. Here, we demonstrate the qubit properties of a photogenerated radical (1a) based on 2,4,6-Tri(4-pyridyl)-1,3,5-triazine (tpt, 1). More importantly, the photogenerated radical is a spin self-diluting complex, which the dilution is generally used in the investigation of qubits to reduce the interference of environment on qubits in order to overcome the decoherence of qubits. It is surprised that radical tpt has a stable Tm = 1.1 μs above 20 K, even keep it to room temperature. In addition, the tpt-film prepared by the vacuum evaporation is significantly increase the T1 and Tm at low temperature.
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  • 文章类型: Journal Article
    实现对目标挥发性有机化合物气体的选择性传感在空气质量评估领域至关重要。食品新鲜度评价,并通过呼出气对患者进行诊断。然而,在复杂环境中表现出像生物酶一样的特异性的化学电阻传感器是罕见的。在这里,我们开发了一种优化氧化锡中氧空位结构以诱导特定催化的策略,在室温下激活对胺气体的100%选择性传感。原位技术和理论计算表明,胺分子中的氮原子与桥接氧空位(OVBri)诱导的电子缺失中心之间的“供体-受体”配位是特定催化的本质,并提供了从表面氧化反应到电物理特性演变的桥梁。这使得传感器能够表现出胺特异性传感行为,即使在气体混合物中。此外,OVBri通过实现室温传感途径来增强选择性,其中晶格氧参与胺分子的催化氧化,产生创纪录的高感测值:19,938.92对100ppm的三乙胺,15,236.78对三甲胺,和123.41对二乙胺。我们的发现说明了通过缺陷工程设计特定活性位点的可行性,并且可以促进基于催化过程的高选择性传感器的发展。
    Achieving selective sensing toward target volatile organic compound gases is of vital importance in the fields of air quality assessment, food freshness evaluation, and diagnosis of patients via exhaled breath. However, chemiresistive sensors that exhibit specificity like biological enzymes in a complex environment are rare. Herein, we developed a strategy of optimizing oxygen vacancy structures in tin oxides to induce specific catalysis, activating 100% selective sensing toward amine gases at room temperature. In situ technologies and theoretical calculations reveal that the \"donor-receptor\" coordination between nitrogen atoms from amine molecules and bridging oxygen vacancies (OVBri)-induced electron-deficient center is the essence of specific catalysis and provides the bridge from the surface oxidation reaction to electrophysical characteristics evolution, which allows the sensor to exhibit amine-specific sensing behavior, even in gas mixtures. Moreover, OVBri enhances the selectivity by enabling a room-temperature sensing pathway where lattice oxygens participate in catalytic oxidation for amine molecules, resulting in record-high sensing values: 19,938.92 toward 100 ppm of triethylamine, 15,236.78 toward trimethylamine, and 123.41 toward diethylamine. Our findings illustrate the feasibility of designing specific active sites through defect engineering and can contribute to the advancement of highly selective sensors based on catalytic processes.
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  • 文章类型: Journal Article
    AgNW网络由于优异的柔韧性而显示出作为导电材料的高前景,低电阻,高透明度,易于大规模制备。然而,AgNW网络的应用受到其固有特性的阻碍,如易氧化降解,化学腐蚀,和高温下的结构不稳定性。在这项研究中,引入源自全氢聚硅氮烷的致密SiOx保护层,通过在室温下的全溶液工艺制造坚固的SiOx/AgNW纳米复合涂层。所获得的纳米复合涂层在高达450°C的温度下显示出出色的热稳定性,抗紫外线辐射,和优异的机械性能,通过在半径为2.5mm的10,000次弯曲后保持稳定性,1000次剥皮循环,和1200次穿着。同时,纳米复合涂层对HCl具有特殊的化学耐受性,Na2S,和有机溶剂。基于纳米复合涂层的透明加热器在20V时的最高温度为400°C,达到了卓越的基准。这些功能凸显了纳米复合涂层在柔性电子产品中的潜力,光电子学,触摸屏,和高性能加热器。
    AgNW networks show high promise as a conductive material due to excellent flexibility, low resistance, high transparency, and ease of large-scale preparation. However, the application of AgNW networks has been hindered by their inherent characteristics, such as easy oxidation degradation, chemical corrosion, and structural instability at high temperatures. In this study, a dense SiOx protective layer derived from perhydropolysilazane was introduced to fabricate a robust SiOx/AgNW nanocomposite coating through an all-solution process at room temperature. The achieved nanocomposite coating shows outstanding thermal stability up to 450 °C, resistance to ultraviolet radiation, and excellent mechanical performance by maintaining stability after 10,000 cycles of bending at a radius of 2.5 mm, 1000 cycles of peeling, and 1200 cycles of wearing. Meanwhile, the nanocomposite coating demonstrates exceptional chemical tolerance against HCl, Na2S, and organic solvents. A transparent heater based on the nanocomposite coating achieves a remarkable benchmark with a maximum temperature of 400 °C at 20 V. These features highlight the potential of the nanocomposite coating in flexible electronics, optoelectronics, touch screens, and high-performance heaters.
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  • 文章类型: Journal Article
    基于聚(环氧乙烷)(PEO)的电解质与超高镍正极材料的匹配对于设计新一代高能量密度固态锂金属电池(SLMB)至关重要。但是它受到PEO和超高镍材料之间严重的界面副反应的限制。这里,在阴极和电解质之间构建具有定制Li+溶剂化护套的高浓度电解质(HCE)界面。它诱导形成阴离子调节的强大的阴极/电解质界面(CEI),减少不稳定的自由状态溶剂,最终实现了PEO基电解液与超高镍正极材料的相容性。同时,通过二氟(草酸)硼酸锂(LiDFOB)离子防止由双(三氟甲磺酰基)酰亚胺锂(LiTFSI)离子引起的Al集电器的腐蚀。双锂盐的协同效应通过在Li+的第一溶剂化鞘中TFSI-和DFOB-的良好定制的比率来实现。与报道的与超高镍(Ni≥90%)阴极匹配的基于PEO的SLMB相比,这项工作中的SLMB即使在室温下也能提供216.4mAhg-1(0.1C)的高放电比容量。这项工作指出了优化阴极/电解质界面的方向。
    The matching of poly(ethylene oxide) (PEO)-based electrolytes with ultrahigh-nickel cathode materials is crucial for designing new-generation high-energy-density solid-state lithium metal batteries (SLMBs), but it is limited by serious interfacial side reactions between PEO and ultrahigh-nickel materials. Here, a high-concentration electrolyte (HCE) interface with a customized Li+ solvation sheath is constructed between the cathode and the electrolyte. It induces the formation of an anion-regulated robust cathode/electrolyte interface (CEI), reduces the unstable free-state solvent, and finally achieves the compatibility of PEO-based electrolytes with ultrahigh-nickel cathode materials. Meanwhile, the corrosion of the Al current collector caused by lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) ions is prevented by lithium difluoro(oxalato)borate (LiDFOB) ions. The synergistic effect of the double lithium salt is achieved by a well-tailored ratio of TFSI- and DFOB- in the first solvation sheath of Li+. Compared with reported PEO-based SLMBs matched with ultrahigh-nickel (Ni ≥ 90%) cathodes, the SLMB in this work delivers a high discharge specific capacity of 216.4 mAh g-1 (0.1C) even at room temperature. This work points out a direction to optimize the cathode/electrolyte interface.
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  • 文章类型: Journal Article
    我们开发了一种HPLC系统,其中相分离多相流在分离柱中作为洗脱液工作。我们将新型分离机制称为相分离模式。水/乙腈/乙酸乙酯三元混合溶液,这是两相分离混合溶液之一,通过温度效应(从20到0°C)从均质到非均质的相变引起相分离多相流。在这项研究中,我们试图用压力效应代替温度效应进行相分离多相流。将熔融石英毛细管(长度为50厘米,内径为50μm)与色谱柱的下游相连,以对系统施加5.5MPa的压力。研究了2,6-萘二磺酸(2,6-NDS)和1-萘酚(1-NA)的模型分析物。例如,溶液(体积%的水/乙腈/乙酸乙酯;20:55:25,富含有机物)和(60:30:10,富含水)用作洗脱剂。在1.5MPa和20°C的压力下用两种溶液不分离模型分析物。但是有了富含有机物的溶液,1-NA和2,6-NDS按此顺序分离,并与富含水的溶液,它们在5.5MPa和20°C的压力下以相反的顺序分离。相分离模式可以在高压下甚至在室温下进行。
    We have developed a HPLC system where phase-separation multiphase flow works in the separation column as an eluent. We call the novel separation mechanism a phase-separation mode. The ternary mixed solution of water/acetonitrile/ethyl acetate, which is one of the two-phase-separation mixed solutions, caused the phase-separation multiphase flow via phase change from homogeneous to heterogeneous with the temperature effect (from 20 to 0 °C). In this study, we tried to perform phase-separation multiphase flow with the pressure effect instead of the temperature one. The fused-silica capillary tube (50 cm length and 50 µm inner diameter) was allied to the downstream of the column to apply the pressure of 5.5 MPa to the system. Model analytes of 2,6-naphthalenedisulfonic acid (2,6-NDS) and 1-naphthol (1-NA) were examined. For example, solutions (the volume% of water/acetonitrile/ethyl acetate; 20:55:25, organic-rich) and (60:30:10, water-rich) were used as eluent. The model analytes were not separated with both solutions at the pressure of 1.5 MPa and 20 °C. But with the organic-rich solution, 1-NA and 2,6-NDS were separated in this order and with the water-rich solution, they were separated in the reverse order at the pressure of 5.5 MPa and 20 °C. The phase-separation mode could be performed at the high pressure even at the room temperature.
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  • 文章类型: Journal Article
    结构生物学的进步在很大程度上依赖于同步加速器冷冻晶体学和低温电子显微镜来阐明生物过程和药物发现。然而,低温和室温(RT)晶体结构之间的差异带来了挑战。这里,Cryo2RT,一种利用冷冻晶体学工作流程的冷冻晶体高通量RT数据收集方法,是介绍的。用四个浸泡过的碎片在内硫肽晶体上测试,thaumatin和SARS-CoV-23CLpro,Cryo2RT揭示了独特的配体结合姿势,提供了一个相当的吞吐量,以冷冻晶体学和简化在各种温度下的结构动力学的探索。
    Advances in structural biology have relied heavily on synchrotron cryo-crystallography and cryogenic electron microscopy to elucidate biological processes and for drug discovery. However, disparities between cryogenic and room-temperature (RT) crystal structures pose challenges. Here, Cryo2RT, a high-throughput RT data-collection method from cryo-cooled crystals that leverages the cryo-crystallography workflow, is introduced. Tested on endothiapepsin crystals with four soaked fragments, thaumatin and SARS-CoV-2 3CLpro, Cryo2RT reveals unique ligand-binding poses, offers a comparable throughput to cryo-crystallography and eases the exploration of structural dynamics at various temperatures.
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  • 文章类型: Journal Article
    为了减轻抗生素等各种污染物对水资源的污染,不可避免地需要进行废水处理。MOFs是具有光催化活性的新型材料。在这项研究中,通过对其合成路线的修改,优化了铈基MOF(Ce-MOF)对四环素(TC)的超声催化降解。Ce-MOF合成室温(RT),热液(HT),和声化学合成(SC)进行了研究。TC降解实验揭示了SC合成的优越性。主要合成参数的相互作用,即,初始配体浓度,超声(US)功率和时间对Ce-MOF,利用中心复合实验设计(CCD)通过响应面方法模型(RSM)进行了研究。最佳的SC合成条件是配体的初始浓度为8.4mmol/L,50振幅的超声处理能力,和美国时间60分钟。通过红外光谱对最佳合成的Ce-MOF进行了表征,FTIR,XRD,FE-SEM,TEM,zeta电位分析,漫反射光谱,粒度分析,Mott-Schottky分析,光电流分析,电化学阻抗谱,和光致发光光谱。结果表明,在初始TC浓度为120ppm和1g/LCe-MOF的水溶液中,在pH为7的条件下,TC的去除效率在120min内可以达到81.75%。根据COD测量,该工艺的矿化效率为71%。Ce-MOF催化剂保留了其化学稳定性,并在TC降解后保持活性,这使其成为废水处理的有希望的候选物。
    Wastewater treatment is inevitably required to alleviate the pollution of water resources by various contaminants such as antibiotics. MOFs are novel materials with photocatalytic activities. In this study, sonophotocatalytic degradation of tetracycline (TC) by the Cerium-based MOF (Ce-MOF) is optimized by modification of its synthesis route. Ce-MOF synthesis by room temperature (RT), hydrothermal (HT), and sonochemical synthesis (SC) are studied. TC degradation experiments revealed the superiority of SC synthesis. The interplay of main synthesis parameters, namely, initial ligand concentration, ultrasound (US) power and time on sonophotocatalytic activity of Ce-MOF, were investigated by response surface methodology model (RSM) utilizing the central composite experimental design (CCD). The optimum SC synthesis conditions are an initial ligand concentration of 8.4 mmol/L, a sonication power of 50 amplitude, and a US time of 60 min. The optimally synthesized Ce-MOF was characterized by infrared spectroscopy, FTIR, XRD, FE-SEM, TEM, zeta potential analysis, diffuse reflectance spectroscopy, particle size analysis, Mott-Schottky analysis, photocurrent analysis, electrochemical impedance spectra, and photoluminescence spectroscopy. The findings indicate that the removal efficiency of TC can reach up to 81.75% within 120 min in an aqueous solution containing an initial TC concentration of 120 ppm and 1 g/L Ce-MOF at pH of 7. Mineralization efficiency of the process is 71% according to COD measurements. The Ce-MOF catalyst retained its chemical stability and remained active upon TC degradation which makes it a promising candidate for wastewater treatment.
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  • 文章类型: Journal Article
    在室温下操作的NO2传感器的不良恢复特性的持续挑战仍然是显著的。然而,基于In2O3的气敏材料的开发提供了一种有希望的方法来加速室温下NO2亚ppm检测的响应和恢复。在这里,我们提出了一种简单的两步法来合成具有中空微管的一维(1D)In2O3@ZnO异质结构材料,通过偶联金属-有机骨架(MOFs)(MIL-68(In))和锌离子。同时,基于In2O3@ZnO复合材料的气体传感器在可见光激活下对NO2表现出优异的灵敏度性能。室温下对5ppmNO2的响应值高达1800,是纯In2O3基传感器的35倍。此外,与基于纯In2O3的传感器(74s/235s)相比,基于In2O3@ZnO异质结构的气体传感器显着减少了30s/67s的响应/恢复时间。In2O3@ZnO异质结构传感器的出色气敏特性可归因于异质结构效应导致的光生电荷分离效率提高,并改善了对NO2的受体功能,这可以增加反应位点和气体吸附能力。总之,这项工作提出了一种低成本,高效的方法来合成具有微管结构的一维异质结构材料,它可以作为开发高性能室温气体传感器的基本技术。
    The persistent challenge of poor recovery characteristics of NO2 sensors operated at room temperature remains significant. However, the development of In2O3-based gas sensing materials provides a promising approach to accelerate response and recovery for sub-ppm of NO2 detection at room temperature. Herein, we propose a simple two-step method to synthesize a one-dimensional (1D) In2O3@ZnO heterostructure material with hollow microtubes, by coupling metal-organic frameworks (MOFs) (MIL-68 (In)) and zinc ions. Meanwhile, the In2O3@ZnO composite-based gas sensor exhibits superior sensitivity performance to NO2 under visible light activation. The response value to 5 ppm of NO2 at room temperature is as high as 1800, which is 35 times higher than that of the pure In2O3-based sensor. Additionally, the gas sensor based on the In2O3@ZnO heterostructure demonstrates a significantly reduced response/recovery time of 30 s/67 s compared to the sensor based on pure In2O3 (74 s/235 s). The outstanding gas sensing properties of the In2O3@ZnO heterostructure-based sensors can be attributed to the enhanced photogenerated charge separation efficiency resulting from the heterostructure effect, and the improved receptor function toward NO2, which can increase the reactive sites and gas adsorption capacity. In summary, this work proposes a low-cost and efficient method to synthesize a 1D heterostructure material with microtube structures, which can serve as a fundamental technique for developing high-performance room-temperature gas sensors.
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  • 文章类型: Journal Article
    将磷掺杂的碳纳米管(CNT)气凝胶作为载体材料,在燃料电池型气体传感器中负载Pt纳米颗粒,用于超灵敏的H2检测。CNT支架的高表面积有利于提供丰富的活性位点,和高导电性促进由电化学反应产生的载流子的传输。此外,在CNT气凝胶中掺杂磷(P)以进一步提高导电性和电化学催化活性。因此,使用掺杂有最佳P含量的Pt/CNT气凝胶作为传感材料的燃料电池型气体传感器在室温下对H2检测显示出相当大的性能。该传感器表现出-921.9μA至15,000ppm的H2的超高响应。灵敏度为-0.063μA/ppm,是常规Pt/CF对应物的21倍。该传感器还具有出色的可重复性和耐湿性,以及快速响应/恢复;响应/恢复时间分别为31和4s到3000ppm的H2。载体材料的结构和催化性能的调制负责传感器性能的改善,从而为优化燃料电池型气体传感器的性能提供了可行的解决方案。
    A phosphorus-doped carbon nanotube (CNT) aerogel as the support material was loaded with Pt nanoparticles in fuel cell-type gas sensors for ultrasensitive H2 detection. The high surface area of the CNT scaffold is favorable to providing abundant active sites, and the high electrical conductivity facilitates the transport of carriers generated by electrochemical reactions. In addition, the CNT aerogel was doped with phosphorus (P) to further enhance the conductivity and electrochemical catalytic activity. As a result, the fuel cell-type gas sensor using the Pt/CNT aerogel doped with the optimal P content as the sensing material shows considerable performance for H2 detection at room temperature. The sensor exhibits an ultrahigh response of -921.9 μA to 15,000 ppm of H2. The sensitivity is -0.063 μA/ppm, which is 21 times higher than that of the conventional Pt/CF counterpart. The sensor also exhibits excellent repeatability and humidity resistance, as well as fast response/recovery; the response/recovery times are 31 and 4 s to 3000 ppm of H2, respectively. The modulation of the structure and catalytic properties of the support material is responsible for the improvement of the sensor performance, thus providing a feasible solution for optimizing the performance of fuel cell-type gas sensors.
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