intermediate phase

中间相
  • 文章类型: Journal Article
    脊髓损伤(SCI)的中期是SCI治疗介导的重要靶位点。然而,对SCI中间阶段的机制缺乏了解。本研究旨在探讨SCI中期的分子机制和可行的治疗靶点。我们从GEO下载GSE2599,鉴定出416个显著的差异表达基因(DEG),包括206个下调的DEG和210个上调的DEG。对DEGs的进一步富集分析表明,在损伤的脊髓中触发了许多重要的生物学过程和信号通路。此外,构建了蛋白质-蛋白质相互作用(PPI)网络,并鉴定了前10个高度枢纽节点.此外,鉴定了27个预测的转录因子(TF)和136个预测的基序。然后我们选择胰岛素样生长因子1(IGF1)及其预测的转录因子,转录因子A,线粒体(TFAM)进行进一步研究。我们推测并初步证实,TFAM可能调节IGF1的基因转录,并影响SCI后大鼠功能恢复的变化。这些发现共同提供了新的信息,可以提高我们对SCI中期病理生理过程的理解。
    The intermediate phase of spinal cord injury (SCI) serves as an important target site for therapeutic mediation of SCI. However, there is a lack of insight into the mechanism of the intermediate phase of SCI. The present study aimed to investigate the molecular mechanism and the feasible treatment targets in the intermediate phase of SCI. We downloaded GSE2599 from GEO and identified 416 significant differentially expressed genes (DEGs), including 206 downregulated and 210 upregulated DEGs. Further enrichment analysis of DEGs revealed that many important biological processes and signal pathways were triggered in the injured spinal cord. Furthermore, a protein-protein interaction (PPI) network was constructed and the top 10 high-degree hub nodes were identified. Furthermore, 27 predicted transcription factors (TFs) and 136 predicted motifs were identified. We then selected insulin-like growth factor 1 (IGF1) and its predicted transcription factor, transcription factor A, mitochondrial (TFAM) for further investigation. We speculated and preliminarily confirmed that TFAM may regulate gene transcription of IGF1 and effected alterations in the function recovery of rats after SCI. These findings together provide novel information that may improve our understanding of the pathophysiological processes during the intermediate phase of SCI.
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  • 文章类型: Journal Article
    宽带隙(WBG)钙钛矿可以通过调整带隙以克服单结钙钛矿太阳能电池(PSC)的Shockley-Queisser限制来构建具有窄带隙太阳能电池的串联电池。然而,WBG钙钛矿仍然遭受严重的非辐射载流子复合和大的开路电压损失。这里,我们使用原位光致发光(PL)测量来监测中间相的演变和结晶过程通过刀片涂层。我们报告了一种通过掺杂长碳链分子辛烷-1,8-二胺二氢碘化物(ODADI)来制造高效且稳定的WBG钙钛矿太阳能电池的策略。我们发现,ODADI掺杂不仅抑制了中间相,而且促进了刀片涂覆的1.67eVWBGFA0.7Cs0.25MA0.05Pb(I0.8Br0.2)3钙钛矿薄膜中钙钛矿的结晶和钝化缺陷。因此,冠军单结反向PSC提供的效率为22.06%和19.63%的0.07cm2和1.02cm2的有效面积,分别,通过刀片涂覆,这是WBGPSC中最高的PCE。未封装的器件在空气中表现出优异的稳定性,在恒定的AM1.5G照明下,在露天近500小时内保持其初始效率在最大功率点。所得的半透明WBG装置提供20.06%的高PCE,4端全钙钛矿串联器件的PCE为28.35%。本文受版权保护。保留所有权利。
    Wide bandgap (WBG) perovskite can construct tandem cells with narrow bandgap solar cells by adjusting the band gap to overcome the Shockley-Queisser limitation of single junction perovskite solar cells (PSCs). However, WBG perovskites still suffer from severe nonradiative carrier recombination and large open-circuit voltage loss. Here, this work uses an in situ photoluminescence (PL) measurement to monitor the intermediate phase evolution and crystallization process via blade coating. This work reports a strategy to fabricate efficient and stable WBG perovskite solar cells through doping a long carbon chain molecule octane-1,8-diamine dihydroiodide (ODADI). It is found that ODADI doping not only suppresses intermediate phases but also promote the crystallization of perovskite and passivate defects in blade coated 1.67 eV WBG FA0.7Cs0.25MA0.05Pb(I0.8Br0.2)3 perovskite films. As a result, the champion single junction inverted PSCs deliver the efficiencies of 22.06% and 19.63% for the active area of 0.07 and 1.02 cm2, respectively, which are the highest power conversion efficiencies (PCEs) in WBG PSCs by blade coating. The unencapsulated device demonstrates excellent stability in air, which maintains its initial efficiency at the maximum power points under constant AM 1.5G illumination in open air for nearly 500 h. The resulting semitransparent WBG device delivers a high PCE of 20.06%, and the 4-terminal all-perovskite tandem device delivers a PCE of 28.35%.
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  • 文章类型: Journal Article
    准2D钙钛矿作为光伏器件显示出巨大的潜力,具有优越的稳定性,但是功率转换效率(PCE)受限于较差的载波传输。这里,通过将吡啶基材料掺入聚(3,4-亚乙基二氧噻吩):聚苯乙烯磺酸盐(PEDOT:PSS)中同时影响空穴传输层(HTL)和钙钛矿层,以解决上述2D钙钛矿中的关键问题。通过这种方法,新型PEDOT:PSS的增强的光电性能是由于添加剂与PEDOT或PSS之间的电子转移,以及基于实验和理论研究的PEDOT和PSS之间的分离,这有利于电荷提取和转移。同时,原位X射线散射研究表明,吡啶基分子的引入改变了钙钛矿中间相的转化过程,导致Pb─N化学桥引起的择优取向和有序分布,实现高效的电荷传输。因此,吡啶处理的器件实现了超过17%的增加的短路电流密度(Jsc)和PCE。
    Quasi-2D perovskites show great potential as photovoltaic devices with superior stability, but the power conversion efficiency (PCE) is limited by poor carrier transport. Here, it is simultaneously affected the hole transport layer (HTL) and the perovskite layer by incorporating pyridine-based materials into poly(3,4-ethylenedioxythiophene): polystyrene sulfonate (PEDOT:PSS) to address the key problem above in 2D perovskites. With this approach, the enhanced optoelectronic performance of the novel PEDOT:PSS is due to electron transfer between the additives and PEDOT or PSS, as well as a dissociation between PEDOT and PSS based on experimental and theoretical studies, which facilitates the charge extraction and transfer. Concurrently, in-situ X-ray scattering studies reveal that the introduction of pyridine-based molecules alters the transformation process of the perovskite intermediate phase, which leads to a preferred orientation and ordered distribution caused by the Pb─N chemical bridge, achieving efficient charge transport. As a result, the pyridine-treated devices achieve an increased short-circuit current density (Jsc) and PCE of over 17%.
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  • 文章类型: Journal Article
    反溶剂工程通常用于调节钙钛矿膜的结晶,因为它们可以为成核提供额外的驱动力。事实上,反溶剂对成核的干预被认为涉及一些相对快速和复杂的过程,which,然而,到目前为止还没有完全理解。这里,通过计算流体动力学(CFD)模型模拟了有机胺阳离子FA(一种占主导地位的前体)的扩散及其在旋涂过程中在不同反溶剂中的分布。建议适度的扩散速率(就像甲苯作为反溶剂的情况一样)不仅可以在基材上形成非常均匀的FA离子分布,有利于中间相的均匀成核,而且还可以平衡中间相的成核和生长速率,从而抑制不期望的异质成核和生长。结果表明,以甲苯为反溶剂制备的钙钛矿薄膜具有较高的质量,在此基础上,钙钛矿太阳能电池实现了高达24.32%的更高的功率转换效率。
    Antisolvent engineering is routinely used to modulate the crystallization of perovskite films as they can offer an additional driving force for nucleation. Actually, the intervention of antisolvent into nucleation is thought to involve some relatively fast and complex processes, which, however, are not fully understood so far. Here, the diffusion of the organic amine cation FA+ (one dominated precursor) and its distribution in a spin-coating process in different antisolvents is simulated by the computational fluid dynamics (CFD) model. It is suggested that a moderate diffusion rate (like that in the case of toluene as an antisolvent) not only enables to form a very uniform distribution of FA+ ions on the substrate, beneficial to the uniform nucleation of the intermediate phase, but also can balance the nucleation and growth rates of the intermediate phase, thereby suppressing undesired heterogeneous nucleation and growth. Results show that the perovskite film fabricated using toluene as an antisolvent has a high quality, based on which higher power conversion efficiencies of up to 24.32% are achieved for perovskite solar cells.
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  • 文章类型: Journal Article
    光滑致密的光吸收层是多晶太阳能电池实现高光伏性能的重要因素,虽然在钙钛矿太阳能电池中仍然具有挑战性,因为难以平衡晶体成核和生长的速度。这里,我们通过操纵正己胺(NHA)分子诱导的中间复合物,探索了钙钛矿成核/生长相容模型,指导我们调整钙钛矿成核和生长过程。我们发现NHA可以充当类似变速箱的分子,以依次降低钙钛矿成核屏障,促进成核速度,同时延缓钙钛矿生长,获得均匀的钙钛矿薄膜;相应地,这种调制还产生具有较少空隙和低缺陷密度的掩埋界面。此外,具有长烷基链的疏水性NHA提高了钙钛矿的耐湿性。经处理的太阳能电池功率转换效率为21.91%。重要的是,在25°C的70%湿度下持续30天,设备的效率下降不到5%,表现出良好的稳定性能。
    The smooth and dense light-absorbing layer is an essential factor in polycrystalline solar cells to achieve high photovoltaic performance, while it remains challenging in perovskite solar cells because of the difficulty balancing the speed of crystal nucleation and growth in a solution way. Here, we explored a perovskite nucleation/growth compatible model via manipulating the intermediate complex induced by n-hexylamine (NHA) molecule, guiding us to adjustments perovskite nucleation and growth process. We found that the NHA can act as a gearbox-like molecule to sequentially reduce the perovskite nucleation barrier, promote the nucleation velocity, and retard the perovskite growth simultaneously to obtain uniform perovskite films; correspondingly, this modulation also yields the buried interface with fewer voids and low defects density. In addition, the hydrophobic NHA with long alkyl chain improves the moisture tolerance of the perovskite. The treated solar cell power conversion efficiency was 21.91 %. Importantly, in ∼ 70 % humidity at 25 °C for 30 days, the efficiency of the device declined less than 5 %, exhibiting a good stability performance.
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  • 文章类型: Journal Article
    具有3DLi+扩散通道的尖晶石Mn基阴极,高电压,和低成本显示出开发高功率锂离子电池(LIB)的前景。但是不成比例和Jahn-Teller扭曲导致结构退化和容量衰减,特别是在高工作温度下。在这里,考虑到单晶的优点和暴露晶面的取向,单晶截头八面体LiMn2O4(TO-LMO),露出{111},{100}和{110}方面设计合理,其中主要暴露的{111}面被{100}和{110}面的一小部分截断。创新性地提出了缺锂中间相制备单晶TO-LMO。单晶的协同作用和暴露的晶面的取向显着减少了Mn3离子的歧化,从而提高了它们的结构稳定性。因此,单晶TO-LMO的循环稳定性显著增强,在2000次循环后获得84.3%的出色容量保留,八面体LiMn2O4的61.2%要好得多。用裸露的{111}制备单晶截头八面体LiNi0.5Mn1.5O4的可行性,{100},和{110}方面通过锂缺乏的中间相被进一步证明。这些发现为调节暴露晶面的取向和改善LIB中Mn基氧化还原对的可逆性提供了新的见解。
    The spinel Mn-based cathodes with 3D Li+ diffusion channels, high voltage, and low-cost show promise for developing high-power lithium-ion batteries (LIBs). But the disproportionation and Jahn-Teller distortion lead to structural degeneration and capacity decay, especially at high working temperatures. Herein, considering the merits of single crystals and orientation of exposed crystal planes, single-crystal truncated octahedral LiMn2 O4 (TO-LMO) with exposed {111}, {100} and {110} facets is rationally designed, in which the mainly exposed {111} facets are truncated by a small portion of {100} and {110} facets. The Li-deficient intermediate phase is innovatively proposed to prepare the single-crystal TO-LMO. The synergistic effects of single crystals and the orientation of exposed crystal planes significantly reduce the disproportionation of Mn3+ ions and thereby improve their structural stability. Consequently, the cycling stability of the single-crystal TO-LMO is remarkably enhanced, obtaining outstanding capacity retention of 84.3% after 2000 cycles, much better than that of 61.2% for octahedral LiMn2 O4 . The feasibility of preparing single-crystal truncated octahedral LiNi0.5 Mn1.5 O4 with exposed {111}, {100}, and {110} facets via the Li-deficient intermediate phase is further demonstrated. These findings offer new insight into regulating the orientation of exposed crystal planes and improving the reversibility of Mn-based redox couples in LIBs.
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  • 文章类型: Journal Article
    铪酸铅(PbHfO3)由于其作为反铁电(AFE)储能材料的潜力而引起了很多新的兴趣。然而,它的室温(RT)储能性能尚未得到很好的确立,也没有关于其高温中间相(IM)储能特性的报告。在这项工作中,通过固态合成路线制备了高质量的PbHfO3陶瓷。根据高温X射线衍射数据,发现PbHfO3的IM是正交的,Imma空间群,Pb2+离子沿[001]立方方向反平行排列。PbHfO3的极化-电场(P-E)关系在RT以及IM的温度范围内显示。典型的AFE回路显示出最佳的可恢复储能密度(Wrec)为2.7J/cm3,比报告的数据高286%,在RT下235kV/cm时效率(η)为65%。在190°C下发现0.7J/cm3的相对高的Wrec值,在65kV/cm下的η为89%。这些结果表明,从RT到200°C,PbHfO3是典型的AFE,使其成为在宽温度范围内储能应用的合适材料。
    Lead hafnate (PbHfO3) has attracted a lot of renewed interest due to its potential as antiferroelectric (AFE) material for energy storage. However, its room temperature (RT) energy-storage performance has not been well established and no reports on the energy-storage feature of its high-temperature intermediate phase (IM) are available. In this work, high-quality PbHfO3 ceramics were prepared via the solid-state synthesis route. Based on high-temperature X-ray diffraction data, the IM of PbHfO3 was found to be orthorhombic, Imma space group, with antiparallel alignment of Pb2+ ions along the [001]cubic directions. The polarization-electric field (P-E) relation of PbHfO3 is displayed at RT as well as in the temperature range of the IM. A typical AFE loop revealed an optimal recoverable energy-storage density (Wrec) of 2.7 J/cm3, which is 286% higher than the reported data with an efficiency (η) of 65% at 235 kV/cm at RT. A relatively high Wrec value of 0.7 J/cm3 was found at 190 °C with an η of 89% at 65 kV/cm. These results demonstrate that PbHfO3 is a prototypical AFE from RT up to 200 °C, making it a suitable material for energy-storage applications in a wide temperature range.
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  • 文章类型: Journal Article
    全无机CsPbI3钙钛矿由于其高热稳定性和适合串联器件的带隙而成为重要的光伏材料。目前,CsPbI3太阳能电池的电池性能主要受到大的开路电压(VOC)亏空的影响。在这里,一种多功能的室温熔盐,证明了乙酸二甲胺(DMAAc),它不仅直接充当前体溶液的溶剂,而且还调节了用于高效光伏的CsPbI3薄膜的相转换过程。DMAAc可以稳定DMAPbI3结构,消除Cs4PbI6中间相,很容易在空间上隔离。同时,一种新的均匀中间相DMAPb(I,Ac)3已形成,最终提供高质量的CsPbI3薄膜。通过这种方法,CsPbI3膜中缺陷的电荷捕获活性被显著抑制。因此,实现了1.25V的VOC和>21%的功率转换效率,这是迄今为止报道的最高记录。这种中间相位调节策略被认为适用于其他钙钛矿材料系统。
    All-inorganic CsPbI3 perovskite has emerged as an important photovoltaic material due to its high thermal stability and suitable bandgap for tandem devices. Currently, the cell performance of CsPbI3 solar cells is mainly subject to a large open-circuit voltage (VOC ) deficit. Herein, a multifunctional room-temperature molten salt, dimethylamine acetate (DMAAc) is demonstrated, which not only directly acts as a solvent for precursor solutions, but also regulates the phase conversion process of the CsPbI3 film for high-efficiency photovoltaics. DMAAc can stabilize the DMAPbI3 structure and eliminate the Cs4 PbI6 intermediate phase, which is easily spatially segregated. Meanwhile, a new homogeneous intermediate phase DMAPb(I,Ac)3 is formed, which finally affords high-quality CsPbI3 films. With this approach, the charge capture activity of defects in the CsPbI3 film is significantly suppressed. Consequently, a VOC of 1.25 V and >21% power conversion efficiency are achieved, which is the record highest reported thus far. This intermediate phase-regulation strategy is believed to be applicable to other perovskite material systems.
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  • 文章类型: Journal Article
    Sn-Pb复合材料中甲基铵(MA)阳离子的完全消除可以扩展其光和热稳定性。不幸的是,无MA的Sn-Pb合金钙钛矿薄膜表面起皱,结晶不良,由于混合中间相的共存。这里,我们报告了一种添加剂策略,用于精细调节Cs0.25FA0.75Pb0.6Sn0.4I3和中间相中的杂质,因此,获得高性能太阳能电池。我们引入d-高丝氨酸内酯盐酸盐(D-HLH)与钙钛矿前体形成氢键和强Pb-O/Sn-O键,从而削弱极性非质子溶剂之间的不完全络合效应(例如,DMSO)和有机(FAI)或无机(CsI,PbI2和SnI2)组件,平衡它们的成核过程。在热退火之前,这种处理将混合的中间相完全转化为纯的预制钙钛矿核。此外,这种D-HLH基本上抑制了Sn2+物质的氧化。这一策略产生了创纪录的21.61%的效率,对于无MA的Sn-Pb器件,Voc为0.88V,其串联装置的效率为23.82%。
    The complete elimination of methylammonium (MA) cations in Sn-Pb composites can extend their light and thermal stabilities. Unfortunately, MA-free Sn-Pb alloyed perovskite thin films suffer from wrinkled surfaces and poor crystallization, due to the coexistence of mixed intermediate phases. Here, we report an additive strategy for finely regulating the impurities in the intermediate phase of Cs0.25FA0.75Pb0.6Sn0.4I3 and, thereby, obtaining high-performance solar cells. We introduced d-homoserine lactone hydrochloride (D-HLH) to form hydrogen bonds and strong Pb-O/Sn-O bonds with perovskite precursors, thereby weakening the incomplete complexation effect between polar aprotic solvents (e.g., DMSO) and organic (FAI) or inorganic (CsI, PbI2, and SnI2) components, and balancing their nucleation processes. This treatment completely transformed mixed intermediate phases into pure preformed perovskite nuclei prior to thermal annealing. Besides, this D-HLH substantially inhibited the oxidation of Sn2+ species. This strategy generated a record efficiency of 21.61%, with a Voc of 0.88 V for an MA-free Sn-Pb device, and an efficiency of 23.82% for its tandem device. The unencapsulated devices displayed impressive thermal stability at 85 °C for 300 h and much improved continuous operation stability at MPP for 120 h.
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  • 文章类型: Journal Article
    基于碳的介观钙钛矿太阳能电池(MPSC)由于其较低的制造成本和优异的稳定性而成为最具竞争力的光伏技术之一。在这项工作中,甲基乙酸铵(MAAc),离子液体添加剂,将其添加到甲基铵三碘化铅(MAPbI3)钙钛矿中,并用于制造高性能MPSC。系统和详细的研究表明,MAAc优先与PbI2相互作用,形成MAPbI3-x(Ac)x中间相,可以有效控制三介观层中MAPbI3的结晶动力学。具有适量MAAc的MAPbI3薄膜表现出更高的结晶度,较低的缺陷密度,和致密的孔隙填充,能有效减少MPSCs中载体非辐射重组的损失。因此,基于优化的MAAc工程MPSC获得13.54%的冠军功率转换效率(PCE)。PCE比控制设备的10.90%高24%。此外,未封装的MAAc工程MPSCs在黑暗环境下储存50天后保留了90%的初始PCE,这表明比控制设备更好的空气稳定性。这项工作为开发具有生态友好型离子液体添加剂的高效和稳定的碳基MPSCs提供了有效的策略。
    Carbon-based mesoscopic perovskite solar cells (MPSCs) are becoming one of the most competitive photovoltaic technologies owing to their lower manufacturing cost and excellent stability. In this work, methylammonium acetate (MAAc), an ionic liquid additive, is added into methylammonium lead triiodide (MAPbI3) perovskite and is used to fabricate high-performance MPSCs. Systematic and detailed studies have shown that the MAAc interacts with PbI2 preferentially to form a MAPbI3-x(Ac)x intermediate phase that can effectively control the crystallization kinetics of MAPbI3 in the triple-mesoscopic layer. MAPbI3 films with an appropriate amount of MAAc exhibit higher crystallinity, lower defect density, and dense pore filling, which effectively reduce carrier non-radiative recombination loss in MPSCs. As a result, a champion power conversion efficiency (PCE) of 13.54% is obtained based on the optimized MAAc-engineered MPSCs. The PCE is 24% higher than 10.90% of the control devices. Moreover, unencapsulated MAAc-engineered MPSCs retain 90% of their initial PCE after being stored in the dark for 50 days under ambient atmosphere, which demonstrates much better air stability than control devices. This work provides an effective strategy for developing efficient and stable carbon-based MPSCs with an eco-friendly ionic liquid additive.
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