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Remembering the Old Propensity Rules of the Electromagnetic Enhancement Mechanism of SERS: Reorientation of Pyridine on a Silver Electrode Induced by the Applied Potential 牢记 SERS 电磁增强机制的旧倾向规则:应用电位诱导吡啶在银电极上重新定向
IF 4.126 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-19 DOI: 10.1021/acs.jpcc.4c03084
Samuel Valdivia, Francisco García-González, Daniel Aranda, Francisco J. Ávila Ferrer, Isabel López-Tocón, Juan Soto, Juan Carlos Otero
Electrochemical SERS of pyridine adsorbed on a silver electrode has been analyzed by comparing the spectra to the calculated normal Raman and resonance Raman intensities of model systems of pyridine bonded to linear silver clusters with different densities of charge through the nitrogen (Ag-NPy) or flipped through the hydrogen in the para-position (Ag-HPy). The changes observed in the ν(CH) region of the SERS have been investigated for the first time and related to a molecular reorientation at negative surface excess of charge of the metal in such a way that the ν(CH) bands with the highest (mode 2) and lowest (mode 13) wavenumber dominate this spectral region at positive or negative electrode potentials, respectively. The calculations support that the ν(CH) region is dominated by a specific vibration depending on pyridine orientation and suggest that both species coexist in the SERS recorded at negative potentials. This conclusion is supported by the SERS of centrosymmetric pyrazine which do not show this behavior and remembers the predictions from the old propensity rules of the so-called electromagnetic mechanism of SERS.
通过将吸附在银电极上的吡啶的光谱与通过氮键(Ag-NPy)或通过对位氢键(Ag-HPy)与线性银簇键合的吡啶模型系统的计算正常拉曼强度和共振拉曼强度进行比较,分析了吡啶的电化学 SERS。我们首次研究了在 SERS 的 ν(CH)区域观察到的变化,这些变化与金属负表面过量电荷时的分子重新定向有关,因此在电极电位为正或负时,具有最高(模式 2)和最低(模式 13)文波数的ν(CH)带分别主导该光谱区域。计算结果表明,ν(CH) 区域主要由吡啶取向所决定的特定振动所支配,并表明在负电位时记录的 SERS 中两种物质共存。这一结论得到了吡嗪中心对称 SERS 的支持,因为吡嗪中心对称的 SERS 并没有显示出这种行为,这也让人想起了所谓 SERS 电磁机制的旧倾向规则的预测。
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引用次数: 0
Fourier Law Fidelity Contrasted by Infrared Imaging as Heat Flows through Metals and Polymers 热量流经金属和聚合物时的红外成像对比傅立叶定律保真度
IF 4.126 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-19 DOI: 10.1021/acs.jpcc.4c02759
Kaikai Zheng, Steve Granick
Using a home-built imaging system to map by infrared detection the surface temperature of a metallic material, we fail to confirm the generality of previously reported deviations, for translucent polymers and quartz, from Fourier’s law at the macroscale. This discrepancy is explained by the fact that unlike polymers and quartz, metals are optically opaque. Comparing the environments of air and vacuum quantitatively, we show the advantage of the latter environment. Of special interest is that thermal gradients reveal surface features otherwise concealed under uniform temperature conditions. Our findings not only confirm the classical heat conduction model for metal but also highlight the often-overlooked impact of material optical properties on thermal behavior.
我们利用自制的成像系统,通过红外探测绘制了金属材料的表面温度图,但未能证实之前报道的半透明聚合物和石英在宏观尺度上偏离傅里叶定律的普遍性。造成这种差异的原因是,与聚合物和石英不同,金属在光学上是不透明的。通过定量比较空气和真空环境,我们发现后者的优势。特别令人感兴趣的是,热梯度揭示了在均匀温度条件下被掩盖的表面特征。我们的研究结果不仅证实了金属的经典热传导模型,还强调了经常被忽视的材料光学特性对热行为的影响。
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引用次数: 0
Characterizing Joule Heating Effects on Single Suspended Carbon Fibers: Calculating the Temperature Coefficient of Resistance for Localized Carbon Nanotube Growth 描述单根悬浮碳纤维的焦耳加热效应:计算局部碳纳米管生长的电阻温度系数
IF 4.126 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-19 DOI: 10.1021/acs.jpcc.4c01116
Sura Nguyen, Alejandro Montesinos-Castellanos, Marc J. Madou, Sergio O. Martínez-Chapa, Nancy Ornelas-Soto, Claudia B. Flores, Arnoldo Salazar
This work investigates the impact of Joule heating (JH) on single suspended carbon fibers (CFs) and their role in facilitating the growth of carbon nanotubes (CNTs) on the surface of the fiber. The key innovation lies in identifying specific temperature thresholds linked to observable phenomena on the CFs during Joule heating. These observations allowed us to make reasonable estimations, in real time, of the temperatures on the CFs. Our method was validated by using the obtained temperature information to grow CNTs localized to the surface of a single suspended CF. Raman analysis confirms improved structural quality after JH, and the resulting hybrid CNTs/CF exhibit an increased maximum electrical conductivity of 476 S/cm, demonstrating the potential applications of this technique in the development of high-performance carbon devices.
这项工作研究了焦耳加热(JH)对单根悬浮碳纤维(CF)的影响,以及它们在促进碳纳米管(CNT)在纤维表面生长方面的作用。关键的创新在于确定了焦耳加热过程中与碳纤维上可观察到的现象相关的特定温度阈值。这些观察结果使我们能够实时合理地估计 CF 上的温度。我们利用获得的温度信息,在单个悬浮 CF 表面局部生长 CNT,从而验证了我们的方法。拉曼分析证实了 JH 后结构质量的改善,由此产生的混合碳纳米管/碳化纤维的最大电导率提高到了 476 S/cm,证明了该技术在开发高性能碳器件方面的潜在应用。
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引用次数: 0
Investigating Static–Dynamic Heterogeneities and Enhanced Charge-Separation in CdS QDs with a Phenothiazine-Based Donor−π–Acceptor (D−π–A) Molecular System 利用基于吩噻嗪的供体-π-受体(D-π-A)分子体系研究 CdS QD 中的静态-动态异质性和增强的电荷分离功能
IF 4.126 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-18 DOI: 10.1021/acs.jpcc.4c01856
Malay Krishna Mahato, Soumi Roy, Edamana Prasad
The majority of the analysis of the interfacial hole-transfer process in QD-phenothiazine-based molecular systems has focused on cases where the acceptor moiety is either physisorbed or covalently attached to the QDs’ surface. However, the role of a dynamic hole-acceptor moiety at the interface in facilitating the hole-transfer process is not well understood yet. To address this, a detailed photophysical study of CdS QDs was conducted in the presence of a phenothiazine-based donor−π–acceptor (D−π–A) molecular system (S2), at varied temperatures and concentrations, using steady-state and time-resolved spectroscopy. The charge-separation process in the excited state was explored using transient absorption analysis, which revealed that the hole-transfer process occurred within 3.04 ps, while the charge-separated state relaxed to the ground state over nanoseconds, indicating the presence of a long-lived charge-separated species. Results taken together indicate that the hole-transfer mechanism in the QD–S2 system at higher concentrations of S2 can be achieved through an apparent static model, whereas the same might happen in a dynamic fashion at lower concentrations. The mechanism of charge transfer dynamics has been proposed to account for the kinetics obtained from the time-resolved spectroscopy experiments. The findings of this study are expected to advance the design of efficient photovoltaic and photocatalytic cells for clean energy research.
对基于 QD-吩噻嗪分子体系的界面空穴传输过程的分析大多集中在受体分子物理吸附或共价连接到 QD 表面的情况。然而,人们对界面上的动态空穴受体分子在促进空穴传输过程中的作用还不甚了解。为了解决这个问题,我们利用稳态和时间分辨光谱法,在不同温度和浓度下,在基于吩噻嗪的供体-π-受体(D-π-A)分子体系(S2)存在下,对 CdS QDs 进行了详细的光物理研究。利用瞬态吸收分析探究了激发态的电荷分离过程,结果表明空穴传输过程发生在 3.04 ps 内,而电荷分离态则在纳秒级的时间内弛豫到基态,这表明存在长寿命的电荷分离物种。这些结果综合表明,在 S2 浓度较高的 QD-S2 系统中,空穴传输机制可以通过明显的静态模型实现,而在浓度较低时,则可能以动态方式发生。我们提出了电荷转移动力学机制,以解释时间分辨光谱实验所获得的动力学。这项研究的发现有望推动高效光伏电池和光催化电池的设计,从而促进清洁能源研究。
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引用次数: 0
Evidence of Superionic Na+ Conductivity in Partially Hydrolyzed NaBH4 部分水解 NaBH4 中超离子 Na+ 传导性的证据
IF 4.126 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-18 DOI: 10.1021/acs.jpcc.4c01191
Xiaoxuan Luo, Aditya Rawal, Kondo-Francois Aguey-Zinsou
Sodium borohydride (NaBH4) has been found to display superionic Na+ conductivity upon partial oxidation. Herein, by controlling the hydrolysis of NaBH4 and by thermally stabilizing the oxide phase formed, i.e., NaB(OH)4, Na+ ionic conductivity increased from ∼10–10 S cm–1 for unmodified NaBH4 to 2.2 × 10–5 S cm–1 at room temperature and 2.6 × 10–3 S cm–1 at 75 °C for hydrolyzed NaBH4. More remarkably, this approach allowed for a comprehensive multidimensional 23Na–1H and 11B–1H solid-state NMR analysis and determination of the interplay between pristine α-NaBH4 and NaB(OH)4 in leading to high Na+ ionic conductivity. Not only NMR analysis confirmed that the superionic behavior observed in partially hydrolyzed NaBH4 was the result of Na+ hopping, but 2D NMR also revealed that the hopping mechanism was the result of the formation of a highly defective structure at the α-NaBH4/NaB(OH)4 interface, leading to high Na+ conductivity. Given the simplicity of the oxidation process reported here, this finding opens novel and facile methodologies for the development of promising solid-state electrolytes for sodium-based batteries.
研究发现,硼氢化钠(NaBH4)在部分氧化后会显示出超离子 Na+ 导电性。在这里,通过控制 NaBH4 的水解和热稳定所形成的氧化物相(即 NaB(OH)4),Na+ 离子电导率从未修改的 NaBH4 的 ∼10-10 S cm-1 增加到室温下的 2.2 × 10-5 S cm-1,以及水解的 NaBH4 在 75 °C 时的 2.6 × 10-3 S cm-1。更值得注意的是,这种方法允许进行全面的多维 23Na-1H 和 11B-1H 固态核磁共振分析,并确定原始 α-NaBH4 和 NaB(OH)4 在导致高 Na+ 离子电导率方面的相互作用。核磁共振分析不仅证实了在部分水解的 NaBH4 中观察到的超离子行为是 Na+ 跳跃的结果,而且二维核磁共振还揭示了跳跃机制是在α-NaBH4/NaB(OH)4 界面形成高度缺陷结构的结果,从而导致高 Na+ 导电性。鉴于本文报告的氧化过程非常简单,这一发现为钠基电池固态电解质的开发开辟了新颖而简便的方法。
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引用次数: 0
Platinum Nanoparticle Formation Kinetics and Mechanistic Studies: Evidence for an Alternative 4-Step Mechanism Involving Size-Dependent Growth and Chloride Anion and Room-Dust-Dependent Nucleation 铂纳米粒子形成动力学和机理研究:尺寸依赖性生长和氯阴离子及室尘依赖性成核的另一种四步机制的证据
IF 4.126 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-18 DOI: 10.1021/acs.jpcc.4c02718
Luke T. MacHale, Christopher B. Whitehead, Richard G. Finke
Platinum nanoparticles (NPs) are utilized extensively in myriad applications ranging from biotechnology and optoelectronics to industrial catalysis. However, precise control over their particle size, size distribution, and shape remains reliant on empirical approaches rather than on the desired kinetics, mechanism-based insight, and associated differential equations. The present study examines the synthesis and underlying mechanism of Pt NPs, emphasizing a second-generation system addressing the previously ill-defined nucleation rate constant (k1) and its previous large (108) uncertainty. After testing nine pseudoelementary step mechanisms in the second-generation synthesis system, the best-fitting mechanism is found to be an alternative 4-step mechanism, X = PtII, as shown in the table-of-content graphic. That mechanism differs from the previously established, classic 4-step mechanism by replacing size-dependent aggregation (X = Pt0n) with size-dependent autocatalytic surface growth (X = PtII). Importantly, employing the alternative 4-step mechanism results in a 107 reduction in the uncertainty of k1, thereby providing one line of evidence for that mechanism. The second-generation system and its kinetics also reveal a strong chloride anion-dependent slowing of the nucleation step as well as microfiltration-based evidence for room-dust-dependent─and hence heterogeneous─nucleation. As such, the present study and its disproof-based approach to the minimalistic Pt0n NP formation mechanism advance our knowledge of Pt0n NP syntheses and their condition- and impurity-dependent mechanisms.
铂纳米粒子(NPs)被广泛应用于从生物技术、光电子学到工业催化等众多领域。然而,对其粒度、粒度分布和形状的精确控制仍然依赖于经验方法,而不是所需的动力学、基于机理的洞察力和相关的微分方程。本研究考察了铂氮氧化物的合成和基本机理,强调采用第二代系统来解决以前定义不清的成核速率常数 (k1) 及其以前的巨大不确定性 (108)。在第二代合成系统中测试了九个伪元素步骤机制后,发现最佳拟合机制是另一种四步骤机制,即 X = PtII,如内容表图形所示。该机制与之前建立的经典 4 步机制不同,它将尺寸依赖性聚集(X = Pt0n)替换为尺寸依赖性自催化表面生长(X = PtII)。重要的是,采用替代的 4 步机制后,k1 的不确定性降低了 107,从而为该机制提供了一条证据线。第二代系统及其动力学还揭示了成核步骤的减慢与氯阴离子的强相关性,以及基于微过滤的室内粉尘依赖性--从而异质--成核的证据。因此,本研究及其基于反证的最小化 Pt0n NP 形成机制的方法,增进了我们对 Pt0n NP 合成及其与条件和杂质有关的机制的了解。
{"title":"Platinum Nanoparticle Formation Kinetics and Mechanistic Studies: Evidence for an Alternative 4-Step Mechanism Involving Size-Dependent Growth and Chloride Anion and Room-Dust-Dependent Nucleation","authors":"Luke T. MacHale, Christopher B. Whitehead, Richard G. Finke","doi":"10.1021/acs.jpcc.4c02718","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c02718","url":null,"abstract":"Platinum nanoparticles (NPs) are utilized extensively in myriad applications ranging from biotechnology and optoelectronics to industrial catalysis. However, precise control over their particle size, size distribution, and shape remains reliant on empirical approaches rather than on the desired kinetics, mechanism-based insight, and associated differential equations. The present study examines the synthesis and underlying mechanism of Pt NPs, emphasizing a second-generation system addressing the previously ill-defined nucleation rate constant (<i>k</i><sub>1</sub>) and its previous large (10<sup>8</sup>) uncertainty. After testing nine pseudoelementary step mechanisms in the second-generation synthesis system, the best-fitting mechanism is found to be an alternative 4-step mechanism, X = Pt<sup>II</sup>, as shown in the table-of-content graphic. That mechanism differs from the previously established, classic 4-step mechanism by replacing size-dependent aggregation (X = Pt<sup>0</sup><sub><i>n</i></sub>) with size-dependent autocatalytic surface growth (X = Pt<sup>II</sup>). Importantly, employing the alternative 4-step mechanism results in a 10<sup>7</sup> reduction in the uncertainty of <i>k</i><sub>1</sub>, thereby providing one line of evidence for that mechanism. The second-generation system and its kinetics also reveal a strong chloride anion-dependent slowing of the nucleation step as well as microfiltration-based evidence for room-dust-dependent─and hence heterogeneous─nucleation. As such, the present study and its disproof-based approach to the minimalistic Pt<sup>0</sup><i><sub>n</sub></i> NP formation mechanism advance our knowledge of Pt<sup>0</sup><i><sub>n</sub></i> NP syntheses and their condition- and impurity-dependent mechanisms.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":null,"pages":null},"PeriodicalIF":4.126,"publicationDate":"2024-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141726392","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Microscopic Structure and Dynamic Study in Amorphous InGaZnO Focusing on Oxygen-Centered Complex 以氧中心络合物为重点的非晶 InGaZnO 微观结构与动力学研究
IF 4.126 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-18 DOI: 10.1021/acs.jpcc.4c02162
Minhwan Lee, Juho Lee, Sungduk Hong, Sung Jin Kim, Dae Sin Kim
Amorphous InGaZnO (a-IGZO) has been widely studied for its excellent electrical properties and stable amorphous structure, making it suitable for various electrical devices. Using molecular dynamics simulations, we investigated its subnanoscale structure and dynamics, especially focusing on O atoms and its local environment. A previously developed force field was used for all-atomic simulations, allowing us to study various oxygen-centered complexes (OCCs). We analyzed the coordination structures using radial distribution functions and nearest neighbor analysis to identify the characteristics of each metal element when it was coordinated with the O atoms. The OCCs were categorized, and their populations and compositions were investigated. The lifetimes of the OCCs were calculated as a function of temperature, providing insights into their stability. The conditional probabilities of the OCC transitions were calculated, identifying two distinct groups based on the presence or absence of another O atom. Differences in the dynamics of the O atoms within these groups were observed, where O atoms with another O atom in complexes exhibit faster speeds and larger mean squared displacements. These findings contribute to a deeper understanding of a-IGZO’s fundamental properties and potential applications in electronic devices such as DRAM and displays.
非晶 InGaZnO(a-IGZO)因其优异的电气性能和稳定的非晶结构而被广泛研究,使其适用于各种电气设备。我们利用分子动力学模拟研究了它的亚纳尺度结构和动力学,尤其关注 O 原子及其局部环境。我们使用之前开发的力场进行全原子模拟,从而研究了各种氧中心络合物(OCC)。我们利用径向分布函数和近邻分析对配位结构进行了分析,以确定每个金属元素与 O 原子配位时的特征。我们对 OCC 进行了分类,并研究了它们的数量和组成。计算了 OCC 的寿命与温度的函数关系,从而深入了解了它们的稳定性。计算了 OCC 转变的条件概率,根据是否存在另一个 O 原子确定了两个不同的组别。在这些组中观察到了 O 原子的动力学差异,在复合物中含有另一个 O 原子的 O 原子显示出更快的速度和更大的平均平方位移。这些发现有助于深入了解 a-IGZO 的基本特性以及在 DRAM 和显示器等电子设备中的潜在应用。
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引用次数: 0
Effects of Strain on Diborane Dissociative Adsorption and Boron Incorporation on Si0.5Ge0.5(001)-2 × 1 Surfaces 应变对 Si0.5Ge0.5(001)-2 × 1 表面二硼烷离解吸附和硼掺杂的影响
IF 4.126 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-17 DOI: 10.1021/acs.jpcc.4c03110
Gianluca Rengo, Geoffrey Pourtois, Clement Porret, Roger Loo, André Vantomme
This study investigates the surface reaction pathway of the diborane dissociative adsorption on the Si0.5Ge0.5(001)-2 × 1 surface by using density functional theory. The impact of biaxial strain on the kinetics and thermodynamics of the reactions and on the subsequent boron incorporation in the lattice is additionally evaluated. The strain affects both the thermodynamic drive for boron incorporation and the activation energies of surface reactions involving BH3 fragments. Specifically, as the strain changes from compressive to tensile, the energy barrier for BH3 dissociation on the surface progressively increases, resulting in a rate reduction of the B adsorption process. Concurrently, the driving force for incorporating B atoms into the first atomic layers of the surface decreases, reducing the probability of its occurrence. The reported mechanisms are studied on two different surface models, either having a Si or a Ge subsurface atomic layer. The simulations on these two surface configurations reveal that the embedding of B atoms is favored in substitutional sites with larger numbers of Si nearest-neighbors.
本研究利用密度泛函理论研究了二硼烷在 Si0.5-Ge0.5(001)-2×1 表面离解吸附的表面反应途径。此外,还评估了双轴应变对反应动力学和热力学的影响,以及对随后晶格中硼键合的影响。应变既影响硼加入的热力学驱动力,也影响涉及 BH3 片段的表面反应的活化能。具体来说,当应变从压缩变为拉伸时,BH3 在表面解离的能量势垒逐渐增加,导致硼吸附过程的速率降低。与此同时,将 B 原子吸附到表面第一原子层的驱动力也会减小,从而降低其发生的概率。所报告的机制是在两种不同的表面模型上进行研究的,这两种表面模型都有一个 Si 或一个 Ge 亚表面原子层。对这两种表面构型的模拟显示,B 原子的嵌入更倾向于硅近邻数目较多的置换位点。
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引用次数: 0
Interfacial Degradation Analysis via the Combined In Situ Method of Gas Monitoring and Electrochemical Impedance Spectroscopy upon Fast-Aging Cycling at 45 °C 通过气体监测和电化学阻抗光谱原位结合法分析 45 °C 快速老化循环过程中的界面降解情况
IF 4.126 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-17 DOI: 10.1021/acs.jpcc.4c03471
Siqi Lyu, Jian Yu, Xiao-Hua Guo, Yufeng Meng, Meirong Gu, Xiaoxiao Huang, Zhenhe Feng, Tao Geng, Hao-Sen Chen, Wei-Li Song, Shuqiang Jiao
In situ analysis methods have been widely developed to investigate the degradation of high-energy density lithium-ion batteries with NMC811 as a positive electrode. The in situ/operando monitoring method is based on sensors, and impedance is an effective strategy for detecting electrolyte-related gas and interface variations upon cycling. However, the correlation between the liquid and solid interface variation with gas evolution and battery degradation during operation remains ambiguous. To understand such a relationship, we developed the combined in situ method of gas monitoring and electrochemical impedance spectra (EIS) to study the NMC811 materials coated with Al2O3 and borides. The operando gas evolution analysis indicates that CO2 and CO related to electrolyte decomposition show similar evolution behavior during cycling, which is opposite to that of H2 and CH4. The increase of resistance via in situ EIS analysis implies that interface degradation leads to changes in the ratios of CO2 to CO and CO2 to H2. The compositional variation of the interfaces via X-ray photoelectron spectroscopy (XPS) depth profiling suggests that aluminum shuttled to the negative electrode within the Li-ion batteries (LIBs) assembled with U-Al/B-NMC and prevents the interface from degradation, forming stable inorganic species, i.e., LiF and Li2O. This work provides a novel in situ/operando method to analyze the relationship between interface variation, gas evolution, and battery degradation.
为了研究以 NMC811 为正极的高能量密度锂离子电池的降解情况,人们广泛开发了原位分析方法。原位/运行监测方法以传感器为基础,阻抗是检测循环过程中与电解质相关的气体和界面变化的有效策略。然而,液态和固态界面变化与气体演化和电池在运行过程中的降解之间的相关性仍不明确。为了了解这种关系,我们开发了气体监测和电化学阻抗谱(EIS)的原位组合方法,以研究涂有 Al2O3 和硼化物的 NMC811 材料。操作气体演化分析表明,与电解质分解有关的 CO2 和 CO 在循环过程中表现出相似的演化行为,这与 H2 和 CH4 的演化行为相反。通过原位 EIS 分析发现的电阻增加意味着界面降解导致 CO2 与 CO 和 CO2 与 H2 的比例发生变化。通过 X 射线光电子能谱(XPS)深度剖面分析得出的界面成分变化表明,铝穿梭到用 U-Al/B-NMC 组装的锂离子电池(LIB)的负极,阻止了界面降解,形成了稳定的无机物,即 LiF 和 Li2O。这项研究为分析界面变化、气体演化和电池降解之间的关系提供了一种新颖的原位/操作步骤方法。
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引用次数: 0
Concentric Structure of Coexistent KCl Core Solution and Water Adlayer Inside a Highly Hydrophobic Single-Wall Carbon Nanotube 高疏水性单壁碳纳米管内共存的氯化钾核心溶液和水外层的同心结构
IF 4.126 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-17 DOI: 10.1021/acs.jpcc.4c01944
Yuma Kawamata, Taku Iiyama, Ryusuke Futamura, Hayato Otsuka, Katsumi Kaneko
The concept of hydrated ions, which is described by the hydration number and the size of the hydrated ion determined with X-ray diffraction measurements, has contributed to understanding ionic solutions. However, we do not understand the effect of ions on the hydrogen-bonded quasi-tetrahedral (Td) clusters of H2O molecules and the beyond-hydrated ion structures, regardless of their crucial importance. The present study applied the intensive confinement effect of a highly hydrophobic single-wall carbon nanotube (SWCNT) to elucidate the correlation of ions with quasi-Td clusters and beyond-hydrated ion structures using KCl solution at 298 K. In situ X-ray diffraction revealed that the water structure confined inside the SWCNT was insensitive to the presence of ions confined in the SWCNT. The GCMC simulation studies showed the stably separated structure of the KCl solution in the central core and the adsorbed water layer akin to the graphene wall of the SWCNT. Newly clarified coexistence of the KCl solution and the water adlayer inside the SWCNT should give new insights into understanding localized heterogeneities in bulk ionic solutions.
水合离子的概念由水合数和通过 X 射线衍射测量确定的水合离子大小来描述,这一概念有助于人们理解离子溶液。然而,我们并不了解离子对 H2O 分子的氢键准四面体(Td)团簇和超水合离子结构的影响,尽管它们至关重要。本研究利用高疏水性单壁碳纳米管(SWCNT)的密集约束效应,在 298 K 的 KCl 溶液中阐明了离子与准 Td 簇和超水合离子结构的相关性。GCMC 模拟研究表明,KCl 溶液在中心管芯中的结构与吸附水层稳定分离,类似于 SWCNT 的石墨烯壁。澄清了氯化钾溶液和水吸附层在 SWCNT 内部共存的新情况,这将为理解块状离子溶液中的局部异质性提供新的视角。
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引用次数: 0
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The Journal of Physical Chemistry C
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