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Operando XANES Reveals the Chemical State of Iron-Oxide Monolayers During Low-Temperature CO Oxidation. Operando XANES 揭示了氧化铁单层在低温 CO 氧化过程中的化学状态。
IF 2.3 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-10-15 DOI: 10.1002/cphc.202400835
Dorotea Gajdek, Harald J Wallander, Giuseppe Abbondanza, Gary S Harlow, Johan Gustafson, Sara Blomberg, Per-Anders Carlsson, Justus Just, Edvin Lundgren, Lindsay R Merte

We have used grazing incidence X-ray absorption near edge spectroscopy (XANES) to investigate the behavior of monolayer FeO x ${_x }$ films on Pt(111) under near ambient pressure CO oxidation conditions with a total gas pressure of 1 bar. Spectra indicate reversible changes during oxidation and reduction by O 2 ${_2 }$ and CO at 150 °C, attributed to a transformation between FeO bilayer and FeO 2 ${_2 }$ trilayer phases. The trilayer phase is also reduced upon heating in CO+O 2 ${_2 }$ , consistent with a Mars-van-Krevelen type mechanism for CO oxidation. At higher temperatures, the monolayer film dewets the surface, resulting in a loss of the observed reducibility. A similar iron oxide film prepared on Au(111) shows little sign of reduction or oxidation under the same conditions. The results highlight the unique properties of monolayer FeO and the importance of the Pt support in this reaction. The study furthermore demonstrates the power of grazing-incidence XAFS for in situ studies of these model catalysts under realistic conditions.

我们使用掠入射 X 射线吸收近缘光谱 (XANES) 研究了 Pt(111) 上的单层 FeOx 薄膜在总气压为 1 巴的近环境压力 CO 氧化条件下的行为。光谱显示了在 150ºC 下被 O2 和 CO 氧化和还原过程中发生的可逆变化,这些变化归因于 FeO 双层相和 FeO2 三层相之间的转变。在 CO+O2 中加热时,三层相也会还原,这与 Mars-van-Krevelen 类型的 CO 氧化机制相一致。在较高温度下,单层膜表面会产生露珠,从而失去观察到的还原性。在相同条件下,在 Au(111)上制备的类似氧化铁薄膜几乎没有还原或氧化的迹象。这些结果凸显了单层氧化铁的独特性质以及铂支撑在该反应中的重要性。该研究进一步证明了掠入射 XAFS 在实际条件下对这些模型催化剂进行原位研究的能力。
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引用次数: 0
Front Cover: Disentangling Acid-Base Chemistry through Blue Shifting Hydrogen Bond Contributions (ChemPhysChem 20/2024) 封面:通过蓝移氢键贡献解析酸碱化学(ChemPhysChem 20/2024)
IF 2.3 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-10-15 DOI: 10.1002/cphc.202482001
John T. Kelly, Louis E. McNamara, William E. Gilbraith, Chelsea M. Goetzman, Megan E. Hoover, Robert J. Lascola

The Front Cover shows a complex relationship of acid–base chemistry in aqueous solutions. Here, Savannah River National Laboratory describes an elusive charge transfer between pyridine and the aqueous environment through Raman spectroscopy and computational chemistry. It builds on concepts that hydrogen bonding can induce blue-shifting features in vibrational spectra, and that excess protons found in acidic solutions are confined to acid–base pairing. More information can be found in the Research Article by J. T. Kelly, L. E. McNamara and co-workers (DOI: 10.1002/cphc.202400029). Image: Ella Maru Studio.

封面展示了水溶液中酸碱化学的复杂关系。在这里,萨凡纳河国家实验室通过拉曼光谱和计算化学描述了吡啶与水环境之间难以捉摸的电荷转移。它建立在氢键能诱导振动光谱中的蓝移特征,以及酸性溶液中发现的过量质子仅限于酸碱配对的概念之上。更多信息请参阅 J. T. Kelly, L. E. 的研究文章。Kelly, L. E.McNamara 及其合作者的研究文章中(DOI: 10.1002/cphc.202400029)。图片:Ella Maru Studio。
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引用次数: 0
Insights Into the Gas-Phase Structure and Internal Dynamics of Diphenylsilane: A Broadband Rotational Spectroscopy Study. 二苯基硅烷气相结构和内部动力学透视:宽带旋转光谱研究。
IF 2.3 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-10-15 DOI: 10.1002/cphc.202400790
Gayatri Batra, Melanie Schnell

The rotational spectrum of diphenylsilane was investigated using chirped-pulse Fourier transform microwave spectroscopy in the frequency range of 2-8 GHz. The lowest energy structure of diphenylsilane has C 2 ${_2 }$ point group symmetry with the C 2 ${_2 }$ symmetry axis coinciding with the b ${b}$ -inertial axis of the molecule. Through the assignment of the main isotopologue as well as singly substituted heavy-atom isotopologues, including 13 ${^{13} }$ C, 29 ${^{29} }$ Si, and 30 ${^{30} }$ Si, we were able to obtain a comprehensive gas-phase structure of diphenylsilane. The structure of diphenylsilane was compared with its oxygen analogue, diphenylether, including a discussion of the barrier height to the large-amplitude motion of the phenyl rings. Furthermore, the structural comparison was extended to include a range of C-Si bond lengths and bond angles from other organosilicon molecules where the silicon atom is bonded to aliphatic and/or aromatic moieties.

利用啁啾脉冲傅立叶变换微波光谱仪研究了二苯基硅烷的旋转光谱,频率范围为 2-8 GHz。二苯基硅烷的最低能量结构具有 C2 点群对称性,C2 对称轴与分子的双惯性轴重合。通过对主同位素以及单取代重原子同位素(包括 13C、29Si 和 30Si)的分配,我们获得了二苯基硅烷的全面气相结构。我们将二苯基硅烷的结构与其氧类似物二苯醚进行了比较,包括讨论了苯环大振幅运动的障碍高度。此外,结构比较还扩展到了硅原子与脂肪族和/或芳香族成键的其他有机硅分子的一系列 C-Si 键长度和键角。
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引用次数: 0
Electric-Field Controlled Switchable and Efficient Separation of Radioactive Xe/Kr on Borophene: A Theoretical Study. 电场控制硼吩上放射性 Xe/Kr 的可切换高效分离:理论研究。
IF 4.6 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-10-14 DOI: 10.1002/cphc.202400720
Wenxi Zhang, Mengnan Qu, Aijun Du, Qiao Sun

The efficient and reversible separation of radioactive Xe/Kr during spent fuel reprocessing is important and challenging for the rapid development of nuclear energy. In this study, we firstly report a strategy of applying an electric field on the solid adsorbent borophene to realize efficient and switchable Xe/Kr separation via a density functional theory (DFT) investigation. Based on the calculational results, the adsorption energies for Xe and Kr on borophene without an electric field are -0.25 eV and -0.18 eV, respectively, indicating that Xe and Kr can only form weak adsorption on borophene. However, by applying an electric field (0.006 a.u.) to the systems, the adsorption energies for Xe and Kr on borophene are -0.98 eV and -0.47 eV, respectively, which shows that the interaction between Xe and borophene has increased dramatically compared with that of Kr, so Xe can be separated from radioactive Xe/Kr mixtures. What's more, when the electric field is removed, desorption of Xe from the surface of borophene is exothermic without an energy barrier. The adsorbent is recyclable. In summary, this theoretical study provides novel information for experimental researches, the highly efficient Xe/Kr separation can be controlled by turning on/off the applied electric field.

在乏燃料后处理过程中高效、可逆地分离放射性 Xe/Kr 对核能的快速发展既重要又具有挑战性。在本研究中,我们通过密度泛函理论(DFT)研究,首次报道了在固体吸附剂硼吩上施加电场以实现高效、可切换的 Xe/Kr 分离的策略。根据计算结果,在没有电场的情况下,Xe 和 Kr 在硼吩上的吸附能分别为 -0.25 eV 和 -0.18 eV,这表明 Xe 和 Kr 在硼吩上只能形成弱吸附。然而,在系统中施加电场(0.006 a.u.)后,Xe 和 Kr 在硼吩上的吸附能分别为 -0.98 eV 和 -0.47 eV,这表明 Xe 和硼吩之间的相互作用比 Kr 的作用显著增强,因此 Xe 可以从放射性 Xe/Kr 混合物中分离出来。更重要的是,当电场移除时,Xe 从硼吩表面的解吸是放热的,没有能量障碍。该吸附剂可循环使用。总之,这项理论研究为实验研究提供了新的信息,通过开启/关闭外加电场可以控制 Xe/Kr 的高效分离。
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引用次数: 0
Scanning Transmission Soft X-Ray Microscopy Probes Topical Drug Delivery of Rapamycin Facilitated by Microneedles. 扫描透射软 X 射线显微镜探测微针对雷帕霉素局部给药的促进作用
IF 2.3 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-10-14 DOI: 10.1002/cphc.202400819
J A Laux, T Ohigashi, M R Bittermann, T Araki, H Yuzawa, F Rancan, A Vogt, E Rühl

Scanning Transmission X-ray microscopy (STXM) is a sensitive and selective probe for the penetration of rapamycin which is topically applied to human skin ex vivo and is facilitated by skin treatment with microneedles puncturing the skin. Inner-shell excitation serves as a selective probe for detecting rapamycin by changes in optical density as well as linear combination modeling using reference spectra of the most abundant species. The results indicate that mechanical damage induced by microneedles allows this drug to accumulate in the stratum corneum without reaching the viable skin layers. This is unlike intact skin which shows no drug penetration at all and underscores the mechanical impact of microneedle skin treatment. These results are compared to drug penetration profiles of other drugs highlighting the importance of skin barriers. High spatial resolution studies also indicate that the lipophilic drug rapamycin is observed in corneocytes. Attempts in data evaluation are reported to probe rapamycin also in the lipid layers between the corneocytes, which was not accomplished before. These results are compared to recent results on rapamycin uptake in skin where barrier impairment was induced by pre-treatment with the enzyme trypsin and drug formulations leading to occlusion.

扫描透射 X 射线显微镜(STXM)是一种灵敏的选择性探针,可用于探测雷帕霉素的渗透情况,雷帕霉素可在体外局部应用于人体皮肤,并可通过微针穿刺皮肤进行治疗。通过光密度的变化以及使用最丰富物种的参考光谱进行线性组合建模,内壳激发可作为检测雷帕霉素的选择性探针。结果表明,微针引起的机械损伤可使这种药物在角质层积聚,而不会到达有活力的皮肤层。这与完全没有药物渗透的完整皮肤不同,突出了微针治疗对皮肤的机械影响。这些结果与其他药物的药物渗透情况进行了比较,突出了皮肤屏障的重要性。高空间分辨率研究还表明,在角质细胞中观察到了亲脂性药物雷帕霉素。数据评估报告尝试在角质细胞之间的脂质层中也探测雷帕霉素,这在以前是没有实现过的。这些结果与最近有关雷帕霉素在皮肤中吸收的结果进行了比较,后者是通过胰蛋白酶预处理和导致闭塞的药物配方引起屏障受损。
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引用次数: 0
Nitrogen and Sulfur Doped Porous Carbon Sheet with Trace Amount of Iron as Efficient Polysulfide Conversion Catalyst for High Loading Lithium-Sulfur Batteries. 含微量铁的氮和硫掺杂多孔碳板作为高负载锂硫电池的高效多硫化物转化催化剂。
IF 2.3 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-10-12 DOI: 10.1002/cphc.202400406
Jeevanantham Sivaraj, Bosubabu Dasari, Prakash Subramani, Jayashree Pitchai, Sreekuttan M Unni, K Ramesha

The major challenges in enhancing the cycle life of lithium-sulfur (Li-S) batteries are polysulfide (PS) shuttling and sluggish reaction kinetics (S to Li2S, Li2S to S). To alleviate the above issues, the use of heteroatom-doped carbon as a cathode host matrix is a low-cost and efficient approach, as it works as a dual-functional framework for PS anchoring as well as an electrocatalyst for faster redox kinetics. Here, the dual role of heteroatom-doped carbon sheets (CS) in the chemisorption of Li2S6 and catalysis of its faster conversion to Li2S is established. To substantiate the catalytic effect, composite cathodes were prepared by encapsulating sulfur in CS which is further blended with carbon nanotubes (CNTs) to form a free-standing cathode. The electrochemical performances of the three cathodes (S@Fe-N-CS-CNT, S@Fe-S-CS-CNT, and S@Fe-NS-CS-CNT) were evaluated by constructing Li-S cells. The S@Fe-NS-CS-CNT delivers a high initial discharge capacity of 1017 mAh g-1 at 0.5 C rate and sustains a capacity of 751 mAh g-1 after 260 cycles with a capacity retention of 73.8 %. Even at a high S loading (12 mg cm-2), it delivers an initial discharge capacity of 892 mAh g-1 and retained 575 mAh g-1 after 200 cycles.

提高锂硫(Li-S)电池循环寿命的主要挑战在于多硫化物(PS)穿梭和反应动力学迟缓(S 到 Li2S,Li2S 到 S)。为了缓解上述问题,使用掺杂杂原子的碳作为阴极主基质是一种低成本、高效率的方法,因为它既能作为锚定 PS 的双功能框架,又能作为加快氧化还原动力学的电催化剂。在这里,通过紫外可见光、XPS 和 CV 研究,确定了含铁杂原子掺杂碳片(CS)在化学吸附 Li2S6 和催化其快速转化为 Li2S 方面的双重作用。为了证实催化作用,研究人员在 CS 中封装了硫,并进一步与碳纳米管(CNT)混合形成独立的阴极,从而制备出复合阴极。通过构建锂-S 电池评估了三种阴极(即 S@Fe-N-CS-CNT、S@Fe-S-CS-CNT 和 S@Fe-NS-CS-CNT)的电化学性能。其中,S@Fe-NS-CS-CNT 在 0.5 C 速率下可提供 1017 mAh g-1 的高初始放电容量,在 260 个循环后可维持 751 mAh g-1 的容量,容量保持率为 73.8%。即使在高 S 负载(12 毫克 cm-2)条件下,它也能提供 892 mAh g-1 的初始放电容量,并在 200 次循环后保持 575 mAh g-1 的容量。
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引用次数: 0
Structurally-Modulated Substrate of MXene for Surface-Enhanced Raman Scattering Sensing. 用于表面增强拉曼散射传感的 MXene 结构调整基底。
IF 2.3 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-10-11 DOI: 10.1002/cphc.202400604
Zhiwei Gao, Wei Lai

The distinctive structure of MXene offers exceptional electron transport properties, abundant surface chemistry, and robust mechanical attributes, thereby bestowing it with remarkable advantages and promising prospects in the realm of surface-enhanced Raman scattering (SERS). This review comprehensively outlines the evolution, synthesis methodologies, and characterization techniques employed for MXene-based SERS substrates. It delves into the intricacies of its SERS enhancement mechanism, substrate variants, and performance metrics, alongside showcasing its diverse applications spanning molecular detection, biosensing, and environmental monitoring. Furthermore, it endeavors to pinpoint the research bottlenecks and chart the future research trajectories for MXene-based SERS substrates.

MXene 的独特结构具有优异的电子传输特性、丰富的表面化学性质和坚固的机械属性,因此在表面增强拉曼散射 (SERS) 领域具有显著的优势和广阔的前景。本综述全面概述了基于 MXene 的 SERS 基底的演变、合成方法和表征技术。它深入探讨了 SERS 增强机制、基底变体和性能指标的复杂性,同时展示了其在分子检测、生物传感和环境监测等方面的多种应用。此外,该报告还致力于指出基于 MXene 的 SERS 基底的研究瓶颈,并描绘出未来的研究轨迹。
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引用次数: 0
Assessment of Edge Modification of Nanographene. 评估纳米石墨烯的边缘改性。
IF 2.3 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-10-09 DOI: 10.1002/cphc.202400792
Ryo Sekiya, Takeharu Haino

Carboxy groups on the edges of nanographene (NG) enable functionalization for realizing NG-organic hybrid materials. Therefore, assessment of the edge-functionalization of the electronic structures of NGs is valuable for the rational design of functional carbon materials. In this study, the structures of model NGs comprising 174 carbon atoms with armchair edges and various functional groups at the edges were computed. To achieve the greatest possible similarity between the computed structure and the real one, the carbon framework was designed based on experimental observations. The functional groups can be accessed via suitable chemical reactions. The computations predicted that although the conversion of carboxyl groups with electron-withdrawing/donating groups influences the orbital energies, the HOMO-LUMO (H-L) gap is not significantly affected, except in a few cases. Among the evaluated examples, π-extension had the greatest influence on the H-L gap. Interestingly, for the Pd2+-coordinated NG, the participation of the low-lying LUMO localized on Pd2+ in the surface-to-metal transitions seemingly narrowed the H-L gap, and a surface-to-ligand transition was observed.

纳米石墨烯(NG)边缘的羧基可实现功能化,从而实现 NG 有机杂化材料。因此,对 NG 电子结构边缘功能化的评估对于合理设计功能碳材料具有重要价值。本研究计算了由 174 个碳原子组成的模型 NG 的结构,这些 NG 具有扶手椅边缘,边缘上有各种官能团。为了使计算出的结构与实际结构尽可能相似,我们根据实验观察结果设计了碳框架。官能团可通过适当的化学反应获得。计算结果表明,虽然羧基与吸电子/捐电子基团的转换会影响轨道能量,但除了少数情况外,HOMO-LUMO(H-L)间隙不会受到明显影响。在评估的例子中,π-扩展对 H-L 间隙的影响最大。有趣的是,对于 Pd2+ 配位的 NG,Pd2+ 上的低洼 LUMO 参与了表面到金属的转变,这似乎缩小了 H-L 间隙,并观察到了表面到配体的转变。
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引用次数: 0
Conformational and Solvent Effects on the Photoinduced Electron Transfer Dynamics of a Zinc Phthalocyanine-Benzoperylenetriimide Conjugate: A Nonadiabatic Dynamics Simulation. 构象和溶剂对酞菁锌-苯并吡啶三亚胺共轭物光诱导电子转移动力学的影响:非绝热动力学模拟。
IF 2.3 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-10-09 DOI: 10.1002/cphc.202400631
Sha-Sha Liu, Xin Wei, Yan Zheng, Shuai Liu, Dong-Hui Xu, Laicai Li, Ganglong Cui, Xiang-Yang Liu

Herein, we employed a combination of static electronic structure calculations and nonadiabatic dynamics simulations at linear-response time dependent density functional theory (LR-TDDFT) level with the optimally tuned range-separated hybrid (OT-RSH) functional to explore the ultrafast photoinduced dynamics of a zinc phthalocyanine-benzoperylenetriimide (ZnPc-BPTI) conjugate. Due to the flexibility of the linker, we identified two major conformations: the stacked conformation (ZnPc-BPTI-1) and the extended conformation (ZnPc-BPTI-2). Since the charge transfer states are much lower than the lowest local excitation in ZnPc-BPTI-1, which is contrary to ZnPc-BPTI-2, the ultrafast electron transfer (~3.6 ps) is only observed in the nonadiabatic simulations of ZnPc-BPTI-1 upon local excitation around the absorption maximum of ZnPc. However, when considering the solvent effects in benzonitrile: the lowest S1 states are both charge transfer states from ZnPc to BPTI for different conformers. Subsequent nonadiabatic dynamics simulations indicate that both conformers experience ultrafast electron transfer in benzonitrile with two time constants of 90 [100] fs and 1.40 [1.43] ps. Our present work not only agrees well with previous experimental study, but also points out the important role of conformational changes and solvent effects in regulating the photodynamics of organic donor-acceptor conjugates.

在此,我们采用线性响应时间相关密度泛函理论(LR-TDDFT)水平上的静态电子结构计算和非绝热动力学模拟,结合优化调谐范围分离混合(OT-RSH)函数,探索了酞菁锌-苯并吡啶三亚胺(ZnPc-BPTI)共轭物的超快光诱导动力学。由于连接体的灵活性,我们确定了两种主要构象:堆叠构象(ZnPc-BPTI-1)和扩展构象(ZnPc-BPTI-2)。由于 ZnPc-BPTI-1 中的电荷转移态远低于最低局域激发,这与 ZnPc-BPTI-2 相反,因此只有在 ZnPc 吸收最大值附近的局域激发时,才能在 ZnPc-BPTI-1 的非绝热模拟中观察到超快电子转移(约 3.6 ps)。然而,当考虑到苯甲腈中的溶剂效应时:对于不同的构象,最低 S1 态都是从 ZnPc 到 BPTI 的电荷转移态。随后的非绝热动力学模拟表明,两种构象在苯甲腈中都经历了超快电子转移,两个时间常数分别为 90 [100] fs 和 1.40 [1.43] ps。我们目前的工作不仅与之前的实验研究完全吻合,而且还指出了构象变化和溶剂效应在调节有机供体-受体共轭物光动力学中的重要作用。
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引用次数: 0
Stretch-Induced Ordering of Prochiral Dimethyl Sulfoxide in Anisotropic Hydrogels Analysed by 1H and 2H Nuclear Magnetic Resonance. 通过 1H 和 2H 核磁共振分析手性二甲基亚砜在各向异性水凝胶中的拉伸有序性。
IF 2.3 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-10-09 DOI: 10.1002/cphc.202400731
Stuart James Elliott, Philip W Kuchel, Thomas R Eykyn

Nuclear spins in small molecules dissolved in stretched hydrogels typically have population-averaged residual interactions. The nuclear magnetic resonance (NMR) spectra of these systems often show additional peaks and splittings compared with free solutions. Residual dipolar couplings (RDCs) and quadrupolar couplings (RQCs) are observed for guest 1H or 2H nuclear spins, respectively. Dimethyl sulfoxide (DMSO) is an exquisitely sensitive probe of such biologically relevant environments since it is prochiral and becomes effectively chiral when embedded in anisotropic gelatin-based hydrogels. Measured 1H RDCs and 2H RQCs were used to estimate bond order parameters over a wide range of stretching extents. At the largest extent of stretching, the 2H splittings were -73.0 and -9.4 Hz, similar to those found for guest molecules in liquid crystals. Inhomogeneous line broadening of the 2H resonances was related to the size of the RQC due to a spatial distribution of RQCs, which was revealed using a one-dimensional slice selective imaging experiment along the stretching direction. 1H NMR spectra exhibited homogeneous line broadening, with resonance integrals that indicated concealed multiplet structure. Understanding molecular bond ordering in mechanically oriented environments provides a conceptual framework for investigating more complex systems including zeolites and those found in vivo.

溶解在拉伸水凝胶中的小分子核自旋通常具有群体平均残余相互作用。与自由溶液相比,这些系统的核磁共振(NMR)光谱通常会出现额外的峰值和分裂。在客体 1H 或 2H 核自旋中分别观察到残余二极耦合(RDC)和四极耦合(RQC)。二甲基亚砜(DMSO)对这种生物相关环境非常敏感,因为它是原手性的,嵌入各向异性的明胶基水凝胶后会有效地变成手性。测量到的 1H RDCs 和 2H RQCs 被用来估算各种拉伸延伸范围内的键序参数。在最大的拉伸范围内,2H分裂为-73.0和-9.4 Hz,与液晶中客体分子的分裂相似。2H 共振的不均匀线宽与 RQC 的大小有关,这是由于 RQC 的空间分布造成的,使用沿拉伸方向的一维切片选择性成像实验揭示了这一点。1H NMR 光谱显示出均匀的线展宽,共振积分显示出隐藏的多重结构。了解机械定向环境中的分子键排序为研究更复杂的系统(包括沸石和体内发现的系统)提供了一个概念框架。
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引用次数: 0
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