A single-molecule van der Waals compass

Shen, Boyuan; Chen, Xiao; Wang, Huiqiu; Xiong, Hao; Bosch, Eric; Lazić, Ivan; Cai, Dali; Qian, Weizhong; Jin, Shifeng; Liu, Xin; Han, Yu; Wei, Fei

doi:10.1038/s41586-021-03429-y

Cited by 92 publications

(76 citation statements)

References 48 publications

(36 reference statements)

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“…Previous studies on the exact form of Zn species and their exact locations are all based on spectroscopic analysis, such as X‐ray absorption, electron spin resonance, and UV‐vis DR spectra, [12b,d, 19] and the direct imaging evidence of Zn present in the micropores of ZSM‐5 has not been reported thus far. Using cutting‐edge integrated differential phase contrast STEM (iDPC‐STEM), which is more sensitive to the guest components in the porous structure than the commonly used HAADF‐STEM, [2c, 3d, 20] we directly observed isolated single‐Zn complexes residing in the microporous channels of ZSM‐5 for the first time (Figure 4). The enlarged images of the three representative channels (Figure 4b–d), together with the intensity profiles (Figure 4e), show an obvious separation in the Zn position between the two channels (Figure 4b, c), illustrating that the single‐Zn oxides anchor on different T‐sites.…”

Section: Resultsmentioning

confidence: 99%

Rational Design of Zinc/Zeolite Catalyst: Selective Formation of p‐Xylene from Methanol to Aromatics Reaction

Wang

Sun

et al. 2022

Angew Chem Int Ed

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The production of p-xylene from the methanol to aromatics (MTA) reaction is challenging. The catalytic stability, which is inversely proportional to the particle size of the zeolite, is not always compatible with p-xylene selectivity, which is inversely proportional to the external acid sites. In this study, based on a nano-sized zeolite, we designed hollow triple-shelled Zn/MFI single crystals using the ultra-dilute liquid-phase growth technique. The obtained composites possessed one ZSM-5 layer ( � 30 nm) in the middle and two silicalite-1 layers ( � 20 nm) epitaxially grown on two sides of ZSM-5, which exhibited a considerably long lifetime (100 % methanol conversion > 40 h) as well as an enhanced shape selectivity of p-xylene (> 35 %) with a p-xylene/xylene ratio of � 90 %. Importantly, using this sandwich-like zeolite structure, we directly imaged the Zn species in the micropores of only the ZSM-5 layer and further determined the specific structure and anchor location of the Zn species.

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Section: Resultsmentioning

confidence: 99%

Rational Design of Zinc/Zeolite Catalyst: Selective Formation of p‐Xylene from Methanol to Aromatics Reaction

Wang

Sun

et al. 2022

Angew Chem Int Ed

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“…Note that there are some other factors that affect the significance of the current model switching and the r-SMES, such as the short time scale of the transition-state solvation, which cannot achieved by our sampling rate. Nonetheless, the rise of single-molecule probes 33 gives us confidence that the electrical single-molecule platform is promising to detect the supercritical fluid, microphase transition, 34 nucleation mechanism, 35 and chemical oscillation systems from single-molecule insight.…”

Section: Resultsmentioning

confidence: 99%

Accurate Single-Molecule Indicator of Solvent Effects

Guo

Yang

Jia

et al. 2021

JACS Au

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The study of the microscopic structure of solvents is of significant importance for deciphering the essential solvation in chemical reactions and biological processes. Yet conventional technologies, such as neutron diffraction, have an inherent averaging effect as they analyze a group of molecules. In this study, we report a method to analyze the microstructure and interaction in solvents from a single-molecule perspective. A single-molecule electrical nanocircuit is used to directly analyze the dynamic microscopic structure of solvents. Through a single-molecule model reaction, the heterogeneity or homogeneity of solvents is precisely detected at the molecular level. Both the thermodynamics and the kinetics of the model reaction demonstrate the microscopic heterogeneity of alcohol–water and alcohol– n -hexane solutions and the microscopic homogeneity of alcohol–carbon tetrachloride solutions. In addition, a real-time event spectroscopy has been developed to study the dynamic characteristics of the segregated phase and the internal intermolecular interaction in microheterogeneous solvents. The development of such a unique high-resolution indicator with single-molecule and single-event accuracy provides infinite opportunities to decipher solvent effects in-depth and optimizes chemical reactions and biological processes in solution.

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“…The method makes it easier to analyze small structure distortions in crystalline materials, like some improper ferroelectrics ( 49 ) and high-entropy alloys ( 20 ). In addition, for nanoparticles ( 50 ) and beam-sensitive materials like zeolites ( 51 , 52 ), it is usually hard to accurately align the crystals to the direction of electron beam. Under these circumstances, mistilt can be relatively large and our method offers an effective way to get high-quality atomic-resolved images.…”

Section: Discussionmentioning

confidence: 99%

Deep sub-angstrom resolution imaging by electron ptychography with misorientation correction

Sha

Cui

2022

Sci. Adv.

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Superresolution imaging of solids is essential to explore local symmetry breaking and derived material properties. Electron ptychography is one of the most promising schemes to realize superresolution imaging beyond aberration correction. However, to reach both deep sub-angstrom resolution imaging and accurate measurement of atomic structures, it is still required for the electron beam to be nearly parallel to the zone axis of crystals. Here, we report an efficient and robust method to correct the specimen misorientation in electron ptychography, giving deep sub-angstrom resolution for specimens with large misorientations. The method largely reduces the experimental difficulties of electron ptychography and paves the way for widespread applications of ptychographic deep sub-angstrom resolution imaging.

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A single-molecule van der Waals compass

Cited by 92 publications

References 48 publications

Rational Design of Zinc/Zeolite Catalyst: Selective Formation of p‐Xylene from Methanol to Aromatics Reaction

Rational Design of Zinc/Zeolite Catalyst: Selective Formation of p‐Xylene from Methanol to Aromatics Reaction

Accurate Single-Molecule Indicator of Solvent Effects

Deep sub-angstrom resolution imaging by electron ptychography with misorientation correction

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