Rational design and observation of the tight interface between graphene and ligand protected nanocrystals

Kim, Byung Hyo; Bae, Hyeonhu; Park, Hyesung; Lee, Hoonkyung; Ercius, Peter

doi:10.1039/c8cp05844j

Cited by 3 publications

(1 citation statement)

References 48 publications

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“…A tight interface presumably promotes the electron transfer between binary materials. It should be pointed out that in many examples of heterostructures used as catalysts and in electronic devices, , the interface structure will be complicated by the presence of another interlayer with different properties from the desired constituent when containing a solution-synthesis step. However, there is scarce report that concerns low-cost Fe 2 O 3 –Fe 3 C heterostructure with tight interface connection between themselves to realize simultaneous trapping and conversion of LiPSs efficiently.…”

Section: Introductionmentioning

confidence: 99%

Integrating Polar and Conductive Fe₂O₃–Fe₃C Interface with Rapid Polysulfide Diffusion and Conversion for High-Performance Lithium–Sulfur Batteries

Cao¹,

Jia²,

Chen³

et al. 2019

ACS Appl. Mater. Interfaces

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A low-cost in situ formed Fe 2 O 3 −Fe 3 C heterostructure highly dispersed in carbon nanofiber was delicately designed via a facile one-pot electrospinning method. The intense anchoring (by Fe 2 O 3 ) and rapid electron transfer (by Fe 3 C) for lithium polysulfides transformation can be simultaneously achieved on the Fe 2 O 3 −Fe 3 C heterostructure interface, thus preventing the amassment of lithium polysulfides benefiting from its excellent interfacial contact and improving sulfur utilization. Experimental characterizations and DFT calculations confirmed the restrained polysulfides shuttle and enhanced redox kinetics. Therefore, the battery containing optimal Fe 2 O 3 −Fe 3 C heterostructure delivered a high capacity of 776.2 mA h g −1 after 300 cycles at 1 C at a low fading rate of 0.037% per cycle. Even at a high sulfur loading of 3.5 and 4.5 mg cm −2 , high capacities of 773.6 and 533.6 mA h g −1 at 0.5 C can be achieved with capacity retentions of 91.7 and 94.2%, respectively. This distinctive heterostructure proposes an effective design of high-performance lithium−sulfur batteries contributing to the excellent electrochemical performance, which can synergize the virtues of effectively adsorptive metal oxides and appealing conductive metal carbides.

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Section: Introductionmentioning

confidence: 99%

Integrating Polar and Conductive Fe₂O₃–Fe₃C Interface with Rapid Polysulfide Diffusion and Conversion for High-Performance Lithium–Sulfur Batteries

Cao¹,

Jia²,

Chen³

et al. 2019

ACS Appl. Mater. Interfaces

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Lattice-Disordered Boron Nitride Colloidal Catalyst for Low-Temperature Selective Methane Oxidation

Kim,

Choi,

Kim

et al. 2024

ACS Catal.

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Metal-free boron nitride (BN) catalysts hold great potential in numerous significant reactions, particularly in the selective oxidation of light alkanes, due to their unique ability to suppress overoxidation. However, the chemically stable BN catalysts often require high reaction temperatures, resulting in elevated energy consumption and less favorable for valuable oxygenate production. Enhancing the structural disorder within BN, increasing the density and refining the operational system are crucial for low-temperature applications, but modifying the inherently inert BN structure remains a significant challenge. Here, we report the controllable synthesis of lattice-disordered BN colloids by tailoring the defects. Spectroscopic, microscopic, and theoretical experiments revealed that increasing the number of vacancies in adjacent layers of hexagonal or porous BN leads to the formation of lattice-disordered structures. By employing the colloidal BN catalysts in the direct conversion of methane, an important greenhouse gas, into C1 oxygenates below 100 °C using H 2 O 2 as a green oxidant, we achieved both high mass activity and selectivity (exceeding 90%), which is an order of magnitude higher than fresh hexagonal BN powder and rivaling conventional metal catalysts. Mechanistic investigations highlighted that the lattice-disordered BN catalyst follows a radical pathway for the C1 oxygenate production. Moreover, the disordered boron species are proposed to enable facile activation of reactants due to their enhanced structural flexibility.

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Imaging the kinetics of anisotropic dissolution of bimetallic core–shell nanocubes using graphene liquid cells

et al. 2020

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Chemical design of multicomponent nanocrystals requires atomic-level understanding of reaction kinetics. Here, we apply single-particle imaging coupled with atomistic simulation to study reaction pathways and rates of Pd@Au and Cu@Au core-shell nanocubes undergoing oxidative dissolution. Quantitative analysis of etching kinetics using in situ transmission electron microscopy (TEM) imaging reveals that the dissolution mechanism changes from predominantly edge-selective to layer-by-layer removal of Au atoms as the reaction progresses. Dissolution of the Au shell slows down when both metals are exposed, which we attribute to galvanic corrosion protection. Morphological transformations are determined by intrinsic anisotropy due to coordination-number-dependent atom removal rates and extrinsic anisotropy induced by the graphene window. Our work demonstrates that bimetallic core-shell nanocrystals are excellent probes for the local physicochemical conditions inside TEM liquid cells. Furthermore, single-particle TEM imaging and atomistic simulation of reaction trajectories can inform future design strategies for compositionally and architecturally sophisticated nanocrystals.

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Rational design and observation of the tight interface between graphene and ligand protected nanocrystals

Abstract: We rationally designed heterostructures of graphene and ligand protected nanocrystals, and systematically investigated their interface by Cs-TEM.

Cited by 3 publications

References 48 publications

Integrating Polar and Conductive Fe₂O₃–Fe₃C Interface with Rapid Polysulfide Diffusion and Conversion for High-Performance Lithium–Sulfur Batteries

Integrating Polar and Conductive Fe₂O₃–Fe₃C Interface with Rapid Polysulfide Diffusion and Conversion for High-Performance Lithium–Sulfur Batteries

Lattice-Disordered Boron Nitride Colloidal Catalyst for Low-Temperature Selective Methane Oxidation

Imaging the kinetics of anisotropic dissolution of bimetallic core–shell nanocubes using graphene liquid cells

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Rational design and observation of the tight interface between graphene and ligand protected nanocrystals

Abstract: We rationally designed heterostructures of graphene and ligand protected nanocrystals, and systematically investigated their interface by Cs-TEM.

Cited by 3 publications

References 48 publications

Integrating Polar and Conductive Fe2O3–Fe3C Interface with Rapid Polysulfide Diffusion and Conversion for High-Performance Lithium–Sulfur Batteries

Integrating Polar and Conductive Fe2O3–Fe3C Interface with Rapid Polysulfide Diffusion and Conversion for High-Performance Lithium–Sulfur Batteries

Lattice-Disordered Boron Nitride Colloidal Catalyst for Low-Temperature Selective Methane Oxidation

Imaging the kinetics of anisotropic dissolution of bimetallic core–shell nanocubes using graphene liquid cells

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Integrating Polar and Conductive Fe₂O₃–Fe₃C Interface with Rapid Polysulfide Diffusion and Conversion for High-Performance Lithium–Sulfur Batteries

Integrating Polar and Conductive Fe₂O₃–Fe₃C Interface with Rapid Polysulfide Diffusion and Conversion for High-Performance Lithium–Sulfur Batteries