Multifunctional graphene heterogeneous nanochannel with voltage-tunable ion selectivity

Su, Shihao; Zhang, Yifan; Peng, Shengyuan; Guo, Linxin; Liu, Yong; Fu, Engang; Yao, Huijun; Du, Jinlong; Du, Guohao; Xue, Jianming

doi:10.1038/s41467-022-32590-9

Cited by 25 publications

(17 citation statements)

References 82 publications

(180 reference statements)

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“… 43 Such theoretical predictions agreed with the pores observed in experiments using a scanning transmission electron microscope, where most subnanopores with several atoms missed were found. 44 Besides, the averaged pore diameter predicted in the MD simulations is 5 Å for Au ions with an energy of 500 keV, which is also consistent with our experimental result. 43 , 44 It is worth noting that in the MD simulations, vacancies (pores) fabricated under the ion irradiation have not undergone further thermodynamical evolution (migration, coalescence, and dissociation), which are similar to the initial vacancies in this work.…”

Section: Resultssupporting

confidence: 90%

“…The above simulation results show the stability of vacancy distributions after the long-term vacancy evolution in monolayer graphene, which is also confirmed by our previous theoretical and experimental works on subnanopores fabricated using the irradiation of energetic ions in monolayer graphene. , In the classical MD simulations, the irradiation of ions can directly generate subnanopores due to the cascade collisions, and most of the pores, which are essentially vacancies, are with several atoms removed . Such theoretical predictions agreed with the pores observed in experiments using a scanning transmission electron microscope, where most subnanopores with several atoms missed were found . Besides, the averaged pore diameter predicted in the MD simulations is 5 Å for Au ions with an energy of 500 keV, which is also consistent with our experimental result. , It is worth noting that in the MD simulations, vacancies (pores) fabricated under the ion irradiation have not undergone further thermodynamical evolution (migration, coalescence, and dissociation), which are similar to the initial vacancies in this work.…”

Section: Resultssupporting

confidence: 86%

Section: Resultsmentioning

confidence: 99%

“…44 Besides, the averaged pore diameter predicted in the MD simulations is 5 Å for Au ions with an energy of 500 keV, which is also consistent with our experimental result. 43,44 It is worth noting that in the MD simulations, vacancies (pores) fabricated under the ion irradiation have not undergone further thermodynamical evolution (migration, coalescence, and dissociation), which are similar to the initial vacancies in this work. The experimentally observed subnanopores were actually the results after the vacancy evolution because there is a long period of time (at least several hours) between the fabrication and observation of the pores, which is enough for the finishing of the evolution.…”

Section: Stability Of Vacancy Distributionmentioning

confidence: 99%

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Long-Term Evolution of Vacancies in Large-Area Graphene

Liu

et al. 2022

ACS Omega

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Devices based on two-dimensional (2D) materials such as graphene and molybdenum disulfide have shown extraordinary potential in physics, nanotechnology, and electronics. The performances of these applications are heavily affected by defects in utilized materials. Although great efforts have been spent in studying the formation and property of various defects in 2D materials, the long-term evolution of vacancies is still unclear. Here, using a designed program based on the kinetic Monte Carlo method, we systematically investigate the vacancy evolution in monolayer graphene on a long-time and large spatial scale, focusing on the variation of the distribution of different vacancy types. In most cases, the vacancy distribution remains nearly unchanged during the whole evolution, and most of the evolution events are vacancy migrations with a few being coalescences, while it is extremely difficult for multiple vacancies to dissolve. The probabilities of different categories of vacancy evolutions are determined by their reaction rates, which, in turn, depend on corresponding energy barriers. We further study the influences of different factors such as the energy barrier for vacancy migration, coalescence, and dissociation on the evolution, and the coalescence energy barrier is found to be dominant. These findings indicate that vacancies (also subnanopores) in graphene are thermodynamically stable for a long period of time, conducive to subsequent characterizations or applications. Besides, this work provides hints to tune the ultimate vacancy distribution by changing related factors and suggests ways to study the evolution of other defects in various 2D materials.

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Section: Resultssupporting

confidence: 90%

Section: Resultssupporting

confidence: 86%

Section: Resultsmentioning

confidence: 99%

Section: Stability Of Vacancy Distributionmentioning

confidence: 99%

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Long-Term Evolution of Vacancies in Large-Area Graphene

Liu

et al. 2022

ACS Omega

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“…The ion selectivity ( S ) is defined as the ratio of D Cl – / D K + , where D Cl – and D K + mean the diffusion coefficients for Cl – and K + , respectively. The ion selectivity could be quantitatively calculated based on the Goldman–Hodgkin–Katz equation , E = k normalb T e .25em ln ( S a H + a L S a L + a H ) where E , k b , T , and e represent the diffusion potential, Boltzmann constant, absolute temperature, and electron charge, respectively, and a H and a L are the activities of Cl – for the high- and low-concentration solutions, respectively. The selectivity of Cl – toward K + would be calculated to be ∼53, indicating a much faster Cl – migration than K + migration in the P4VP channel.…”

Section: Resultsmentioning

confidence: 99%

Ultra-mechanosensitive Chloride Ion Transport through Bioinspired High-Density Elastomeric Nanochannels

Li,

Liu,

Zhi

et al. 2023

J. Am. Chem. Soc.

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Mechanosensitive ion channels play crucial roles in physiological activities, where small mechanical stimuli induce the membrane tension, trigger the ion channels’ deformation, and are further transformed into significant electrochemical signals. Artificial ion channels with stiff moduli have been developed to mimic mechanosensory behaviors, exhibiting an electrochemical response by the high-pressure-induced flow. However, fabricating flexible mechanosensitive channels capable of regulating specific ion transporting upon dramatic deformation has remained a challenge. Here, we demonstrate bioinspired high-density elastomeric channels self-assembled by polyisoprene-b-poly4-vinylpyridine, which exhibit ultra-mechanosensitive chloride ion transport resulting from nanochannel deformation. The PI-formed continuous elastic matrix can transmit external forces into internal tensions, while P4VP forms transmembrane chloride channels that undergo dramatic deformation and respond to mechanical stimuli. The integrated and flexible chloride channels present a dramatic and stable electrochemical signal toward a low pressure of 0.2 mbar. This research first demonstrates the artificial mechanosensory chloride channels, which could provide a promising avenue for designing flexible and responsive channel systems.

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Advanced Methods for Ion Selectivity Measurement in Nanofluidic Devices

Hou

Zhang

2023

Adv Materials Technologies

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methods [5f ] or by using emerging sub-nanometer porous materials to split large nanochannels [14e,49] and nanopipettes [15a,44a] into multiple sub-nanometer pores or channels. Single-ion selectivity [5f ] has been mainly achieved in sub-1 nm pores with specific ion-binding sites (Figure 1L). At present, a series of artificial single-H + , [19a,50] K + , [51] Li + , [42d,49c,52] Na + , [15c] F − , [14f,53] Cl − , [54] and I −[25b] selective ion channels have been developed to mimic the nature ion channels.To achieve accurate measurement of these unique selectivities in nanofluidic devices, different advanced experimental methods have been developed. For example, drift-diffusion experiment with the Goldman-Hodgkin-Katz (GHK) model [6a,14b,15b,19b,32d,44a,55] and charged molecule permeation experiments [56] have been developed for measuring the charge selectivity of nanofluidic channels and membranes. Ion permeation (diffusion) experiment, electrodialysis, ion current/ conductance/conductivity measurements, and pyranine assays were developed for investigating mono/divalent ion selectivity of nanofluidic devices. Notably, the drift-diffusion experiments, ion permeation (diffusion) experiments, conductance/conductivity measurements, and pyranine assays could also be used for single-ion selectivity measurements. Herein, in this review, research progress to date on investigations of the selective transport properties of the nanofluidic devices is reviewed. We begin by briefly reviewing some of the advanced construction strategies of nanofluidic devices that enable the measurement of their ion transport properties. We also summarize recent advances in experimental methods and theories for ion selectivity measurements and calculations. This is followed by a discussion of the challenge and future development of ion selective nanofluidic devices.

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Multifunctional graphene heterogeneous nanochannel with voltage-tunable ion selectivity

Cited by 25 publications

References 82 publications

Long-Term Evolution of Vacancies in Large-Area Graphene

Long-Term Evolution of Vacancies in Large-Area Graphene

Ultra-mechanosensitive Chloride Ion Transport through Bioinspired High-Density Elastomeric Nanochannels

Advanced Methods for Ion Selectivity Measurement in Nanofluidic Devices

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