Facile Anhydrous Proton Transport on Hydroxyl Functionalized Graphane

Bagusetty, Abhishek; Choudhury, Pabitra Pal; Saidi, Wisssam A; Derksen, Bridget; Gatto, Elizabeth; Johnson, J. Karl

doi:10.1103/physrevlett.118.186101

Cited by 23 publications

(32 citation statements)

References 42 publications

(42 reference statements)

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Inspired by this mechanism, proton transport in synthetic nanofluidic systems attracts broad interest. − For example, Fan et al report surface-governed proton transport in aligned mesoporous silica film, which can be actively modulated by a low gate voltage . Recently, proton transport in 2D layered materials receives considerable attention due to the fantastic application in fuel cells. − Sulfonated, ozonated, and phosphorylated graphene oxide membranes (GOMs) are proposed as solid electrolyte and exhibit excellent proton conductivity. Shao et al further use clay nanosheets to build layered membranes for proton conduction and greatly enhance the thermal stability of the membrane materials .…”

mentioning

confidence: 99%

Asymmetric Electrokinetic Proton Transport through 2D Nanofluidic Heterojunctions

Zhang

Wang

et al. 2019

ACS Nano

View full text Add to dashboard Cite

Nanofluidic ion transport in nacre-like 2D layered materials attracts broad research interest due to subnanometer confined space and versatile surface chemistry for precisely ionic sieving and ultrafast water permeation. Currently, most of the 2D-material-based nanofluidic systems are homogeneous, and the investigations of proton conduction therein are restricted to symmetric transport behaviors. It remains a great challenge to endow the 2D nanofluidic systems with asymmetric proton transport characteristics and adaptive responsibilities. Herein, we report the asymmetric proton transport phenomena through a 2D nanofluidic heterojunction membrane under three different types of electrokinetic driving force, that is, the external electric field, the transmembrane concentration gradient, and the hydraulic pressure difference. The heterogeneous 2D nanofluidic membrane comprises of sequentially stacked negatively and positively charged graphene oxide (n-GO and p-GO) multilayers. We find that the preferential direction for proton transport is opposite under the three types of electrokinetic driving force. The preferential direction for electric-field-driven proton transport is from the n-GO multilayers to the p-GO multilayers, showing rectified behaviors. Intriguingly, when the transmembrane concentration difference and the hydraulic flow are used as the driving force, a preferred diffusive and streaming proton current is found in the reverse direction, from the p-GO to the n-GO multilayers. The asymmetric proton transport phenomena are explained in terms of asymmetric proton concentration polarization and difference in proton selectivity. The membrane-scale heterogeneous 2D nanofluidic devices with electrokinetically controlled asymmetric proton flow provide a facile and general strategy for potential applications in biomimetic energy conversion and chemical sensing.

show abstract

mentioning

confidence: 99%

Asymmetric Electrokinetic Proton Transport through 2D Nanofluidic Heterojunctions

Zhang

Wang

et al. 2019

ACS Nano

View full text Add to dashboard Cite

show abstract

“…Separating of ions based on their ability to dehydrate is feasible as the dehydration-based energy barriers of cations are different when they permeate through nanochannels. Unlike protons that can be transported in the absence of water in hydroxyl functionalized graphene nanochannels 39 or anhydrous transport of K + ions in biological K + -membrane protein ion channels (direct Coulomb knock-on mechnism 40 ), to date, there are no reports that synthetic nanochannels that can conduct ions efficiently under anhydrous conditions have been made.…”

Section: Effect Of Nanochannel Sizementioning

confidence: 99%

Design principles of ion selective nanostructured membranes for the extraction of lithium ions

et al. 2019

View full text Add to dashboard Cite

It is predicted that the continuously increasing demand for the energy-critical element of lithium will soon exceed its availability, rendering it a geopolitically significant resource. The present work critically reviews recent reports on Li+ selective membranes. Particular emphasis has been placed on the basic principles of the materials’ design for the development of membranes with nanochannels and nanopores with Li+ selectivity. Fundamental and practical challenges, as well as prospects for the targeted design of Li+ ion-selective membranes are also presented, with the goal of inspiring future critical research efforts in this scientifically and strategically important field.

show abstract

“…Density functional theory calculations predict remarkably low barriers to diffusion of proton along 1D chain of surface hydroxyl groups [14]. The properties of hydroxygraphane due to the presence of surface network of hydrogen bonds [15] make it a viable candidate for a proton exchange membrane material capable of operating under anhydrous or low-humidity conditions.…”

Section: Introductionmentioning

confidence: 99%

Hydroxygraphene: dynamics of hydrogen bond networks

Savin

2020

Preprint

View full text Add to dashboard Cite

Using the molecular dynamics method, dynamics of hydrogen bond (HB) networks emerging on the surface of a graphene sheet during its functionalization with hydroxyl groups OH are simulated. It is demonstrated that two OH groups form an energetically more advantageous structure when they are covalently attached on one side of the sheet to carbon atoms forming opposite vertices of one hexagon of valence bonds of the sheet. Attaching of OH groups to carbon atoms located at the opposite vertices of hexagons of valence bonds leads to the emergence of hydroxygraphene C4(OH). In such sheet lying on a flat substrate, attached oxygen atoms on its outer surface form a hexagonal lattice, and hydroxyl groups due to their turns can in various ways form chains of hydrogen bonds. The modification of the sheet from two sides results in forming of hydroxygraphene C2(OH) with HB networks on both sides of the graphene sheet. Simulation of the dynamics of these sheets shows that their heat capacity at low temperatures T < T0 increases monotonously when the temperature rises, reaches its maximum at T = T0 and then decreases monotonically. The initial growth is caused by the accumulation of orientational defects in the lattice of hydrogen bonds whereas the decrease at T > T0 is explained by the "melting" of the lattice. For one chain of OH groups connected to the outer side of a nanoribbon the melting temperature is T0 = 500K, while for a graphene sheet C4(OH) modified on one side T0 = 260K, and for a graphene sheet C2(OH) modified on both sides T0 = 485K.

show abstract

Facile Anhydrous Proton Transport on Hydroxyl Functionalized Graphane

Cited by 23 publications

References 42 publications

Asymmetric Electrokinetic Proton Transport through 2D Nanofluidic Heterojunctions

Asymmetric Electrokinetic Proton Transport through 2D Nanofluidic Heterojunctions

Design principles of ion selective nanostructured membranes for the extraction of lithium ions

Hydroxygraphene: dynamics of hydrogen bond networks

Contact Info

Product

Resources

About