Quaternized Graphene Oxide Nanocomposites as Fast Hydroxide Conductors

Zarrin, Hadis; Fu, Jing; Jiang, Gaopeng; Yoo, Skylar; Lenos, Jared; Fowler, Michael; Chen, Zhongwei

doi:10.1021/nn507113c

Cited by 93 publications

(63 citation statements)

References 50 publications

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“…[12,13] In the spectrum of QAFGO, after functionalization, the peaks assigned to the vibration of C O (1739 cm −1 ), C-OH (1224 cm −1 ), C-O-C (1054 cm −1 ), and epoxy rings (856 cm −1 ) disappear. [14] Alternatively, two new small peaks at 2852 and 2921 cm −1 emerge in the spectrum, owing to methyl and long chains of methylene groups in the precursor (DMAOP), which indicates the effective grafting reaction between the oxygen functional groups of GO and QA groups of DMAOP. In the PC spectrum, the peaks at 3342 and 2900 cm −1 are attributed to the O-H and sp 3 hybridized C-H stretch vibration in the PC membrane.…”

Section: Doi: 101002/aenm201600476mentioning

confidence: 99%

“…[9][10][11] To address these challenges, researchers have sought to highly efficient solid-state electrolytes based on graphene oxide (GO), the oxidation product of natural graphite flakes. [12][13][14] GO has been demonstrated as a promising candidate because of its outstanding physicochemical stability and electrochemical properties. [15] Additionally, GO is a well-known wileyonlinelibrary.com step 2, Supporting Information).…”

Section: Doi: 101002/aenm201600476mentioning

confidence: 99%

“…Finally, these silanols and their oligomers are covalently bound to the oxygen-containing groups of nanocellulose/GO by losing water ( Figure S1, step 3, Supporting Information). [14] In the next step, the water-based suspensions of QA-functionalized GO nanosheets and cellulose nanofibers alternately go through vacuum filtration to form a laminate-structured membrane (Figure 1b) supported by QAfunctionalized GO at the top and bottom with a flat and uniform surface (Figure 1c). During the filtration process, the numerous cellulose nanofibers tend to construct a dense interwined porous network (Figure 1d), and perform as binder layers to integrate each single thin GO film into a robust membrane.…”

Section: Doi: 101002/aenm201600476mentioning

confidence: 99%

See 2 more Smart Citations

Laminated Cross‐Linked Nanocellulose/Graphene Oxide Electrolyte for Flexible Rechargeable Zinc–Air Batteries

Zhang

Song

et al. 2016

Advanced Energy Materials

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173

128

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electronic insulator with abundant oxygen-containing groups (epoxy, hydroxyl, and carboxyl groups), which can be easily functionalized to improve its ionic conductivity. [12,16] Owing to the wide range of oxygen functional groups on its basal planes and edges, GO is also readily exfoliated to yield well-dispersed solution of individual GO sheets in both water and organic solvents, and then flow-directed assembled into a free-standing paper-like material by vacuum filtration. [12,17] However, despite all the progress of the development of a free-standing GO electrolyte membrane, its advantages are diminished with the difficulty to form a mechanically robust membrane. [17,18] Consequently, that makes the free-standing GO membranes less attractive for being used as practical solid-state electrolytes in energy storage systems. To enhance the mechanical strength, several fillers can be incorporated into GO matrix. Among the multifarious materials, cellulose-the most abundant renewable material-is recognized as a good binder and surface modifier thanks to its low cost, high hygroscopicity, flexibility, ad porous substrate that allows strong binding of other materials. Particularly, considerable interest has been directed to nanocellulose fiber because of its low thermal expansion, high surface area, high surface area-to-volume ratio, strengthening effect, good mechanical and optical properties which may find many applications in nanocomposites. [19] Meanwhile, due to its highly reactive area rich in hydroxyl groups, cellulose can be easily refashioned through a surface-functionalization to conduct ions and be utilized in advanced batteries. [7] Herein, for the first time, we report on a laminate-structured nanocellulose/GO membrane functionalized with highly hydroxide-conductive quaternary ammonium (QA) groups to be applied as a robust solid-state electrolyte in flexible, rechargeable zinc-air batteries. The QA-functionalized nanocellulose/GO (QAFCGO) membrane is fabricated through chemical functionalization, layer-by-layer filtration, cross-linking, and ion-exchange processes (Figure 1a). For the functionalization process, dimethyloctadecyl [3-(trimethoxysilyl)-propyl] ammonium chloride (DMAOP) has been selected as the functional precursor containing QA moieties. The hydroxide conductivity and the alkaline stability in the highly surface-active DMAOP are provided by quaternary ammonium groups which are already attached to this organic compound. Thus, the hydroxide conducting characteristic of the electrolyte membrane can be achieved directly through the precursor DMAOP without complex organic synthesis. First, the trimethoxy groups of trimethoxysilyl are hydrolyzed to form the corresponding silanols, and the hydrolyzed silanols undergo self-condensation to yield silanol oligomers intermediates ( Figure S1, step 1, Supporting Information). Then, these intermediates are adsorbed onto nanocellulose/GO surface rich in oxygen-containing groups through hydrogen bonding ( Figure S1,

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Section: Doi: 101002/aenm201600476mentioning

confidence: 99%

Section: Doi: 101002/aenm201600476mentioning

confidence: 99%

Section: Doi: 101002/aenm201600476mentioning

confidence: 99%

See 1 more Smart Citation

Laminated Cross‐Linked Nanocellulose/Graphene Oxide Electrolyte for Flexible Rechargeable Zinc–Air Batteries

Zhang

Song

et al. 2016

Advanced Energy Materials

Self Cite

173

128

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show abstract

“…[41][42][43] Recently, potassium hydroxide equilibrated membranes based on m-PBI 44,45 and derivatives thereof 46 have been demonstrated to outperform conventional porous diaphragms in alkaline water electrolysis tests. Chemically, the m-PBI shows excellent stability in aqueous KOH in the lower concentration range and seems virtually unaffected after treatment in 5-10 wt% KOH at 88…”

Section: 32mentioning

confidence: 99%

Zero-Gap Alkaline Water Electrolysis Using Ion-Solvating Polymer Electrolyte Membranes at Reduced KOH Concentrations

Kraglund

Aili

Jankova

et al. 2016

J. Electrochem. Soc.

118

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Membranes based on poly(2,2 -(m-phenylene)-5,5-bibenzimidazole) (m-PBI) can dissolve large amounts of aqueous KOH to give electrolyte systems with ion conductivity in a practically useful range. The conductivity of the membrane strongly depends on the concentration of the aqueous KOH phase, reaching about 10 −1 S cm −1 or higher in 15-25 wt% KOH. Herein, m-PBI membranes are systematically characterized with respect to performance and short-term stability as electrolyte in a zero-gap alkaline water electrolyzer at different KOH concentrations. Using plain uncatalyzed nickel foam electrodes, the cell based on m-PBI outperforms the cell based on the commercially available state-of-the-art diaphragm and reaches a current density of 1500 mA cm −2 at 2.4 V in 20 wt% KOH at 80 • C. The cell performance remained stable during two days of operation, though post analysis of the membrane using size exclusion chromatography and spectroscopy reveal evidence of oxidative degradation of the base polymer at KOH concentrations of 15 wt% and higher. Converting surplus electrical energy into hydrogen by water electrolysis represents an attractive approach to balance the electric grid when an increasing fraction of the power input originates from fluctuating renewable sources.1 Characterized by their robustness and durability, alkaline electrolyzers have been available for a long time on a commercial basis for large scale hydrogen and oxygen production through electrochemical water splitting.2,3 The alkaline environment allows for a cell construction completely free from noble metals, where the oxygen 4-6 and hydrogen 7-9 evolution reactions readily occur on nickel and other transition metal-based materials. The electrodes are separated by an aqueous solution of potassium hydroxide confined in a porous diaphragm to reduce the intermixing of the product gasses. Between the diaphragm and the electrode is an electrolyte-filled gap to facilitate gas removal. This cell design gives an interelectrode distance in the range of a few millimeters and therefore a relatively large internal resistance, 3,10 even though the specific conductivity of the aqueous potassium hydroxide electrolyte used is remarkably high. Replacing the diaphragm with an ion-conducting membrane represents a new direction in the development of advanced alkaline electrolyzers as recently discussed by Pletcher and Li. 23 It allows for a zero-gap design with an inter-electrode distance of less than 100 μm, in which the membrane is sandwiched in between two porous electrodes. One approach in this connection is to use alkaline ion exchange membranes (AEM) based on quaternary ammoniumfunctionalized polymers, [24][25][26] but improving the stability of the polymer backbone 27 as well as of the anion exchange moieties 28 are apparent challenges.An alternative approach is to use a membrane based on an aqueous electrolyte dissolved in a polymer matrix. The ion-solvating polymer electrolytes are often soluble in water, 29 but as first demonstrated by Xing and Savadogo, 30 poly(2,2...

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“…Alternatively, the pristine form of m-PBI can be equilibrated in aqueous solutions of alkali metal hydroxides to form apparently homogenous ternary systems composed of the hydroxide salt and water dissolved in the polymer matrix. Such semi-solid materials exhibit remarkably high ion conductivity [34], excellent chemical stability at low alkali concentrations [35] and have been tested as electrolytes in hydrogen [34,36,37] and direct alcohol [38][39][40][41][42] fuel cells, water electrolysers [43,44] and as anion conducting phase in alkaline fuel cell catalyst layers [45][46][47]. Despite the recent efforts to develop electrochemical systems around this electrolyte system, the physicochemical chemistry of polybenzimidazoles in alkaline environment remains unexplored to a large extent.…”

Section: Introductionmentioning

confidence: 99%

Understanding ternary poly(potassium benzimidazolide)-based polymer electrolytes

Aili

Jankova

Han

et al. 2016

Polymer

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Quaternized Graphene Oxide Nanocomposites as Fast Hydroxide Conductors

Cited by 93 publications

References 50 publications

Laminated Cross‐Linked Nanocellulose/Graphene Oxide Electrolyte for Flexible Rechargeable Zinc–Air Batteries

Laminated Cross‐Linked Nanocellulose/Graphene Oxide Electrolyte for Flexible Rechargeable Zinc–Air Batteries

Zero-Gap Alkaline Water Electrolysis Using Ion-Solvating Polymer Electrolyte Membranes at Reduced KOH Concentrations

Understanding ternary poly(potassium benzimidazolide)-based polymer electrolytes

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