Interconversion of acid-base neutralization energy as electrical driving force can spontaneously desalinate saline water during electric power production without a net redox reaction. This entropically favorable chemistry performs desalination by reversible redox reactions involving only gases, water, H + , and OH À such that the products and reactants of the reaction will not contaminate the desalinated water.
We utilize proton-coupled electron transfer in hydrogen storage molecules to unlock a rechargeable battery chemistry based on the cleanest chemical energy carrier molecule, hydrogen. Electrochemical, spectroscopic, and spectroelectrochemical analyses evidence the participation of protons during charge-discharge chemistry and extended cycling. In an era of anthropogenic global climate change and paramount pollution, a battery concept based on a virtually nonpolluting energy carrier molecule demonstrates distinct progress in the sustainable energy landscape.
We report a rechargeable sodium-ion battery in an aqueous environment with hydrophobic few-layer graphene as the capacitive anode and hexacyanometallate as the insertion cathode. Owing to the lack of hydrophilic functionalities, sodium-ion adsorption is selectively favored over H + adsorption at the hydrophobic anode/electrolyte interface without the complexity of widely encountered hydrogen-ion insertion/H 2 evolution. Hydrophobicity precludes chemical bond formation with sodium ions, thereby improving reversibility and extended cyclability during charge discharge chemistry.In the context of the geographic and temporal variations of renewable energy resources, metal ion batteries and new generation supercapacitors assume larger space as efficient energy storage modules. [1][2][3][4][5][6][7][8][9][10][11][12][13][14][15][16] So far non-aqueous metal ion batteries have dominated the consumer electronics, transport technologies and electrical grid as the prime storage technology. [17][18][19] Aqueous metal ion batteries though being environmentally benign, are rare in these contexts mainly due to serious instability of the state of the art anode materials in aquatic environment. [20][21][22] They suffer from spontaneous deinsertion reactions, unwanted swelling, undesirable proton insertion and parasitic H 2 evolution reactions, consequently degrading the anode entity during the long run. [23][24][25][26] The seminal works of Goodenough et. al., Wainwright et al, Yi Cui et. al, and Kang Kisuk et al., on anode materials for aqueous metal ion batteries are noteworthy in this direction. [23,[27][28][29][30][31][32][33] Here we report an aqueous sodium ion battery with extended cyclability using hydrophobic few layer graphene (FLG) as sodium ion adsorption anode and metal hexacyanoferrate (MHF) as the insertion cathode in aquatic environment. Hydrophobic FLG was produced by the reduction of graphene oxide's (GO) hydrophilic functionalities using Fe powder over conventionally used chemical reducing agents such as hydrazine and NaBH 4 [34,35] which predominantly yielded incompletely reduced GO thereby affecting its electrical and electronic properties. [34][35][36] We show here that the mode of reduction and therefore the hydrophobicity of FLG noticeably affect metal ion adsorption and charge-discharge chemistry at the anode/ electrolyte interface.FLG formed by two types of reduction processes are compared here, one by the Fe powder reduction method and the other by the conventional borohydride reduction method (see experimental section for more details). Few layers structure of graphene formed by the two reduction methods are evident in their atomic force microscopy images and the corresponding line profiles, Figures 1a and 1b, indicating that each flake approximately contains 3-4 graphene layers.The Raman spectra demonstrate a higher I D /I G ratio (intensity of defect band/intensity of graphitic band) for the FLG formed by borohydride reduction method compared to the corresponding FLG obtained by Fe powder reduction m...
The interfacial electrochemistry of reversible redox molecules is central to state-of-the-art flow batteries, outer-sphere redox species-based fuel cells, and electrochemical biosensors. At electrochemical interfaces, because mass transport and interfacial electron transport are consecutive processes, the reaction velocity in reversible species is predominantly mass-transport-controlled because of their fast electron-transfer events. Spatial structuring of the solution near the electrode surface forces diffusion to dominate the transport phenomena even under convective fluid-flow, which in turn poses unique challenges to utilizing the maximum potential of reversible species by either electrode or fluid characteristics. We show Coulombic force gated molecular flux at the interface to target the transport velocity of reversible species; that in turn triggers a directional electrostatic current over the diffusion current within the reaction zone. In an iron-based redox flow battery, this gated molecular transport almost doubles the volumetric energy density without compromising the power capability.
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