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Layered double hydroxide membrane with high hydroxide conductivity and ion selectivity for energy storage device.

ABSTRACT: Membranes with fast and selective ions transport are highly demanded for energy storage devices. Layered double hydroxides (LDHs), bearing uniform interlayer galleries and abundant hydroxyl groups covalently bonded within two-dimensional (2D) host layers, make them superb candidates for high-performance membranes. However, related research on LDHs for ions separation is quite rare, especially the deep-going study on ions transport behavior in LDHs. Here, we report a LDHs-based composite membrane with fast and selective ions transport for flow battery application. The hydroxide ions transport through LDHs via vehicular (standard diffusion) & Grotthuss (proton hopping) mechanisms is uncovered. The LDHs-based membrane enables an alkaline zinc-based flow battery to operate at 200 mA cm^-2, along with an energy efficiency of 82.36% for 400 cycles. This study offers an in-depth understanding of ions transport in LDHs and further inspires their applications in other energy-related devices.

SUBMITTER: Hu J

PROVIDER: S-EPMC8184958 | biostudies-literature | 2021 Jun

REPOSITORIES: biostudies-literature

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Layered double hydroxide membrane with high hydroxide conductivity and ion selectivity for energy storage device.

Hu Jing J Tang Xiaomin X Dai Qing Q Liu Zhiqiang Z Zhang Huamin H Zheng Anmin A Yuan Zhizhang Z Li Xianfeng X

Nature communications 20210607 1

Membranes with fast and selective ions transport are highly demanded for energy storage devices. Layered double hydroxides (LDHs), bearing uniform interlayer galleries and abundant hydroxyl groups covalently bonded within two-dimensional (2D) host layers, make them superb candidates for high-performance membranes. However, related research on LDHs for ions separation is quite rare, especially the deep-going study on ions transport behavior in LDHs. Here, we report a LDHs-based composite membrane ...[more]

PMID: 34099700

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Project description:Nitrate electroreduction (NO3RR) holds promise as an energy-efficient strategy for the removal of toxic nitrate to restore the natural nitrogen cycle and mitigate the adverse impacts caused by overfertilization from suboptimal agricultural practices. However, existing catalysts suffer from limited electrocatalytic activity, poor selectivity, inadequate durability, and low scalability. To address this quadrilemma, in this study, we developed a cost-effective layered double hydroxide (LDH) electrocatalyst with a lamellar structure that presents trimetallic CuCoAl active sites on the nanomaterial surface. This codoping design enabled electrochemical upcycling of nitrate into ammonia exclusively and efficiently with an onset potential at 0 V vs RHE, where the electrocatalytic process is less energy intensive and has a lower carbon footprint than conventional practices. The synergistic interaction among Cu, Co, and Al further afforded a 99.5% Faradic efficiency (FE) and a yield rate of 0.22 mol h-1 g-1 for nitrate-to-ammonia electroreduction, surpassing the performance of state-of-the-art nonprecious metal NO3RR electrocatalysts over an extended operation period. To gain insights into the origin of the catalytic performance observed on LDH, control materials were employed to elucidate the roles of Cu and Co. Cu was found to improve the NO3RR onset potential despite displaying limited FE for ammonia synthesis, while Co was discovered to suppress the formation of nitrite byproduct though requiring large overpotential. Simulated wastewater containing phosphate and sulfate, which are typically present in industrial effluents, was used to further investigate the effect of electrolytes on NO3RR. Intriguingly, the use of phosphate buffer resulted in a superior yield rate and FE for ammonia production while simultaneously inhibiting nitrite byproduct formation compared with the sulfate case. These experimental findings were supported by density functional theory (DFT) calculations, which explored the adsorption strength of nitrate adducts adjacent to coadsorbed electrolytes on the LDH surface. Additionally, the relative free energies of NO3RR species were also computed to examine the proton-coupled electron transfer (PCET) mechanism on CuCoAl LDH, shedding light on the potential-dependent step (PDS) and the exclusive selectivity for nitrate-to-ammonia conversion. The CuCoAl LDH developed here offers scalability by eliminating the need for precious metals, rendering this earth-abundant catalyst particularly appealing for sustainable nitrate electrovalorization technology.

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Layered double hydroxide membrane with high hydroxide conductivity and ion selectivity for energy storage device.

Publications

Layered double hydroxide membrane with high hydroxide conductivity and ion selectivity for energy storage device.

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