Langmuir–Blodgett Deposition of Graphite Oxide Nanosheets as Catalysts for Bipolar Membrane Electrochemistry

IF 5.4 3区 材料科学 Q2 CHEMISTRY, PHYSICAL ACS Applied Energy Materials Pub Date : 2024-08-15 DOI:10.1021/acsaem.4c0160210.1021/acsaem.4c01602
Amy S. Metlay, Yein Yoon, Leanna Schulte, Tianyue Gao and Thomas E. Mallouk*, 
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Abstract

Graphite oxide (GO) has been widely studied as an interfacial layer in bipolar membranes because of its activity as a catalyst for the water dissociation and acid–base neutralization reactions. However, the roles of GO nanosheet size, orientation, and surface coverage in controlling its catalytic activity are not well understood. GO nanosheets with lateral dimensions of several microns were prepared by oxidative exfoliation of natural graphite crystals, enabling their orientation and coverage to be observed directly by optical microscopy. The coverage and orientation of the GO nanosheets were measured as a function of different deposition methods, which included solution adsorption, Langmuir–Blodgett transfer from an air–water interface, and spray-coating. Highly oriented GO films made by the Langmuir–Blodgett method gave the best performance metrics. Interestingly, full coverage of the bipolar interface by GO nanosheets resulted in lower performance than partial coverage. This effect could be rationalized in terms of the differential permeability of H+ and OH ions through GO, which leads to concentration polarization of OH on one side of the sheets.

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朗缪尔-布洛杰特沉积氧化石墨纳米片作为双极膜电化学催化剂
由于氧化石墨(GO)在水解离和酸碱中和反应中具有催化剂活性,因此作为双极性膜的界面层被广泛研究。然而,人们对 GO 纳米片的尺寸、取向和表面覆盖率在控制其催化活性方面的作用还不甚了解。通过氧化剥离天然石墨晶体制备了横向尺寸为几微米的GO纳米片,从而可以直接用光学显微镜观察其取向和覆盖情况。根据不同的沉积方法,包括溶液吸附、空气-水界面的朗缪尔-布洛杰特转移和喷涂,测量了 GO 纳米片的覆盖率和取向。采用 Langmuir-Blodgett 方法制成的高取向性 GO 薄膜具有最佳的性能指标。有趣的是,GO 纳米片完全覆盖双极界面的性能低于部分覆盖。这种效应可以用 H+ 和 OH- 离子在 GO 中的渗透性不同来解释,这导致了 OH- 的浓度极化在纳米片的一侧。
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来源期刊
ACS Applied Energy Materials
ACS Applied Energy Materials Materials Science-Materials Chemistry
CiteScore
10.30
自引率
6.20%
发文量
1368
期刊介绍: ACS Applied Energy Materials is an interdisciplinary journal publishing original research covering all aspects of materials, engineering, chemistry, physics and biology relevant to energy conversion and storage. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrate knowledge in the areas of materials, engineering, physics, bioscience, and chemistry into important energy applications.
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