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Effects of Atomic-Layer-Deposition Alumina on Proton Transmission through Single-Layer Graphene in Electrochemical Hydrogen Pump Cells
ACS Applied Energy Materials ( IF 5.4 ) Pub Date : 2020-01-13 00:00:00 , DOI: 10.1021/acsaem.9b01775
Saheed Bukola 1 , Duyen Cao 2 , Alex B. F. Martinson 2 , Stephen Creager 1
Affiliation  

Fifty atomic layer deposition (ALD) cycles of trimethylaluminum and water were applied to single-layer graphene on copper and graphene on Nafion membranes that result in alumina coatings that fully block photoelectron emission from the underlying substrate materials (copper and Nafion, respectively). This finding is consistent with relatively uninhibited alumina ALD nucleation and growth to a thickness of ∼5 nm and further suggests that the alumina layer is continuous with no uncoated regions exposed. The ALD-derived alumina coatings are good barriers to large ions, e.g., from aqueous ferric chloride, but they have a relatively modest effect on proton transmission through graphene as measured in electrochemical hydrogen pump cell experiments. Proton currents of ∼0.5 A cm–2 were obtained through Nafion/graphene/ALD alumina/Nafion at a modest bias voltage of 150 mV, which reflects a diminishment by less than half relative to the value for membranes without the 50 cycles of ALD alumina applied to the graphene. Proton transmission through the ALD alumina layer is thought to occur via hydrated alumina surfaces within the relatively porous ALD alumina layer on the graphene surface and perhaps also at grain boundaries formed in the alumina during the ALD process.

中文翻译:

原子层沉积氧化铝对电化学氢泵电池中质子通过单层石墨烯传输的影响

将三甲基铝和水的五十个原子层沉积(ALD)循环应用于铜上的单层石墨烯和Nafion膜上的石墨烯,从而形成氧化铝涂层,该涂层完全阻挡了下层基材(分别为铜和Nafion)的光电子发射。该发现与相对不受抑制的氧化铝ALD成核和生长至约5nm的厚度相一致,并且进一步表明氧化铝层是连续的,没有未涂覆的区域被暴露。ALD衍生的氧化铝涂层是阻挡较大离子(例如来自氯化铁水溶液的离子)的良好屏障,但如电化学氢泵电池实验中所测,它们对质子通过石墨烯的传输影响相对较小。质子电流〜0.5 A cm –2通过Nafion /石墨烯/ ALD氧化铝/ Nafion在150 mV的适度偏置电压下获得的结果表明,相对于未将ALD氧化铝施加到石墨烯上的50次循环,膜的减小值相对于膜值减少了不到一半。质子通过ALD氧化铝层的传输被认为是通过在石墨烯表面上的相对多孔的ALD氧化铝层内的水合氧化铝表面发生的,并且也可能是在ALD过程中在氧化铝中形成的晶界处发生的。
更新日期:2020-01-13
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