Breaking OER and CER scaling relations via strain and its relaxation in RuO2 (101)

Breaking OER and CER scaling relations via strain and its relaxation in RuO2 (101)
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通过 RuO2 (101) 中的应变及其弛豫打破 OER 和 CER 标度关系

DOI:
10.1016/j.mtener.2022.101087
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发表时间:
2022
影响因子:
9.3
通讯作者:
Stoerzinger, Kelsey A.
Stoerzinger, Kelsey A.
中科院分区:
材料科学3区
文献类型:
--
作者:
Adiga, Prajwal;Nunn, William;Wong, Cindy;Manjeshwar, Anusha K.;Nair, Sreejith;Jalan, Bharat;Stoerzinger, Kelsey A.

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利用丰富的水源进行绿色制氢是可再生能源储存的重要组成部分。水氧化催化剂通常被认为是由吸附质结垢关系束缚的,这限制了它们的析氧反应(OER)的活性,以及在盐水流中竞争的OER和析氯反应(CER)之间的选择性。ruo2对这两种反应都具有高活性,最近的测量表明,与通常研究的最低能量(110)面相比,在欠协调、高指数面的OER活性更大。然而,外延薄膜等取向的生长可以通过其弛豫产生可观的应变和潜在的表面饰面。我们发现外延(101)tio2薄膜对OER和CER的活性和选择性随薄膜厚度的变化而变化:OER活性随着薄膜厚度从8 nm增加到48 nm而下降4倍,而CER活性相当。因此,应变及其弛豫可以用来打破OER和CER之间的结垢关系,突出了缺陷在含氯化物的RuO2in介质上的选择性氧化过程中所起的重要作用。
Green hydrogen production from abundant water sources is an important component of renewable energy storage. Water oxidation catalysts are typically considered bound by adsorbate scaling relations, limiting their activity for the oxygen evolution reaction (OER) as well as selectivity between OER and the chlorine evolution reaction (CER) that compete in saline water streams. RuO2is highly active for both reactions, and recent measurements have shown that the OER activity is greater on undercoordinated, high index facets compared to the lowest energy (110) facet often studied. The growth of such orientations as epitaxial films, however, can result in appreciable strain and potential surface faceting via its relaxation. We find the activity and selectivity toward OER and CER vary with thickness in epitaxial (101) RuO2thin films: OER activity decreases four times as film thickness increases from 8 nm to 48 nm, while CER activity is comparable. Thus, strain and its relaxation can be used to break scaling relationships between OER and CER, highlighting the important role that defects play in selective oxidation processes on RuO2in chloride-containing media.
DOI: 10.1016/j.joule.2021.05.018
发表时间: 2021-08-18
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影响因子: 39.8
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发表时间: 2020
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期刊: Crystal Growth & Design
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