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Dimensionality Control of Electrocatalytic Activity in Perovskite Nickelates
Nano Letters ( IF 9.6 ) Pub Date : 2020-03-24 , DOI: 10.1021/acs.nanolett.0c00553 Cong Cao 1 , Chunyan Shang 1 , Xu Li 1 , Yinyin Wang 1 , Chunxiao Liu 1 , Xinyi Wang 1 , Shiming Zhou 1 , Jie Zeng 1
Nano Letters ( IF 9.6 ) Pub Date : 2020-03-24 , DOI: 10.1021/acs.nanolett.0c00553 Cong Cao 1 , Chunyan Shang 1 , Xu Li 1 , Yinyin Wang 1 , Chunxiao Liu 1 , Xinyi Wang 1 , Shiming Zhou 1 , Jie Zeng 1
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The dimensionality of the crystal structure plays an important role in the electronic structures of materials. Ruddlesden–Popper perovskite oxides offer an attractive platform for studying this role due to dimensional flexibility. The effects of dimensionality on physical properties in those oxides have been widely reported. However, the study of dimensional dependence on the chemical properties is still lacking. Here, we synthesized a series of Ruddlesden–Popper perovskite nickelates LanSrNinO3n+1 (n = 1, 2, 3, and ∞) to explore the role of dimensionality on oxygen-evolution reaction (OER) performance. As the dimensionality increased with n, the nickelates exhibited an enhanced OER activity. We found that the weakening of electron correlations among Ni 3d electrons by increasing the dimensionality induced an insulator-to-metal transition and a strengthened Ni–O hybridization, both of which accelerated the OER kinetics. This work sets up a bridge between the dimensionality and electrocatalysis, which provides guidance for designing highly efficient oxygen-evolving catalysts.
中文翻译：
钙钛矿镍酸盐中电催化活性的尺寸控制
晶体结构的尺寸在材料的电子结构中起重要作用。Ruddlesden-Popper钙钛矿氧化物由于尺寸灵活性而为研究该作用提供了一个有吸引力的平台。尺寸对这些氧化物的物理性质的影响已被广泛报道。但是，仍然缺乏对尺寸依赖性的化学性质的研究。在这里，我们合成了一系列Ruddlesden-Popper钙钛矿镍酸盐La n SrNi n O 3 n +1（n = 1、2、3和∞），以研究尺寸对氧演化反应（OER）性能的作用。随着n的维数增加，镍酸盐显示出增强的OER活性。我们发现，通过增加尺寸来减弱Ni 3 d电子之间的电子相关性会导致绝缘体到金属的转变以及增强的Ni-O杂化，这两者都加速了OER动力学。这项工作在维数和电催化之间架起了一座桥梁，为设计高效的析氧催化剂提供了指导。
更新日期：2020-04-24
中文翻译：
钙钛矿镍酸盐中电催化活性的尺寸控制
晶体结构的尺寸在材料的电子结构中起重要作用。Ruddlesden-Popper钙钛矿氧化物由于尺寸灵活性而为研究该作用提供了一个有吸引力的平台。尺寸对这些氧化物的物理性质的影响已被广泛报道。但是，仍然缺乏对尺寸依赖性的化学性质的研究。在这里，我们合成了一系列Ruddlesden-Popper钙钛矿镍酸盐La n SrNi n O 3 n +1（n = 1、2、3和∞），以研究尺寸对氧演化反应（OER）性能的作用。随着n的维数增加，镍酸盐显示出增强的OER活性。我们发现，通过增加尺寸来减弱Ni 3 d电子之间的电子相关性会导致绝缘体到金属的转变以及增强的Ni-O杂化，这两者都加速了OER动力学。这项工作在维数和电催化之间架起了一座桥梁，为设计高效的析氧催化剂提供了指导。
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