Cao Cong, Shang Chunyan, Li Xu, Wang Yinyin, Liu Chunxiao, Wang Xinyi, Zhou Shiming, Zeng Jie
Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui 230026, P. R. China.
Nano Lett. 2020 Apr 8;20(4):2837-2842. doi: 10.1021/acs.nanolett.0c00553. Epub 2020 Mar 30.
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 LaSrNiO ( = 1, 2, 3, and ∞) to explore the role of dimensionality on oxygen-evolution reaction (OER) performance. As the dimensionality increased with , the nickelates exhibited an enhanced OER activity. We found that the weakening of electron correlations among Ni 3 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.
晶体结构的维度在材料的电子结构中起着重要作用。由于维度的灵活性，Ruddlesden-Popper钙钛矿氧化物为研究这一作用提供了一个有吸引力的平台。这些氧化物中维度对物理性质的影响已被广泛报道。然而，关于维度对化学性质影响的研究仍然缺乏。在此，我们合成了一系列Ruddlesden-Popper钙钛矿镍酸盐LaSrNiO（ = 1、2、3和∞），以探索维度对析氧反应（OER）性能的作用。随着维度随 增加，镍酸盐表现出增强的OER活性。我们发现，通过增加维度削弱Ni 3电子之间的电子关联会引发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。这项工作在维度与电催化之间架起了一座桥梁，为设计高效析氧催化剂提供了指导。
