Abstract
In this work, we reported the synthesis of two-dimensional spinel structure of ultrathin Co2AlO4 nanosheets via dealloying and subsequent annealing processes. Oxygen vacancy defects were further introduced into Co2AlO4 nanosheets by a mild solvothermal reduction method, resulting in large electrochemical surface area and high active site densities, making the related Co atoms get electrons, and producing more empty orbitals. The positive charge of Co and Al atoms adjacent to the O vacancies in VO-rich Co2AlO4 reduced significantly, that is, more electrons are concentrated on the Co and Al atoms. Those electrons closed to the Fermi level have a promoting effect during the H2O activation. As a result, the obtained ultrathin Co2AlO4 nanosheets with oxygen vacancies show a low overpotential of 280 mV at the current density of 10 mA cm−2 and a small Tafel slope of 70.98 mV dec−1. Moreover, it also displays a remarkable stability in alkaline solution, which is superior to most of the reported Co3O4 electrocatalysts. The present work paves a new way to achieve efficient new energetic materials for sustainable community.
摘要
本文报道了通过脱合金和后续退火工艺合成一种新型超薄二维尖晶石结构的Co2AlO4纳米片. 通过温和的溶剂热还原法将氧空位缺陷引入Co2AlO4纳米片中, 使得电化学表面积增大, 活性位密度变高, 钴原子得到电子而产生更多的空轨道. 这些空轨道有利于接受水分子中氧原子的孤对电子, 促进水分子的活化. 含有氧空位的超薄Co2AlO4纳米片在10 mA cm−2时的过电位为280 mV, 塔菲尔斜率为70.98 mV dec−1. 此外, 其在碱性溶液中也表现出显著的稳定性, 并且优于多数已报道的Co3O4电催化剂. 该工作为制备高效的可持续新能源材料提供了新思路.
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Acknowledgements
The authors gratefully acknowledge the financial support by the National Natural Science Foundation of China (21771137), the Natural Science Foundation of Tianjin City (18JCJQJC47700), 111 project (D17003) and the Training Project of Innovation Team of Colleges and Universities in Tianjin (TD13-5020)
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An C conceived the idea of systhesizing Co2AlO4 spinel for oxygen evolution reaction, Wang J and An C designed the project; and Wang J performed the experiments; Shen Y conducted the theoretical simulations; Wei G, Xi W and Ma X took part in the characterizations of samples; Wang J, Zhu P and Wei G analyzed the data and discussed the results. Wang J wrote the paper with support from An C and Zhang W.
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Supporting data are available in the online version of the paper.
Jiayang Wang received her BSc degree in chemical engineering and technology from Shijiazhuang College in 2017. Now she is a master student majored in chemical engineering in Tianjin University of Technology under the supervision of Prof. Changhua An. Her current interests focus on the synthesis of 2D materials for electrochemical hydrogen and oxygen evolution reaction.
Weiqing Zhang received her PhD degree from National University of Singapore (NUS) in 2013. She currently works as an associate professor at Tianjin University of Technology. Her research interests focus on noble metal nanomaterials and their atomic origins for electrochemical energy conversion.
Changhua An received his PhD degree from the University of Science and Technology of China (USTC) in 2003 with Prof. Yitai Qian. After he did postdoc with Prof. Taeghwan Hyeon in Seoul National University from 2004 to 2005, he joined China University of Petroleum as an associate professor. In 2013, he was promoted to full professor of materials science and chemistry. From 2016, he has been a Tianjin distinguished professor at Tianjin University of Technology. His research interests focus on the synthesis, characterization, and explorations of efficient catalysts in the fields of clean energy production and environmental purification.
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Wang, J., Shen, Y., Wei, G. et al. Synthesis of ultrathin Co2AlO4 nanosheets with oxygen vacancies for enhanced electrocatalytic oxygen evolution. Sci. China Mater. 63, 91–99 (2020). https://doi.org/10.1007/s40843-019-9490-x
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DOI: https://doi.org/10.1007/s40843-019-9490-x