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Regulating the electronic structure of NiFe layered double hydroxide/reduced graphene oxide by Mn incorporation for high-efficiency oxygen evolution reaction

Mn调控NiFe LDH/rGO活性位点的电子结构作为高效水氧化催化剂

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Abstract

The development of highly efficient and cost-effective oxygen evolution reaction (OER) electrocatalysts for renewable energy systems is vitally essential. Modulation of the electronic structure through heteroatom doping is considered as one of the most potential strategies to boost OER performances. Herein, a rational design of Mn-doped NiFe layered double hydroxide/reduced graphene oxide (Mn-NiFe LDH/rGO) is demonstrated by a facile hydrothermal approach, which exhibits outstanding OER activity and durability. Experimental results and density functional theory (DFT) calculations manifest that the introduction of Mn can reprogram the electronic structure of surface active sites and alter the intermediate adsorption energy, consequently reducing the potential limiting activation energy for OER. Specifically, the optimal Mn-NiFe LDH/rGO composite shows an enhanced OER performance with an ultralow overpotential of 240 mV@10 mA cm−2, Tafel slope of 40.0 mV dec−1 and excellent stability. Such superior OER activity is comparable to those of the recently reported state-of-the-art OER catalysts. This work presents an advanced strategy for designing electrocatalysts with high activity and low cost for energy conversion applications.

摘要

发展廉价、 高效的水氧化(OER)催化剂对发展可持续能源具有重要意义. 杂原子掺杂调节活性位点的电子结构提高催化剂的OER性能被认为是一种高效的策略. 本文通过水热法制备得到Mn掺杂的层状镍铁氢氧化物/还原氧化石墨烯(Mn-NiFe LDH/rGO)作为高效、 稳定的水氧化催化剂. 实验和模拟计算研究都表明Mn能调整活性位点的电子结构, 改善其对水氧化反应中中间产 物的吸附能垒, 从而减小OER反应中决速步骤的反应势垒. 具体而 言, 最优的Mn-NiFe LDH/rGO复合材料在过电位仅为240 mV就能 驱动10 mA cm−2的电流密度, Tafel斜率低至40.0 mV dec−1, 并且具有良好的稳定性. 该催化剂优异的活性优于最近报道的OER电催化剂. 本工作为制备用于能源转换领域的高活性、 廉价的电催化剂提供了新的思路.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (51902003 and 21771003), Anhui Province Natural Science Foundation (2008085QB53), and the Natural Science Research Project of Anhui Province Education Department (KJ2019A0581).

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  1. These authors contributed equally to this work.

Authors and Affiliations

  1. Institute of Clean Energy and Advanced Nanocatalysis (iClean), School of Chemistry and Chemical Engineering, Anhui University of Technology, Maanshan, 243002, China

    Binbin Jiang  (江彬彬), Konglin Wu  (吴孔林), Hengshuai Shang  (尚恒帅), Miao Wang  (王淼) & Xianwen Wei  (魏先文)

  2. Department of Chemistry, Tsinghua University, Beijing, 100084, China

    Weng-Chon Cheong  (张永臻), Renyong Tu  (屠仁勇), Kaian Sun  (孙凯安) & Chen Chen  (陈晨)

  3. Anhui Key Laboratory of Functional Coordination Compounds, Anqing Normal University, Anqing, 246011, China

    Binbin Jiang  (江彬彬)

  4. Department of Physics and Chemistry, Faculty of Science and Technology, University of Macau, Macao, China

    Weng-Chon Cheong  (张永臻)

  5. Chemistry and Chemical Engineering of Guangdong Laboratory, Shantou, 515063, China

    Shoujie Liu  (柳守杰)

  6. School of Electronics Science and Engineering, University of Electronic Science and Technology of China, Chengdu, 610054, China

    Aijian Huang  (黄爱鉴)

  7. Beijing Synchrotron Radiation Facility (NSRF), Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, 100049, China

    Lirong Zheng  (郑黎荣)

Authors
  1. Binbin Jiang  (江彬彬)
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Contributions

Author contributions Jiang B, Cheong WC and Wu K designed and carried out the synthesis and characterizations of samples, tested the electrochemical performance, analyzed the data and wrote the manuscript. Tu R, Sun K and Zheng L performed the TEM and XAFS characterization. Liu S analyzed the XAFS data. Shang H and Wang M synthesized the materials. Huang A did the DFT calculations, wrote and revised the manuscript. Wei X revised the manuscript and gave suggestions. Chen C supervised this work.

Corresponding authors

Correspondence to Konglin Wu  (吴孔林), Aijian Huang  (黄爱鉴) or Chen Chen  (陈晨).

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Conflict of interest The authors declare that they have no conflict of interest.

Additional information

Binbin Jiang received his PhD degree from the Institute of Functional Nano & Soft Materials (FUNSOM) of Soochow University in 2018. He has been a lecturer at the School of Chemistry and Chemical Engineering, Anqing Normal University since 2018. His research direction focuses on the field of energy sources.

Weng-Chon (Max) Cheong received his BSc and PhD degrees from the Department of Chemistry, Tsinghua University in 2013 and 2019, respectively, under the direction of Prof. Yadong Li. He is now a lecturer (UM Macao Fellow) at the Department of Physics and Chemistry, University of Macau. His research interests focus on nanosynthesis and electrocatalysis.

Konglin Wu is an associate professor at the School of Chemistry and Chemical Engineering, Anhui University of Technology. He received his PhD degree from the Department of Chemistry at Tsinghua University in 2019 under the supervision of Prof. Yadong Li. His research interest focuses on the design and preparation of single atom, clusters and micro/nanomaterials for energy storage and conversion, and organic catalysis.

Aijian Huang received his BSc degree in electronic information science and technology from the University of Electronic Science and Technology of China (UESTC) in 2018. Currently, he is a PhD candidate at the School of Electronics Science and Engineering, UESTC. His research interests include computer modeling of the electronic, thermal, mechanical, defect and doping properties of semiconductor, catalyst electrode materials with DFT simulation.

Chen Chen received his BSc degree from the Department of Chemistry, Beijing Institute of Technology in 2006, and his PhD degree from the Department of Chemistry, Tsinghua University in 2011 under the direction of Prof. Yadong Li. After postdoctoral work at Lawrence Berkeley National Laboratory with Prof. Peidong Yang, he joined the Department of Chemistry, Tsinghua University as an associate professor in 2015. His research interests focus on nanomaterials and catalysis.

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Regulating the electronic structure of NiFe layered double hydroxide/reduced graphene oxide by Mn incorporation for high-efficiency oxygen evolution reaction

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Jiang, B., Cheong, WC., Tu, R. et al. Regulating the electronic structure of NiFe layered double hydroxide/reduced graphene oxide by Mn incorporation for high-efficiency oxygen evolution reaction. Sci. China Mater. 64, 2729–2738 (2021). https://doi.org/10.1007/s40843-021-1678-y

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