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Synergistic electronic and morphological modulation on ternary Co1−xVxP nanoneedle arrays for hydrogen evolution reaction with large current density

具有协同电子结构和形貌调控功能的三元 Co1−xVxP纳米针阵列在大电流下的析氢性能研究

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Abstract

It is a great challenge to prepare non-noble metal electrocatalysts toward hydrogen evolution reaction (HER) with large current density. Synergistic electronic and morphological structures of the catalyst have been considered as an effective method to improve the catalytic performance, due to the enhanced intrinsic activity and enlarged accessible active sites. Herein, we present novel ternary Co1−xVxP nano-needle arrays with modulated electronic and morphological structures as an electrocatalyst for highly efficient HER in alkaline solution. The NF@Co1−xVxP catalyst shows a remarkable catalytic ability with low overpotentials of 46 and 226 mV at current densities of 10 and 400 mA cm−2, respectively, as well as a small Tafel slope and superior stability. Combining the experimental and computational study, the excellent catalytic performance was attributed to the improved physical and chemical properties (conductivity and surface activity), large active surface area, and fast reaction kinetics. Furthermore, the assembled Co-V based electrolyzer (NF@Co1−xVx-HNNs(+)||NF@Co1−xVxP(−)) delivers small full-cell voltages of 1.58, 1.75, and 1.92 V at 10, 100, and 300 mA cm−2, respectively. Our findings provide a systematic understanding on the V-incorporation strategy to promote highly efficient ternary electrocatalysts via synergistic control of morphology and electronic structures.

摘要

制备具有大电流析氢性能的非贵金属电催化剂是一个巨大 挑战. 协同调控催化剂的电子结构和形貌能够增强其本征催化能 力和增加活性位点, 被认为是提高催化性能的有效方法. 本文以具 有协同电子结构和形貌调控功能的三元Co1−xVxP纳米针阵列作为 碱性析氢的高效电催化剂. 试验和理论计算结果表明, 其优异的催 化性能来源于物理化学性质的提高、活性表面积的增加及反应动 力学的加速. 此外, 组装的(NF@Co1−xVx–HNNs(+)||NF@Co1−xVxP (−))电解池在1.58、1.75和1.92 V的电压下, 能够分别得到10、100 和300 mA cm−2的电流密度.

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (21671096, 21603094 and 21905180), the Natural Science Foundation of Guangdong Province (2018B030322001 and 2018A030310225), Shenzhen Peacock Plan (KQTD2016022620054656), Shenzhen Key Laboratory Project (ZDSYS201603311013489), the Basic Research Project of the Science and Technology Innovation Commission of Shenzhen (JCYJ20190809115413414), the Science and Technology Development Fund from Macau SAR (FDCT-0102/2019/A2, FDCT-0035/2019/AGJ and FDCT-0154/2019/A3) and the Multi-Year Research Grants (MYRG2017-00027-FST and MYRG2018-00003-IAPME) from the University of Macau. The DFT calculations were performed at the High Performance Computing Cluster (HPCC) of Information and Communication Technology Office (ICTO) at the University of Macau.

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  1. These authors contributed equally to this work.

Authors and Affiliations

  1. Department of Materials Science and Engineering, Shenzhen Key Laboratory of Hydrogen Energy, Southern University of Science and Technology, Shenzhen, 518055, China

    Mingyang Yang  (杨明阳), Zhenyu Wang  (王振宇), Shuai Gu  (顾帅), Lujie Cao  (曹鲁杰), Junjun Zhang  (张钧君) & Zhouguang Lu  (卢周广)

  2. Institute of Applied Physics and Materials Engineering, University of Macau, Macau SAR, China

    Mingyang Yang  (杨明阳), Feifei Li  (李菲菲), Di Liu  (刘地), Lujie Cao  (曹鲁杰) & Hui Pan  (潘晖)

  3. Shenzhen Key Laboratory of Polymer Science and Technology, College of Materials Science and Engineering, Shenzhen University, Shenzhen, 518060, China

    Mingyang Yang  (杨明阳) & Chen Liu  (刘琛)

  4. International Academy of Optoelectronics at Zhaoqing, South China Normal University, Zhaoqing, 526060, China

    Chaoqun Shang  (商超群)

  5. Department of Physics and Chemistry, Faculty of Science and Technology, University of Macau, Macau SAR, China

    Hui Pan  (潘晖)

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  1. Mingyang Yang  (杨明阳)
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Contributions

Yang M, Liu C, Lu Z and Pan H designed the research. Yang M, Shang C, Wang Z, Gu S, Cao L and Zhang J carried out the experiments and discussions. Li F, Liu D and Pan H finished the DFT calculations and analysis. Yang M, Shang C, Lu Z and Pan H wrote the manuscript. All authors revised the manuscript.

Corresponding authors

Correspondence to Chen Liu  (刘琛), Zhouguang Lu  (卢周广) or Hui Pan  (潘晖).

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Conflict of interest

The authors declare no conflict of interest.

Mingyang Yang received his PhD degree from the University of Macau in 2020. He was a visiting scholar at the Southern University of Science and Technology in 2015. Now he is a postdoc at Shenzhen University. His research interests focus on the design and synthesis of nanomaterials for energy conversion and storage, such as electrocatalysis for water splitting.

Chaoqun Shang is an associate research fellow at the South China Academy of Advanced Optoelectronics, South China Normal University. He received his PhD degree from Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences (2015). His research interests mainly focus on designing high-performance electrode materials for energy conversion and storage systems.

Feifei Li is a PhD student at the Institute of Applied Physics and Materials Engineering, University of Macau. Her research interest focuses on the first-principles design of materials for energy harvesting and storage.

Chen Liu received her PhD degree from the City University of Hong Kong in 2017. She is an assistant professor at the School of Materials Science and Engineering, Shenzhen University. Her research interest focuses on nanomaterials/polymer composites for electrochemical and energy applications.

Zhouguang Lu is now a professor at the Department of Materials Science and Engineering, Southern University of Science and Technology. He obtained his BE from the Central South University (CSU) in 2001 and got his MSc under the joint master program between Tsinghua University and CSU in 2004, and PhD from the City University of Hong Kong in 2009. His research mainly covers the design and synthesis of nanostructures and their application in energy storage and conversion.

Hui Pan is a professor at the Institute of Applied Physics and Materials Engineering, University of Macau. He obtained his PhD from the National University of Singapore in 2006. He was a scientist at the Institute of High Performance Computing (Singapore) from 2009 to 2013. His research mainly focuses on energy harvesting and storage (photocatalysis, electrocatalysis, biomass, CO2 and N2 reductions, battery, supercapacitor, and hydrogen production/storage).

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Synergistic electronic and morphological modulation on ternary Co1−xVxP nanoneedle arrays for hydrogen evolution reaction with large current density

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Yang, M., Shang, C., Li, F. et al. Synergistic electronic and morphological modulation on ternary Co1−xVxP nanoneedle arrays for hydrogen evolution reaction with large current density. Sci. China Mater. 64, 880–891 (2021). https://doi.org/10.1007/s40843-020-1495-x

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