能源化学(英文版)

能源化学(英文) ›› 2019, Vol. 28 ›› Issue (7): 57-63.DOI: 10.1016/j.jechem.2018.09.011

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Ultrafine monolayer Co-containing layered double hydroxide nanosheets for water oxidation

Xiaodan Jiaa,c, Xin Zhanga,b, Jiaqing Zhaoa, Yufei Zhaoa, Yunxuan Zhaoa,b, Geoffrey I. N. Waterhoused, Run Shia,b, Li-Zhu Wua, Chen-Ho Tunga, Tierui Zhanga,b   

  1. a Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing 100190, China;
    b University of Chinese Academy of Sciences, Beijing 100049, China;
    c School of Chemistry and Chemical Engineering, Xi'an University of Science and Technology, Xi'an 710054, Shaanxi, China;
    d School of Chemical Sciences, The University of Auckland, Auckland 1142, New Zealand
  • 收稿日期:2018-07-09 修回日期:2018-09-14 出版日期:2019-07-15 发布日期:2019-07-15
  • 通讯作者: Tierui Zhang
  • 基金资助:
    The authors are grateful for the financial support from the National Key R&D Program of China (Grant Nos.:2017YFA0206904, 2017YFA0206900, and 2016YFB0600901), the National Program on Key Basic Research Project (Grant No.:2014CB239402), the National Natural Science Foundation of China (Grant Nos.:51772305, 51572270, U1662118, 31671489, U1332205, and 21701131), the Strategic Priority Research Program of the Chinese Academy of Sciences (Grant No.:XDB17000000), the Royal Society Newton Advanced Fellowship (Grant No.:NA170422), the Young Elite Scientist Sponsorship Program by CAST (Grant No.:YESS20160137), the Youth Innovation Promotion Association of the CAS, and the Fund of Xi'an University of Science and Technology (Grant No.:2018QDJ014).

Ultrafine monolayer Co-containing layered double hydroxide nanosheets for water oxidation

Xiaodan Jiaa,c, Xin Zhanga,b, Jiaqing Zhaoa, Yufei Zhaoa, Yunxuan Zhaoa,b, Geoffrey I. N. Waterhoused, Run Shia,b, Li-Zhu Wua, Chen-Ho Tunga, Tierui Zhanga,b   

  1. a Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing 100190, China;
    b University of Chinese Academy of Sciences, Beijing 100049, China;
    c School of Chemistry and Chemical Engineering, Xi'an University of Science and Technology, Xi'an 710054, Shaanxi, China;
    d School of Chemical Sciences, The University of Auckland, Auckland 1142, New Zealand
  • Received:2018-07-09 Revised:2018-09-14 Online:2019-07-15 Published:2019-07-15
  • Contact: Tierui Zhang
  • Supported by:
    The authors are grateful for the financial support from the National Key R&D Program of China (Grant Nos.:2017YFA0206904, 2017YFA0206900, and 2016YFB0600901), the National Program on Key Basic Research Project (Grant No.:2014CB239402), the National Natural Science Foundation of China (Grant Nos.:51772305, 51572270, U1662118, 31671489, U1332205, and 21701131), the Strategic Priority Research Program of the Chinese Academy of Sciences (Grant No.:XDB17000000), the Royal Society Newton Advanced Fellowship (Grant No.:NA170422), the Young Elite Scientist Sponsorship Program by CAST (Grant No.:YESS20160137), the Youth Innovation Promotion Association of the CAS, and the Fund of Xi'an University of Science and Technology (Grant No.:2018QDJ014).

摘要： For many two-dimensional (2D) materials, low coordination edges and corner sites offer greatly enhanced catalytic performance compared to basal sites, motivating the search for new synthetic approaches towards ultrathin and ultrafine 2D nanomaterials with high specific surface areas. To date, the synthesis of catalysts that are both ultrathin (monolayer) and ultrafine (lateral size <10 nm) has proven extremely challenging. Herein, using a facile ultrasonic exfoliation procedure, we describe the successful synthesis of ultrafine ZnCo-LDH nanosheets (denoted as ZnCo-UF) with a size~3.5 nm and thickness~0.5 nm. The single layer ZnCo-UF nanosheets possess an abundance of oxygen vacancies (VO) and unsaturated coordination sites, thereby affording outstanding electrocatalytic water oxidation performance. DFT calculations confirmed that VO on the surface of ZnCo-UF enhanced H2O adsorption via increasing the electropositivity of the nanosheets.

关键词: Layered double hydroxides, Ultrafine nanosheets, Oxidation evolution reaction

Abstract: For many two-dimensional (2D) materials, low coordination edges and corner sites offer greatly enhanced catalytic performance compared to basal sites, motivating the search for new synthetic approaches towards ultrathin and ultrafine 2D nanomaterials with high specific surface areas. To date, the synthesis of catalysts that are both ultrathin (monolayer) and ultrafine (lateral size <10 nm) has proven extremely challenging. Herein, using a facile ultrasonic exfoliation procedure, we describe the successful synthesis of ultrafine ZnCo-LDH nanosheets (denoted as ZnCo-UF) with a size~3.5 nm and thickness~0.5 nm. The single layer ZnCo-UF nanosheets possess an abundance of oxygen vacancies (VO) and unsaturated coordination sites, thereby affording outstanding electrocatalytic water oxidation performance. DFT calculations confirmed that VO on the surface of ZnCo-UF enhanced H2O adsorption via increasing the electropositivity of the nanosheets.

Key words: Layered double hydroxides, Ultrafine nanosheets, Oxidation evolution reaction