Defect-induced Pt-Co-Se coordinated sites with highly asymmetrical electronic distribution for boosting oxygen-involving electrocatalysis

Zhuang, Linzhou and Jia, Yi and Liu, Hongli and Wang, Xing and Hocking, Rosalie K. and Liu, Hongwei and Chen, Jun and Ge, Lei and Zhang, Longzhou and Li, Mengran and Dong, Chung-Li and Huang, Yu-cheng and Chen, Shaohua and Yang, Dongjiang and Zhu, Zhonghua and Yao, Xiangdong (2019) Defect-induced Pt-Co-Se coordinated sites with highly asymmetrical electronic distribution for boosting oxygen-involving electrocatalysis. Advanced Materials, 31 (4 (1805581)). pp. 1-10. ISSN 0935-9648

Abstract

Rational design and synthesis of hetero-coordinated moieties at the atomic scale can significantly raise the performance of the catalyst and obtain mechanistic insight into the oxygen-involving electrocatalysis. Here, a facile plasma-photochemical strategy is applied to construct atomically coordinated Pt-Co-Se moieties in defective CoSe2 (CoSe2-x) through filling the plasma-created Se vacancies in CoSe2-x with single Pt atomic species (CoSe2-x-Pt) under ultraviolet irradiation. The filling of single Pt can remarkably enhance the oxygen evolution reaction (OER) activity of CoSe2. Optimal OER specific activity is achieved with a Pt content of 2.25 wt% in CoSe2-x-Pt, exceeding that of CoSe2-x by a factor of 9. CoSe2-x-Pt shows much better OER performance than CoSe2-x filled with single Ni and even Ru atomic species (CoSe2-x-Ni and CoSe2-x-Ru). Noticeably, it is general that Pt is not a good OER catalyst but Ru is; thus the design of active sites for electrocatalysis at an atomic level should follow a different intrinsic mechanism. Mechanism studies unravel that the single Pt can induce much higher electronic distribution asymmetry degree than both single Ni and Ru, and benefit the interaction between the Co sites and adsorbates (OH*, O*, and OOH*) during the OER process, leading to a better OER activity.


Statistics for USQ ePrint 35440
Statistics for this ePrint Item
Item Type: Article (Commonwealth Reporting Category C)
Refereed: Yes
Item Status: Live Archive
Additional Information: Published version cannot be displayed due to copyright restrictions.
Faculty/School / Institute/Centre: Current - Institute for Advanced Engineering and Space Sciences - Centre for Future Materials
Date Deposited: 26 Feb 2019 01:16
Last Modified: 12 Mar 2019 05:13
Uncontrolled Keywords: asymmetrical electronic distribution; atomic metal species; oxygen evolution; selenium vacancies; synergetic interaction; nitrogen-doped graphene; single-atom; reduction reaction; water-oxidation; catalyst; nanosheets; hydrogen; transition; selenium; surface
Fields of Research : 03 Chemical Sciences > 0303 Macromolecular and Materials Chemistry > 030301 Chemical Characterisation of Materials
03 Chemical Sciences > 0303 Macromolecular and Materials Chemistry > 030306 Synthesis of Materials
09 Engineering > 0912 Materials Engineering > 091205 Functional Materials
Socio-Economic Objective: E Expanding Knowledge > 97 Expanding Knowledge > 970103 Expanding Knowledge in the Chemical Sciences
Identification Number or DOI: 10.1002/adma.201805581
URI: http://eprints.usq.edu.au/id/eprint/35440

Actions (login required)

View Item Archive Repository Staff Only