期刊
JOURNAL OF MATERIALS CHEMISTRY A
卷 9, 期 14, 页码 9010-9017出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d0ta12277g
关键词
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资金
- National Natural Science Foundation of China [NSFC-22078293, 21776251, 21625604, 2017R5203, 91934302]
- Fundamental Research Funds for the Provincial Universities of Zhejiang [RF-A2020015]
- Zhejiang Collaborative Innovation Center (Ningbo Polytechnic College) [NZXT201801]
The study investigates the influence of lattice oxygen on beta-PbO2 during electrochemical ozone production, showing that all three oxygen atoms in ozone originate from lattice oxygen. The EOP reaction pathway on beta-PbO2 follows the lattice oxygen mechanism, with different reactivity observed on different crystal surfaces. This insight can be applied to other applications of metal oxide-based electrocatalysts.
The on-site production of ozone via electrochemical water electrolysis has attracted increasing interest because of its security and efficiency. However, the underlying mechanism of the facet effect and the influence of lattice oxygen on beta-PbO2 for electrochemical ozone production (EOP) remain unclear. Here, beta-PbO2-120 nanorods (beta-PbO2-120 NRs) were prepared to investigate the mechanism of the facet effect and the influence of lattice oxygen during the EOP process. The beta-PbO2-120 NRs assembled as an anode in a membrane electrode assembly show a remarkable EOP performance. Measurements using in situ(18)O isotope-labeling differential electrochemical mass spectrometry confirm that all three oxygen atoms in the ozone originate from the lattice oxygen of beta-PbO2. Theoretical calculations verify that the EOP reaction pathway on beta-PbO2 follows the lattice oxygen mechanism (LOM), and surface lattice oxygen migration and coupling to O-2/O-3 are favorable on the (101) and (110) surfaces of beta-PbO2. Different reaction mechanisms are proposed on the two surfaces, and (101) exhibits higher reactivity for O-2 and the formation of O-3. This valuable insight into the facet effect and LOM of metal oxide-based electrocatalysts can be extended to other applications.
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