期刊
ACS APPLIED MATERIALS & INTERFACES
卷 12, 期 3, 页码 3642-3653出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.9b19614
关键词
biomimetic method; oxygen reduction reaction; biochar; CeO2; oxygen vacancies
资金
- National Natural Science Foundation of China [51778505, 51908375]
- Department of Science and Technology in Guangdong Province [2017B090901029]
This study reports the superior performance of novel carbonaceous materials, CeO2-encapsulated nitrogen-doped biochars [BC-Ce-X (X = 1 and 2)], for oxygen reduction reaction (ORR). The biomass precursor of this value-added biochar material was biomimetically prepared via a hydroponic operation in the Ce-enriched solution. The characterization results showed that CeO2 with large amounts of oxygen vacancies was stably embedded in the N self-doped biochars during the pyrolytic processes. The measured specific surface areas of cerium-free biochar (BC sample), BC-Ce-1, and BC-Ce-2 were 79, 566, and 518 m(2)/g, respectively. The BC-Ce-X (X = 1 and 2) showed excellent ORR performances with onset potentials of similar to 0.90-0.91 V, which outperformed the commercial 10 wt % Pt/C and BC. Compared with Pt/C, the BC-Ce-2 had better methanol tolerance and stability. Also, BC-Ce-2 displayed excellent electrochemical activity for Zn/air batteries. Controlled experiments and density functional theoretical calculations illustrated the synergistic effect between the pyri-N/C centers and CeO2 with oxygen vacancies in ORR The Lewis base sites, created by pyri-N and oxygen vacancies, greatly facilitated the chemisorption of O-2 molecules.
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