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| Carbon charge population and oxygen molecular transport regulated by program-doping for highly efficient 4e-ORR | |
| Zhang, Tong1,2,3; Wang, Huanhuan1,4; Zhang, Jintao1,5; Ma, Jing4; Wang, Zhi1,2,3; Liu, Junhao1,3; Gong, Xuzhong1,2,3 | |
| 2022-09-15 | |
| Source Publication | CHEMICAL ENGINEERING JOURNAL
 |
| ISSN | 1385-8947 |
| Volume | 444Pages:11 |
| Abstract | Oxygen reduction reaction (ORR) is a key reaction in both hydrogen peroxide (H2O2) generation and fuel cells system. Carbon is a promising catalyst to overcome the sluggish kinetics of ORR, while its intrinsic activity is contentious. It has been verified that both heteroatoms doping and intrinsic defects upgrade the carbon performance. Nevertheless, the charge population is the fundamental origin of carbon activity. In this work, N and S are used to co-regulate the carbon charge population. Results demonstrate that the N in the six-member ring and thiophene-S are electron-withdrawing configurations, leading to more positive charge distribution. Nevertheless, pyrrole-N is an electron-donor and destroys the charge delocalization when it co-existed with a six-member N ring or thiophene-S. Consequently, S is preferentially released to inhabit the five-membered ring formation site, inducing the precise formation of six-membered N ring. Importantly, the transfer enhancement of O-2 molecules by physical absorption and reaction consumption is confirmed by in-situ concentration detection. The synthesized material possesses more positive half-wave potential (E-1/2~0.851 VRHE), high selectivity and stability than that of Pt/C (E-1/2~0.823 VRHE). |
| Keyword | Charge population
Precise synthesis
N,S co-doping 4e-ORR |
| DOI | 10.1016/j.cej.2022.136560 |
| Language | 英语 |
| WOS Keyword | METAL-FREE ELECTROCATALYSTS ; DOPED GRAPHENE ; REDUCTION REACTION ; NITROGEN ; BATTERIES ; DEFECTS ; ORR |
| Funding Project | National Key R&D Program of China[2018YFE0183600] ; Natural Science Foundation of China[21878299] |
| WOS Research Area | Engineering |
| WOS Subject | Engineering, Environmental ; Engineering, Chemical |
| Funding Organization | National Key R&D Program of China ; Natural Science Foundation of China |
| WOS ID | WOS:000800420400001 |
| Publisher | ELSEVIER SCIENCE SA |
| Citation statistics | |
| Document Type | 期刊论文 |
| Identifier | http://ir.ipe.ac.cn/handle/122111/53562 |
| Collection | 中国科学院过程工程研究所 |
| Corresponding Author | Wang, Zhi; Gong, Xuzhong |
| Affiliation | 1.Chinese Acad Sci, Inst Proc Engn, Natl Engn Res Ctr Green Recycling Strateg Met Reso, Beijing 100190, Peoples R China 2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 3.Chinese Acad Sci, Innovat Acad Green Manufacture, Beijing 100190, Peoples R China 4.Taiyuan Univ Technol, Sch Mat Sci & Engn, Taiyuan 030024, Peoples R China 5.Univ Sci & Technol Beijing, Beijing 100083, Peoples R China |
| Recommended Citation GB/T 7714 | Zhang, Tong,Wang, Huanhuan,Zhang, Jintao,et al. Carbon charge population and oxygen molecular transport regulated by program-doping for highly efficient 4e-ORR[J]. CHEMICAL ENGINEERING JOURNAL,2022,444:11. |
| APA | Zhang, Tong.,Wang, Huanhuan.,Zhang, Jintao.,Ma, Jing.,Wang, Zhi.,...&Gong, Xuzhong.(2022).Carbon charge population and oxygen molecular transport regulated by program-doping for highly efficient 4e-ORR.CHEMICAL ENGINEERING JOURNAL,444,11. |
| MLA | Zhang, Tong,et al."Carbon charge population and oxygen molecular transport regulated by program-doping for highly efficient 4e-ORR".CHEMICAL ENGINEERING JOURNAL 444(2022):11. |
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