Ultra-Rapid Electrocatalytic H2O2 Fabrication over Mono-Species and High-Density Polypyrrolic-N Sites | |
Peng, Wei1; Chen, Rui1; Liu, Xiaoqing1; Tan, Haotian1; Yin, Lichang2; Hou, Feng1; Yang, De'an1; Liang, Ji1 | |
通讯作者 | Yin, Lichang(lcyin@imr.ac.cn) ; Hou, Feng(houf@tju.edu.cn) ; Yang, De'an(dayang@tju.edu.cn) ; Liang, Ji(liangji@tju.edu.cn) |
2024-06-21 | |
发表期刊 | SMALL
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ISSN | 1613-6810 |
页码 | 9 |
摘要 | Electrocatalytic hydrogen peroxide (H2O2) production via two-electron oxygen reduction reaction (2e(-)-ORR) features energy-saving and eco-friendly characteristics, making it a promising alternative to the anthraquinone oxidation process. However, the common existence of numerous 2e(-)-ORR-inactive sites/species on electrocatalysts tends to catalyze side reactions, especially under low potentials, which compromises energy efficiency and limits H2O2 yield. Addressing this, a high surface density of mono-species pyrrolic nitrogen configurations is formed over a polypyrrole@carbon nanotube composite. Thermodynamic and kinetic calculation and experimental investigation collaboratively confirm that these densely distributed and highly selective active sites effectively promote high-rate 2e(-)-ORR electrocatalysis and inhibit side reactions over a wide potential range. Consequently, an ultra-high and stable H2O2 yield of up to 67.9/51.2 mol g(-1) h(-1) has been achieved on this material at a current density of 200/120 mA cm(-1), corresponding Faradaic efficiency of 72.8/91.5%. A maximum H2O2 concentration of 13.47 g L-1 can be accumulated at a current density of 80 mA cm(-1) with satisfactory stability. The strategy of surface active site densification thus provides a promising and universal avenue toward designing highly active and efficient electrocatalysts for 2e(-)-ORR as well as a series of other similar electrochemical processes. |
关键词 | electrocatalysts high-density hydrogen peroxide mono-species polypyrrole |
资助者 | National Natural Science Foundation of China ; Tianjin University International Education Program for Outstanding Doctoral Thesis |
DOI | 10.1002/smll.202403261 |
收录类别 | SCI |
语种 | 英语 |
资助项目 | National Natural Science Foundation of China ; Tianjin University International Education Program for Outstanding Doctoral Thesis[C2-2021-004] ; [22379111] ; [22179093] |
WOS研究方向 | Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics |
WOS类目 | Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter |
WOS记录号 | WOS:001252058700001 |
出版者 | WILEY-V C H VERLAG GMBH |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://ir.imr.ac.cn/handle/321006/187249 |
专题 | 中国科学院金属研究所 |
通讯作者 | Yin, Lichang; Hou, Feng; Yang, De'an; Liang, Ji |
作者单位 | 1.Tianjin Univ, Sch Mat Sci & Engn, Key Lab Adv Ceram & Machining Technol, Minist Educ, Tianjin 300072, Peoples R China 2.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Liaoning, Peoples R China |
推荐引用方式 GB/T 7714 | Peng, Wei,Chen, Rui,Liu, Xiaoqing,et al. Ultra-Rapid Electrocatalytic H2O2 Fabrication over Mono-Species and High-Density Polypyrrolic-N Sites[J]. SMALL,2024:9. |
APA | Peng, Wei.,Chen, Rui.,Liu, Xiaoqing.,Tan, Haotian.,Yin, Lichang.,...&Liang, Ji.(2024).Ultra-Rapid Electrocatalytic H2O2 Fabrication over Mono-Species and High-Density Polypyrrolic-N Sites.SMALL,9. |
MLA | Peng, Wei,et al."Ultra-Rapid Electrocatalytic H2O2 Fabrication over Mono-Species and High-Density Polypyrrolic-N Sites".SMALL (2024):9. |
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