Highly Selective Hydrogen Peroxide Electrosynthesis on Carbon: In Situ Interface Engineering with Surfactants | |
Wu, Kuang-Hsu1,2; Wang, Dan1; Lu, Xingyu1; Zhang, Xuefei3; Xie, Zailai3; Liu, Yuefeng4; Su, Bing-Jian5; Chen, Jin-Ming1; Su, Dang-Sheng1,4; Qi, Wei1; Guo, Shaojun6 | |
通讯作者 | Xie, Zailai(zlxie@fzu.edu.cn) ; Qi, Wei(wqi@imr.ac.cn) ; Guo, Shaojun(guosj@pku.edu.cn) |
2020-06-11 | |
发表期刊 | CHEM
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ISSN | 2451-9294 |
卷号 | 6期号:6页码:1443-1458 |
摘要 | In situ modulation of surface reaction is a powerful approach to drive high-yield H2O2 electrosynthesis on metal-free carbon. Here, we discover that cationic surfactants can work efficiently as an in situ kinetic promoter for the oxygen-to-peroxide reaction on a car bon black electrode, achieving a peroxide yield above 90% (up to 95.2%) across a >0.8 V window in alkaline media, the best among reported H2O2 electrocatalysts. Our characterizations and kinetic model analysis show that the high peroxide selectivity is attributable to surface carboxylates (-COO-) with weak peroxide binding under a Coulombic pull imposed by an adsorbed cationic layer. Although surface carbonyls (-C=O) also participate in the peroxide synthesis, they exhibit strong binding to peroxide and promote on-site reduction at moderate-to-high overpotential. At only a minute amount of cationic surfactant, a chronoamperometry experiment with a carbonyl-free system can deliver a peroxide production at a sustainably high selectivity (similar to 96%) over 10h. |
资助者 | NSFC, China ; Youth Innovation Promotion Association, Chinese Academy of Sciences, China ; UNSW, Sydney (UNSW Faculty Research Fellowship), Australia |
DOI | 10.1016/j.chempr.2020.04.002 |
收录类别 | SCI |
语种 | 英语 |
资助项目 | NSFC, China[21761132010] ; NSFC, China[91645114] ; NSFC, China[21573256] ; Youth Innovation Promotion Association, Chinese Academy of Sciences, China ; UNSW, Sydney (UNSW Faculty Research Fellowship), Australia |
WOS研究方向 | Chemistry |
WOS类目 | Chemistry, Multidisciplinary |
WOS记录号 | WOS:000540905600030 |
出版者 | CELL PRESS |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://ir.imr.ac.cn/handle/321006/139572 |
专题 | 中国科学院金属研究所 |
通讯作者 | Xie, Zailai; Qi, Wei; Guo, Shaojun |
作者单位 | 1.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China 2.Univ New South Wales, Sch Chem Engn, Kensington, NSW 2052, Australia 3.Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350016, Peoples R China 4.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China 5.Natl Synchrotron Radiat Res Ctr, Hsinchu 300, Taiwan 6.Peking Univ, Coll Engn, Dept Mat Sci & Engn, Beijing 100871, Peoples R China |
推荐引用方式 GB/T 7714 | Wu, Kuang-Hsu,Wang, Dan,Lu, Xingyu,et al. Highly Selective Hydrogen Peroxide Electrosynthesis on Carbon: In Situ Interface Engineering with Surfactants[J]. CHEM,2020,6(6):1443-1458. |
APA | Wu, Kuang-Hsu.,Wang, Dan.,Lu, Xingyu.,Zhang, Xuefei.,Xie, Zailai.,...&Guo, Shaojun.(2020).Highly Selective Hydrogen Peroxide Electrosynthesis on Carbon: In Situ Interface Engineering with Surfactants.CHEM,6(6),1443-1458. |
MLA | Wu, Kuang-Hsu,et al."Highly Selective Hydrogen Peroxide Electrosynthesis on Carbon: In Situ Interface Engineering with Surfactants".CHEM 6.6(2020):1443-1458. |
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