Tailoring the Atomic-Local Environment of Carbon Nanotube Tips for Selective H2O2 Electrosynthesis at High Current Densities
文献类型:期刊论文
作者 | Long, Yongde5; Lin, Jinguo4; Ye, Fenghui5; Liu, Wei3; Wang, Dan5; Cheng, Qingqing2; Paul, Rajib1; Cheng, Daojian5; Mao, Baoguang5; Yan, Riqing5 |
刊名 | ADVANCED MATERIALS |
出版日期 | 2023-10-15 |
页码 | 11 |
ISSN号 | 0935-9648 |
关键词 | carbon nanotubes electrocatalysis hydrogen peroxide pure H2O2 solution production tip atomic environment |
DOI | 10.1002/adma.202303905 |
通讯作者 | Mao, Baoguang(bgmao@buct.edu.cn) ; Liu, Feng(liufeng@imech.ac.cn) ; Hu, Chuangang(chuangang.hu@mail.buct.edu.cn) |
英文摘要 | The atomic-local environment of catalytically active sites plays an important role in tuning the activity of carbon-based metal-free electrocatalysts (C-MFECs). However, the rational regulation of the environment is always impeded by synthetic limitations and insufficient understanding of the formation mechanism of the catalytic sites. Herein, the possible cleavage mechanism of carbon nanotubes (CNTs) through the crossing points during ball-milling is proposed, resulting in abundant CNT tips that are more susceptible to be modified by heteroatoms, achieving precise modulation of the atomic environment at the tips. The obtained CNTs with N,S-rich tips (N,S-TCNTs) exhibit a wide potential window of 0.59 V along with H2O2 selectivity for over 90.0%. Even using air as the O-2 source, the flow cell system with N,S-TCNTs catalyst attains high H2O2 productivity up to 30.37 mol g(cat.)(-1) h(-1)@350 mA cm(-2), superior to most reported C-MFECs. From a practical point of view, a solid electrolyzer based on N,S-TCNTs is further employed to realize the in-situ continuous generation of pure H2O2 solution with high productivity (up to 4.35 mmol cm(-2) h(-1)@300 mA cm(-2); over 300 h). The CNTs with functionalized tips hold great promise for practical applications, even beyond H2O2 generation. |
WOS关键词 | OXYGEN REDUCTION REACTION ; FUNCTIONALIZED GRAPHENE NANOPLATELETS ; METAL-FREE ELECTROCATALYSTS ; HYDROGEN-PEROXIDE ; EFFICIENT ELECTROCATALYST ; ACTIVE-SITES ; FUEL-CELL ; NITROGEN ; OXIDATION ; TRENDS |
资助项目 | This work was partly financially supported by the National Natural Science Foundation of China (52172179), the Fundamental Research Funds for the Central Universities (buctrc202118), an open fund of the Key Lab of Organic Optoelectronics and Molecular Engi[11972349] ; This work was partly financially supported by the National Natural Science Foundation of China (52172179), the Fundamental Research Funds for the Central Universities (buctrc202118), an open fund of the Key Lab of Organic Optoelectronics and Molecular Engi[11790292] ; National Natural Science Foundation of China[buctrc202118] ; Fundamental Research Funds for the Central Universities[53223000122] ; Key Lab of Organic Optoelectronics and Molecular Engineering of Ministry of Education[XDB22040503] ; Strategic Priority Research Program of the Chinese Academy of Sciences |
WOS研究方向 | Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics |
语种 | 英语 |
WOS记录号 | WOS:001084814800001 |
资助机构 | This work was partly financially supported by the National Natural Science Foundation of China (52172179), the Fundamental Research Funds for the Central Universities (buctrc202118), an open fund of the Key Lab of Organic Optoelectronics and Molecular Engi ; National Natural Science Foundation of China ; Fundamental Research Funds for the Central Universities ; Key Lab of Organic Optoelectronics and Molecular Engineering of Ministry of Education ; Strategic Priority Research Program of the Chinese Academy of Sciences |
源URL | [http://dspace.imech.ac.cn/handle/311007/93240] |
专题 | 力学研究所_非线性力学国家重点实验室 |
通讯作者 | Mao, Baoguang; Liu, Feng; Hu, Chuangang |
作者单位 | 1.Kent State Univ, Adv Mat & Liquid Crystal Inst, Kent, OH 44242 USA 2.Chinese Acad Sci, Shanghai Adv Res Inst, Shanghai 201210, Peoples R China 3.Beijing Univ Chem Technol, Coll Mat Sci & Engn, Beijing 100029, Peoples R China 4.Chinese Acad Sci, Inst Mech, State Key Lab Nonlinear Mech, Beijing 100190, Peoples R China 5.Beijing Univ Chem Technol, Coll Chem Engn, State Key Lab Organ Inorgan Composites, Beijing 100029, Peoples R China |
推荐引用方式 GB/T 7714 | Long, Yongde,Lin, Jinguo,Ye, Fenghui,et al. Tailoring the Atomic-Local Environment of Carbon Nanotube Tips for Selective H2O2 Electrosynthesis at High Current Densities[J]. ADVANCED MATERIALS,2023:11. |
APA | Long, Yongde.,Lin, Jinguo.,Ye, Fenghui.,Liu, Wei.,Wang, Dan.,...&林金国.(2023).Tailoring the Atomic-Local Environment of Carbon Nanotube Tips for Selective H2O2 Electrosynthesis at High Current Densities.ADVANCED MATERIALS,11. |
MLA | Long, Yongde,et al."Tailoring the Atomic-Local Environment of Carbon Nanotube Tips for Selective H2O2 Electrosynthesis at High Current Densities".ADVANCED MATERIALS (2023):11. |
入库方式: OAI收割
来源:力学研究所
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