Tailoring the Atomic-Local Environment of Carbon Nanotube Tips for Selective H<sub>2</sub>O<sub>2</sub> Electrosynthesis at High Current Densities

doi:10.1002/adma.202303905

CORC > 力学研究所 > 中国科学院力学研究所 > 非线性力学国家重点实验室

	Tailoring the Atomic-Local Environment of Carbon Nanotube Tips for Selective H₂O₂ Electrosynthesis at High Current Densities
	Long, Yongde 5; Lin, Jinguo 4; Ye, Fenghui 5; Liu, Wei 3; Wang, Dan 5; Cheng, Qingqing 2; Paul, Rajib 1; Cheng, Daojian 5; Mao, Baoguang 5; Yan, Riqing 5
刊名	ADVANCED MATERIALS
	2023-10-15
页码	11
关键词	carbon nanotubes electrocatalysis hydrogen peroxide pure H2O2 solution production tip atomic environment
ISSN号	0935-9648
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.
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关键词	OXYGEN REDUCTION REACTION ; FUNCTIONALIZED GRAPHENE NANOPLATELETS ; METAL-FREE ELECTROCATALYSTS ; HYDROGEN-PEROXIDE ; EFFICIENT ELECTROCATALYST ; ACTIVE-SITES ; FUEL-CELL ; NITROGEN ; OXIDATION ; TRENDS
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
内容类型	期刊论文
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.,...&Hu, Chuangang.(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.