气候变化领域集成服务门户(CCPortal): Regulating the allocation of N and P in codoped graphene: Via supramolecular control to remarkably boost hydrogen evolution

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DOI	10.1039/c9ee00555b
	Regulating the allocation of N and P in codoped graphene: Via supramolecular control to remarkably boost hydrogen evolution
	Wu H.; Chen Z.; Wang Y.; Cao E.; Xiao F.; Chen S.; Du S.; Wu Y.; Ren Z.
发表日期	2019
ISSN	1754-5692
起始页码	2697
结束页码	2705
卷号	12 期号:9
英文摘要	Although, as early as 2014, theoretical investigations have illuminated that nonmetallic heteroatom doped graphene (NHDG) is anticipated to achieve excellent catalytic activity approaching that of platinum for the hydrogen evolution reaction (HER), its actual HER performance, even today, is still worse than that of the transition metal-based catalysts used as benchmarks. The lack of an effective way capable of extensively and precisely modulating the allocation (e.g., the proportion, content and configuration) of heteroatoms in NHDG presents a substantial impediment. Herein, encouraged by our systematic theoretical result that optimizing the heteroatom allocation in graphene could significantly boost the HER performance, we regulate, for the first time, the proportion and content of heteroatoms in N, P codoped graphene (G-NP) accurately by a judiciously designed supramolecular architecture. The key to implementation lies in the well-built H-bonded supramolecular architecture (melamine-phosphoric acid)/graphene oxide assemblies, in which, during the pyrolysis, the architecture of melamine and phosphoric acid functions as not only a "spacer" to suppress the stacking of graphene nanosheets, but also a self-sacrificial dopant for extensively tuning the allocation of N and P in a wide range. The optimal G-NP can acquire a moderate hydrogen adsorption Gibbs free-energy, an enhanced conductivity and a large electrochemical surface area, and display an extremely low overpotential of 106 mV at 10 mA cm-2 in 0.5 M H2SO4 solution, ranking first in the reported NHDG catalysts and outperforming many state-of-the-art metallic catalysts. This work not only presents a cost-effective, efficient strategy to regulate the allocation of heteroatoms in doped graphene but also offers insight for better design and fabrication of advanced NHDG for different applications. © 2019 The Royal Society of Chemistry.
语种	英语
scopus关键词	Benchmarking; Catalyst activity; Cost effectiveness; Free energy; Gas adsorption; Gibbs free energy; Phosphoric acid; Supramolecular chemistry; Transition metals; Electrochemical surface area; Enhanced conductivity; Graphene nanosheets; Hydrogen adsorption; Hydrogen evolution reactions; Metal-based catalysts; Supramolecular architectures; Theoretical investigations; Graphene; adsorption; catalysis; catalyst; chemical compound; electrochemical method; Gibbs free energy; hydrogen; nitrogen; performance assessment; phosphorus
来源期刊	Energy and Environmental Science
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/162847
作者单位	Key Laboratory of Functional Inorganic Material Chemistry (Ministry of Education of China), School of Chemistry and Materials Science, Heilongjiang University, Harbin, 150080, China; Shanghai Institutes of Optics and Fine Mechanics, Chinese Academy of Sciences, Shanghai, 201800, China
推荐引用方式 GB/T 7714	Wu H.,Chen Z.,Wang Y.,et al. Regulating the allocation of N and P in codoped graphene: Via supramolecular control to remarkably boost hydrogen evolution[J],2019,12(9).
APA	Wu H..,Chen Z..,Wang Y..,Cao E..,Xiao F..,...&Ren Z..(2019).Regulating the allocation of N and P in codoped graphene: Via supramolecular control to remarkably boost hydrogen evolution.Energy and Environmental Science,12(9).
MLA	Wu H.,et al."Regulating the allocation of N and P in codoped graphene: Via supramolecular control to remarkably boost hydrogen evolution".Energy and Environmental Science 12.9(2019).