Control of Surface and Edge Oxidation on Phosphorene

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	Control of Surface and Edge Oxidation on Phosphorene
	Kuntz, Kaci L. ; Wells, Rebekah A. ; Hu, Jun ; Yang, Teng ; Dong, Baojuan ; Guo, Huaihong ; Woomer, Adam H. ; Druffel, Daniel L. ; Alabanza, Anginelle ; Tomanek, David ; Warren, Scott C.
刊名	ACS APPLIED MATERIALS & INTERFACES
	2017-03-15
卷号	9 期号:10 页码:9126-9135
关键词	2D materials black phosphorus phosphorene oxidation surface functionalization edge functionalization DFT binding energy shift
ISSN号	1944-8244
通讯作者	Warren, SC (reprint author), Univ North Carolina Chapel Hill, Dept Chem, Chapel Hill, NC 27599 USA. ; Warren, SC (reprint author), Univ North Carolina Chapel Hill, Dept Appl Phys Sci, Chapel Hill, NC 27599 USA.
中文摘要	Phosphorene is emerging as an important two-dimensional semiconductor, but controlling the surface chemistry of phosphorene remains a significant challenge. Here, we show that controlled oxidation of phosphorene determines the composition and spatial distribution of the resulting oxide. We used X-ray photoemission spectroscopy to measure the binding energy shifts that accompany oxidation. We interpreted these spectra by calculating the binding energy shift for 24 likely bonding configurations, including phosphorus oxides and hydroxides located on the basal surface or edges of flakes. After brief exposure to high-purity oxygen or high-purity water vapor at room temperature, we observed phosphorus in the +1 and +2 oxidation states; longer exposures led to a large population of phosphorus in the +3 oxidation state. To provide insight into the spatial distribution of the oxide, transmission electron microscopy was performed at several stages during the oxidation. We found crucial differences between oxygen and water oxidants: while pure oxygen produced an oxide layer on the van der Waals surface, water oxidized the material at pre-existing defects such as edges or steps. We propose a mechanism based on the thermodynamics of electron transfer to interpret these observations. This work opens a route to functionalize the basal surface or edges of two-dimensional (2D) black phosphorus through site-selective chemical reactions and presents the opportunity to explore the synthesis of 2D phosphorene oxide by oxidation.
学科主题	Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary
收录类别	SCI
资助信息	UNC Chapel Hill startup funds; ACS Petroleum Research Fund [55497-DNI3]; NSFC [51331006, U1537204]; NSF/AFOSR EFRI 2-DARE Grant [EFMA-1433459]; Liaoning Province Doctor Startup Fund [201601325]; Liaoning Shihua University Grant [2016XJJ-044]; National Science Foundation as part of the National Nanotechnology Coordinated Infrastructure, NNCI [ECCS-1542015]; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001011]
语种	英语
公开日期	2017-08-17
内容类型	期刊论文
源URL	[http://ir.imr.ac.cn/handle/321006/78232]
专题	金属研究所_中国科学院金属研究所
推荐引用方式 GB/T 7714	Kuntz, Kaci L.,Wells, Rebekah A.,Hu, Jun,et al. Control of Surface and Edge Oxidation on Phosphorene[J]. ACS APPLIED MATERIALS & INTERFACES,2017,9(10):9126-9135.
APA	Kuntz, Kaci L..,Wells, Rebekah A..,Hu, Jun.,Yang, Teng.,Dong, Baojuan.,...&Warren, Scott C..(2017).Control of Surface and Edge Oxidation on Phosphorene.ACS APPLIED MATERIALS & INTERFACES,9(10),9126-9135.
MLA	Kuntz, Kaci L.,et al."Control of Surface and Edge Oxidation on Phosphorene".ACS APPLIED MATERIALS & INTERFACES 9.10(2017):9126-9135.