Abstract
Due to integrated advantages in electrochemical functionalities for energy conversion, 2D nonlayered heterostructure nanosheets offer new and fascinating opportunities for electrocatalysis but their fabrication is challenging when compared with the widely studied 2D layered heterostructure. Herein, a bottom-up approach is established for facile synthesis of holey 2D transition metal carbide/nitride heterostructure nanosheets (h-TMCN) with regulated hole sizes by controlled thermal annealing of the Mo/Zn bimetallic imidazolate frameworks (Mo/Zn BIFs). Ex situ phase and structural identifications disclose that the Mo/Zn BIFs precursor experiences interconnected three steps of transformation to produce h-TMCN. Especially, the slow successive solid-state diffusion of nitrogen and carbon into immediate noncrystalline molybdenum oxides allows the intergrowth of Mo 2 C and Mo 2 N into the 2D nonlayered heterostructure. X-ray fine structure analysis coupled with high resolution X-ray photoelectron spectroscopy demonstrate that Mo 2 C and Mo 2 N in the microdomains can chemically bond with each other, producing the abundant active N–Mo–C interfaces toward water splitting. Consequently, h-TMCN affords low overpotentials, high turnover frequencies, rapid charge transfer, and superior long-term stability toward electrocatalytic water oxidation. The present work demonstrates the feasibility of developing a broad range of 2D nonlayered heterostructures for high efficiency chemical energy conversion.
| Original language | English |
|---|---|
| Article number | 1803768 |
| Journal | Advanced Energy Materials |
| DOIs | |
| Publication status | Published - 1 Jan 2019 |
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Keywords
- 2D nonlayered structure
- carbide
- heterostructure
- nitride
- water splitting
ASJC Scopus subject areas
- Renewable Energy, Sustainability and the Environment
- Materials Science(all)
Cite this
Rational Design of Holey 2D Nonlayered Transition Metal Carbide/Nitride Heterostructure Nanosheets for Highly Efficient Water Oxidation. / Kou, Zongkui; Wang, Tingting; Gu, Qilin; Xiong, Mo; Zheng, Lirong; Li, Xin; Pan, Zhenghui; Chen, Hao; Verpoort, Francis; Cheetham, Anthony K.; Mu, Shichun; Wang, John.
In: Advanced Energy Materials, 01.01.2019.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Rational Design of Holey 2D Nonlayered Transition Metal Carbide/Nitride Heterostructure Nanosheets for Highly Efficient Water Oxidation
AU - Kou, Zongkui
AU - Wang, Tingting
AU - Gu, Qilin
AU - Xiong, Mo
AU - Zheng, Lirong
AU - Li, Xin
AU - Pan, Zhenghui
AU - Chen, Hao
AU - Verpoort, Francis
AU - Cheetham, Anthony K.
AU - Mu, Shichun
AU - Wang, John
PY - 2019/1/1
Y1 - 2019/1/1
N2 - Due to integrated advantages in electrochemical functionalities for energy conversion, 2D nonlayered heterostructure nanosheets offer new and fascinating opportunities for electrocatalysis but their fabrication is challenging when compared with the widely studied 2D layered heterostructure. Herein, a bottom-up approach is established for facile synthesis of holey 2D transition metal carbide/nitride heterostructure nanosheets (h-TMCN) with regulated hole sizes by controlled thermal annealing of the Mo/Zn bimetallic imidazolate frameworks (Mo/Zn BIFs). Ex situ phase and structural identifications disclose that the Mo/Zn BIFs precursor experiences interconnected three steps of transformation to produce h-TMCN. Especially, the slow successive solid-state diffusion of nitrogen and carbon into immediate noncrystalline molybdenum oxides allows the intergrowth of Mo 2 C and Mo 2 N into the 2D nonlayered heterostructure. X-ray fine structure analysis coupled with high resolution X-ray photoelectron spectroscopy demonstrate that Mo 2 C and Mo 2 N in the microdomains can chemically bond with each other, producing the abundant active N–Mo–C interfaces toward water splitting. Consequently, h-TMCN affords low overpotentials, high turnover frequencies, rapid charge transfer, and superior long-term stability toward electrocatalytic water oxidation. The present work demonstrates the feasibility of developing a broad range of 2D nonlayered heterostructures for high efficiency chemical energy conversion.
AB - Due to integrated advantages in electrochemical functionalities for energy conversion, 2D nonlayered heterostructure nanosheets offer new and fascinating opportunities for electrocatalysis but their fabrication is challenging when compared with the widely studied 2D layered heterostructure. Herein, a bottom-up approach is established for facile synthesis of holey 2D transition metal carbide/nitride heterostructure nanosheets (h-TMCN) with regulated hole sizes by controlled thermal annealing of the Mo/Zn bimetallic imidazolate frameworks (Mo/Zn BIFs). Ex situ phase and structural identifications disclose that the Mo/Zn BIFs precursor experiences interconnected three steps of transformation to produce h-TMCN. Especially, the slow successive solid-state diffusion of nitrogen and carbon into immediate noncrystalline molybdenum oxides allows the intergrowth of Mo 2 C and Mo 2 N into the 2D nonlayered heterostructure. X-ray fine structure analysis coupled with high resolution X-ray photoelectron spectroscopy demonstrate that Mo 2 C and Mo 2 N in the microdomains can chemically bond with each other, producing the abundant active N–Mo–C interfaces toward water splitting. Consequently, h-TMCN affords low overpotentials, high turnover frequencies, rapid charge transfer, and superior long-term stability toward electrocatalytic water oxidation. The present work demonstrates the feasibility of developing a broad range of 2D nonlayered heterostructures for high efficiency chemical energy conversion.
KW - 2D nonlayered structure
KW - carbide
KW - heterostructure
KW - nitride
KW - water splitting
UR - http://www.scopus.com/inward/record.url?scp=85062356129&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85062356129&partnerID=8YFLogxK
U2 - 10.1002/aenm.201803768
DO - 10.1002/aenm.201803768
M3 - Article
JO - Advanced Energy Materials
JF - Advanced Energy Materials
SN - 1614-6832
M1 - 1803768
ER -