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C: Surfaces, Interfaces, Porous Materials, and Catalysis x
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The Role of ReO Species in Ni-Re/AlO Catalyst for Amination of Monoethanolamine Lei Ma, Keju Sun, Mi Luo, Li Yan, Zheng Jiang, An-Hui Lu, and Yunjie Ding J. Phys. Chem. C, Just Accepted Manuscript • DOI: 10.1021/acs.jpcc.8b06748 • Publication Date (Web): 24 Sep 2018 Downloaded from http://pubs.acs.org on September 25, 2018
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The Journal of Physical Chemistry
The Role of ReOx Species in Ni-Re/Al2O3 Catalyst for Amination of Monoethanolamine Lei Ma,abd Keju Sun,e Mi Luo,f Li Yan,*a Zheng Jiang,f An-Hui Lu,b and Yunjie Ding*ac a
Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese
Academy of Sciences, 457 Zhongshan Road, Dalian, 116023, China. E-mail:
[email protected];
[email protected]; Fax: +86 411 84379143; Tel: +86 411 84379143 b
State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of
Technology, No. 2 Linggong Road, Dalian 116024, P. R. China c
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of
Sciences, 457 Zhongshan Road, Dalian, 116023, China d
University of Chinese Academy of Sciences, No.19A Yuquan Road, Beijing 100049, China
e
Key Laboratory of Applied Chemistry, College of Environmental and Chemical Engineering,
Yanshan University, Qinhuangdao 066004, China f
Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese
Academy of Sciences, Shanghai 201204, China
Abstract: The role of ReOx species in Ni-Re/Al2O3 catalyst for amination of monoethanolamine (MEA) were investigated using a combination of experimental
(Raman
spectroscopy,
in-situ
XPS,
TEM,
XRD,
STEM-EDX line scan, and EXAFS) and theoretical (DFT) methods. Characterization and simulation results indicate that rhenium oxide specie prefers to atomically disperse on the surface of NiO in calcined Ni-Re/Al2O3 catalyst. After reduction, the surface of metallic Ni is decorated by ReOx with multiple valence states, meanwhile, a small amount of Ni-Re alloy was detected by EXAFS. DFT results indicate that
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different valent ReOx species in Ni-Re/Al2O3 catalyst have different functions during reaction. The high valent ReOx (x≥3) distributed on the Ni0 particle surface play an important role in decreasing the surface energy of Ni0 particle, thus stabilizing Ni0 particles against sintering and increasing the lifetime of Ni-Re/Al2O3 catalyst during amination reaction. The synergistic effect between Ni0 and low valent ReOx (x
