DOI: 10.1073/pnas.1917237117
论文题名: Defects in nanosilica catalytically convert CO2 to methane without any metal and ligand
作者: Mishra A.K. ; Belgamwar R. ; Jana R. ; Datta A. ; Polshettiwar V.
刊名: Proceedings of the National Academy of Sciences of the United States of America
ISSN: 0027-8424
出版年: 2020
卷: 117, 期: 12 起始页码: 6383
结束页码: 6390
语种: 英语
英文关键词: Climate change
; CO2
; Defects
; Methane
; Nanosilica
Scopus关键词: carbon dioxide
; dendritic fibrous nanosilica
; hydrogen
; ligand
; magnesium
; magnesium oxide
; magnesium silicide
; metal
; methane
; silica nanoparticle
; unclassified drug
; adsorption
; Article
; catalysis
; controlled study
; density functional theory
; diffuse reflectance infrared Fourier transform spectroscopy
; diffuse reflectance spectroscopy
; dissociation
; electron diffraction
; electron spin resonance
; energy dispersive X ray spectroscopy
; hydrogenation
; nanocatalyst
; photoluminescence
; priority journal
; reaction optimization
; surface area
; thermogravimetry
; transmission electron microscopy
; ultraviolet visible diffuse reflectance spectroscopy
; ultraviolet visible spectroscopy
; X ray photoemission spectroscopy
; X ray powder diffraction
英文摘要: Active and stable metal-free heterogeneous catalysts for CO2 fixation are required to reduce the current high level of carbon dioxide in the atmosphere, which is driving climate change. In this work, we show that defects in nanosilica (E′ centers, oxygen vacancies, and nonbridging oxygen hole centers) convert CO2 to methane with excellent productivity and selectivity. Neither metal nor complex organic ligands were required, and the defect alone acted as catalytic sites for carbon dioxide activation and hydrogen dissociation and their cooperative action converted CO2 to methane. Unlike metal catalysts, which become deactivated with time, the defect-containing nanosilica showed significantly better stability. Notably, the catalyst can be regenerated by simple heating in the air without the need for hydrogen gas. Surprisingly, the catalytic activity for methane production increased significantly after every regeneration cycle, reaching more than double the methane production rate after eight regeneration cycles. This activated catalyst remained stable for more than 200 h. Detailed understanding of the role of the various defect sites in terms of their concentrations and proximities as well as their cooperativity in activating CO2 and dissociating hydrogen to produce methane was achieved. © 2020 National Academy of Sciences. All rights reserved. Citation statistics:
资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/164277
Appears in Collections: 气候变化与战略
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作者单位: Mishra, A.K., Department of Chemical Sciences, Tata Institute of Fundamental Research, Mumbai, 400005, India; Belgamwar, R., Department of Chemical Sciences, Tata Institute of Fundamental Research, Mumbai, 400005, India; Jana, R., School of Chemical Sciences, Indian Association for the Cultivation of Science, Kolkata, 700032, India; Datta, A., School of Chemical Sciences, Indian Association for the Cultivation of Science, Kolkata, 700032, India; Polshettiwar, V., Department of Chemical Sciences, Tata Institute of Fundamental Research, Mumbai, 400005, India
Recommended Citation:
Mishra A.K.,Belgamwar R.,Jana R.,et al. Defects in nanosilica catalytically convert CO2 to methane without any metal and ligand[J]. Proceedings of the National Academy of Sciences of the United States of America,2020-01-01,117(12)