Selectivity and direct visualization of carbon dioxide and sulfur dioxide in a decorated porous host

Sihai Yang; Junliang Sun; Anibal J. Ramirez-Cuesta; Samantha K. Callear; William I.F. David; Daniel P. Anderson; Ruth Newby; Alexander J. Blake; Julia E. Parker; Chiu C. Tang; Martin Schröder

doi:10.1038/nchem.1457

Selectivity and direct visualization of carbon dioxide and sulfur dioxide in a decorated porous host

Sihai Yang, Junliang Sun, Anibal J. Ramirez-Cuesta, Samantha K. Callear, William I.F. David, Daniel P. Anderson, Ruth Newby, Alexander J. Blake, Julia E. Parker, Chiu C. Tang, Martin Schröder

Research output: Contribution to journal › Article › peer-review

469 Scopus citations

Abstract

Understanding the mechanism by which porous solids trap harmful gases such as CO ₂ and SO ₂ is essential for the design of new materials for their selective removal. Materials functionalized with amine groups dominate this field, largely because of their potential to form carbamates through H ₂N(δ ^-) ⋯C(δ ⁺)O ₂ interactions, thereby trapping CO ₂ covalently. However, the use of these materials is energy-intensive, with significant environmental impact. Here, we report a non-amine-containing porous solid (NOTT-300) in which hydroxyl groups within pores bind CO ₂ and SO ₂ selectively. In situ powder X-ray diffraction and inelastic neutron scattering studies, combined with modelling, reveal that hydroxyl groups bind CO ₂ and SO ₂ through the formation of O=C(S)=O(δ ^-)⋯H(δ ⁺)-O hydrogen bonds, which are reinforced by weak supramolecular interactions with C-H atoms on the aromatic rings of the framework. This offers the potential for the application of new 'easy-on/easy-off' capture systems for CO ₂ and SO ₂ that carry fewer economic and environmental penalties.

Original language	English
Pages (from-to)	887-894
Number of pages	8
Journal	Nature Chemistry
Volume	4
Issue number	11
DOIs	https://doi.org/10.1038/nchem.1457
State	Published - Nov 2012
Externally published	Yes

Funding

S.Y. acknowledges receipt of a Leverhulme Trust Early Career Research Fellowship, and M.S. the receipt of an ERC Advanced Grant and EPSRC Programme Grant. The authors acknowledge funding from the EPSRC and the University of Nottingham, and are especially grateful to Diamond Light Source and ISIS Neutron Centre for access to Beamlines I11 and TOSCA, respectively. The authors thank the user support group at ISIS (C. Goodway and M. Kibble) for technical help at ISIS beamline TOSCA, M. Fray for help with TEM measurements, and K. Refson for discussions on DFT modelling. J.S. acknowledges support from the Swedish Research Council (VR).

Funders	Funder number
Diamond Light Source
Engineering and Physical Sciences Research Council
Leverhulme Trust
European Research Council
University of Nottingham
Vetenskapsrådet

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1038/nchem.1457

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title = "Selectivity and direct visualization of carbon dioxide and sulfur dioxide in a decorated porous host",

abstract = "Understanding the mechanism by which porous solids trap harmful gases such as CO 2 and SO 2 is essential for the design of new materials for their selective removal. Materials functionalized with amine groups dominate this field, largely because of their potential to form carbamates through H 2N(δ -) ⋯C(δ +)O 2 interactions, thereby trapping CO 2 covalently. However, the use of these materials is energy-intensive, with significant environmental impact. Here, we report a non-amine-containing porous solid (NOTT-300) in which hydroxyl groups within pores bind CO 2 and SO 2 selectively. In situ powder X-ray diffraction and inelastic neutron scattering studies, combined with modelling, reveal that hydroxyl groups bind CO 2 and SO 2 through the formation of O=C(S)=O(δ -)⋯H(δ +)-O hydrogen bonds, which are reinforced by weak supramolecular interactions with C-H atoms on the aromatic rings of the framework. This offers the potential for the application of new 'easy-on/easy-off' capture systems for CO 2 and SO 2 that carry fewer economic and environmental penalties.",

author = "Sihai Yang and Junliang Sun and Ramirez-Cuesta, {Anibal J.} and Callear, {Samantha K.} and David, {William I.F.} and Anderson, {Daniel P.} and Ruth Newby and Blake, {Alexander J.} and Parker, {Julia E.} and Tang, {Chiu C.} and Martin Schr{\"o}der",

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doi = "10.1038/nchem.1457",

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AU - Sun, Junliang

AU - Ramirez-Cuesta, Anibal J.

AU - Callear, Samantha K.

AU - David, William I.F.

AU - Anderson, Daniel P.

AU - Newby, Ruth

AU - Blake, Alexander J.

AU - Parker, Julia E.

AU - Tang, Chiu C.

AU - Schröder, Martin

PY - 2012/11

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N2 - Understanding the mechanism by which porous solids trap harmful gases such as CO 2 and SO 2 is essential for the design of new materials for their selective removal. Materials functionalized with amine groups dominate this field, largely because of their potential to form carbamates through H 2N(δ -) ⋯C(δ +)O 2 interactions, thereby trapping CO 2 covalently. However, the use of these materials is energy-intensive, with significant environmental impact. Here, we report a non-amine-containing porous solid (NOTT-300) in which hydroxyl groups within pores bind CO 2 and SO 2 selectively. In situ powder X-ray diffraction and inelastic neutron scattering studies, combined with modelling, reveal that hydroxyl groups bind CO 2 and SO 2 through the formation of O=C(S)=O(δ -)⋯H(δ +)-O hydrogen bonds, which are reinforced by weak supramolecular interactions with C-H atoms on the aromatic rings of the framework. This offers the potential for the application of new 'easy-on/easy-off' capture systems for CO 2 and SO 2 that carry fewer economic and environmental penalties.

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Selectivity and direct visualization of carbon dioxide and sulfur dioxide in a decorated porous host

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UN SDGs

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