Dramatic enhancement of CO 2 uptake by poly(ethyleneimine) using zirconosilicate supports

Yasutaka Kuwahara; Dun Yen Kang; John R. Copeland; Nicholas A. Brunelli; Stephanie A. Didas; Praveen Bollini; Carsten Sievers; Takashi Kamegawa; Hiromi Yamashita; Christopher W. Jones

doi:10.1021/ja303136e

Dramatic enhancement of CO ₂ uptake by poly(ethyleneimine) using zirconosilicate supports

Yasutaka Kuwahara, Dun Yen Kang, John R. Copeland, Nicholas A. Brunelli, Stephanie A. Didas, Praveen Bollini, Carsten Sievers, Takashi Kamegawa, Hiromi Yamashita, Christopher W. Jones

Chemical Engineering and Materials Science

Research output: Contribution to journal › Article

154 Scopus citations

Abstract

The CO ₂ adsorption characteristics of prototypical poly(ethyleneimine)/silica composite adsorbents can be drastically enhanced by altering the acid/base properties of the oxide support via incorporation of Zr into the silica support. Introduction of an optimal amount of Zr resulted in a significant improvement in the CO ₂ capacity and amine efficiency under dilute (simulated flue gas) and ultradilute (simulated ambient air) conditions. Adsorption experiments combined with detailed characterization by thermogravimetric analysis, temperature-programmed desorption, and in situ FT-IR spectroscopy clearly demonstrate a stabilizing effect of amphoteric Zr sites that enhances the adsorbent capacity, regenerability, and stability over continued recycling. It is suggested that the important role of the surface properties of the oxide support in these polymer/oxide composite adsorbents has been largely overlooked and that the properties may be even further enhanced in the future by tuning the acid/base properties of the support.

Original language	English (US)
Pages (from-to)	10757-10760
Number of pages	4
Journal	Journal of the American Chemical Society
Volume	134
Issue number	26
DOIs	https://doi.org/10.1021/ja303136e
State	Published - Jul 4 2012

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Dramatic enhancement of CO ₂ uptake by poly(ethyleneimine) using zirconosilicate supports. / Kuwahara, Yasutaka; Kang, Dun Yen; Copeland, John R.; Brunelli, Nicholas A.; Didas, Stephanie A.; Bollini, Praveen; Sievers, Carsten; Kamegawa, Takashi; Yamashita, Hiromi; Jones, Christopher W.

In: Journal of the American Chemical Society, Vol. 134, No. 26, 04.07.2012, p. 10757-10760.

Research output: Contribution to journal › Article

Kuwahara, Yasutaka ; Kang, Dun Yen ; Copeland, John R. ; Brunelli, Nicholas A. ; Didas, Stephanie A. ; Bollini, Praveen ; Sievers, Carsten ; Kamegawa, Takashi ; Yamashita, Hiromi ; Jones, Christopher W. / Dramatic enhancement of CO ₂ uptake by poly(ethyleneimine) using zirconosilicate supports. In: Journal of the American Chemical Society. 2012 ; Vol. 134, No. 26. pp. 10757-10760.

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title = "Dramatic enhancement of CO 2 uptake by poly(ethyleneimine) using zirconosilicate supports",

abstract = "The CO 2 adsorption characteristics of prototypical poly(ethyleneimine)/silica composite adsorbents can be drastically enhanced by altering the acid/base properties of the oxide support via incorporation of Zr into the silica support. Introduction of an optimal amount of Zr resulted in a significant improvement in the CO 2 capacity and amine efficiency under dilute (simulated flue gas) and ultradilute (simulated ambient air) conditions. Adsorption experiments combined with detailed characterization by thermogravimetric analysis, temperature-programmed desorption, and in situ FT-IR spectroscopy clearly demonstrate a stabilizing effect of amphoteric Zr sites that enhances the adsorbent capacity, regenerability, and stability over continued recycling. It is suggested that the important role of the surface properties of the oxide support in these polymer/oxide composite adsorbents has been largely overlooked and that the properties may be even further enhanced in the future by tuning the acid/base properties of the support.",

author = "Yasutaka Kuwahara and Kang, {Dun Yen} and Copeland, {John R.} and Brunelli, {Nicholas A.} and Didas, {Stephanie A.} and Praveen Bollini and Carsten Sievers and Takashi Kamegawa and Hiromi Yamashita and Jones, {Christopher W.}",

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AU - Kuwahara, Yasutaka

AU - Kang, Dun Yen

AU - Copeland, John R.

AU - Brunelli, Nicholas A.

AU - Didas, Stephanie A.

AU - Bollini, Praveen

AU - Sievers, Carsten

AU - Kamegawa, Takashi

AU - Yamashita, Hiromi

AU - Jones, Christopher W.

PY - 2012/7/4

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N2 - The CO 2 adsorption characteristics of prototypical poly(ethyleneimine)/silica composite adsorbents can be drastically enhanced by altering the acid/base properties of the oxide support via incorporation of Zr into the silica support. Introduction of an optimal amount of Zr resulted in a significant improvement in the CO 2 capacity and amine efficiency under dilute (simulated flue gas) and ultradilute (simulated ambient air) conditions. Adsorption experiments combined with detailed characterization by thermogravimetric analysis, temperature-programmed desorption, and in situ FT-IR spectroscopy clearly demonstrate a stabilizing effect of amphoteric Zr sites that enhances the adsorbent capacity, regenerability, and stability over continued recycling. It is suggested that the important role of the surface properties of the oxide support in these polymer/oxide composite adsorbents has been largely overlooked and that the properties may be even further enhanced in the future by tuning the acid/base properties of the support.

AB - The CO 2 adsorption characteristics of prototypical poly(ethyleneimine)/silica composite adsorbents can be drastically enhanced by altering the acid/base properties of the oxide support via incorporation of Zr into the silica support. Introduction of an optimal amount of Zr resulted in a significant improvement in the CO 2 capacity and amine efficiency under dilute (simulated flue gas) and ultradilute (simulated ambient air) conditions. Adsorption experiments combined with detailed characterization by thermogravimetric analysis, temperature-programmed desorption, and in situ FT-IR spectroscopy clearly demonstrate a stabilizing effect of amphoteric Zr sites that enhances the adsorbent capacity, regenerability, and stability over continued recycling. It is suggested that the important role of the surface properties of the oxide support in these polymer/oxide composite adsorbents has been largely overlooked and that the properties may be even further enhanced in the future by tuning the acid/base properties of the support.

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