Selective nitrogen capture by porous hybrid materials containing accessible transition metal ion sites

Ji Woong Yoon, Hyunju Chang, Seung Joon Lee, Young Kyu Hwang, Do Young Hong, Su Kyung Lee, Ji Sun Lee, Seunghun Jang, Tae Ung Yoon, Kijeong Kwac, Yousung Jung, Renjith S. Pillai, Florian Faucher, Alexandre Vimont, Marco Daturi, Gérard Férey, Christian Serre, Guillaume Maurin, Youn-Sang Bae, Jong San Chang

Research output: Contribution to journalArticle

45 Citations (Scopus)

Abstract

Selective dinitrogen binding to transition metal ions mainly covers two strategic domains: biological nitrogen fixation catalysed by metalloenzyme nitrogenases, and adsorptive purification of natural gas and air. Many transition metal-dinitrogen complexes have been envisaged for biomimetic nitrogen fixation to produce ammonia. Inspired by this concept, here we report mesoporous metal-organic framework materials containing accessible Cr(III) sites, able to thermodynamically capture N2 over CH4 and O2. This fundamental study integrating advanced experimental and computational tools confirmed that the separation mechanism for both N2/CH4 and N2/O2 gas mixtures is driven by the presence of these unsaturated Cr(III) sites that allows a much stronger binding of N2 over the two other gases. Besides the potential breakthrough in adsorption-based technologies, this proof of concept could open new horizons to address several challenges in chemistry, including the design of heterogeneous biomimetic catalysts through nitrogen fixation.

Original languageEnglish
Pages (from-to)526-531
Number of pages6
JournalNature materials
Volume16
Issue number5
DOIs
Publication statusPublished - 2017 May 1

Fingerprint

Nitrogen fixation
nitrogenation
Hybrid materials
Transition metals
Metal ions
Porous materials
metal ions
Nitrogen
transition metals
biomimetics
Biomimetics
nitrogen
Nitrogenase
natural gas
Metal complexes
organic materials
Ammonia
purification
Gas mixtures
horizon

All Science Journal Classification (ASJC) codes

  • Chemistry(all)
  • Materials Science(all)
  • Condensed Matter Physics
  • Mechanics of Materials
  • Mechanical Engineering

Cite this

Yoon, J. W., Chang, H., Lee, S. J., Hwang, Y. K., Hong, D. Y., Lee, S. K., ... Chang, J. S. (2017). Selective nitrogen capture by porous hybrid materials containing accessible transition metal ion sites. Nature materials, 16(5), 526-531. https://doi.org/10.1038/nmat4825
Yoon, Ji Woong ; Chang, Hyunju ; Lee, Seung Joon ; Hwang, Young Kyu ; Hong, Do Young ; Lee, Su Kyung ; Lee, Ji Sun ; Jang, Seunghun ; Yoon, Tae Ung ; Kwac, Kijeong ; Jung, Yousung ; Pillai, Renjith S. ; Faucher, Florian ; Vimont, Alexandre ; Daturi, Marco ; Férey, Gérard ; Serre, Christian ; Maurin, Guillaume ; Bae, Youn-Sang ; Chang, Jong San. / Selective nitrogen capture by porous hybrid materials containing accessible transition metal ion sites. In: Nature materials. 2017 ; Vol. 16, No. 5. pp. 526-531.
@article{0d3f1b25f4be409cb83345ef89555607,
title = "Selective nitrogen capture by porous hybrid materials containing accessible transition metal ion sites",
abstract = "Selective dinitrogen binding to transition metal ions mainly covers two strategic domains: biological nitrogen fixation catalysed by metalloenzyme nitrogenases, and adsorptive purification of natural gas and air. Many transition metal-dinitrogen complexes have been envisaged for biomimetic nitrogen fixation to produce ammonia. Inspired by this concept, here we report mesoporous metal-organic framework materials containing accessible Cr(III) sites, able to thermodynamically capture N2 over CH4 and O2. This fundamental study integrating advanced experimental and computational tools confirmed that the separation mechanism for both N2/CH4 and N2/O2 gas mixtures is driven by the presence of these unsaturated Cr(III) sites that allows a much stronger binding of N2 over the two other gases. Besides the potential breakthrough in adsorption-based technologies, this proof of concept could open new horizons to address several challenges in chemistry, including the design of heterogeneous biomimetic catalysts through nitrogen fixation.",
author = "Yoon, {Ji Woong} and Hyunju Chang and Lee, {Seung Joon} and Hwang, {Young Kyu} and Hong, {Do Young} and Lee, {Su Kyung} and Lee, {Ji Sun} and Seunghun Jang and Yoon, {Tae Ung} and Kijeong Kwac and Yousung Jung and Pillai, {Renjith S.} and Florian Faucher and Alexandre Vimont and Marco Daturi and G{\'e}rard F{\'e}rey and Christian Serre and Guillaume Maurin and Youn-Sang Bae and Chang, {Jong San}",
year = "2017",
month = "5",
day = "1",
doi = "10.1038/nmat4825",
language = "English",
volume = "16",
pages = "526--531",
journal = "Nature Materials",
issn = "1476-1122",
publisher = "Nature Publishing Group",
number = "5",

}

Yoon, JW, Chang, H, Lee, SJ, Hwang, YK, Hong, DY, Lee, SK, Lee, JS, Jang, S, Yoon, TU, Kwac, K, Jung, Y, Pillai, RS, Faucher, F, Vimont, A, Daturi, M, Férey, G, Serre, C, Maurin, G, Bae, Y-S & Chang, JS 2017, 'Selective nitrogen capture by porous hybrid materials containing accessible transition metal ion sites', Nature materials, vol. 16, no. 5, pp. 526-531. https://doi.org/10.1038/nmat4825

Selective nitrogen capture by porous hybrid materials containing accessible transition metal ion sites. / Yoon, Ji Woong; Chang, Hyunju; Lee, Seung Joon; Hwang, Young Kyu; Hong, Do Young; Lee, Su Kyung; Lee, Ji Sun; Jang, Seunghun; Yoon, Tae Ung; Kwac, Kijeong; Jung, Yousung; Pillai, Renjith S.; Faucher, Florian; Vimont, Alexandre; Daturi, Marco; Férey, Gérard; Serre, Christian; Maurin, Guillaume; Bae, Youn-Sang; Chang, Jong San.

In: Nature materials, Vol. 16, No. 5, 01.05.2017, p. 526-531.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Selective nitrogen capture by porous hybrid materials containing accessible transition metal ion sites

AU - Yoon, Ji Woong

AU - Chang, Hyunju

AU - Lee, Seung Joon

AU - Hwang, Young Kyu

AU - Hong, Do Young

AU - Lee, Su Kyung

AU - Lee, Ji Sun

AU - Jang, Seunghun

AU - Yoon, Tae Ung

AU - Kwac, Kijeong

AU - Jung, Yousung

AU - Pillai, Renjith S.

AU - Faucher, Florian

AU - Vimont, Alexandre

AU - Daturi, Marco

AU - Férey, Gérard

AU - Serre, Christian

AU - Maurin, Guillaume

AU - Bae, Youn-Sang

AU - Chang, Jong San

PY - 2017/5/1

Y1 - 2017/5/1

N2 - Selective dinitrogen binding to transition metal ions mainly covers two strategic domains: biological nitrogen fixation catalysed by metalloenzyme nitrogenases, and adsorptive purification of natural gas and air. Many transition metal-dinitrogen complexes have been envisaged for biomimetic nitrogen fixation to produce ammonia. Inspired by this concept, here we report mesoporous metal-organic framework materials containing accessible Cr(III) sites, able to thermodynamically capture N2 over CH4 and O2. This fundamental study integrating advanced experimental and computational tools confirmed that the separation mechanism for both N2/CH4 and N2/O2 gas mixtures is driven by the presence of these unsaturated Cr(III) sites that allows a much stronger binding of N2 over the two other gases. Besides the potential breakthrough in adsorption-based technologies, this proof of concept could open new horizons to address several challenges in chemistry, including the design of heterogeneous biomimetic catalysts through nitrogen fixation.

AB - Selective dinitrogen binding to transition metal ions mainly covers two strategic domains: biological nitrogen fixation catalysed by metalloenzyme nitrogenases, and adsorptive purification of natural gas and air. Many transition metal-dinitrogen complexes have been envisaged for biomimetic nitrogen fixation to produce ammonia. Inspired by this concept, here we report mesoporous metal-organic framework materials containing accessible Cr(III) sites, able to thermodynamically capture N2 over CH4 and O2. This fundamental study integrating advanced experimental and computational tools confirmed that the separation mechanism for both N2/CH4 and N2/O2 gas mixtures is driven by the presence of these unsaturated Cr(III) sites that allows a much stronger binding of N2 over the two other gases. Besides the potential breakthrough in adsorption-based technologies, this proof of concept could open new horizons to address several challenges in chemistry, including the design of heterogeneous biomimetic catalysts through nitrogen fixation.

UR - http://www.scopus.com/inward/record.url?scp=85007092545&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85007092545&partnerID=8YFLogxK

U2 - 10.1038/nmat4825

DO - 10.1038/nmat4825

M3 - Article

VL - 16

SP - 526

EP - 531

JO - Nature Materials

JF - Nature Materials

SN - 1476-1122

IS - 5

ER -