Runaway Carbon Dioxide Conversion Leads to Enhanced Uptake in a Nanohybrid Form of Porous Magnesium Borohydride

Noemie Marius; Thomas Gennett; Sohee Jeong; Phillip Milner; Liwen Wan; Yi-Sheng Liu; Julia Oktawiec; Edmond Zaia; Alexander Forse; Jinghua Guo; David Prendergast; Jeffrey Long; Jeffrey Urban

doi:10.1002/adma.201904252

Runaway Carbon Dioxide Conversion Leads to Enhanced Uptake in a Nanohybrid Form of Porous Magnesium Borohydride

Noemie Marius, Thomas Gennett, Sohee Jeong, Phillip Milner, Liwen Wan, Yi-Sheng Liu, Julia Oktawiec, Edmond Zaia, Alexander Forse, Jinghua Guo, David Prendergast, Jeffrey Long, Jeffrey Urban

Chemistry and Nanoscience

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

11 Scopus Citations

Abstract

Leveraging molecular-level controls to enhance CO₂ capture in solid-state materials has received tremendous attention in recent years. Here, a new class of hybrid nanomaterials constructed from intrinsically porous γ-Mg(BH₄)₂ nanocrystals and reduced graphene oxide (MBHg) is described. These nanomaterials exhibit kinetically controlled, irreversible CO₂ uptake profiles with high uptake capacities (>19.9 mmol g⁻¹) at low partial pressures and temperatures between 40 and 100 °C. Systematic experiments and first-principles calculations reveal the mechanism of reaction between CO₂ and MBHg and unveil the role of chemically activated, metastable (BH₃-HCOO)⁻ centers that display more thermodynamically favorable reaction and potentially faster reaction kinetics than the parent BH₄ ⁻ centers. Overall, it is demonstrated that size reduction to the nanoscale regime and the generation of reactive, metastable intermediates improve the CO₂ uptake properties in metal borohydride nanomaterials.

Original language	American English
Article number	1904252
Number of pages	9
Journal	Advanced Materials
Volume	31
Issue number	44
DOIs	https://doi.org/10.1002/adma.201904252 https://doi.org/10.1002/adma.201904252
State	Published - 2019

Bibliographical note

Publisher Copyright:
© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

NREL Publication Number

NREL/JA-5900-74987

Keywords

carbon dioxide capture
kinetics
magnesium borohydride gamma phase (γ-Mg(BH ))
nanomaterials
reduced graphene oxide

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Marius, N., Gennett, T., Jeong, S., Milner, P., Wan, L., Liu, Y.-S., Oktawiec, J., Zaia, E., Forse, A., Guo, J., Prendergast, D., Long, J., & Urban, J. (2019). Runaway Carbon Dioxide Conversion Leads to Enhanced Uptake in a Nanohybrid Form of Porous Magnesium Borohydride. Advanced Materials, 31(44), Article 1904252. https://doi.org/10.1002/adma.201904252, https://doi.org/10.1002/adma.201904252

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title = "Runaway Carbon Dioxide Conversion Leads to Enhanced Uptake in a Nanohybrid Form of Porous Magnesium Borohydride",

abstract = "Leveraging molecular-level controls to enhance CO2 capture in solid-state materials has received tremendous attention in recent years. Here, a new class of hybrid nanomaterials constructed from intrinsically porous γ-Mg(BH4)2 nanocrystals and reduced graphene oxide (MBHg) is described. These nanomaterials exhibit kinetically controlled, irreversible CO2 uptake profiles with high uptake capacities (>19.9 mmol g−1) at low partial pressures and temperatures between 40 and 100 °C. Systematic experiments and first-principles calculations reveal the mechanism of reaction between CO2 and MBHg and unveil the role of chemically activated, metastable (BH3-HCOO)− centers that display more thermodynamically favorable reaction and potentially faster reaction kinetics than the parent BH4 − centers. Overall, it is demonstrated that size reduction to the nanoscale regime and the generation of reactive, metastable intermediates improve the CO2 uptake properties in metal borohydride nanomaterials.",

keywords = "carbon dioxide capture, kinetics, magnesium borohydride gamma phase (γ-Mg(BH )), nanomaterials, reduced graphene oxide",

author = "Noemie Marius and Thomas Gennett and Sohee Jeong and Phillip Milner and Liwen Wan and Yi-Sheng Liu and Julia Oktawiec and Edmond Zaia and Alexander Forse and Jinghua Guo and David Prendergast and Jeffrey Long and Jeffrey Urban",

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year = "2019",

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language = "American English",

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Marius, N , Gennett, T, Jeong, S, Milner, P, Wan, L, Liu, Y-S, Oktawiec, J, Zaia, E, Forse, A, Guo, J, Prendergast, D, Long, J & Urban, J 2019, 'Runaway Carbon Dioxide Conversion Leads to Enhanced Uptake in a Nanohybrid Form of Porous Magnesium Borohydride', Advanced Materials, vol. 31, no. 44, 1904252. https://doi.org/10.1002/adma.201904252, https://doi.org/10.1002/adma.201904252

TY - JOUR

T1 - Runaway Carbon Dioxide Conversion Leads to Enhanced Uptake in a Nanohybrid Form of Porous Magnesium Borohydride

AU - Marius, Noemie

AU - Gennett, Thomas

AU - Jeong, Sohee

AU - Milner, Phillip

AU - Wan, Liwen

AU - Liu, Yi-Sheng

AU - Oktawiec, Julia

AU - Zaia, Edmond

AU - Forse, Alexander

AU - Guo, Jinghua

AU - Prendergast, David

AU - Long, Jeffrey

AU - Urban, Jeffrey

PY - 2019

Y1 - 2019

N2 - Leveraging molecular-level controls to enhance CO2 capture in solid-state materials has received tremendous attention in recent years. Here, a new class of hybrid nanomaterials constructed from intrinsically porous γ-Mg(BH4)2 nanocrystals and reduced graphene oxide (MBHg) is described. These nanomaterials exhibit kinetically controlled, irreversible CO2 uptake profiles with high uptake capacities (>19.9 mmol g−1) at low partial pressures and temperatures between 40 and 100 °C. Systematic experiments and first-principles calculations reveal the mechanism of reaction between CO2 and MBHg and unveil the role of chemically activated, metastable (BH3-HCOO)− centers that display more thermodynamically favorable reaction and potentially faster reaction kinetics than the parent BH4 − centers. Overall, it is demonstrated that size reduction to the nanoscale regime and the generation of reactive, metastable intermediates improve the CO2 uptake properties in metal borohydride nanomaterials.

AB - Leveraging molecular-level controls to enhance CO2 capture in solid-state materials has received tremendous attention in recent years. Here, a new class of hybrid nanomaterials constructed from intrinsically porous γ-Mg(BH4)2 nanocrystals and reduced graphene oxide (MBHg) is described. These nanomaterials exhibit kinetically controlled, irreversible CO2 uptake profiles with high uptake capacities (>19.9 mmol g−1) at low partial pressures and temperatures between 40 and 100 °C. Systematic experiments and first-principles calculations reveal the mechanism of reaction between CO2 and MBHg and unveil the role of chemically activated, metastable (BH3-HCOO)− centers that display more thermodynamically favorable reaction and potentially faster reaction kinetics than the parent BH4 − centers. Overall, it is demonstrated that size reduction to the nanoscale regime and the generation of reactive, metastable intermediates improve the CO2 uptake properties in metal borohydride nanomaterials.

KW - carbon dioxide capture

KW - kinetics

KW - magnesium borohydride gamma phase (γ-Mg(BH ))

KW - nanomaterials

KW - reduced graphene oxide

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SN - 0935-9648

VL - 31

JO - Advanced Materials

JF - Advanced Materials

IS - 44

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ER -

Runaway Carbon Dioxide Conversion Leads to Enhanced Uptake in a Nanohybrid Form of Porous Magnesium Borohydride

Abstract

Bibliographical note

NREL Publication Number

Keywords

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