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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 CO 2 capture in solid-state materials has received tremendous attention in recent years. Here, a new class of hybrid nanomaterials constructed from intrinsically porous y-Mg(BH 4) 2 nanocrystals and reduced graphene oxide (MBHg) is described. These nanomaterials exhibit kinetically controlled, irreversible CO 2 uptake profiles with high uptake capacities (>19.9 mmol g -1) at low partial pressures and temperatures between 40 and 100 degrees C. Systematic experiments and first-principles calculations reveal the mechanism of reaction between CO 2 and MBHg and unveil the role of chemically activated, metastable (BH 3-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 CO 2 uptake properties in metal borohydride nanomaterials.

Authors:
 [1];  [2];  [3];  [1];  [4];  [1];  [5];  [6];  [7];  [8];  [1];  [4];  [1]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Cornell Univ., Ithaca, NY (United States)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
  4. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  5. Univ. of California, Berkeley, CA (United States)
  6. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  7. National Renewable Energy Lab. (NREL), Golden, CO (United States); Colorado School of Mines, Golden, CO (United States)
  8. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Santa Cruz, CA (United States)
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1567036
Alternate Identifier(s):
OSTI ID: 1563023
Report Number(s):
NREL/JA-5900-74987
Journal ID: ISSN 0935-9648
Grant/Contract Number:  
AC36-08GO28308; AC02‐05CH11231; SC0001015; AC36‐08GO28308; AC52‐07NA27344
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Name: Advanced Materials; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; carbon dioxide capture; kinetics; magnesium borohydride gamma phase; nanomaterials; reduced graphene oxide

Citation Formats

Jeong, Sohee, Milner, Phillip J., Wan, Liwen F., Liu, Yi-Sheng, Oktawiec, Julia, Zaia, Edmond W., Forse, Alexander C., Marius, Noemie, Gennett, Thomas, Guo, Jinghua, Prendergast, David, Long, Jeffrey R., and Urban, Jeffrey J. Runaway Carbon Dioxide Conversion Leads to Enhanced Uptake in a Nanohybrid Form of Porous Magnesium Borohydride. United States: N. p., 2019. Web. doi:10.1002/adma.201904252.
Jeong, Sohee, Milner, Phillip J., Wan, Liwen F., Liu, Yi-Sheng, Oktawiec, Julia, Zaia, Edmond W., Forse, Alexander C., Marius, Noemie, Gennett, Thomas, Guo, Jinghua, Prendergast, David, Long, Jeffrey R., & Urban, Jeffrey J. Runaway Carbon Dioxide Conversion Leads to Enhanced Uptake in a Nanohybrid Form of Porous Magnesium Borohydride. United States. doi:10.1002/adma.201904252.
Jeong, Sohee, Milner, Phillip J., Wan, Liwen F., Liu, Yi-Sheng, Oktawiec, Julia, Zaia, Edmond W., Forse, Alexander C., Marius, Noemie, Gennett, Thomas, Guo, Jinghua, Prendergast, David, Long, Jeffrey R., and Urban, Jeffrey J. Fri . "Runaway Carbon Dioxide Conversion Leads to Enhanced Uptake in a Nanohybrid Form of Porous Magnesium Borohydride". United States. doi:10.1002/adma.201904252.
@article{osti_1567036,
title = {Runaway Carbon Dioxide Conversion Leads to Enhanced Uptake in a Nanohybrid Form of Porous Magnesium Borohydride},
author = {Jeong, Sohee and Milner, Phillip J. and Wan, Liwen F. and Liu, Yi-Sheng and Oktawiec, Julia and Zaia, Edmond W. and Forse, Alexander C. and Marius, Noemie and Gennett, Thomas and Guo, Jinghua and Prendergast, David and Long, Jeffrey R. and Urban, Jeffrey J.},
abstractNote = {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 y-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 degrees 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.},
doi = {10.1002/adma.201904252},
journal = {Advanced Materials},
number = ,
volume = ,
place = {United States},
year = {2019},
month = {9}
}

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Works referenced in this record:

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