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

Journal Article · · Advanced Materials
 [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)
+ Show Author Affiliations

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.

Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Center for Gas Separations Relevant to Clean Energy Technologies (CGS); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
AC02-05CH11231; AC36-08GO28308; AC52-07NA27344; SC0001015
OSTI ID:
1567036
Report Number(s):
LLNL-JRNL--762420; NREL/JA--5900-74987
Journal Information:
Advanced Materials, Journal Name: Advanced Materials Journal Issue: 44 Vol. 31; ISSN 0935-9648
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

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36 MATERIALS SCIENCE
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nanomaterials
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