Precipitation-Based Nanoscale Enzyme Reactor with Improved Loading, Stability, and Mass Transfer for Enzymatic CO2 Conversion and Utilization

Han Sol Kim, Sung Gil Hong, Kie Moon Woo, Vanesa Teijeiro Seijas, Seongbeen Kim, Jinwoo Lee, Jungbae Kim

Research output: Contribution to journalArticle

2 Citations (Scopus)

Abstract

Enzymatic CO2 conversion has gathered a growing attention due to its fast kinetics in converting CO2 to bicarbonate, but the carbonic anhydrase enzymes easily lose their activities in CO2 conversion processes. Here, we propose a "precipitation-based nanoscale enzyme reactor (p-NER)" approach, which stabilizes the activity of carbonic anhydrase, prepared via the two steps of enzyme adsorption into magnetic mesoporous silica and simultaneous enzyme precipitation/cross-linking. The simple addition of enzyme precipitation during cross-linking step resulted in the formation of cross-linked enzyme aggregates (CLEAs) not only inside the mesopores but also on the surface of mesoporous silica. External CLEAs of p-NER contributed to the improvement of enzyme loading (32.9% (w/w)) and mass transfer (KM = 3.68 mM) compared to those of NER (20.1% (w/w) and 4.29 mM, respectively), prepared without enzyme precipitation step and showing no external CLEAs. p-NER was stable under vigorous shaking (200 rpm) with no activity decrease for 160 days after the inactivation of 25% labile enzyme population at the initial stage of incubation. It suggests that external CLEAs were tightly bound on the surface of mesoporous silica by having roots of CLEAs in the internal mesopores. p-NER of carbonic anhydrase was used to convert CO2 to bicarbonate, and the resulting bicarbonate was further utilized for the generation of calcium carbonate. The addition of p-NER into the CO2 bubbling reactor resulted in 6.5-fold higher production of calcium carbonate than the control with no enzyme, revealing the accelerated kinetics of CO2 conversion in the presence of p-NER. p-NER can be easily recycled via magnetic separation, and retained 89% of initial activity after 10 recycled uses. This study has demonstrated great potential of p-NER not only for enzymatic CO2 conversion but also in various other applications where the short lifetimes of enzymes hamper their practical applications.

Original languageEnglish
Pages (from-to)6526-6536
Number of pages11
JournalACS Catalysis
Volume8
Issue number7
DOIs
Publication statusPublished - 2018 Jul 6

Fingerprint

Mass transfer
Enzymes
Carbonic anhydrase
Carbonic Anhydrases
Bicarbonates
Silicon Dioxide
Calcium Carbonate
Silica
Calcium carbonate
Enzyme kinetics
Magnetic separation
Kinetics

Keywords

  • Calcium carbonate
  • Carbonic anhydrase
  • CO conversion
  • CO utilization
  • Precipitation-based nanoscale enzyme reactor

ASJC Scopus subject areas

  • Catalysis

Cite this

Precipitation-Based Nanoscale Enzyme Reactor with Improved Loading, Stability, and Mass Transfer for Enzymatic CO2 Conversion and Utilization. / Kim, Han Sol; Hong, Sung Gil; Woo, Kie Moon; Teijeiro Seijas, Vanesa; Kim, Seongbeen; Lee, Jinwoo; Kim, Jungbae.

In: ACS Catalysis, Vol. 8, No. 7, 06.07.2018, p. 6526-6536.

Research output: Contribution to journalArticle

Kim, Han Sol ; Hong, Sung Gil ; Woo, Kie Moon ; Teijeiro Seijas, Vanesa ; Kim, Seongbeen ; Lee, Jinwoo ; Kim, Jungbae. / Precipitation-Based Nanoscale Enzyme Reactor with Improved Loading, Stability, and Mass Transfer for Enzymatic CO2 Conversion and Utilization. In: ACS Catalysis. 2018 ; Vol. 8, No. 7. pp. 6526-6536.
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AU - Teijeiro Seijas, Vanesa

AU - Kim, Seongbeen

AU - Lee, Jinwoo

AU - Kim, Jungbae

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AB - Enzymatic CO2 conversion has gathered a growing attention due to its fast kinetics in converting CO2 to bicarbonate, but the carbonic anhydrase enzymes easily lose their activities in CO2 conversion processes. Here, we propose a "precipitation-based nanoscale enzyme reactor (p-NER)" approach, which stabilizes the activity of carbonic anhydrase, prepared via the two steps of enzyme adsorption into magnetic mesoporous silica and simultaneous enzyme precipitation/cross-linking. The simple addition of enzyme precipitation during cross-linking step resulted in the formation of cross-linked enzyme aggregates (CLEAs) not only inside the mesopores but also on the surface of mesoporous silica. External CLEAs of p-NER contributed to the improvement of enzyme loading (32.9% (w/w)) and mass transfer (KM = 3.68 mM) compared to those of NER (20.1% (w/w) and 4.29 mM, respectively), prepared without enzyme precipitation step and showing no external CLEAs. p-NER was stable under vigorous shaking (200 rpm) with no activity decrease for 160 days after the inactivation of 25% labile enzyme population at the initial stage of incubation. It suggests that external CLEAs were tightly bound on the surface of mesoporous silica by having roots of CLEAs in the internal mesopores. p-NER of carbonic anhydrase was used to convert CO2 to bicarbonate, and the resulting bicarbonate was further utilized for the generation of calcium carbonate. The addition of p-NER into the CO2 bubbling reactor resulted in 6.5-fold higher production of calcium carbonate than the control with no enzyme, revealing the accelerated kinetics of CO2 conversion in the presence of p-NER. p-NER can be easily recycled via magnetic separation, and retained 89% of initial activity after 10 recycled uses. This study has demonstrated great potential of p-NER not only for enzymatic CO2 conversion but also in various other applications where the short lifetimes of enzymes hamper their practical applications.

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