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Fast CO2 hydration kinetics impair heterogeneous but improve enzymatic CO2 reduction catalysis
by
Pereira, Inês A. C.
, Wagner, Andreas
, Reisner, Erwin
, Badiani, Vivek M.
, Dharani, Azim M.
, Zacarias, Sónia
, Cobb, Samuel J.
, Oliveira, Ana Rita
in
639/638/161/886
/ 639/638/224/685
/ 639/638/45/607/1168
/ 639/638/77/886
/ Analytical Chemistry
/ Biochemistry
/ Carbon dioxide
/ Carbon dioxide concentration
/ Carbonic anhydrase
/ Carbonic anhydrases
/ Catalysis
/ Catalysts
/ Chemistry
/ Chemistry and Materials Science
/ Chemistry/Food Science
/ Dehydrogenase
/ Dehydrogenases
/ Electrocatalysts
/ Formate dehydrogenase
/ Hydration
/ Hydrogen evolution
/ Immobilization
/ Inorganic Chemistry
/ Kinetics
/ Organic Chemistry
/ Physical Chemistry
/ Reduction
/ Selectivity
/ Side reactions
2022
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Fast CO2 hydration kinetics impair heterogeneous but improve enzymatic CO2 reduction catalysis
by
Pereira, Inês A. C.
, Wagner, Andreas
, Reisner, Erwin
, Badiani, Vivek M.
, Dharani, Azim M.
, Zacarias, Sónia
, Cobb, Samuel J.
, Oliveira, Ana Rita
in
639/638/161/886
/ 639/638/224/685
/ 639/638/45/607/1168
/ 639/638/77/886
/ Analytical Chemistry
/ Biochemistry
/ Carbon dioxide
/ Carbon dioxide concentration
/ Carbonic anhydrase
/ Carbonic anhydrases
/ Catalysis
/ Catalysts
/ Chemistry
/ Chemistry and Materials Science
/ Chemistry/Food Science
/ Dehydrogenase
/ Dehydrogenases
/ Electrocatalysts
/ Formate dehydrogenase
/ Hydration
/ Hydrogen evolution
/ Immobilization
/ Inorganic Chemistry
/ Kinetics
/ Organic Chemistry
/ Physical Chemistry
/ Reduction
/ Selectivity
/ Side reactions
2022
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Fast CO2 hydration kinetics impair heterogeneous but improve enzymatic CO2 reduction catalysis
by
Pereira, Inês A. C.
, Wagner, Andreas
, Reisner, Erwin
, Badiani, Vivek M.
, Dharani, Azim M.
, Zacarias, Sónia
, Cobb, Samuel J.
, Oliveira, Ana Rita
in
639/638/161/886
/ 639/638/224/685
/ 639/638/45/607/1168
/ 639/638/77/886
/ Analytical Chemistry
/ Biochemistry
/ Carbon dioxide
/ Carbon dioxide concentration
/ Carbonic anhydrase
/ Carbonic anhydrases
/ Catalysis
/ Catalysts
/ Chemistry
/ Chemistry and Materials Science
/ Chemistry/Food Science
/ Dehydrogenase
/ Dehydrogenases
/ Electrocatalysts
/ Formate dehydrogenase
/ Hydration
/ Hydrogen evolution
/ Immobilization
/ Inorganic Chemistry
/ Kinetics
/ Organic Chemistry
/ Physical Chemistry
/ Reduction
/ Selectivity
/ Side reactions
2022
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Fast CO2 hydration kinetics impair heterogeneous but improve enzymatic CO2 reduction catalysis
Journal Article
Fast CO2 hydration kinetics impair heterogeneous but improve enzymatic CO2 reduction catalysis
2022
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Overview
The performance of heterogeneous catalysts for electrocatalytic CO
2
reduction suffers from unwanted side reactions and kinetic inefficiencies at the required large overpotential. However, immobilized CO
2
reduction enzymes—such as formate dehydrogenase—can operate with high turnover and selectivity at a minimal overpotential and are therefore ‘ideal’ model catalysts. Here, through the co-immobilization of carbonic anhydrase, we study the effect of CO
2
hydration on the local environment and performance of a range of disparate CO
2
reduction systems from enzymatic (formate dehydrogenase) to heterogeneous systems. We show that the co-immobilization of carbonic anhydrase increases the kinetics of CO
2
hydration at the electrode. This benefits enzymatic CO
2
reduction—despite the decrease in CO
2
concentration—due to a reduction in local pH change, whereas it is detrimental to heterogeneous catalysis (on Au) because the system is unable to suppress the H
2
evolution side reaction. Understanding the role of CO
2
hydration kinetics within the local environment on the performance of electrocatalyst systems provides important insights for the development of next-generation synthetic CO
2
reduction catalysts.
Carbonic anhydrase enzymatically catalyses CO
2
hydration, and its effect on enzymatic and heterogeneous CO
2
reduction has now been studied. Through the co-immobilization of carbonic anhydrase, it has been shown that faster CO
2
hydration kinetics are beneficial for enzymatic catalysis (using formate dehydrogenase) but detrimental for heterogeneous catalysts, such as gold.
Publisher
Nature Publishing Group UK,Nature Publishing Group
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