Dissolved carbonic anhydrase for enhancing post-combustion carbon dioxide hydration in aqueous ammonia

摘要

Aqueous ammonia solvents that capture CO_2 as ionic complexes of carbonates with ammonium have recently been advanced as alternatives to amine-based solvents due to their lower energy requirements for thermal regeneration. In ammonia based solvents, the hydration of CO_2 to form bicarbonate may become a rate-limiting step as the CO_2 loading increases and the resulting pH level of the solvent decreases. Variants of the enzyme carbonic anhydrase can accelerate the reversible hydration of CO_2 to yield bicarbonate by more than 106-fold. The possible benefit of bovine carbonic anhydrase (BCA) addition to solutions of aqueous ammonia to enhance CO_2 hydration was investigated in semi-batch reactions within continuously stirred tank reactors or in a bubble column gas-liquid contactor. Adding 154 mg/liter of BCA to 2 M aqueous ammonia provided a 34.1% overall increase in the rate of CO_2 hydration (as indicated by the production of [H+]) as the pH declined from 9.6 to 8.6 during sparging with a 15% CO2, 85% N2 gas at a flow rate of 3 lpm. The benefits of adding BCA to enhance CO_2 hydration were only discernable below ~pH 9. The implications of the apparent pH limitations on the utility of BCA are discussed in the context of absorber unit operation design. Possible embodiments of carbonic anhydrase as either an immobilized catalyst or as a dissolved, recirculating catalyst in potential plant scale aqueous ammonia systems are considered as well.