Pickering interfacial biocatalysis with enhanced diffusion processes for CO2 mineralization

doi:10.1016/S1872-2067(21)63998-0

Abstract

Abstract:

Utilization of carbon dioxide (CO₂) has become a crucial and anticipated solution to address environmental and ecological issues. Enzymes such as carbonic anhydrase (CA) can efficiently convert CO₂ into various platform chemicals under ambient conditions, which offers a promising way for CO₂ utilization. Herein, we constructed a Pickering interfacial biocatalytic system (PIBS) stabilized by CA-embedded MOFs (ZIF-8 and ZIF-L) for CO₂ mineralization. Through structure engineering of MOFs and incorporation of Pickering emulsion, the internal and external diffusion processes of CO₂ during the enzymatic mineralization were greatly intensified. When CO₂ was ventilated at a flow rate of 50 mL min^-1for 1 h, the pH value of PIBS dropped from ~8.00 to ~6.50, while the average pH value of free system only dropped to ~7.15, indicating that the initial reaction rate of CO₂ mineralization of PIBS is nearly twice that of the free system. After the 8^thcycle reaction, PIBS can still produce more than 9.8 mg of CaCO₃ in 5 min, realizing efficient and continuous mineralization of CO₂.

Key words: Carbon dioxide conversion, Carbonic anhydrase, Pickering emulsion, Metal-organic frameworks, Diffusion intensification

Boyu Zhang, Jiafu Shi, Yang Zhao, Han Wang, Ziyi Chu, Yu Chen, Zhenhua Wu, Zhongyi Jiang. Pickering interfacial biocatalysis with enhanced diffusion processes for CO₂ mineralization[J]. Chinese Journal of Catalysis, 2022, 43(4): 1184-1191.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63998-0

https://www.cjcatal.com/EN/Y2022/V43/I4/1184

Figures/Tables 7

Fig. 1. Schematic preparation process of (a) CA@ZIF-L and (b) CA@ZIF-8 particles.

Fig. 2. SEM images of ZIF-L (a), CA@ZIF-L (b), ZIF-8 (c), and CA@ZIF-8 (d). FTIR spectra (e) and XRD patterns (f) of CA@ZIF-L, ZIF-L, CA@ZIF-8, and ZIF-8; SAXS data of CA@ZIF-L (g) and CA@ZIF-8 (h) with schemes showing the size of the mesopore.

Fig. 3. Bright-field images (left) and EDS elemental mapping (right) of N, Zn, and S for CA@ZIF-8 (a) and CA@ZIF-L (b).

Fig. 4. (a) Schematic diagram of CO2 conversion catalyzed by CA@ZIF-L and CA@ZIF-8 particles. (b) Degradation rate of 4-NPA by CA@ZIF-L, CA@ZIF-8, and free CA. (c) Relative activity of CA@ZIF-L and CA@ZIF-8 particles. (d) Adsorption rate of coumarin by BSA@ZIF-L and BSA@ZIF-8 particles. Notably, bovine serum albumin (BSA) that commonly applied as the substitute for expensive enzymes was adopted to prepare BSA@ZIFs particles for the adsorption experiment [44].

Fig. 5. (a) Schematic construction process of PIBS enabled by CA@ZIF-L particles. (b) Water contact angles of CA@ZIF-L, CA@ZIF-8, ZIF-L, and ZIF-8 particles. (c) Photograph and optical microscope images of Pickering emulsion stabilized by CA@ZIF-L particles.

Fig. 6. Schematic conversion of CO2 by PIBS (a) and free system (b). When CO2 was introduced at a flow rate of 50 (c) and 100 (d) mL min-1, the pH curve of the PIBS or free system constructed by CA@ZIF-L and CA@ZIF-8 particles.

Fig. 7. (a) Schematic conversion and mineralization of CO2 by CA@ZIFs PIBS. (b) CaCO3 production catalyzed by the PIBS and free systems. (c) Recyclability of CA@ZIF-L PIBS and CA@ZIF-8 PIBS.

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Pickering interfacial biocatalysis with enhanced diffusion processes for CO₂ mineralization

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