Co anchored on porphyrinic triazine-based frameworks with excellent biocompatibility for conversion of CO<sub>2</sub> in H<sub>2</sub>-mediated microbial electrosynthesis

doi:10.1007/s11705-022-2195-6

Front. Chem. Sci. Eng.

2022, Vol. 16

Issue (12) : 1761-1771 https://doi.org/10.1007/s11705-022-2195-6

RESEARCH ARTICLE

Co anchored on porphyrinic triazine-based frameworks with excellent biocompatibility for conversion of CO₂ in H₂-mediated microbial electrosynthesis

Folin Liu¹, Shaohua Feng¹, Siyuan Xiu¹, Bin Yang^1,², Yang Hou^1,², Lecheng Lei^1,², Zhongjian Li^1,^2,³(

)

¹. College of Chemical and Biological Engineering, Key Laboratory of Biomass Chemical Engineering of Ministry of Education, Zhejiang University, Hangzhou 310027, China
². Institute of Zhejiang University—Quzhou, Quzhou 324000, China
³. Academy of Ecological Civilization, Zhejiang University, Hangzhou 310027, China

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Abstract

Microbial electrosynthesis is a promising alternative to directly convert CO₂ into long-chain compounds by coupling inorganic electrocatalysis with biosynthetic systems. However, problems arose that the conventional electrocatalysts for hydrogen evolution may produce extensive by-products of reactive oxygen species and cause severe metal leaching, both of which induce strong toxicity toward microorganisms. Moreover, poor stability of electrocatalysts cannot be qualified for long-term operation. These problems may result in poor biocompatibility between electrocatalysts and microorganisms. To solve the bottleneck problem, Co anchored on porphyrinic triazine-based frameworks was synthesized as the electrocatalyst for hydrogen evolution and further coupled with Cupriavidus necator H16. It showed high selectivity for a four-electron pathway of oxygen reduction reaction and low production of reactive oxygen species, owing to the synergistic effect of Co–N_x modulating the charge distribution and adsorption energy of intermediates. Additionally, low metal leaching and excellent stability were observed, which may be attributed to low content of Co and the stabilizing effect of metalloporphyrins. Hence, the electrocatalyst exhibited excellent biocompatibility. Finally, the microbial electrosynthesis system equipped with the electrocatalyst successfully converted CO₂ to poly-β-hydroxybutyrate. This work drew up a novel strategy for enhancing the biocompatibility of electrocatalysts in microbial electrosynthesis system.

Keywords microbial electrosynthesis hydrogen evolution reaction metalloporphyrins biocompatibility CO₂ conversion

Corresponding Author(s): Zhongjian Li

Online First Date: 09 October 2022 Issue Date: 19 December 2022

Cite this article:

Folin Liu,Shaohua Feng,Siyuan Xiu, et al. Co anchored on porphyrinic triazine-based frameworks with excellent biocompatibility for conversion of CO₂ in H₂-mediated microbial electrosynthesis[J]. Front. Chem. Sci. Eng., 2022, 16(12): 1761-1771.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-022-2195-6
https://academic.hep.com.cn/fcse/EN/Y2022/V16/I12/1761

Fig.1 (a) Schematic illustration of the fabrication procedures for M@PTF; (b) LSV curves; (c) corresponding Tafel slopes of M@PTF (M = Fe, Co, Ni, Cu) in MM without IR correction.

Fig.2 (a) TEM image and (b) elemental mapping images of Co, C, N, and O, (c) XRD pattern, (d) FTIR spectrum, (e) Raman spectrum, (f) N₂ adsorption–desorption isotherm and pore size distribution (inset) of Co@PTF.

Fig.3 (a) XPS survey spectrum and high-resolution XPS spectra of (b) Co 2p, (c) N 1s and (d) C 1s of Co@PTF.

Fig.4 Concentration of (a) ·O₂^–, (b) H₂O₂, (c) ·OH of Co@PTF using SS and Co@PTF as cathode at the current density of –1 mA·cm^–2 (Error bars denote SEM, n = 3). (d) H₂O₂ yield, n and LSV curve for ORR (inset) of Co@PTF obtained from RRDE measurements.

Fig.5 (a) Spot assays of Co@PTF and SS before starting electrolysis (0 h), after 3 and 24 h of electrolysis at the current density of –1 mA·cm^–2. (b) Growth curves of the MES systems equipped with Co@PTF and SS as the cathodes at current densities of –1, –2 and –4 mA·cm^–2. (c) Dissolution concentration of Co in the electrolyte of Co@PTF and spot assays of C. necator for different concentrations of Co²⁺ (inset). (All the samples of spot assays were grown on plates with different dilution factors. Error bars denote SEM, n = 3).

Fig.6 The profiles of (a) OD₆₀₀ and (b) concentration of PHB. (c) Proportion of PHB in chemicals and (d) ECE during MES systems operation under the current density of –6 mA·cm^–2 equipped with Co@PTF and SS (Error bars denote SEM, n = 3). (e) LSV curves and Tafel slopes (inset) of Co@PTF before and after MES system operation. (f) LSV curves and Tafel slopes (inset) of SS before and after MES system operation.

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