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

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

参考文献

[1] ShindellD, SmithC J. Climate and air-quality benefits of a realistic phase-out of fossil fuels. Nature, 2019, 573( 7774): 408– 411

[2] PetersG P, AndrewR M, CanadellJ G, FriedlingsteinP, JacksonR B, KorsbakkenJ I, LeQuéré C, PeregonA. Carbon dioxide emissions continue to grow amidst slowly emerging climate policies. Nature Climate Change, 2020, 10( 1): 3– 6

[3] RauG H, WillauerH D, RenZ J. The global potential for converting renewable electricity to negative-CO₂-emissions hydrogen. Nature Climate Change, 2018, 8( 7): 621– 625

[4] YanY L, BorhaniT N, SubravetiS G, PaiK N, PrasadV, RajendranA, NkulikiyinkaP, AsiborJ O, ZhangZ E, ShaoD, WangL, ZhangW, YanY, AmpomahW, YouJ, WangM, AnthonyE J, ManovicV, CloughP T. Harnessing the power of machine learning for carbon capture, utilisation, and storage (CCUS)—a state-of-the-art review. Energy & Environmental Science, 2021, 14( 12): 6122– 6157

[5] FangX, KalathilS, ReisnerE. Semi-biological approaches to solar-to-chemical conversion. Chemical Society Reviews, 2020, 49( 14): 4926– 4952

[6] PrévoteauA, Carvajal-ArroyoJ M, GaniguéR, RabaeyK. Microbial electrosynthesis from CO₂: forever a promise?. Current Opinion in Biotechnology, 2020, 62 : 48– 57

[7] Perona-VicoE, Feliu-ParadedaL, PuigS, BañerasL. Bacteria coated cathodes as an in-situ hydrogen evolving platform for microbial electrosynthesis. Scientific Reports, 2020, 10( 1): 19852

[8] LiH, OpgenorthP H, WernickD G, RogersS, WuT Y, HigashideW, MalatiP, HuoY X, ChoK M, LiaoJ C. Integrated electromicrobial conversion of CO₂ to higher alcohols. Science, 2012, 335( 6076): 1596

[9] KriegT, SydowA, FaustS, HuthI, HoltmannD. CO₂ to terpenes: autotrophic and electroautotrophic α-humulene production with Cupriavidus necator. Angewandte Chemie International Edition, 2018, 57( 7): 1879– 1882

[10] SakimotoK K, WongA B, YangP D. Self-photosensitization of nonphotosynthetic bacteria for solar-to-chemical production. Science, 2016, 351( 6268): 74– 77

[11] XiuS Y, YaoJ N, WuG M, HuangY M, YangB, HuangY, LeiL C, LiZ J, HouY. Hydrogen-mediated electron transfer in hybrid microbial-inorganic systems and application in energy and the environment. Energy Technology (Weinheim), 2019, 7( 8): 1800987

[12] LiuC, ColónB C, ZiesackM, SilverP A, NoceraD G. Water splitting-biosynthetic system with CO₂ reduction efficiencies exceeding photosynthesis. Science, 2016, 352( 6290): 1210– 1213

[13] WangM, ZhongW, ZhangS S, LiuR J, XingJ M, ZhangG J. An overall water-splitting polyoxometalate catalyst for the electromicrobial conversion of CO₂ in neutral water. Journal of Materials Chemistry A, 2018, 6( 21): 9915– 9921

[14] RodriguesR M, GuanX, IñiguezJ A, EstabrookD A, ChapmanJ O, HuangS Y, SlettenE M, LiuC. Perfluorocarbon nanoemulsion promotes the delivery of reducing equivalents for electricity-driven microbial CO₂ reduction. Nature Catalysis, 2019, 2( 5): 407– 414

[15] SakimotoK K, KornienkoN, Cestellos-BlancoS, LimJ, LiuC, YangP D. Physical biology of the materials—microorganism interface. Journal of the American Chemical Society, 2018, 140( 6): 1978– 1985

[16] TorellaJ P, GagliardiC J, ChenJ S, BediakoD K, ColónB, WayJ C, SilverP A, NoceraD G. Efficient solar-to-fuels production from a hybrid microbial—water-splitting catalyst system. Proceedings of the National Academy of Sciences of the United States of America, 2015, 112( 8): 2337– 2342

[17] SinghN, SavanurM A, SrivastavaS, D’SilvaP, MugeshG. A redox modulatory Mn₃O₄ nanozyme with multi-enzyme activity provides efficient cytoprotection to human cells in a Parkinson’s disease model. Angewandte Chemie International Edition, 2017, 56( 45): 14267– 14271

[18] LiuY, CaoX, GeJ. Antioxidative composites based on multienzyme systems encapsulated in metal−organic frameworks. ACS Applied Materials & Interfaces, 2021, 13( 39): 46431– 46439

[19] AbdiZ, BalaghiS E, SologubenkoA S, WillingerM G, VandichelM, ShenJ R, AllakhverdievS I, PatzkeG R, NajafpourM M. Understanding the dynamics of molecular water oxidation catalysts with liquid-phase transmission electron microscopy: the case of Vitamin B₁₂. ACS Sustainable Chemistry & Engineering, 2021, 9( 28): 9494– 9505

[20] SlavinY N, AsnisJ, HäfeliU O, BachH. Metal nanoparticles: understanding the mechanisms behind antibacterial activity. Journal of Nanobiotechnology, 2017, 15( 1): 65

[21] BianB, BajracharyaS, XuJ, PantD, SaikalyP E. Microbial electrosynthesis from CO₂: challenges, opportunities and perspectives in the context of circular bioeconomy. Bioresource Technology, 2020, 302 : 122863

[22] YiJ D, XuR, ChaiG L, ZhangT, ZangK T, NanB, LinH, LiangY L, LvJ Q, LuoJ, SiR, HuangY B, CaoR. Cobalt single-atoms anchored on porphyrinic triazine-based frameworks as bifunctional electrocatalysts for oxygen reduction and hydrogen evolution reactions. Journal of Materials Chemistry A, 2019, 7( 3): 1252– 1259

[23] AyedC, HuangW, ZhangK A. Covalent triazine framework with efficient photocatalytic activity in aqueous and solid media. Frontiers of Chemical Science and Engineering, 2020, 14( 3): 397– 404

[24] XiangZ H, XueY H, CaoD P, HuangL, ChenJ F, DaiL M. Highly efficient electrocatalysts for oxygen reduction based on 2D covalent organic polymers complexed with non-precious metals. Angewandte Chemie International Edition, 2014, 53( 9): 2433– 2437

[25] LiuJ L, HuY J, CaoJ J. Covalent triazine-based frameworks as efficient metal-free electrocatalysts for oxygen reduction reaction in alkaline media. Catalysis Communications, 2015, 66 : 91– 94

[26] GarcíaÁ, RetuertoM, DominguezC, PascualL, FerrerP, GianolioD, SerranoA, AßmannP, SanchezD G, PeñaM A, RojasS. Fe doped porous triazine as efficient electrocatalysts for the oxygen reduction reaction in acid electrolyte. Applied Catalysis B: Environmental, 2020, 264 : 118507

[27] ZhuoH Y, ZhangX, LiangJ X, YuQ, XiaoH, LiJ. Theoretical understandings of graphene-based metal single-atom catalysts: stability and catalytic performance. Chemical Reviews, 2020, 120( 21): 12315– 12341

[28] FengS H, ZhengW Z, ZhuJ K, LiZ J, YangB, WenZ H, LuJ G, LeiL C, WangS B, HouY. Porous metal-porphyrin triazine-based frameworks for efficient CO₂ electroreduction. Applied Catalysis B: Environmental, 2020, 270 : 118908

[29] AlarawiA, RamalingamV, HeJ H. Recent advances in emerging single atom confined two-dimensional materials for water splitting applications. Materials Today. Energy, 2019, 11 : 1– 23

[30] GaoC, LowJ X, LongR, KongT T, ZhuJ F, XiongY J. Heterogeneous single-atom photocatalysts: fundamentals and applications. Chemical Reviews, 2020, 120( 21): 12175– 12216

[31] LaBelleE V, MarshallC W, MayH D. Microbiome for the electrosynthesis of chemicals from carbon dioxide. Accounts of Chemical Research, 2020, 53( 1): 62– 71

[32] ZhouR F, ZhengY, JaroniecM, QiaoS Z. Determination of the electron transfer number for the oxygen reduction reaction: from theory to experiment. ACS Catalysis, 2016, 6( 7): 4720– 4728

[33] YaoJ, ChengY, ZhouM, ZhaoS, LinS C, WangX Y, WuJ J X, LiS R, WeiH. ROS scavenging Mn₃O₄ nanozymes for in vivo anti-inflammation. Chemical Science (Cambridge), 2018, 9( 11): 2927– 2933

[34] ChenM, ZhouX F, ChenX Y, CaiQ H, ZengR J X, ZhouS G. Mechanisms of nitrous oxide emission during photoelectrotrophic denitrification by self-photosensitized Thiobacillus denitrificans. Water Research, 2020, 172 : 115501

[35] HuangJ W, SuY, ZhangY D, WuW Q, WuC Y, SunY H, LuR F, ZouG F, LiY R, XiongJ. FeO_x/FeP hybrid nanorods neutral hydrogen evolution electrocatalysis: insight into interface. Journal of Materials Chemistry A, 2018, 6( 20): 9467– 9472

[36] TanY W, LuoM, LiuP, ChengC, HanJ H, WatanabeK, ChenM W. Three-dimensional nanoporous Co₉S₄P₄ pentlandite as a bifunctional electrocatalyst for overall neutral water splitting. ACS Applied Materials & Interfaces, 2019, 11( 4): 3880– 3888

[37] WangN, ChengG, GuoL P, TanB E, JinS B. Hollow covalent triazine frameworks with variable shell thickness and morphology. Advanced Functional Materials, 2019, 29( 43): 1904781

[38] DaiK, HuT P, ZhangJ F, LuL H. Carbon nanotube exfoliated porous reduced graphene oxide/CdS-diethylenetriamine heterojunction for efficient photocatalytic H₂ production. Applied Surface Science, 2020, 512 : 144783

[39] ZhengY, ChenS, SongH, GuoH, ZhangK A I, ZhangC, LiuT. Nitrogen-doped hollow carbon nanoflowers from a preformed covalent triazine framework for metal-free bifunctional electrocatalysis. Nanoscale, 2020, 12( 27): 14441– 14447

[40] LuM, QianY J, YangC C, HuangX, LiH, XieX J, HuangL, HuangW. Nitrogen-enriched pseudographitic anode derived from silk cocoon with tunable flexibility for microbial fuel cells. Nano Energy, 2017, 32 : 382– 388

[41] ZhuY P, LiJ J, ChenY B, ZouJ, ChengQ Q, ChenC, HuW B, ZouL L, ZouZ Q, YangB, YangH. Switching the oxygen reduction reaction pathway via tailoring the electronic structure of FeN₄/C catalysts. ACS Catalysis, 2021, 11( 21): 13020– 13027

[42] BallB, ChakravartyC, SarkarP. Silicon and phosphorus Co-doped bipyridine-linked covalent triazine framework as a promising metal-free catalyst for hydrogen evolution reaction: a theoretical investigation. Journal of Physical Chemistry Letters, 2020, 11( 4): 1542– 1549

[43] PohlmannA, FrickeW F, ReineckeF, KusianB, LiesegangH, CrammR, EitingerT, EweringC, PötterM, SchwartzE, StrittmatterA, VoßI, GottschalkG, SteinbüchelA, FriedrichB, BowienB. Genome sequence of the bioplastic-producing “Knallgas” bacterium Ralstonia eutropha H16. Nature Biotechnology, 2006, 24( 10): 1257– 1262

[44] Fernández-CastroP, VallejoM, SanRomán M F, OrtizI. Insight on the fundamentals of advanced oxidation processes. Role and review of the determination methods of reactive oxygen species. Journal of Chemical Technology and Biotechnology, 2015, 90( 5): 796– 820

[45] NosakaY, NosakaA Y. Generation and detection of reactive oxygen species in photocatalysis. Chemical Reviews, 2017, 117( 17): 11302– 11336

[46] LiuY, ZhaoY, WangJ L. Fenton/Fenton-like processes with in-situ production of hydrogen peroxide/hydroxyl radical for degradation of emerging contaminants: advances and prospects. Journal of Hazardous Materials, 2021, 404 : 124191

[47] LiY, ZhangW, NiuJ F, ChenY S. Mechanism of photogenerated reactive oxygen species and correlation with the antibacterial properties of engineered metal-oxide nanoparticles. ACS Nano, 2012, 6( 6): 5164– 5173

[48] LiY, HuangJ H, HuX, BiL L, CaiP W, JiaJ C, ChaiG L, WeiS Q, DaiL M, WenZ H. Fe vacancies induced surface FeO₆ in nanoarchitectures of N-doped graphene protected β-FeOOH: effective active sites for pH-universal electrocatalytic oxygen reduction. Advanced Functional Materials, 2018, 28( 34): 1803330

Acknowledgements

This project was supported by the National Natural Science Foundation of China (Grant Nos. 22122812, 22075245 and 21961160742).

Electronic Supplementary Material

Supplementary material is available in the online version of this article at https://dx.doi.org/10.1007/s11705-022-2195-6 and is accessible for authorized users.

版权

2022 Higher Education Press