Water‐Soluble Polymers with Appending Porphyrins as Bioinspired Catalysts for the Hydrogen Evolution Reaction

Xie, Lisi; Tian, Jia; Ouyang, Yingjie; Guo, Xinai; Apfel, Ulf‐Peter; Zhang, Wei; Cao, Rui

doi:10.1002/ange.202003836

Cited by 17 publications

(10 citation statements)

References 75 publications

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“…Molecular electrocatalysis has gained increasing interests because catalyst structures are clear and can be systematically modified [1–10] . These features are critical for studying reaction mechanisms and structure‐function relationships, which are of fundamental significance for catalyst design [11–18] .…”

Section: Figurementioning

confidence: 99%

Metal–Organic‐Framework‐Supported Molecular Electrocatalysis for the Oxygen Reduction Reaction

et al. 2021

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Synthesizing molecule@support hybrids is appealing to improve molecular electrocatalysis. We report herein metal–organic framework (MOF)‐supported Co porphyrins for the oxygen reduction reaction (ORR) with improved activity and selectivity. Co porphyrins can be grafted on MOF surfaces through ligand exchange. A variety of porphyrin@MOF hybrids were made using this method. Grafted Co porphyrins showed boosted ORR activity with large (>70 mV) anodic shift of the half‐wave potential compared to ungrafted porphyrins. By using active MOFs for peroxide reduction, the number of electrons transferred per O2 increased from 2.65 to 3.70, showing significantly improved selectivity for the 4e ORR. It is demonstrated that H2O2 generated from O2 reduction at Co porphyrins is further reduced at MOF surfaces, leading to improved 4e ORR. As a practical demonstration, these hybrids were used as air electrode catalysts in Zn‐air batteries, which exhibited equal performance to that with Pt‐based materials.

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Section: Figurementioning

confidence: 99%

Metal–Organic‐Framework‐Supported Molecular Electrocatalysis for the Oxygen Reduction Reaction

et al. 2021

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“…The non-sustainability of platinum, by far the best catalyst for reduction of protons to hydrogen (the hydrogen evolution reaction [HER]), and also inspiration from biology (e.g., Fe-hydrogenases) continues to drive focus on developing catalysts based on cheap, non-toxic, and earth-abundant metal complexes (Abbas and Bang, 2015;Bullock et al, 2014;Fukuzumi et al, 2018;Guo et al, 2020;Mondal et al, 2013;Roger et al, 2017;Xie et al, 2020). Molybdenum may safely be considered the only non-precious heavy transition metal, and it is also essential for human life due to its presence and roles in more than 30 enzymes (e.g., DMSO reductase, sulfite oxidase, xanthine oxidase) (Schwarz et al, 2009).…”

Section: Introductionmentioning

confidence: 99%

Hydrogen evolution catalysis by terminal molybdenum-oxo complexes

et al. 2021

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Summary Stable complexes with terminal triply bound metal-oxygen bonds are usually not considered as valuable catalysts for the hydrogen evolution reaction (HER). We now report the preparation of three conceptually different (oxo)molybdenum(V) corroles for testing if proton-assisted 2-electron reduction will lead to hyper-reactive molybdenum(III) capable of converting protons to hydrogen gas. The upto 670 mV differences in the [(oxo)Mo(IV)] - /[(oxo)Mo(III)] −2 redox potentials of the dissolved complexes came into effect by the catalytic onset potential for proton reduction thereby, significantly earlier than their reduction process in the absence of acids, but the two more promising complexes were not stable at practical conditions. Under heterogeneous conditions, the smallest and most electron-withdrawing catalyst did excel by all relevant criteria, including a 97% Faradaic efficiency for catalyzing HER from acidic water. This suggests complexes based on molybdenum, the only sustainable heavy transition metal, as catalysts for other yet unexplored green-energy-relevant processes.

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“…Co‐1 (cobalt copolymerized with methacrylate‐functionalized free base tetraphenylporphyrin with methacrylic acid) generated a 98% Faradic efficiency of HER while Co‐2 (2‐(dimethylamino)ethyl methacrylate) achieved the highest photocatalytic HER performance with a turnover number of 2.7 × 10 4 . [ 88 ] Ainsworth and colleagues coated Ru II ‐dye‐sensitized TiO 2 nanoparticles with surface exposed MtrC and OmcA from S. oneidensis MR‐1 eliciting photocatalytic reduction of these proteins. [ 89 ] The inclusion of these cytochromes into abiotic Ru‐sensitized TiO 2 nanoparticles improved the ability of these nanoparticles to reduce protein complexes paving the way for the development of strategies that use surface‐exposed proteins for solar microbial synthesis.…”

Section: Nanoenzyme Tailoring and Synthesismentioning

confidence: 99%

Engineered Nanoenzymes with Multifunctional Properties for Next‐Generation Biological and Environmental Applications

Mishra

Lee

Kumar

et al. 2021

Adv Funct Materials

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As a powerful tool, nanoenzyme electrocatalyst broadens the ways to explore bioinspired solutions to the world's energy and environmental concerns. Efforts of fashioning novel nanoenzymes for effective electrode functionalization is generating innovative viable catalysts with high catalytic activity, low cost, high stability and versatility, and ease of production. High chemo‐selectivity and broad functional group tolerance of nanoenzyme with an intrinsic enzyme like activity make them an excellent environmental tool. The catalytic activities and kinetics of nanoenzymes that benefit the development of nanoenzyme‐based energy and environmental technologies by effectual electrode functionalization are discussed in this article. Further, a deep‐insight on recent developments in the state‐of‐art of nanoenzymes either in terms of electrocatalytic redox reactions (viz. oxygen evolution reaction, oxygen reduction reaction, nitrogen reduction reaction and hydrogen evolution reaction) or environmental remediation /treatment of wastewater/or monitoring of a variety of pollutants. The complex interdependence of the physicochemical properties and catalytic characteristics of nanoenzymes are discussed along with the exciting opportunities presented by nanomaterial‐based core structures adorned with nanoparticle active‐sites shell for enhanced catalytic processes. Thus, such modular architecture with multi‐enzymatic potential introduces an immense scope of making its economical scale‐up for multielectron‐fuel or product recovery and multi‐pollutant or pesticide remediation as reality.

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Water‐Soluble Polymers with Appending Porphyrins as Bioinspired Catalysts for the Hydrogen Evolution Reaction

Cited by 17 publications

References 75 publications

Metal–Organic‐Framework‐Supported Molecular Electrocatalysis for the Oxygen Reduction Reaction

Metal–Organic‐Framework‐Supported Molecular Electrocatalysis for the Oxygen Reduction Reaction

Hydrogen evolution catalysis by terminal molybdenum-oxo complexes

Engineered Nanoenzymes with Multifunctional Properties for Next‐Generation Biological and Environmental Applications

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