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<p>Cobalt-based systems are among the most extensively studied catalyst materials for both half-reactions of water oxidation and CO<sub>2</sub> reduction in artificial photosynthesis applications. Notably, cobalt porphyrin complexes have emerged as promising candidates for facilitating these half-reactions, using sunlight as an energy source. In this study, we evaluated the efficacy of the anionic porphyrin complex cobalt (II)-<i>meso</i>-tetra(4-carboxyphenyl) porphyrin (CoTCPP) as a molecular catalyst-sensitized system (MCSS) for water oxidation and CO<sub>2</sub> reduction. Molecular characterization of CoTCPP indicated that its catalytic activity was predominantly influenced by spontaneous aggregation under pH and solvent conditions, as confirmed by spectrophotometric analysis. Electrochemical investigations demonstrated that CoTCPP operates effectively as a homogeneous catalyst for water oxidation in 5% aqueous acetonitrile; however, its catalytic performance diminishes at water concentrations above 10% due to increased aggregation. Interestingly, the heterogeneous electrocatalytic activity of CoTCPP is robust and highly promising. The utilization of CoTCPP as a molecular catalyst and sensitizer in photoelectrodes was investigated using a 420-nm LED light with a power of 3.5&#xa0;mW/cm<sup>2</sup>. This resulted in a stable photocurrent, achieving an IPCE of 0.03% for CO<sub>2</sub> reduction and 0.08% for H<sub>2</sub>O oxidation under zero bias in aqueous conditions.</p> Graphical abstract <p></p>

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Activity of anionic cobalt porphyrin as a bifunctional molecular catalyst for the redox reactions in artificial photosynthesis: a consideration of the role of aggregation

  • 期刊论文

  • 发表日期：

    2026年2月2日

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  • Haritha Baby,
  • Manaved Kannamvelli Manoj,
  • Shalom Varghese,
  • Reshma Joseph,
  • Athira Mohan,
  • Haritha Anamangattupurakkal,
  • Jayachandran Kaippully,
  • Fazalurahman Kuttassery,
  • Hiroshi Tachibana,
  • Haruo Inoue,
  • Sebastian Nybin Remello

摘要

Cobalt-based systems are among the most extensively studied catalyst materials for both half-reactions of water oxidation and CO2 reduction in artificial photosynthesis applications. Notably, cobalt porphyrin complexes have emerged as promising candidates for facilitating these half-reactions, using sunlight as an energy source. In this study, we evaluated the efficacy of the anionic porphyrin complex cobalt (II)-meso-tetra(4-carboxyphenyl) porphyrin (CoTCPP) as a molecular catalyst-sensitized system (MCSS) for water oxidation and CO2 reduction. Molecular characterization of CoTCPP indicated that its catalytic activity was predominantly influenced by spontaneous aggregation under pH and solvent conditions, as confirmed by spectrophotometric analysis. Electrochemical investigations demonstrated that CoTCPP operates effectively as a homogeneous catalyst for water oxidation in 5% aqueous acetonitrile; however, its catalytic performance diminishes at water concentrations above 10% due to increased aggregation. Interestingly, the heterogeneous electrocatalytic activity of CoTCPP is robust and highly promising. The utilization of CoTCPP as a molecular catalyst and sensitizer in photoelectrodes was investigated using a 420-nm LED light with a power of 3.5 mW/cm2. This resulted in a stable photocurrent, achieving an IPCE of 0.03% for CO2 reduction and 0.08% for H2O oxidation under zero bias in aqueous conditions.

Graphical abstract