Theoretical investigation of tandem catalysts utilizing S-modified metalloporphyrin two-dimensional carbon-rich conjugated frameworks for the electrocatalytic reduction synthesis of l-erythrulose

Abstract

Notwithstanding consistent advancements in CO₂ upgrading and recycling using diverse catalytic methodologies, the production of intricate goods, such as sugars, remains unexamined. L-Erythrulose is a natural keto sugar utilized for various purposes, including natural tanning, streak mitigation, prolonged coloration, and moisturizing properties, making it prevalent in the cosmetic industry. This study presents the innovative development of a tandem catalyst system comprising an S-modified metalloporphyrin and an expanded-structure metalloporphyrin, with a thorough theoretical exploration of the reaction pathway for converting CO₂ to L-erythrulose. To systematically assess the catalytic efficiency of the catalyst, the stability, catalytic activity, product selectivity, and reactivity characteristics during the reaction process have been analyzed using DFT calculations, with the objective of providing theoretical support for the optimal design and performance enhancement of catalysts in carbon dioxide conversion applications. Of the catalysts examined, four demonstrated effective electrocatalysis for the production of L-erythrulose: Fe–SPor–CoRh–SN₅TPor, Fe–SPor–CoIr–SN₅TPor, Co–SPor–CoRh–SN₅TPor, and Co–SPor–CoIr–SN₅TPor. This work proposes an effective electrocatalytic synthesis of L-erythrulose from CO₂ as a precursor for its production. This study broadens the spectrum of product complexity attainable by the electrocatalytic conversion of CO₂, which has been effectively transformed into essential sugars.