CO 2 Electrochemical reduction on the two dimensional transition metal coordinated by 2,3,6,7,10,11-triphenylenehexathiol and 2,3,6,7,10,11-triphenylenehexamine, a computational survey

Electrochemical CO2 reduction reaction (CO2RR) provides a feasible technology for alleviating global warming, energy crisis and sustainable energy production. In this work, CO2RR reaction mechanism on TM-THTA (TM = Fe, Co, Ni, Ru, Rh, Pd, THTA is composed by two types of building blocks of 2,3,6,7,10,11-triphenylenehexathiol and 2,3,6,7,10,11-triphenylenehexamine) has been studied by using density functional method. Our study showed that the studied catalysts are stable both thermodynamically and electrochemically. Rh-THTA is a good CO2 reduction catalyst in producing CH4. Pd-THTA is a potential CO2 reduction catalyst in producing HCOOH. Solvent effect plays important role in reaction mechanism. The strong hydrogen evolution reaction in Rh-THTA and Pd-THTA can be refrained by adjusting the pH values of electrolyte. We hope this study could provide a useful way to develop 2D-MOF-based CO2RR electrocatalysts.