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

Abstract

AbstractElectrochemical 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.KEYWORDS: CO2 reduction; two-dimensional metal-organic frameworks; density functional study; reaction mechanism Disclosure statementNo potential conflict of interest was reported by the author(s).Additional informationFundingThis work is supported by The National Natural Science Foundation of China (21963009 and 22373097), The Program for Innovative Research Program of Science and Technology at Universities of Inner Mongolia Autonomous Region Team in Universities of Inner Mongolia Autonomous Region (NMGIRT2214), The Local Scientific and Technological Development Plan guided by the Central Government (2021ZY0025), The Grassland Talents Engineering of Inner Mongolia and The Light of West China Program by Chinese Academy of Sciences. The computational time is supported by the computing centre of Changchun Institute of Applied Chemistry.