Metal-free boron-doped graphene for selective electroreduction of carbon dioxide to formic acid/formate

Abstract

Herein we report the electrocatalytic activity of boron-doped graphene for the reduction of CO2. Electrolysis takes place at low overpotentials leading exclusively to formate as the product (vis-à-vis benchmark Bi catalyst). Computational studies reveal mechanistic details of CO2 adsorption and subsequent conversion to formic acid/formate.

Carbon Solving Carbon's Problems: Recent Progress of Nanostructured Carbon‐Based Catalysts for the Electrochemical Reduction of CO2

“…which alter local electron density, active sites for the CO 2 RR can be formed. [29,50,51] Graphene materials have also been used as effective supports for metal nanoparticles active toward the CO 2 RR due to their large surface areas and excellent network conductivities, affording a metal-support synergy that enhances catalytic activity.…”

“…Graphene has also found a promising role in the field of catalysis due to the ability to fine tune its electronic structure through techniques like heteroatom doping and its excellent stability during catalytic operation. [47][48][49] Although graphene itself has been shown to possess no intrinsic catalytic activity toward CO 2 reduction, [50] by introducing atomic defects (through doping with heteroatoms like N, S, B etc.) which alter local electron density, active sites for the CO 2 RR can be formed.…”

“…Similar findings have also been found for boron doped graphene (B-graphene). [50] Synthesis of graphene for CO 2 reduction catalysts has largely been via high temperature pyrolysis of GO, [50,51] but CVD methods have also been used, [29] and doping of heteroatoms has been performed with post treatment methods. N-doping in this way provides better control over final N content and moiety type, and has direct implications on electrochemical performance.…”

Carbon-Based Metal-Free Electrocatalysis for Energy Conversion, Energy Storage, and Environmental Protection

“…Pyrrolic N is believed to 4 as the main product with a FE as high as 93.5% and a more than 6 times higher current density than metal Cu-based catalysts [216]. Along with N-doped carbon fibers and CNTs, borondoped graphene (BG) has also been studied for the reduction of CO 2 to formate [207]. Even boron-doped diamonds (BDD) have been demonstrated to show promising catalytic activity for the reduction of CO 2 to methanol, despite diamonds being often considered chemically inert [208].…”

“…In this context, carbon-based metal-free catalysts have also been used for CO 2 RR. Figure 11 and Table 1 represent recent advances in the development of carbon-based metal-free catalysts for CO 2 RR [36,37,[207][208][209][210][211][212][213][214].…”