Premium
Electrocatalytic Reduction of Carbon Dioxide to Methane on Single Transition Metal Atoms Supported on a Defective Boron Nitride Monolayer: First Principle Study
Author(s) -
Tan Xin,
Tahini Hassan A.,
Arandiyan Hamidreza,
Smith Sean C.
Publication year - 2019
Publication title -
advanced theory and simulations
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.068
H-Index - 17
ISSN - 2513-0390
DOI - 10.1002/adts.201800094
Subject(s) - boron nitride , monolayer , transition metal , catalysis , boron , materials science , electrochemical reduction of carbon dioxide , chemistry , electron transfer , nitride , methane , electrochemistry , carbon fibers , methanol , inorganic chemistry , photochemistry , nanotechnology , electrode , carbon monoxide , organic chemistry , layer (electronics) , composite number , composite material
The electrochemical conversion of carbon dioxide (CO 2 ) and water into useful multi‐electron transfer products, such as methanol (CH 3 OH) and methane (CH 4 ), is a major challenge in facilitating a closed carbon cycle. Here, a systematic first principle study of the potential of single transition metal atoms (Sc to Zn, Mo, Rh, Ru, Pd, Ag, Pt, and Au) supported on experimentally available defective boron nitride monolayers with a boron monovacancy (TM/defective BN) to achieve highly efficient electrocatalytic CO 2 reduction (ECR) to CH 4 is carried out. Our computations reveal that Fe/defective BN, Co/defective BN, and Pt/defective BN nanosheets possess outstanding ECR activities with quite low (less negative) onset potentials of −0.52, −0.68, and −0.60 V, respectively. Given that Fe and Co are nonprecious metals, Fe/defective BN and Co/defective BN may provide cost‐effective electrocatalysts. The high ECR activities of these TM/defective BN catalyst systems stem from the moderate electrocatalysts’ affinities for C and O, which modulate the free energies of ECR intermediates in the reaction pathways. Moreover, it is found that Fe/defective BN and Pt/defective BN show high selectivity of ECR to CH 4 . This finding highlights a strategy to design highly active and selective single‐atom electrocatalysts for ECR to CH 4 .