Density functional theory-based screening of Ti4C3O2-loaded single atoms for efficient selective catalytic oxidation of formaldehyde
Zheng Zhao, Cheng Zhang, Junchen Li, Dingli Fang, Peng Tan, Qingyan Fang, Gang Chen
Abstract
Indoor formaldehyde (HCHO) pollution poses a major risk to human health. Low-temperature catalytic oxidation is an effective method for HCHO removal. The high activity and selectivity of single atomic catalysts provide a possibility for the development of efficient non-precious metal catalysts . In this study, the most stable single-atom catalyst Ti–Ti 4 C 3 O 2 was screened by density functional theory among many single atomic catalysts with two-dimensional (2D) monolayer Ti 4 C 3 O 2 as the support. The computational results show that Ti–Ti 4 C 3 O 2 is highly selective to HCHO and O 2 in complex environments. The HCHO oxidation reaction pathways are proposed based on the Eley-Rideal (E-R) and Langmuir-Hinshelwood (L-H) mechanisms. According to the reaction energy and energy span models, the E-R mechanism has a lower maximum energy barrier and higher catalytic efficiency than the L-H mechanism. In addition, the stability of the Ti–Ti 4 C 3 O 2 structure and active center was verified by diffusion energy barrier and ab initio molecular dynamics simulations . The above results indicate that Ti–Ti 4 C 3 O 2 is a promising non-precious metal catalyst. The present study provides detailed theoretical insights into the catalytic oxidation of HCHO by Ti–Ti 4 C 3 O 2 , as well as an idea for the development of efficient non-precious metal catalysts based on 2D materials .