First-principles study of ferroelectric properties and CO2 reduction reaction capabilities in two-dimensional monolayers and heterostructures

Author

Mo Li, New Jersey Institute of TechnologyFollow

Author ORCID Identifier

0000-0002-1828-3964

Document Type

Dissertation

Date of Award

12-31-2024

Degree Name

Doctor of Philosophy in Materials Science and Engineering - (Ph.D.)

Department

Chemical and Materials Engineering

First Advisor

Joshua Young

Second Advisor

Xianqin Wang

Third Advisor

Gennady Gor

Fourth Advisor

Mengqiang Zhao

Fifth Advisor

Farnaz A .Shakib

Sixth Advisor

Lucas Dorazio

Abstract

Two-dimensional (2D) materials hold significant potential for CO₂ reduction reactions (CO₂RR) due to their high surface-to-volume ratio. However, achieving high selectivity for desired products and overcoming limitations posed by scaling relationships remain challenging. Recent studies suggest that ferroelectric (FE) materials with switchable out-of-plane polarization (OOP) can effectively tune the adsorption behavior, thermodynamics, and kinetics of CO₂RR, offering promising solutions to these challenges. Using density functional theory (DFT) and the Berry phase approach, this work expands the family of 2D ferroelectrics by theoretically identifying Y₂CO₂, Y₂CS₂, and Sc₂CS₂—members of the MXenes family—as stable ferroelectric materials. Y₂CO₂ was selected for its photocatalytic suitability in CO₂RR, demonstrating that switchable polarization can optimize CO adsorption and modulate selectivity between CO and formic acid. Additionally, In₂Se₂—an experimentally realized FE material—was studied as a substrate for graphene-embedded Fe single-atom catalyst (SAC) and 2Fe dual-atom catalyst (DAC). The findings reveal that the ferroelectric polarization in In₂Se₂ enhances CO selectivity on Fe SAC and promotes ethanol production on 2Fe DAC. This work advances understanding of the mechanisms by which ferroelectric materials improve CO₂RR efficiency and provides theoretical guidance for future experimental study.

Recommended Citation

Li, Mo, "First-principles study of ferroelectric properties and CO2 reduction reaction capabilities in two-dimensional monolayers and heterostructures" (2024). Dissertations. 1806.
https://digitalcommons.njit.edu/dissertations/1806