Unveiling the Dominant Influence of First-Order Rotational Defects in Molybdenum Ditelluride: Insights into Adsorption of Nonpolar Gas Molecules

Mehrez, Jaafar Abdul-Aziz1,2; Zeng, Min1; Liu, Xue1,2; Zhang, Yongwei1,2; Wu, Jian1,2; Yang, Jianhua1,2; Hu, Nantao1,2; Xu, Lin4,5; Cai, Wei3; Yang, Zhi1

2024-06-12

10.1021/acs.jpcc.4c00507

JOURNAL OF PHYSICAL CHEMISTRY C   影响因子和分区

1932-7447

1932-7455

Structural defects exert a significant influence in shaping the functionality of materials. However, the structure-activity relationship between rotational defects in transition metal dichalcogenides and their gas-sensing performance remains unclear, necessitating further research to systematically reveal the sensing mechanism of these materials. In this study, we address this knowledge gap by examining the impact of first-order rotational defects, specifically trefoil-shaped defects in molybdenum ditelluride (MoTe2), in detecting nonpolar gas molecules. Thus, employing first-principles theory, we unveil the enhanced adsorption phenomenon of the gas molecules [(acetylene (C2H2), ethylene (C2H4), methane (CH4), carbon dioxide (CO2), and hydrogen (H-2)] facilitated by first-order rotational defects in MoTe2. Our comprehensive studies reveal the exceptional selectivity of MoTe2 with first-order rotational defects toward C2H4, surpassing other gas molecules. Investigating the adsorption process of C2H4 over MoTe2 with a trefoil-like defect, heightened adsorption energy, and charge transfer are observed compared to pristine and single-point defect monolayers, highlighting the superior performance of the trefoil defect. Furthermore, we calculate the electrical conductivity using a semiclassical approach based on the Boltzmann transport equation, demonstrating a markedly higher relative response of 53.9% for MoTe2 with rotational defect, outperforming single-point defect (2.59%) and pristine MoTe2 (0.7%). Remarkably, ab initio molecular dynamics simulations and transition state theory analysis confirm the thermodynamic stability of the gas/substrate complex. Notably, the trefoil defect material exhibits efficient gas desorption without disrupting the dynamic response process, rendering it ideal for nonpolar gas-sensing applications. These findings deepen our understanding of nonpolar gas adsorption on MoTe2 with first-order rotational defects, offering insights into designing defect-optimized materials and advancing gas-sensing capabilities across diverse applications.

SCI ; EI

英语

其他

Natural Science Foundation of Shanghai Municipality[2022YFC3104700] ; National Key Research and Development Program of China["62371299","62301314","62101329"] ; National Natural Science Foundation of China[2023M732198] ; China Postdoctoral Science Foundation[23ZR1430100]

Chemistry ; Science & Technology - Other Topics ; Materials Science

Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary

WOS:001246075700001

AMER CHEMICAL SOC

20242516273724

Charge transfer ; Chemical detection ; Defects ; Ethylene ; Gas detectors ; Gases ; Molecular dynamics ; Molecules ; Molybdenum compounds ; Thermodynamic stability ; Transition metals

Metallurgy and Metallography:531 ; Thermodynamics:641.1 ; Chemistry:801 ; Physical Chemistry:801.4 ; Chemical Reactions:802.2 ; Organic Compounds:804.1 ; Inorganic Compounds:804.2 ; Accidents and Accident Prevention:914.1 ; Atomic and Molecular Physics:931.3 ; Special Purpose Instruments:943.3 ; Materials Science:951

Web of Science

1.Shanghai Jiao Tong Univ, Natl Key Lab Adv Micro & Nano Manufacture Technol, Shanghai 200240, Peoples R China
2.Shanghai Jiao Tong Univ, Sch Elect Informat & Elect Engn, Dept Micro Nano Elect, Shanghai 200240, Peoples R China
3.Southern Univ Sci & Technol, Dept Ocean Sci & Engn, Shenzhen 518055, Peoples R China
4.Shanghai Eye Hosp, Shanghai Eye Dis Prevent & Treatment Ctr, Shanghai, Peoples R China
5.Shanghai Jiao Tong Univ, Shanghai Gen Hosp, Shanghai Engn Ctr Visual Sci & Photomed, Natl Clin Res Ctr Eye Dis,Sch Med,Dept Ophthalmol,, Shanghai 200080, Peoples R China

Mehrez, Jaafar Abdul-Aziz,Zeng, Min,Liu, Xue,et al. Unveiling the Dominant Influence of First-Order Rotational Defects in Molybdenum Ditelluride: Insights into Adsorption of Nonpolar Gas Molecules[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2024,128(25):10595-10613.

Mehrez, Jaafar Abdul-Aziz.,Zeng, Min.,Liu, Xue.,Zhang, Yongwei.,Wu, Jian.,...&Yang, Zhi.(2024).Unveiling the Dominant Influence of First-Order Rotational Defects in Molybdenum Ditelluride: Insights into Adsorption of Nonpolar Gas Molecules.JOURNAL OF PHYSICAL CHEMISTRY C,128(25),10595-10613.

Mehrez, Jaafar Abdul-Aziz,et al."Unveiling the Dominant Influence of First-Order Rotational Defects in Molybdenum Ditelluride: Insights into Adsorption of Nonpolar Gas Molecules".JOURNAL OF PHYSICAL CHEMISTRY C 128.25(2024):10595-10613.