Heterojunctions formed by polyoxometalates and 2D materials draw attention owing to their remarkable photoelectric and catalytic properties. However, the intrinsic mechanisms of polyoxometalates regulating the heterojunction photoelectric properties are unclear. Herein, we constructed two types of heterojunctions by integrating polyoxometalates (Keggin-type HPWO and Lindqvist-type HWO) on g-CN monolayers, exploring photoexcited carrier dynamics in these heterojunctions by ab initio calculations combined with nonadiabatic molecular dynamics (NAMD) simulations. Our results show that electrons and holes in HPWO on g-CN monolayers relax within 583 and 760 fs, respectively. The electron-hole recombination occurs at 342 fs, faster than carrier separation, aligning with the behavior of Z-type heterojunctions. Contrarily, the HWO/g-CN heterojunction exhibits the typical characteristics of type II heterojunctions, with a long photogenerated carrier lifetime reaching 652 fs. These findings show tunable band alignment in polyoxometalate-supported systems by modulating polyoxometalate type, influencing hot electron dynamics, and guiding 0D/2D heterojunction design.
Download full-text PDF |
Source |
|---|---|
| http://dx.doi.org/10.1021/acs.jpclett.4c02102 | DOI Listing |
Publication Analysis
Top Keywords
Similar Publications
Theoretical Investigation of Single-, Double-, and Triple- -block Metals Anchored on g-CN Monolayer for Oxygen Electrocatalysis.
J Phys Chem Lett
November 2024
Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion and Synergetic Innovation Centre of Quantum Information and Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026, China.
The design and development of highly active non-noble metal electrocatalysts for the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) are crucial for metal-air batteries. In this work, the electrocatalytic performance of different -block metal (PM = Sn, Sb, Pb and Bi) atoms embedded in the g-CN monolayer (PM@g-CN, = 1-3) for the OER and ORR was systematically investigated by density functional theory (DFT). The strong interaction between PM atoms and g-CN substrates indicates the good stability of PM@g-CN catalysts.
View Article and Find Full Text PDFSiCN monolayer as a universal anode for alkali metal-ion batteries.
Dalton Trans
August 2023
College of Chemistry, Fuzhou University, Fuzhou, 350108 Fujian, China.
Our density functional theory calculations show that silicon doping in g-CN (SiCN) can improve the electrochemical performance of g-CN as an anode of alkali metal-ion batteries and solve the problems of too high adsorption ability and migration energy barrier commonly found in porous carbon nitride. The stability of SiCN was verified by molecular dynamics simulations and phonon spectroscopy. Elastic constant calculations revealed that the Si doping in g-CN can improve its mechanical properties.
View Article and Find Full Text PDFReversible Hydrogen Storage Media by g-CN Monolayer Decorated with NLi: A First-Principles Study.
Nanomaterials (Basel)
February 2023
Material Science and Engineering Department, City University of Hongkong, Hongkong 999077, China.
A two-dimensional graphene-like carbon nitride (g-CN) monolayer decorated with the superatomic cluster NLi was studied for reversible hydrogen storage by first-principles calculations. Molecular dynamics simulations show that the g-CN monolayer has good thermal stability at room temperature. The NLi is firmly anchored on the g-CN monolayer with a binding energy of -6.
View Article and Find Full Text PDFEnhanced performance of hydroxyl and cyano group functionalized graphitic carbon nitride for efficient removal of crystal violet and methylene blue from wastewater.
RSC Adv
December 2022
Chemistry Department, Faculty of Science, Mansoura University Mansoura 35516 Egypt
Article Synopsis
- Researchers developed a new multifunctional carbon nitride adsorbent (f/g-CN) for effectively removing dyes like crystal violet and methylene blue from wastewater.
- The f/g-CN was created through pyrolysis of melamine and further treatment, resulting in significantly higher dye adsorption capacities compared to standard carbon nitride.
- The adsorbent achieved 100% removal of the dyes at low concentrations in just 60 seconds, maintained about 90% effectiveness after seven uses, and operates based on specific interactions between its functional groups and the dye molecules.
Ultrafast Charge Transfer and Delayed Recombination in Graphitic-CN/WTe van der Waals Heterostructure: A Time Domain Ab Initio Study.
J Phys Chem Lett
September 2022
Department of Chemistry, Visva-Bharati University, Santiniketan 731235, India.
In search of an efficient solar energy harvester, we herein performed a time domain density functional study coupled with nonadiabatic molecular dynamics (NAMD) simulation to gain atomistic insight into the charge carrier dynamics of a graphitic carbon nitride (g-CN)-tungsten telluride (WTe) van der Waals heterostructure. Our NAMD study predicted ultrafast electron (589 fs) and hole-transfer (807 fs) dynamics in g-CN/WTe heterostructure and a delayed electron-hole recombination process (2.404 ns) as compared to that of the individual g-CN (3 ps) and WTe (0.
View Article and Find Full Text PDFWant AI Summaries of new PubMed Abstracts delivered to your In-box?
Enter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!