Insights into Photogenerated Carrier Dynamics and Overall Water Splitting of the CrS₃/GeSe Heterostructure

Abstract

Based on the nonadiabatic molecular dynamics (NAMD) simulations and the first-principles calculations, we explore the overall water-splitting schemes and the photogenerated carrier dynamics for two configurations (CG and C y G) of the CrS3/GeSe van der Waals heterostructures. The photocatalytic direct Z-schemes and carrier migration pathways for hydrogen and oxygen evolution reactions (HER/OER) are constructed based on the electronic properties. The solar-to-hydrogen efficiency (η′STH values) of the schemes can reach 10.60% and 10.17% and further rise under tensile strain. The NAMD results demonstrate similar transfer times of the electron/hole for HER/OER and more rapid electron–hole recombination in CG enables it to be superior to C y G in photocatalytic performance. Moreover, the Gibbs free energy indicates that both the HERs and OERs turn to spontaneously proceed with CG and C y G at pH = 0–12.37 and pH = 2.55–11.01, respectively. These facts reveal that the CrS3/GeSe heterostructure is promising in photocatalytic overall water splitting.

Two-dimensional trilayer heterostructures with cascade dual Z-schemes to achieve efficient hydrogen evolution reaction

“…Notably, the η ′ STH 's of Bi/HfSeTe/ZrSe 2 -I, Bi/HfSeTe/ZrSe 2 -II, and InAs 3 /HfSeTe/ZrSe 2 -II were much larger than those of ZrS 2 /MoSSe (6.4%), 64 HfSe 2 /InSe (25.24%), 15 and AlP 3 /GaP 3 (16.89%). 65 Moreover, the η ′ STH can also be compared with the experimental data if the AQE and experimental STH conversion efficiency (STH exp ) are available in the literature, 66 although the ideal quantum efficiency was used in eqn (3). For example, the GaN:Mg/InGaN:Mg nanowires 67 and Rh/Cr 2 O 3 /Co 3 O 4 -loaded InGaN/GaN nanowires 68 had STH exp 's of 3.3% and 9% corresponding to the η ′ STH 's of 7.5% and 17.7%, respectively.…”

Heterostructures stacked with X2SY (X = In, Ga; Y = Se, Te) and g-C2N monolayers for high power conversion efficiency solar cells: insight from electronic properties and nonadiabatic dynamics

“…5a–c, 3 processes including electron transfer (①), hole transfer (②), and interlayer/intralayer e–h recombination (③) occur in the three heterostructures under light. The time population evolutions of carriers for the three processes in the three heterostructures can be simulated by NAMD with the DISH method 32 based on the nonadiabatic coupling (NAC) factor defined as 53,54 …”

Self-trapped holes, oxygen vacancies and electrocatalytic performance of Zn-doped β-Ga2O3 microspindles

“…5 However, due to the presence of self-trapped holes (STHs), the mobility of carriers in β-Ga 2 O 3 micro- or nanostructure is greatly limited, which could reduce the effective utilization rate of the active sites during photocatalytic or electrocatalytic processes. 6,7…”