Ferroelectric switching driven photocatalytic overall water splitting in the As/In₂Se₃ heterostructure

Journal of Materials Chemistry A, Год журнала: 2025, Номер unknown

Опубликована: Янв. 1, 2025

The photocatalytic overall water splitting can be achieved in the As/In 2 Se 3 vdW heterostructure by regulating polarization direction of In layer.

Язык: Английский

---

Recent Progress in Computational Design of Single-Atom/Cluster Catalysts for Electrochemical and Solar-Driven N₂ Fixation

ACS Catalysis, Год журнала: 2022, Номер 12(24), С. 15541 - 15575

Опубликована: Дек. 5, 2022

Fixation of dinitrogen into ammonia is an essential biological process for the evolution life, and at same time component many industrial processes, including fertilizers, plastics, so on. NH3 also known as best alternative to H2 in fuel cells. However, due chemical inertness, direct conversion N2 not possible; a suitable catalyst required. The century-old Haber–Bosch process, utilizing Fe-based catalyst, extremely energy-intensive eco-unfriendly consumption fossil fuels. In recent years, huge development has taken place design applications electro- photocatalysts artificial fixation. First-principles calculations have been considered powerful avenue theoretical screening promising catalysts through rational analysis plausible mechanisms or pathways reactions. present review focuses on developments various unsupported nanoclusters supported single-atom cluster application photochemical reduction support substrates include oxides, carbides, nitrides metal-based 2D materials, porous carbonaceous metal-free materials containing main-group elements like B, C, N, P. Although some reviews already made, focusing research related either photocatalytic fixation different catalysts, here we give comprehensive account both electrochemical nitrogen reaction (NRR) activities selectivities polyatomic catalysts. Additionally, comparative assessment made basis free energy adsorption, most favorable pathway, potential limiting step, corresponding NRR.

Язык: Английский

---

Emergence of Z-Scheme Photocatalysis for Total Water Splitting: An Improvised Route to High Efficiency

The Journal of Physical Chemistry Letters, Год журнала: 2024, Номер 15(26), С. 6841 - 6851

Опубликована: Июнь 25, 2024

Photocatalytic water splitting to spontaneously produce H2 and O2 is a long-standing goal in solar energy conversion, presenting significant challenge without using sacrificial electron donors or external biases. Inspired by natural photosynthesis, the design of artificial Z-scheme photocatalytic systems at forefront this field. These achieve higher redox potential separating photogenerated electrons holes through fast interlayer recombination process between valence conduction band edges. photocatalysis involves two different semiconductors with distinct bandgap energies. Here, we explore based on two-dimensional (2D) heterostructures composed carbon, nitrogen, similar main group elements. The advantages disadvantages these are discussed, focus enhancing their efficiency strategic design. Special emphasis placed dynamics excited charge carrier transfer processes, which crucial for developing efficient overall splitting.

Язык: Английский

---

Exploring the Ti₂CO₂–WSe₂ Heterostructure as a Direct Z-Scheme Photocatalyst for Water Splitting: A Non-Adiabatic Study

The Journal of Physical Chemistry C, Год журнала: 2022, Номер 126(49), С. 20852 - 20863

Опубликована: Дек. 2, 2022

One of the potential strategies to solve renewable energy shortage is design low-cost efficient photocatalysts for water splitting aid hydrogen and oxygen evolution reactions (HER OER). Two-dimensional (2D) materials like MXenes transition metal dichalcogenides (TMDs) have caught special attention owing their unique optical, electrical, mechanical properties, but come with issues photocorrosion poor charge separation. Bilayer vdW heterojunctions suitable constitutive monolayers are coming up as a solution these hazards, accredited tunable band gap In this paper, we investigated possibility Ti2CO2–WX2 (X = S, Se, Te) heterostructures perform Z-scheme by employing first-principle density functional calculations, thereby, Ti2CO–WSe2 heterostructure has emerged most promising material photocatalysis. Further, excited-state dynamics simulation reveals that timescales electron transfer hole greater (1.13 1.22 ps, respectively) than maximum time limit photogenerated electron–hole recombination (1.0 ps) weaker non-adiabatic coupling electron–phonon coupling. This affirms fact electrons holes redox ability preserved drive photocatalytic pathway. addition that, free calculations associated HER OER processes entail occur spontaneously on surface without any co-catalyst. establishes mediator-free direct photocatalyst overall splitting.

Язык: Английский

---

Theoretical prediction of the potential of using two-dimensional V2S2 as an effective anode for alkali metal ion batteries

Surfaces and Interfaces, Год журнала: 2024, Номер 51, С. 104750 - 104750

Опубликована: Июль 6, 2024

Язык: Английский

---

Point defect-mediated hot carrier relaxation dynamics of lead-free FASnI₃ perovskites

Nanoscale, Год журнала: 2024, Номер 16(9), С. 4737 - 4744

Опубликована: Янв. 1, 2024

In search of a promising optoelectronic performance, we herein investigated the hot carrier relaxation dynamics lead-free cubic phased bulk formamidinium tin triiodide (FASnI 3 ) perovskite.

Язык: Английский

---

Hot Carrier Controlled Nitrogen Fixation Reaction in Metal-Free Boron-Anchored Aza-COF: Insight from Nonadiabatic Molecular Dynamics Simulation

The Journal of Physical Chemistry Letters, Год журнала: 2024, Номер 15(18), С. 4898 - 4905

Опубликована: Апрель 29, 2024

Designing highly efficient photocatalysts for the production of renewable energy is a challenging task that necessitates simultaneous control chemical activity and photocarrier dynamics particular reaction. To this end, we have investigated catalytic mechanism real-time nitrogen reduction reaction (NRR) at metal-free boron-functionalized 2D aza-COF (B-aza-COF), an inexpensive environmentally friendly semiconductor. By employing density functional theory (DFT) time-dependent ab initio nonadiabatic molecular simulation, electronic structure, light harvesting ability, free change, photoexcited carriers. Our calculated results reveal gas phase N2 molecule can be effectively reduced into NH3 on B-aza-COF under UV–visible light. Therefore, our investigation design provides cost-effective opportunity sustainable NH3.

Язык: Английский

---

How the Stacking Pattern Influences the Charge Transfer Dynamics of van der Waals Heterostructures: An Answer from a Time-Domain Ab Initio Study

The Journal of Physical Chemistry Letters, Год журнала: 2023, Номер 14(34), С. 7672 - 7679

Опубликована: Авг. 21, 2023

Here, we perform a time domain density functional study in conjunction with non-adiabatic molecular dynamics (NAMD) simulation to investigate the charge carrier series of van der Waals heterostructures made two-dimensional (2D) SnX2 (X = S or Se)-supported ZrS2, ZrSe2, and ZrSSe monolayers. Results from NAMD reveal delayed electron-hole recombination (in range 0.53-2.13 ns) ultrafast electron/hole transfer processes (electron within 108.3-321.5 fs hole between 107.6 258.8 fs). The most interesting finding our is that switching AB AA stacking extends lifespan by significant amount. because pattern can be rationalized weak electron-phonon coupling, lower coupling (NAC), fast decoherence time. Thus, these insightful studies excited carriers variation an effective tool develop efficient photovoltaic devices based on 2D heterostructures.

Язык: Английский

---

Hot carrier relaxation dynamics of an aza-covalent organic framework during photoexcitation: An insight from ab initio quantum dynamics

The Journal of Chemical Physics, Год журнала: 2024, Номер 160(16)

Опубликована: Апрель 22, 2024

In order to develop an efficient metal-free solar energy harvester, we herein performed the electronic structure calculation, followed by hot carrier relaxation dynamics of two dimensional (2D) aza-covalent organic framework time domain density functional calculations in conjunction with non-adiabatic molecular (NAMD) simulation. The calculation shows that (COF) is a direct bandgap semiconductor acute charge separation and effective optical absorption UV-visible region. Our study simulation predicts sufficiently prolonged electron-hole recombination process (6.8 nanoseconds) comparatively faster electron (22.48 ps) hole (0.51 this two-dimensional aza-COF. According our theoretical analysis, strong electron-phonon coupling responsible for rapid relaxation, whereas slowed down relatively weak coupling, lower quick decoherence time. We do hope results NAMD on exciton will be helpful designing photovoltaic devices based

Язык: Английский

---

Rational design of Two-Dimensional Buckled-Hexagonal Nb2S2 monolayer as an efficient anode material for Ca-ion Batteries: A First-Principles study

Computational Materials Science, Год журнала: 2023, Номер 230, С. 112539 - 112539

Опубликована: Окт. 1, 2023

Язык: Английский

---