Materials For Photocatalytic Water Splitting Research Articles

Direct Z-scheme GeC/GaSe heterojunction by first-principles study for photocatalytic water splitting

In this study, we constructed the direct Z-scheme heterojunction by vertically stacking monolayers of GeC and GaSe. And systematically explored its stability, electronic structure, optical absorption characteristics and photocatalytic mechanism with first principles calculations. Our results show that the GeC/GaSe heterojunction possesses an indirect-gap of 1.88 eV and exhibits a staggered energy-band structure. In comparison to the individual monolayers of GeC and GaSe, the GeC/GaSe heterojunction has more excellent absorption of far-ultraviolet and visible light. And the electrons and holes in the GeC/GaSe heterojunction have a transmission path resembling the letter Z. There is also an internal electric field from GeC to GaSe in the heterojunction, which accelerates the photoelectrons and holes along the Z direction when the heterojunction receives light. Furthermore, further studies suggest that the GeC/GaSe heterojunction can be utilized as a photocatalytic material for water splitting under pH = 0–14. Besides, the bandwidth and optical absorption properties of the GeC/GaSe heterojunction can be adjusted by biaxial strains. Moreover, Gibbs free energy calculations during water splitting demonstrate that the GeC/GaSe heterojunction exhibits a highly driven force for both OER and HER. Thus, direct Z-scheme GeC/GaSe heterojunction has the capability to be a promising photocatalyst for water splitting.

Innovative 2D materials for efficient photocatalysis: A comparative study for WSi2N4, WGe2N4, and their janus counterpart WSiGeN4 monolayers

In pursuit of environmentally friendly and effective photocatalytic materials for water splitting, this research paper presents a thorough evaluation of WSi2N4, WGe2N4, and their Janus counterpart WSiGeN4 monolayers through the application of Density Functional Theory. The study elucidates the optical, electronic, and structural characteristics of these monolayers, thereby demonstrating their potential as highly favorable contenders for applications involving photocatalytic water splitting. By means of comprehensive optimization and analysis, it is shown that these monolayers possess advantageous characteristics, such as favorable band gaps, stable work functions, and stability over a broad pH range. These attributes are of utmost importance in ensuring the effectiveness of hydrogen evolution reaction (HER). The inclusion of Janus WSiGeN4, which possesses an intrinsic mirror asymmetry, significantly improves the photocatalytic efficacy of the material. This is achieved by meeting the demands of optimal redox reaction levels in both the conduction and valence bands. In conjunction with machine learning force fields, ab initio molecular dynamics (AIMD) simulations validate the thermal stability of these monolayers at 300 K. In addition, our analysis of the optical properties reveals substantial absorption in the visible spectrum - vital for photocatalytic applications powered by solar energy. In summary, the research highlights the potential of Janus WSiGeN4, WGe2N4, and WSi2N4 monolayers as multifunctional and effective substances for forthcoming photocatalytic water-splitting systems. This advancement indicates of a significant stride in the direction of sustainable energy solution development.

Theoretical Study of the Ternary Compound Monolayer CuP2Se for Photocatalytic Water Splitting with Efficient Optical Absorption.

Utilizing photocatalytic method to produce hydrogen by splitting water is an efficient strategy to solve the hotspot issues of energy crisis and environmental pollution. Herein, we systematically investigate the corresponding properties of the reported Cu-bearing ternary compound monolayer CuP2Se by using the first-principle calculations. The monolayer CuP2Se has quite small cleavage energy of 0.51 J/m2, indicating it can be easily produced by the mechanical exfoliation method experimentally. In addition, it is an indirect bandgap semiconductor material which has a moderate value of 1.91 eV. The conduction band minimum (CBM) and valence band maximum (VBM) can perfectly straddle the redox potentials of water when a biaxial strain of -4% to 4% is applied, unveiling the high photocatalytic thermodynamic stability of monolayer CuP2Se in response to the effect of solvent tension. Remarkably, the monolayer CuP2Se also demonstrates significant sunlight capturing ability in the visible region. The outstanding electronic and optical properties suggest that the monolayer CuP2Se is undoubtedly a viable material for photocatalytic water splitting.

Account of doping photocatalyst for water splitting

In the field of photocatalytic water splitting, the strategy of doping photocatalysts has emerged as a significant and extensively studied approach. Doping can effectively facilitate the modification of both the microstructure and energy band structure of the photocatalyst, addressing key performance limitations such as light absorption, position of the conduction and valence band minima (CBM and VBM), photogenerated carrier separation, and surface chemical reactions. In recent years, we have reported several works about the doping of rare earth elements into bismuth-based composite oxides. These endeavors are aimed at enhancing the conduction band minimum and achieving overall water splitting under visible light. Based on these bismuth-based composite oxides, we studied the effects of doping on the microstructures of photocatalysts, including exposed surfaces, surface properties, and defects. Recently, we introduce an innovative asymmetric doping technique—Selected Local Gradient Doping, intricately placing doped ions within nanocapsules. This approach allows for the gradual, controlled, and localized release of doped ions to the primary photocatalyst. Therefore, this account is to review our related research in the field of doping for photocatalytic water splitting. The primary focus on doping bismuth-based composite oxides and Asymmetry doping would significantly make contribution to the exploration of novel materials for photocatalytic water splitting under visible light and the enhancement of energy conversion efficiency.

NiS modified SrTiO3:Al bifunctional photocatalyst for H2 generation and cathodic protection

Developing low-cost and high-efficiency non-precious metal cocatalysts is the key to the practical application of photocatalysis technology. Here, nickel sulfide (NiS) nanoparticles were synthesized on the surface of strontium titanate (SrTiO3) via a hydrothermal method, identifying the optimal loading molar concentration of NiS as 10 %. The solar-to-hydrogen efficiency (STH) of 10%NiS/SrTiO3:Al was enhanced by 97 times compared to SrTiO3:Al and by 1.62 times compared to RhCrCoOx/SrTiO3:Al. This improvement is primarily attributed to the metallic-like properties of NiS, which enhance the photocatalyst's light absorption capacity and charge transfer capability. Additionally, the STH value of samples loaded with both NiS and RhCrCoOx reached 0.436 %, indicating a positive synergistic effect in photocatalysis between NiS and RhCrCoOx. Their photocathodic protection capability was also studied in simulated seawater conditions, showing a reduced self-corrosion potential (−0.31V) and a low interface charge impedance (5962 KΩ). This work reveals the potential of NiS as an alternative to precious metal cocatalysts, offering new possibilities for developing cost-effective and high-performance materials for photocatalytic water splitting and photocathodic protection.

First-principles study of direct Z-scheme GaS/WTe2 van der Waals heterostructure as photocatalyst for water splitting

The effective separation of charge carriers and the redox capacity for water splitting are two crucial factors that influence photocatalysis. Here, we studied the photocatalytic properties of GaS/WTe2 van der Waals heterostructure (vdWH) using first-principle calculations. The results show that this heterostructure acts as a direct Z-scheme with GaS as the water oxidation photocatalyst and WTe2 as the water reduction photocatalyst. Photogenerated charge carriers are efficiently separated, with electrons in GaS combining with holes in WTe2, while other charge carriers with high redox ability remain in the respective materials for water splitting. More importantly, the heterostructure exhibits excellent performance in all acid and alkali solutions (pH 0–14) and has strong light absorption in the ultraviolet (UV) and visible region. The power conversion efficiency(PCE) reaches 19.73%. This work reveals that GaS/WTe2 heterostructure is a highly promising material for photocatalytic water splitting.

Improved Carrier Separation and Recombination by Ferroelectric Polarization in the CuBiP2Se6/C2N Heterostructure: A Nonadiabatic Molecular Dynamics Study.

The rapid recombination of photogenerated carriers heavily restricts the photocatalytic efficiency. Here, we propose a new strategy to improve catalytic efficiency based on the ferroelectric van der Waals heterostructure (CuBiP2Se6/C2N). Combining density functional theory and the nonadiabatic molecular dynamics (NAMD) method, we have systematically analyzed the ground-state properties and carrier dynamics images in the CuBiP2Se6/C2N heterostructure. Our calculations showed that the ferroelectric polarization of CuBiP2Se6 provides the internal driving force for the photogenerated carriers separation. NAMD results demonstrate that the excited-state carrier transfer and recombination processes in the CuBiP2Se6/C2N are consistent with a type II mechanism. Meanwhile, constructing the ferroelectric heterostructure can effectively prolong the carrier lifetime, from ∼65.98 to ∼124.54 ps. Moreover, the high quantum efficiency and tunable band edge positions mean that the CuBiP2Se6/C2N heterostructure is an excellent potential candidate material for photocatalytic water splitting.

Emerging Light‐Harvesting Materials Based on Organic Photovoltaic D/A Heterojunctions for Efficient Photocatalytic Water Splitting

AbstractPhotocatalytic water splitting to hydrogen is a highly promising method to meet the surging energy consumption globally through the environmentally friendly means. As the initial step before photocatalysis, harvesting photons from sunlight is crucially important, thus making the design of photosensitizers with visible even near‐infrared (NIR) absorptions get more and more attentions. In the past three years, organic donor/acceptor (D/A) heterojunctions with absorptions extending to 950 nm, have emerged as the new star light‐harvesting materials for photocatalytic water splitting, demonstrating exciting advantages over inorganic materials in solar light utilization, hydrogen yielding rate, etc. This Minireview firstly gives a brief discussion about the principle processes and determining factors for photocatalytic water splitting with organic photovoltaic D/A heterojunction as photosensitizers. Thereafter, the current progress is summarized in details by introducing typical and excellent D/A heterojunction‐based photocatalytic systems. Finally, not only the great prospects but also the most challenging issues confronted by organic D/A heterojunctions are indicated along with a perspective on the opportunities and new directions for future material explorations.

Carrier mobility and optical properties of a type-II GaSe/ZnS heterostructure as a photocatalyst: a first-principles study.

In this paper, a new GaSe/ZnS van der Waals heterostructure (vdWH) was constructed and a systematic analysis of the electronic structure, interfacial properties, and transport and photocatalytic capacity of the GaSe/ZnS vdWH was performed by using first-principles calculations. It was found that the heterostructure exhibited excellent photocatalytic performance for water splitting. The direct band gap of the heterostructure calculated using the hybrid HSE06 functional was 2.19 eV, which had a good visible light absorption ability. The electronic structure of the type-II band arrangement effectively reduced the recombination of electron-hole pairs. The heterostructure also showed excellent transport ability, and the carrier mobility of electrons and holes along different directions was greatly improved. Additionally, as the electric field strength increased, the band gap width of the GaSe/ZnS vdWH narrowed and the heterostructure characteristics transitioned from semiconductor to metal properties, which were attributed to the appearance of near-free electronic (NFE) states induced by the strong electric field. Meanwhile, the optical absorption capacity of the heterostructure was greatly improved compared to the ZnS monolayer, reaching 1.44 × 105 cm-1 at an incident photon energy of 8.65 eV. Therefore, the GaSe/ZnS vdWH was proved to be an excellent photocatalytic material for water splitting in the present study.

Dense arrangement of crown ethers in graphene: novel graphitic carbon oxides with enhanced optoelectronic properties.

Incorporating crown ethers into a graphene lattice presents an efficient means of tuning its properties and expanding its range of potential applications. This study employed density functional theory calculations to introduce a series of novel graphitic carbon oxides through the dense arrangement of crown ethers featuring varying cavity sizes within the graphene structure. These newly developed graphitic carbon oxides exhibit thermodynamic and dynamic stability. They also manifest improved stability relative to previously reported graphene oxides with similar oxygen content. Notably, a robust linear relationship is observed between the cohesive energies and the proportion of oxygen atoms. The electronic properties of these graphitic carbon oxides span a spectrum of characteristics, including semi-metallic, metallic, and semi-conducting behavior. Their calculated band gaps range from 0.11 eV to 4.38 eV. Specifically, our analysis reveals that C6G-1, characterized by its largest crown ether-like nanopore with six oxygen atoms, holds potential as a material for photocatalytic water splitting. Moreover, these materials exhibit anisotropic optical properties, showcasing a significant enhancement in absorption within the infrared and visible regions relative to pristine graphene. Given the successful experimental synthesis of crown ether in graphene, we anticipate that our findings will contribute to the widespread utilization of graphene derivatives in low-dimensional electronic, catalytic, and optical devices.

Near-infrared-driven upconversion nanoparticles with photocatalysts through water-splitting towards cancer treatment.

Water splitting is promising, especially for energy and environmental applications; however, there are limited studies on the link between water splitting and cancer treatment. Upconversion nanoparticles (UCNPs) can be used to convert near-infrared (NIR) light to ultraviolet (UV) or visible (Vis) light and have great potential for biomedical applications because of their profound penetration ability, theranostic approaches, low self-fluorescence background, reduced damage to biological tissue, and low toxicity. UCNPs with photocatalytic materials can enhance the photocatalytic activities that generate a shorter wavelength to increase the tissue penetration depth in the biological microenvironment under NIR light irradiation. Moreover, UCNPs with a photosensitizer can absorb NIR light and convert it into UV/vis light and emit upconverted photons, which excite the photoinitiator to create H2, O2, and/or OH˙ via water splitting processes when exposed to NIR irradiation. Therefore, combining UCNPs with intensified photocatalytic and photoinitiator materials may be a promising therapeutic approach for cancer treatment. This review provides a novel strategy for explaining the principles and mechanisms of UCNPs and NIR-driven UCNPs with photocatalytic materials through water splitting to achieve therapeutic outcomes for clinical applications. Moreover, the challenges and future perspectives of UCNP-based photocatalytic materials for water splitting for cancer treatment are discussed in this review.

Monolayers Sn2Te2X4 (X = P, As) as promising materials for photocatalytic water splitting and flexible devices: a DFT study.

First principles calculation was performed to study the Sn2Te2X4 (X = P, As) monolayers. Structural investigation confirms the stability of the two monolayers with Young's modulus in the range of 30.34-33.65 N m-1 and a Poisson's ratio of 0.18-0.21. The two monolayers are semiconductors with a direct band gap of 1.52-1.66 eV. The light absorption rate of the two monolayers is rather high 104-105 cm-1. Both monolayers have high charge carrier mobility and suitable VBM and CBM positions for the redox reaction. The η STH efficiency of both materials (15.76-17.12%) is close to the theoretical limit of 18%. Moreover, moderate strains can improve the light absorption rate, while the suitable VBM and CBM positions are preserved. These characteristics suggest that Sn2Te2X4 (X = P, As) monolayers are good candidates for being applied in flexible devices and for the conversion of solar energy to other types of energy.

Unraveling the photocatalytic potential of transition metal sulfide and selenide monolayers for overall water splitting and photo-corrosion inhibition

A systematic study was carried out to identify transition metal sulfide and selenide (TMSS) monolayers, which resist both photo-degradation and photo-corrosion in a single electrolyte towards overall water splitting (OWS).

Prediction of novel penta-$${\text{Si}}_{3} {\text{P}}_{2} {\text{X}}$$ (X = S, Se) monolayers as photocatalytic materials for water splitting by first principles calculations

Prediction of novel penta-$${\text{Si}}_{3} {\text{P}}_{2} {\text{X}}$$ (X = S, Se) monolayers as photocatalytic materials for water splitting by first principles calculations

First-principles calculations to investigate structural, elastic, electronic, optical, and magnetic properties of Hg2WO4 for photocatalytic applications

In the present work, structural, elastic, electronic, optical, and magnetic properties of Hg2WO4 are investigated using CASTEP simulation tool. Generalized Gradient Approximation (GGA) along with Perdew-Burke-Ernzerhof (PBE) are employed for the calculation of electronic exchange and correlation energy. In structural analysis, Hg2WO4 is found to be stable with C-centered monoclinic structure having space group C2/c. Material’s ductile nature is confirmed with Pugh’s approximation where calculated B/G ratio is greater than 0.75 and Frantsevich’s rule where v is greater than 0.26. The calculations of electronic properties show that Hg2WO4 has indirect band gap of 2.14 eV. While the optical study reveals that Hg2WO4 has a good photosensitivity in visible light region. Furthermore, the spin-polarized treatment shows that Hg2WO4 is antiferromagnetic in nature. The current findings can be of great importance for the development of efficient photocatalytic materials for water splitting and associated applications.

Theoretical prediction of two-dimensional WSi2N4 materials for photocatalytic water splitting

Recently, novel two-dimensional (2D) crystals, MSi2N4 (M = Mo, W) materials, have been successfully synthesized experimentally and have comparable excellent catalytic properties as that of MoS2. The suitability of MA2Z4 family materials in photocatalytic water splitting can't be fully determined by whether the bandgap edge of the material cross the standard redox potential of water. Photoelectric properties and electron–hole separation are also critical factors to be considered. We investigated the bandgap edge positions and the photoelectric and the electron–hole excitation properties of 2D MoSi2N4 and its family of materials (CrSi2N4, WSi2N4) in water by first-principles calculations, and the results indicate that WSi2N4 may be a relatively high-performing photocatalyst. Relative to the MoSi2N4 bandgap (1.74 eV), the bandgap of WSi2N4 is 2.06 eV, and the conduction-band minimum edge band potential (−0.42 eV) is close to the hydrogen precipitation potential in water at pH = 7. The bandgaps of the MSi2N4 (M = Mo, W) materials cross the water redox potential (1.23 eV), and both have favorable adsorption for H2O molecules. However, compared with the absorption spectrum and excited states of MoSi2N4 in water, WSi2N4 exhibits a broader and more enhanced visible light absorption range and intensity as well as a higher electron–hole separation. 2D WSi2N4 could achieve the half-reaction of photocatalytic water splitting under visible light irradiation, and the photogenerated electrons in the conduction band can spontaneously reduce H+ ions to hydrogen, suggesting that WSi2N4 might be composed of a heterogeneous structure with other photocatalysts to accomplish the redox of water.

Asymmetric Embedded Benzene Ring in Graphite Carbon Nitride Enhanced Photocatalytic Hydrogen Evolution in Visible Light

Preventing the high recombination rate of carriers in graphite-carbon nitride (GCN) is essential for hydrogen production. In this work, we break the original symmetry of GCN by embedding benzene ring for enhanced visible-light absorption and carriers transfer efficiency. The new catalyst was prepared by a condensation reaction using dicyandiamide and 5-amino-2,4,6-triiodoisophthalic acid as precursors. It shows photocatalytic hydrogen evolution rate of 690.74[Formula: see text][Formula: see text][Formula: see text]mol[Formula: see text]g[Formula: see text][Formula: see text]h[Formula: see text], 9.3 times enhancement than the original GCN. This work provides a new strategy for designing efficient two-dimensional photocatalytic materials for water splitting.

Study of NiFe2O4/Cu2O p-n heterojunctions for hydrogen production by photocatalytic water splitting with visible light

To date, synthesis of visible light-active materials for photocatalytic water splitting is a promising challenge for future applications, e.g., photocatalytic reactors for hydrogen production with solar energy. Type p-n heterojunctions are an alternative to improve electronic properties of pure phase semiconductors and achieve a higher hydrogen production with photocatalytic water splitting. In this work, heterojunctions of NiFe2O4/Cu2O at mass percentages of 75/25, 50/50 and 25/75, are generated by impregnation method and thermal annealing starting from pristine materials NiFe2O4 and Cu2O synthesized by Pechini's method and Benedict's reaction respectively. A photocatalytic evaluation for hydrogen production was performed by means of gas chromatography for pristine and heterojunctions in order to correlate their textural, structural, chemical and electronic properties with their photocatalytic activity, finding a direct correlation between charge carrier concentration and hydrogen production. Finally, the material that exhibited higher hydrogen production was the 50/50 ratio with a production 120 times greater at 24 h in comparison with pristine photocatalysts.

Reverse Replacement in NH2 -MIL-125 with 1,4-Dicarboxybenzene for Enhanced Photocatalytic Hydrogen Generation.

Metal-organic frameworks (MOFs) constructed by ligands and metal clusters, have been considered as a promising material for photocatalytic water splitting. In this work, a solvent-assisted ligand exchange (SALE) method has been applied through partial reverse substitution of the ligand in NH2 -MIL-125 (Ti) by 1,4-dicarboxybenzene (BDC). This modification strategy can optimize the charge transfer dynamics together with the preserved light absorption, resulting in a 3.3 times higher hydrogen production rate compared to the pristine material under visible-light irradiation. This work broadens the field of ligand modifications of MOFs to boost the photocatalytic performance.

Development of Double Perovskite Oxide Photocatalysts for Efficient Visible-Light Driven Photocatalytic Water Splitting and CO2 Reduction

Energy and environment are the key global challenges in the 21st century. Solar energy is considered the most promising clean and sustainable energy resource due to its university, inexhaustible and environmental friendliness. One of the most viable means of solar energy conversion and utilization is artificially converting solar energy into chemical energy as natural photosynthesis does. H2 produced from water splitting and CO2 reduction, are the major research topics of artificial photosynthesis. However, the effective conversion of solar energy into chemical energy by cost-effective artificial means on a large scale remains elusive. Metal oxide-based photocatalysts are the most studied materials for photocatalytic water splitting and CO2 reduction. Particularly, perovskite oxides with the chemical formula of ABO3 have been intensively studied as semiconductor photocatalysts. However, overwhelmingly of the perovskite oxides are only active under UV-light-irradiation, which limited their potential in solar energy application. Therefore, breakthrough technology and step-change materials, particularly, visible-light-responsive photocatalysts are highly desirable for the development of photocatalytic systems. In recent years, copious progress has been made in designing materials that function under visible-light-irradiation. So far, the most successful strategy is anion doping of oxide semiconductors, such as nitrogen or sulfur dope to form oxynitrides and oxysulfides, respectively. For example, nitrogen-doped oxynitrides such as (Ga1-xZnx)(N1-xOx) and ANbO2N (A=Sr, Ba, and La)1, and sulfur-doped oxysulfides such as Sm2Ti2S2O5 2 showed efficient photocatalytic overall water splitting activities under visible-light-irradiation. Particularly, oxynitrides (Ga1-xZnx)(N1-xOx) based photocatalyst sheet, showed remarkable photocatalytic overall water splitting activity with AQE of more than 30% at l»420 nm3. However, these oxynitrides and oxysulfides suffer stability problems due to photocorrosion, hindering their potential practical application in photocatalytic applications. Recently, it has been theorized that double perovskite oxides (DPOs) with the chemical formula of A2BʹB"O6 can function as efficient and stable visible-light-responsive photocatalysts for photocatalytic water splitting and CO2 reduction. However, DPOs have been rarely studied for photocatalytic water splitting and CO2 reduction due to the difficulty of obtaining pure phase materials and the paucity of exposed active sites. Thus, developing efficient and stable visible-light-responsive DPOs photocatalysts for photocatalytic water splitting and CO2 reduction becomes important. In this regard, recently, we have demonstrated a series of efficient and stable visible-light-responsive DPOs photocatalysts for photocatalytic water splitting. For instance, Sr2CoWO6 and Sr2CoTaO6 can serve as an efficient and stable bifunctional photocatalyst for both photocatalytic oxygen evolution reaction (OER) and hydrogen evolution reaction(HER)4, 5, and Sr2NiWO6 can efficiently drive the photocatalytic OER6. Even though these DPOs have been demonstrated as visible-light-responsive photocatalysts with suitable CB and VB positions that straddle the theoretical potentials for overall water splitting, however, one-step overall water splitting has not been achieved so far, and their potential for photocatalytic CO2 reduction has not been studied yet. Overall water splitting under visible-light-irradiation based on particulate photocatalysts is a challenging reaction, which is regarded as one of the “Holy Grail” of sciences. And oxide semiconductors showing both photocatalytic OER and HER activities are rare. Nevertheless, bifunctional photocatalytic OER and HER were successfully demonstrated based on Sr2CoWO6 and Sr2CoTaO6. Further improvement of the material designs and developing appropriate cocatalysts may play a key role in achieving one-step overall water splitting under visible-light-irradiation based on DPOs photocatalysts. This work is mainly to explore the possibility of utilizing DPOs materials as visible-light-responsive photocatalysts for photocatalytic water splitting and CO2 reduction reaction, which is challenging work but has great potential value in advancing science and technology in photocatalysis. We anticipated that this work will provide a novel and rational strategy for improving the light absorption, charge separation and charge utilization in DPOs photocatalysts. References Maeda, K.; Teramura, K.; Masuda, H.; Takata, T.; Saito, N.; Inoue, Y.; Domen, K. 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