Browse
Submit Data
Databases
API
Help

Dataset Information

29 Views

0 Connections

0 Citations

0 Reanalyses

0 Downloads

Omics score: 0

Overall water splitting by Pt/g-C3N4 photocatalysts without using sacrificial agents.

ABSTRACT: We report the direct splitting of pure water by light-excited graphitic carbon nitride (g-C3N4) modified with Pt, PtO x , and CoO x as redox cocatalysts, while pure g-C3N4 is virtually inactive for overall water splitting by photocatalysis. The novelty is in the selective creation of both H2 and O2 cocatalysts on surface active sites of g-C3N4via photodeposition triggering the splitting of water for the simultaneous evolution of H2 and O2 gases in a stoichiometric ratio of 2?:?1, irradiated with light, without using any sacrificial reagents. The photocatalyst was stable for 510 hours of reaction.

SUBMITTER: Zhang G

PROVIDER: S-EPMC6005136 | biostudies-literature | 2016 May

REPOSITORIES: biostudies-literature

ACCESS DATA

Json Xml

Publications

Overall water splitting by Pt/g-C3N4 photocatalysts without using sacrificial agents.

Zhang Guigang G Lan Zhi-An ZA Lin Lihua L Lin Sen S Wang Xinchen X

Chemical science 20160127 5

We report the direct splitting of pure water by light-excited graphitic carbon nitride (g-C3N4) modified with Pt, PtO x , and CoO x as redox cocatalysts, while pure g-C3N4 is virtually inactive for overall water splitting by photocatalysis. The novelty is in the selective creation of both H2 and O2 cocatalysts on surface active sites of g-C3N4via photodeposition trig ...[more]

PMID: 29997797

Similar Datasets

Monolayer Fullerene Networks as Photocatalysts for Overall Water Splitting.

Project description:Photocatalytic water splitting can produce hydrogen in an environmentally friendly way and provide alternative energy sources to reduce global carbon emissions. Recently, monolayer fullerene networks have been successfully synthesized [Hou et al. Nature2022, 606, 507], offering new material candidates for photocatalysis because of their large surface area with abundant active sites, feasibility to be combined with other 2D materials to form heterojunctions, and the C60 cages for potential hydrogen storage. However, efficient photocatalysts need a combination of a suitable band gap and appropriate positions of the band edges with sufficient driving force for water splitting. In this study, I employ semilocal density functional theory and hybrid functional calculations to investigate the electronic structures of monolayer fullerene networks. I find that only the weakly screened hybrid functional, combined with time-dependent Hartree-Fock calculations to include the exciton binding energy, can reproduce the experimentally obtained optical band gap of monolayer C60. All the phases of monolayer fullerene networks have suitable band gaps with high carrier mobility and appropriate band edges to thermodynamically drive overall water splitting. In addition, the optical properties of monolayer C60 are studied, and different phases of fullerene networks exhibit distinct absorption and recombination behavior, providing unique advantages either as an electron acceptor or as an electron donor in photocatalysis.

| S-EPMC9634807 | biostudies-literature

Bipolar charge collecting structure enables overall water splitting on ferroelectric photocatalysts.

Project description:Ferroelectrics are considered excellent photocatalytic candidates for solar fuel production because of the unidirectional charge separation and above-gap photovoltage. Nevertheless, the performance of ferroelectric photocatalysts is often moderate. A few studies showed that these types of photocatalysts could achieve overall water splitting. This paper proposes an approach to fabricating interfacial charge-collecting nanostructures on positive and negative domains of ferroelectric, enabling water splitting in ferroelectric photocatalysts. The present study observes efficient accumulations of photogenerated electrons and holes within their thermalization length (~50 nm) around Au nanoparticles located in the positive and negative domains of a BaTiO3 single crystal. Photocatalytic overall water splitting is observed on a ferroelectric BaTiO3 single crystal after assembling oxidation and reduction cocatalysts on the positively and negatively charged Au nanoparticles, respectively. The fabrication of bipolar charge-collecting structures on ferroelectrics to achieve overall water splitting offers a way to utilize the energetic photogenerated charges in solar energy conversion.

| S-EPMC9307613 | biostudies-literature

Photocatalytic Overall Water Splitting over MIL-125(Ti) upon CoPi and Pt Co-catalyst Deposition.

Project description:Photocatalytic overall water splitting is realized by taking advantage of the semiconductive and porous properties of MIL-125(Ti). CoPi and Pt are deposited into MIL-125(Ti) in two steps. The co-catalysts CoPi and Pt not only act as reactive sites for oxygen and hydrogen evolution, respectively, but also improve the photogenerated charge separation efficiency. The above conclusions are supported by the photoelectrical and photophysical results.

| S-EPMC5715264 | biostudies-literature

Vapor-Phase Photocatalytic Overall Water Splitting Using Hybrid Methylammonium Copper and Lead Perovskites.

Project description:Films or powders of hybrid methylammonium copper halide perovskite exhibit photocatalytic activity for overall water splitting in the vapor phase in the absence of any sacrificial agent, resulting in the generation of H2 and O2, reaching a maximum production rate of 6 ?mol H2 × g cat-1h-1 efficiency. The photocatalytic activity depends on the composition, degreasing all inorganic Cs2CuCl2Br2 perovskite and other Cl/Br proportions in the methylammonium hybrids. XRD indicates that MA2CuCl2Br2 is stable under irradiation conditions in agreement with the linear H2 production with the irradiation time. Similar to copper analogue, hybrid methylammonium lead halide perovskites also promote the overall photocatalytic water splitting, but with four times less efficiency than the Cu analogues. The present results show that, although moisture is strongly detrimental to the photovoltaic applications of hybrid perovskites, it is still possible to use these materials as photocatalysts for processes requiring moisture due to the lack of relevance in the photocatalytic processes of interparticle charge migration.

| S-EPMC7279556 | biostudies-literature

Single-site Pt-doped RuO2 hollow nanospheres with interstitial C for high-performance acidic overall water splitting.

Project description:Realizing stable and efficient overall water splitting is highly desirable for sustainable and efficient hydrogen production yet challenging because of the rapid deactivation of electrocatalysts during the acidic oxygen evolution process. Here, we report that the single-site Pt-doped RuO2 hollow nanospheres (SS Pt-RuO2 HNSs) with interstitial C can serve as highly active and stable electrocatalysts for overall water splitting in 0.5 M H2SO4. The performance toward overall water splitting have surpassed most of the reported catalysts. Impressively, the SS Pt-RuO2 HNSs exhibit promising stability in polymer electrolyte membrane electrolyzer at 100 mA cm-2 during continuous operation for 100 hours. Detailed experiments reveal that the interstitial C can elongate Ru-O and Pt-O bonds, and the presence of SS Pt can readily vary the electronic properties of RuO2 and improve the OER activity by reducing the energy barriers and enhancing the dissociation energy of *O species.

| S-EPMC8890715 | biostudies-literature

Why Do Sulfone-Containing Polymer Photocatalysts Work So Well for Sacrificial Hydrogen Evolution from Water?

Project description:Many of the highest-performing polymer photocatalysts for sacrificial hydrogen evolution from water have contained dibenzo[b,d]thiophene sulfone units in their polymer backbones. However, the reasons behind the dominance of this building block are not well understood. We study films, dispersions, and solutions of a new set of solution-processable materials, where the sulfone content is systematically controlled, to understand how the sulfone unit affects the three key processes involved in photocatalytic hydrogen generation in this system: light absorption; transfer of the photogenerated hole to the hole scavenger triethylamine (TEA); and transfer of the photogenerated electron to the palladium metal co-catalyst that remains in the polymer from synthesis. Transient absorption spectroscopy and electrochemical measurements, combined with molecular dynamics and density functional theory simulations, show that the sulfone unit has two primary effects. On the picosecond timescale, it dictates the thermodynamics of hole transfer out of the polymer. The sulfone unit attracts water molecules such that the average permittivity experienced by the solvated polymer is increased. We show that TEA oxidation is only thermodynamically favorable above a certain permittivity threshold. On the microsecond timescale, we present experimental evidence that the sulfone unit acts as the electron transfer site out of the polymer, with the kinetics of electron extraction to palladium dictated by the ratio of photogenerated electrons to the number of sulfone units. For the highest-performing, sulfone-rich material, hydrogen evolution seems to be limited by the photogeneration rate of electrons rather than their extraction from the polymer.

| S-EPMC9619400 | biostudies-literature

Laser Synthesis of Iridium Nanospheres for Overall Water Splitting.

Project description:Engineering surface structure of catalysts is an efficient way towards high catalytic performance. Here, we report on the synthesis of regular iridium nanospheres (Ir NSs), with abundant atomic steps prepared by a laser ablation technique. Atomic steps, consisting of one-atom level covering the surface of such Ir NSs, were observed by aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM). The prepared Ir NSs exhibited remarkably enhanced activity both for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) in acidic medium. As a bifunctional catalyst for overall water splitting, they achieved a cell voltage of 1.535 V @ 10 mA/cm2, which is much lower than that of Pt/C-Ir/C couple (1.630 V @ 10 mA/cm2).

| S-EPMC6766323 | biostudies-literature

Gradient tungsten-doped Bi3TiNbO9 ferroelectric photocatalysts with additional built-in electric field for efficient overall water splitting.

Project description:Bi3TiNbO9, a layered ferroelectric photocatalyst, exhibits great potential for overall water splitting through efficient intralayer separation of photogenerated carriers motivated by a depolarization field along the in-plane a-axis. However, the poor interlayer transport of carriers along the out-of-plane c-axis, caused by the significant potential barrier between layers, leads to a high probability of carrier recombination and consequently results in low photocatalytic activity. Here, we have developed an efficient photocatalyst consisting of Bi3TiNbO9 nanosheets with a gradient tungsten (W) doping along the c-axis. This results in the generation of an additional electric field along the c-axis and simultaneously enhances the magnitude of depolarization field within the layers along the a-axis due to strengthened structural distortion. The combination of the built-in field along the c-axis and polarization along the a-axis can effectively facilitate the anisotropic migration of photogenerated electrons and holes to the basal {001} surface and lateral {110} surface of the nanosheets, respectively, enabling desirable spatial separation of carriers. Hence, the W-doped Bi3TiNbO9 ferroelectric photocatalyst with Rh/Cr2O3 cocatalyst achieves an efficient and durable overall water splitting feature, thereby providing an effective pathway for designing excellent layered ferroelectric photocatalysts.

| S-EPMC10692145 | biostudies-literature

Plasmon-Induced Water Splitting on Ag-Alloyed Pt Single-Atom Catalysts.

Project description:A promising route to realize solar-to-chemical energy conversion resorts to water splitting using plasmon photocatalysis. However, the ultrafast carrier dynamics and underlying mechanism in such processes has seldom been investigated, especially when the single-atom catalyst is introduced. Here, from the perspective of quantum dynamics at the atomic length scale and femtosecond time scale, we probe the carrier and structural dynamics of plasmon-assisted water splitting on an Ag-alloyed Pt single-atom catalyst, represented by the Ag19Pt nanocluster. The substitution of an Ag atom by the Pt atom at the tip of the tetrahedron Ag20 enhances the interaction between water and the nanoparticle. The excitation of localized surface plasmons in the Ag19Pt cluster strengthens the charge separation and electron transfer upon illumination. These facts cooperatively turn on more than one charge transfer channels and give rise to enhanced charge transfer from the metal nanoparticle to the water molecule, resulting in rapid plasmon-induced water splitting. These results provide atomistic insights and guidelines for the design of efficient single-atom photocatalysts for plasmon-assisted water splitting.

| S-EPMC8573343 | biostudies-literature

Light illuminated α-Fe2O3/Pt nanoparticles as water activation agent for photoelectrochemical water splitting.

Project description:The photoelectrochemical (PEC) water splitting is hampered by strong bonds of H2O molecules and low ionic conductivity of pure water. The photocatalysts dispersed in pure water can serve as a water activation agent, which provides an alternative pathway to overcome such limitations. Here we report that the light illuminated α-Fe2O3/Pt nanoparticles may produce a reservoir of reactive intermediates including H2O2, ·OH, OH(-) and H(+) capable of promoting the pure water reduction/oxidation half-reactions at cathode and highly photocatalytic-active TiO2/In2S3/AgInS2 photoanode, respectively. Remarkable photocurrent enhancement has been obtained with α-Fe2O3/Pt as water activation agent. The use of α-Fe2O3/Pt to promote the reactivity of pure water represents a new paradigm for reproducible hydrogen fuel provision by PEC water splitting, allowing efficient splitting of pure water without adding of corrosive chemicals or sacrificial agent.

| S-EPMC5390902 | biostudies-literature