The photocatalytic production of H2 in one step is potentially one of the most promising ways for the conversion and storage of solar energy. The paper overviews our recent studies on the photocatalysts splitting water into hydrogen under irradiation. The attention was mainly focused on the promotion effects of nanosized modifications in the interlayer and surface of photocatalysts for hydrogen evolution with visible light. The photocatalytic activity depended significantly on modification techniques, such as loading, proton exchange, and intercalation. The formation of a ‘‘nest’’ on the particle surface promoted a uniform distribution and strong combination of the nanosized particles on the surface of catalysts. By the methods of intercalation and pillaring as well as by selecting both host and guest, a large variety of molecular designed host–guest systems were obtained. Cadmium sulfide (CdS)-intercalated composites showed higher activity and stability. This activity of K4Ce2M10O30 (M = Ta, Nb) evolving H2 under visible light irradiation was enhanced by the incorporation of Pt, RuO2 and NiO as co-catalysts. Especially, the nanosized NiOx (Ni–NiO double-layer structure) greatly prompted the photocatalytic H2 evolution significantly. 相似文献
The simultaneous degradation of real-time industrial effluent and hydrogen production was carried out in this study, taking into account the global clean energy demand. A novel photocatalyst based on a metal–organic framework and spindle-shaped titanium dioxide nanoparticles was synthesized to perform photocatalytic water splitting reactions. The resulting composite (MIL-53@TiO2, MIL: Matériaux de l′Institut Lavoisier) was characterized by standard analytical methods. The photocatalytically active MIL-53@TiO2 composite produced hydrogen without using any sacrificial agents. The hydrogen production was observed to be 0.26 mmol in the presence of TiO2 which increased to 7.9 mmol in the presence of MIL-53@TiO2 composite after 180 min of irradiation. The corresponding hydrogen evolution rate was 26.33 mmol h-1g?1, which was observed 30 times higher than the pristine materials. The remarkable photoactivity was due the superior charge separation property and less recombination of the charge carrier pair in the MIL-53@TiO2 composite. Furthermore, the photocatalyst exhibited excellent reusability for hydrogen production up to 4 cycles. The results shown in the present work may be extended for large-scale applications. 相似文献
It is expected that in the future hydrogen will play a major role in the storage, distribution, and usage of energy involving its various physical states: gaseous—solid hydride—cryogenic liquid. One of the most modern concepts for the production of hydrogen from water, thermochemical cycles, is reviewed and a compilation of 72 published cycles is presented. 相似文献
Enhancing electrocatalytic water splitting performance by modulating the intrinsic electronic structure is of great importance. Here, porous bimetallic oxide and chalcogenide nanosheets grown on carbon paper denoted as NiCo2X4/CP (X = O, S, and Se) are prepared to demonstrate how the anion components affect the electronic structures and thereby disclose the correlation between their intermediates interaction and catalytic activities. The experimental characterization and theoretical calculation demonstrate that Se and S substitution can promote the ratio of Co3+/Co2+ and thereby modulate the electronic structure accompanied with the upshift of d band centers, which not only enhance the inner conductivity but also regulate the interaction between the catalyst surface and intermediates, especially for the adsorption of absorbed H and hydroperoxy intermediates towards respective hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). As a result, a full alkaline electrolyzer using NiCo2Se4/CP and NiCo2S4/CP as cathode and anode delivers a low voltage of 1.51 V at 10 mA·cm−2, which is comparable even superior to most transition metal-based electrolyzers.
Ultrafine porous cellulose triacetate (CTA) fibers were prepared by electrospinning with methylene chloride (MC) and a mixed solvent of MC/ethanol (EtOH) and their intra- and inter-fiber pore structures was investigated. Ultrafine porous CTA fibers electrospun with MC had isolated circular shape pores with a narrow size distribution in the range of 50–100 nm. In the case of ultrafine CTA fibers electrospun with MC/EtOH (90 / 10 v/v), they had interconnected larger pores in the range of 200–500 nm. These porous structures were induced by phase separation resulting from the rapid evaporation of solvent during the electrospinning process. However, non-porous corrugated fibers were obtained from MC/EtOH (85 / 15 v/v) and MC/EtOH (80 / 20 v/v) due to their lower vapor pressure. The pore sizes in ultrafine CTA fibers electrospun with MC showed a bimodal distribution centered at ∼17 and ∼64 nm. CTA fibers electrospun with MC/EtOH (90 / 10 v/v) showed the greatest porosity due to their larger intra-fiber pores and fiber diameter. 相似文献
Large scale synthesis of high-efficiency bifunctional electrocatalyst based on cost-effective and earth-abundant transition metal for overall water splitting in the alkaline environment is indispensable for renewable energy conversion. In this regard, meticulous design of active sites and probing their catalytic mechanism on both cathode and anode with different reaction environment at molecular-scale are vitally necessary. Herein, a coordination environment inheriting strategy is presented for designing low-coordination Ni2+ octahedra (L-Ni-8) atomic interface at a high concentration (4.6 at.%). Advanced spectroscopic techniques and theoretical calculations reveal that the self-matching electron delocalization and localization state at L-Ni-8 atomic interface enable an ideal reaction environment at both cathode and anode. To improve the efficiency of using the self-modification reaction environment at L-Ni-8, all of the structural features, including high atom economy, mass transfer, and electron transfer, are integrated together from atomic-scale to macro-scale. At high current density of 500 mA/cm2, the samples synthesized at gram-scale can deliver low hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) overpotentials of 262 and 348 mV, respectively.