Simultaneous optimization of the number and intensity of oxygen (O) adsorption on gold (Au) cocatalyst is highly required to greatly improve their interfacial hydrogen peroxide (HO)-production activity. However, it is a great challenge to realize the above effective modulation of Au by traditional photodeposition route. In this study, a platinum (Pt)-induced selective photodeposition method was designed to simultaneously regulate the particle size and electronic structure of Au cocatalyst for boosting the photocatalytic HO-production activity of bismuth vanadate (BiVO) via the selective deposition of Pt@Au core-shell cocatalyst.
View Article and Find Full Text PDFGold-based co-catalysts are a promising class of materials with potential applications in photocatalytic HO production. However, current approaches with Au co-catalysts show limited HO production due to intrinsically weak O adsorption at the Au site. We report an approach to strengthen O adsorption at Au sites, and to improve HO production, through the formation of electron-deficient Au sites by modifying the electronic structure.
View Article and Find Full Text PDFThe free electron transfer between cocatalyst and photocatalyst has a great effect on the bonding strength between the active site and adsorbed hydrogen atom (H), but there is still a lack of effective means to purposely manipulate the electron transfer in a beneficial direction of H adsorption/desorption activity. Herein, when ReS cocatalyst is loaded on TiO surface, a spontaneous free-electron transfer from ReS to TiO happens due to the smaller work function of ReS, causing an over-strong S-H bond. To prevent the over-strong S-H bonds of ReS in the ReS/TiO , a free-electron reversal transfer strategy is developed to weaken the strong S-H bonds via increasing the work function of ReS by incorporating O to produce ReOS cocatalyst.
View Article and Find Full Text PDFThe interaction between a co-catalyst and photocatalyst usually induces spontaneous free-electron transfer between them, but the effect and regulation of the transfer direction on the hydrogen-adsorption energy of the active sites have not received attention. Herein, to steer the free-electron transfer in a favorable direction for weakening S-H bonds of sulfur-rich MoS , an electron-reversal strategy is proposed for the first time. The core-shell Au@MoS cocatalyst was constructed on TiO to optimize the antibonding-orbital occupancy.
View Article and Find Full Text PDFLow-cost transition-metal chalcogenides (MS ) are demonstrated to be potential candidate cocatalyst for photocatalytic H generation. However, their H -generation performance is limited by insufficient quantities of exposed sulfur (S) sites and their strong bonding with adsorbed hydrogen atoms (SH ). To address these issues, an efficient coupling strategy of active-site-enriched regulation and electronic structure modification of active S sites is developed by rational design of core-shell Au@NiS nanostructured cocatalyst.
View Article and Find Full Text PDFThe molten salt-assisted route is one of the most important methods to improve the crystallinity of conventionally disordered bulk graphitic carbon nitride (g-CN). However, the residual potassium ions from potassium chloride/lithium chloride molten salt can greatly impact the ordered structure of g-CN and serve as the recombination centers of photoinduced carriers, causing limited photocatalytic hydrogen-evolution performance. In this article, the ethyl acetate-mediated method is first developed to not only further improve the ordered structure of traditional crystalline g-CN, but also produce more cyano groups for preparing highly efficient g-CN photocatalysts.
View Article and Find Full Text PDFA hydroxyl-enriched highly crystalline TiO suspensible photocatalyst was synthesized via a facile ethanol-controlled hydrolysis and following an in situ crystallization method. In the absence of any cocatalysts, the resultant photocatalyst displayed a clearly higher H-evolution rate (622 μmol h g) than the well-known commercial P25 TiO (190 μmol h g).
View Article and Find Full Text PDFFacile and novel strategies to prepare g-C3N4 nanosheets are required to greatly improve their photocatalytic H2-production activity. In this study, a lactic acid-mediated synthesis route has been developed to prepare g-C3N4 nanosheets, which includes the preassembled formation of lactic acid-melamine co-monomers, followed by direct high-temperature calcination. In this case, it is found that during high-temperature calcination, the lactic acid molecules can greatly prevent the serious polymerization of melamine molecules, resulting in the formation of g-C3N4 nanosheets.
View Article and Find Full Text PDF