The semiconductor/electrolyte interface plays a crucial role in photoelectrochemical (PEC) water-splitting devices as it determines both thermodynamic and kinetic properties of the photoelectrode. Interfacial engineering is central for the device performance improvement. Taking the cheap and stable hematite (α-FeO) wormlike nanostructure photoanode as a model system, we design a facile sacrificial interlayer approach to suppress the crystal overgrowth and realize Ti doping into the crystal lattice of α-FeO in one annealing step as well as to avoid the consequent anodic shift of the photocurrent onset potential, ultimately achieving five times increase in its water oxidation photocurrent compared to the bare hematite by promoting the transport of charge carriers, including both separation of photogenerated charge carriers within the bulk semiconductor and transfer of holes across the semiconductor-electrolyte interface. Our research indicates that understanding the semiconductor/electrolyte interfacial engineering mechanism is pivotal for reconciling various strategies in a beneficial way, and this simple and cost-effective method can be generalized into other systems aiming for efficient and scalable solar energy conversion.
The CO2 methanation is an important component of the “power to gas” strategy, and the Ru‐Al2O3 catalyst is considered to be a state‐of‐the‐art catalyst for this reaction. Conventional Ru‐Al2O3 is prepared by wet impregnation. Due to weak interactions between Ru and the Al2O3, construction of a controllable interface between the metal and the substrate is still challenging. In this work, a UV pulse laser is used to controllably construct ultra‐small Ru nanoparticles on defects‐rich Al2O3‐x‐L in situ grown on Al foil (Ru‐Al2O3‐x‐L) for effective photothermal CO2 methanation. The catkin‐like fluff Al2O3‐x‐L efficiently traps light to ensure the light adsorption of Ru‐Al2O3‐x‐L. The defects in Al2O3‐x‐L efficiently anchors Ru. A Strong‐Metal‐Support‐Interaction (SMSI) effect is constructed between the ultra‐small Ru nanoparticles and the Al2O3‐x‐L. The Ru‐Al2O3‐x‐L exhibits remarkable photothermal catalytic performance (CH4 yield of 12.35 mol gRu−1 h−1) in the closed batch system. Then an innovative flow reactor is established based on the one‐piece Ru‐Al2O3‐x‐L microchannel catalyst. Thanks to local pressure on the edge of the microchannels, the CH4 yield is further enhanced to 14.04 mol gRu−1 h−1. Finally, an outdoor setup demonstrates the feasibility of photothermal CO2 methanation (CH4 yield of 18.00 mmol min−1). This work provides novel perspectives for the construction of multi‐level micro/nanostructures integrated catalysts for photothermal CO2 methanation.
With the depletion of fossil fuels and environmental contamination, photocatalytic H2 production has become an essential issue. Co‐catalysts play a critical role in improving photocatalytic H2 generation of photocatalysts. However, co‐catalysts frequently need additional synthesis steps for loading on the surface of photocatalysts, and the interface contact between the co‐catalyst and the photocatalyst is insufficient. Herein, a CdS/MoS2 nanooctahedron heterostructure is prepared through the in situ sulfidation of CdMoO4 nanooctahedrons. MoS2 as the co‐catalyst provides active sites for H2 generation and enhances the separation of photo‐generated carriers. Furthermore, the sulfidation of CdMoO4 precursors ensures a tight contact interface by S atoms between CdS and MoS2, which is beneficial to the electrons transfer from CdS to MoS2, thus markedly improving the photocatalytic H2 evolution activity. The obtained optimum CdS/MoS2 nanooctahedrons exhibit a better photocatalytic H2 generation activity than those of pure CdS, pure MoS2, and even CdS/MoS2 by hydrothermal synthesis under visible light irradiation. In addition, solar‐driven biomass upgrading of furfural alcohol, bacterial cellulose membrane, bioplastic wastes upgrading of polylactic acid (PLA), polyethylene terephthalate (PET), and their reforming to H2 are also performed and demonstrate an inexpensive route to drive aqueous proton reduction to H2 through waste biomass oxidation.
Metal nanoclusters (NCs) are well-known for their distinct
molecule-like
luminescent behaviors. Currently, some research has been conducted
concerning their quenching properties for various dyes, but little
is known about the interaction between metal NCs and other fluorescent
materials such as quantum dots (QDs). In this paper, we report efficient
quenching of fluorescence emission of mercaptoacetic acid (TGA)-coated
CdTe QDs having identical protective layers but differing core diameters
(1.04, 1.61, and 2.11 nm) by the bovine serum albumin (BSA)-protected
Au25 NCs (0.8 nm metal core diameter) that have negligible
plasmon bands in PBS buffer solution at pH 7.4. With UV–vis
absorption spectroscopy and steady-state and time-resolved fluorescence
spectroscopy, we found that fluorescence emission of all QDs decreased
significantly upon addition of Au NCs, in combination with no decrease
in average fluorescence lifetime, which was attributed to static quenching
of QDs by Au NCs. Interestingly, the 515 nm emitting QDs are at least
1 order of magnitude more efficiently quenched than the other two
QDs in spite of the similar degree of spectral overlap of the emission
spectrum with the excitation spectrum of Au NCs. This study not only
has brought to light the quenching properties of metal NCs for QDs
but also provided fundamental guidelines and new opportunities for
further investigations into the interaction between metal NCs and
other materials.
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