Although lead halide perovskites are demonstrated to be promising photocatalysts for hydrogen evolution from hydrogen halide splitting, it still remains challenging to fabricate efficient and stable catalysts. Here MoS 2 nanoflowers with abundant active sites are assembled with methylammonium lead iodide (MAPbI 3 ) microcrystals to form a new heterostructure. Its hydrogen evolution rate can reach up to about 30 000 μmol g −1 h −1 , which is more than 1000-fold higher than pristine MAPbI 3 under visible light irradiation (λ ≥ 420 nm). Importantly, the solar HI splitting efficiency reaches 7.35%, one of the highest efficiencies so far. The introduction of MoS 2 with proper band alignment and unsaturated species can efficiently promote the charge separation and afford more active sites for H 2 production. This finding not only provides a highly efficient and stable photocatalyst for hydrogen evolution but also offers a useful modification strategy on lead halide perovskites.
As an analogue to the vapor–liquid–solid process, the solution–liquid–solid (SLS) method offers a mild solution‐phase route to colloidal 1D nanostructures with controlled sizes, compositions, and properties. However, direct growth of 1D nanostructure arrays through SLS processes remains in its infancy. Herein, this study shows that SLS processes are also suitable for the growth of nanorod arrays on the substrate. As a proof of concept, seedless growth of silica nanorod arrays on a variety of hydrophilic substrates such as pristine and oxide‐modified glass, metal sheets, Si wafers, and biaxially oriented polypropylene film are demonstrated. Also, the silica nanorod arrays can be used as a new platform for the fabrication of catalysts for photothermal CO 2 hydrogenation and the reduction of 4‐nitrophenol reactions. This work offers some fundamental insight into the SLS growth process and opens a new avenue for the mild preparation of functional 1D nanostructure arrays for various applications.
Photothermal CO2 hydrogenation catalyzed by earth‐abundant materials, such as non‐noble metals, has emerged as an industrially viable and sustainable way of effectively converting solar energy into chemical energy stored in fuels and other valuable chemical feedstocks. However, the performance of existing non‐noble metal photocatalysts often suffers from incomplete sunlight utilization, limited photothermal effect, and poor stability under intense light illumination. Herein, the fabrication of all‐earth‐abundant on‐silicon architectures with nearly 100% sunlight harvesting ability is demonstrated. The cobalt‐loading‐optimized architecture exhibits a high photothermal CO2 conversion rate of 0.433 mol·gCo−1·h−1. A spatial confinement strategy based on surface encapsulation with a thin layer of silica is further used to improve the stability of supported Co nanoparticles against sintering. This strategy of maximizing the sunlight absorbance of non‐noble metal photocatalysts lays a foundation for industrial implementation of all‐earth‐abundant photothermal CO2 catalysis.
The rational design of nanoarray‐structured catalysts is an accessible way to increase light absorption ability and boost photothermal CO2 conversion efficiency. However, practical application of current nanoarrays is hindered by complex synthesis procedures, high costs, and low catalyst yields. Herein, we report a simple, robust method to prepare efficient photothermal catalyst by sputtering Co nanoparticles on commercial anodic aluminum oxide (AAO) membrane. The detailed study shows that gas diffusion and catalytic activity can be affected by AAO structures, such as channel size and shape. The optimized Co@dpAAO catalyst reached a record Co‐based photothermal CO2 conversion rate of 1666 mmol ⋅ gCo−1 ⋅ h−1. This study not only provides a facile way to synthesize efficient catalysts, but also promotes the understanding of constructing nanoarray‐based photothermal catalysts.
Photothermal reverse water gas shift (RWGS) catalysis holds promise for efficient conversions of greenhouse gas CO 2 and renewable H 2 , powered solely by sunlight, into CO, an important feedstock for the chemical industry. However, the performance of photothermal RWGS catalysis over existing supported catalysts is limited by the balance between the catalyst loading and dispersity, as well as stability against sintering. Herein, we report a core-shell strategy for the design of photothermal catalysts, by using Ni 12 P 5 as an example, with simultaneously strong light absorption ability, high dispersity and stability. The core-shell structured Ni 12 P 5 @SiO 2 catalyst with a relatively small Ni 12 P 5 particle size of 15 nm at a high Ni 12 P 5 loading of 30 wt% exhibits improved activity, nearly 100% CO selectivity, and superior stability in photothermal RWGS catalysis, particularly under intense illuminations. Our study clearly reveals the effectiveness of the core-shell strategy in breaking the limitation of supported catalysts and boosting the performance of photothermal CO 2 catalysis.
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