A strong sunlight-absorptive ability and high dispersity are considered as two key requirements of supported metal catalysts for efficient photothermal CO 2 conversions. The former can be improved by increasing the metal loading but often at the expense of decreasing the latter. Here we develop an ion-exchange route to supported Ru nanoparticles with both high loadings and dispersity that exhibit enhanced activity and relatively good stability in photothermal CO 2 catalysis. This strategy involves an ionexchange reaction between Ru 3+ and Mg(OH) 2 to form uniformly distributed and chemically bonded Ru precursors on Mg(OH) 2 supports. The subsequent lowtemperature reduction by H 2 produces highly dispersed Ru nanoparticles whose sizes barely change as the loading increases. Our study provides an avenue for the preparation of strongly light-absorptive and highly dispersed metal catalysts for efficient conversion of carbon dioxide into solar fuels.
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.
Interest in the preparation of colloidal heterostructures with complex shapes, structures, and spatial compositions is driven by their unique optical, electrical, magnetic, or rheological properties. Despite recent advances, it is highly desired but challenging to further extend the library of heterostructured particles with increased degrees of complexity.Here we report a general step-by-step strategy for controlled preparations of complex heterostructured colloids with various structures and compositions. A local-curvature-controlled emulsion polymerization method is first employed for siteselective growth of secondary polystyrene nanostructures on different nonspherical colloidal seeds. The following functionalization and selective removal steps further increase the degree of particle complexity. We also demonstrate a new type of chemically powered nanomotors based on heterostructured α-Fe 2 O 3 @SiO 2 /Pt particles. This growth strategy is a versatile, general method suitable for the preparation of complex heterostructured particles with tailored structures, compositions, and functionalities, paving the way for their applications for various purposes.
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