Cu-based high-entropy two-dimensional oxide as stable and active photothermal catalyst

Abstract

Cu-based nanocatalysts are the cornerstone of various industrial catalytic processes. Synergistically strengthening the catalytic stability and activity of Cu-based nanocatalysts is an ongoing challenge. Herein, the high-entropy principle is applied to modify the structure of Cu-based nanocatalysts, and a PVP templated method is invented for generally synthesizing six-eleven dissimilar elements as high-entropy two-dimensional (2D) materials. Taking 2D Cu2Zn1Al0.5Ce5Zr0.5Ox as an example, the high-entropy structure not only enhances the sintering resistance from 400 °C to 800 °C but also improves its CO2 hydrogenation activity to a pure CO production rate of 417.2 mmol g−1 h−1 at 500 °C, 4 times higher than that of reported advanced catalysts. When 2D Cu2Zn1Al0.5Ce5Zr0.5Ox are applied to the photothermal CO2 hydrogenation, it exhibits a record photochemical energy conversion efficiency of 36.2%, with a CO generation rate of 248.5 mmol g−1 h−1 and 571 L of CO yield under ambient sunlight irradiation. The high-entropy 2D materials provide a new route to simultaneously achieve catalytic stability and activity, greatly expanding the application boundaries of photothermal catalysis.

Structure and Activity Comparison of Cu/CeyZr1–yOx Series Catalysts in the Reverse Water–Gas Shift Reaction

“…22,39,40 The Cu/Ce 0.9 Zr 0.1 O x catalyst with a small amount of Zr can generate a large amount of Ce 3+ , significantly increasing the surface oxygen vacancy content of the catalyst. Zr 3d spectra of Cu/CeO 2 and Cu/Ce 0.9 Zr 0.1 O x catalysts, which were mainly in the form of Zr 4+ , were very similar, 9,20 which proved that electron transfer mainly occurred between Cu and Ce rather than between Zr and Ce. The O 1s spectra of the catalysts were deconvoluted into lattice oxygen (O L , 529.5 eV) and oxygen vacancy (O V , 531.2 eV) species.…”

Control of Oxygen Vacancies of 2D-InOx Fabricated by Liquid Metal Printing via Temperature Modulation

“…The revelation of graphene, a hexagonally patterned monolayer of carbon atoms, ignited significant enthusiasm for revolutionizing electronics, 3 leading to the investigation of various 2DMs beyond graphene. Among the assorted categories of 2DMs, the realm of 2D metal oxides has surfaced as an especially captivating area due to their versatile nature and their potential in diverse fields, spanning from electronics 4 and catalysis 5 to energy storage 6 and environmental sustainability. 7 Comprising metal cations linked to oxygen anions, metal oxides, when downscaled to the 2D scale, display unique features distinct from those of their bulk counterparts.…”

A novel strategy for dramatically improving catalytic performance for light-driven thermocatalytic CO2 reduction with CH4 on Ru/MgO: the CO2 molecular fencing effect promoted by photoactivation

“…Effective methods for light-driven thermocatalytic CO 2 reduction using H 2 O, 12–17 CH 4 18–28 and H 2 29–39 as reducing agents have been developed in recent years. They combine well the advantages of thermocatalysis (high catalytic activity) and photocatalysis (low energy consumption).…”