Integrated Photothermal Nanoreactors for Efficient Hydrogenation of CO2

Abstract

To alleviate the energy crisis and global warming, photothermal catalysis is an attractive way to efficiently convert CO2 and renewable H2 into value-added fuels and chemicals. However, the catalytic performance is usually restricted by the trade-off between the dispersity and light absorption property of metal catalysts. Here we demonstrate a simple SiO2-protected metal–organic framework pyrolysis strategy to fabricate a new type of integrated photothermal nanoreactor with a comparatively high metal loading, dispersity, and stability. The core-satellite structured Co@SiO2 exhibits strong sunlight-absorptive ability and excellent catalytic activity in CO2 hydrogenation, which is ascribed to the functional separation of different sizes of Co nanoparticles. Large-sized plasmonic Co nanoparticles are mainly responsible for the light absorption and conversion to heat (nanoheaters), whereas small-sized Co nanoparticles with high intrinsic activities are responsible for the catalysis (nanoreactors). This study provides a new concept for designing efficient photothermal catalytic materials.

Supra‐Photothermal CO2 Methanation over Greenhouse‐Like Plasmonic Superstructures of Ultrasmall Cobalt Nanoparticles

“…Tetraethyl orthosilicate (TEOS) was purchased from TCI. Ammonium hydroxide solution (NH 3 •H 2 O, 28 wt%) and ethanol were purchased from Macklin and Sinopharm Chemical Reagent Co.,Ltd.,18.2 MΩ cm at 25 °C) was used in all experiments.…”

The Current Progresses and Future Perspectives of Photoreactors and Catalysts Used in Photocatalytic Reduction of CO2

“…More importantly, the coupling of Co 3 O 4 quantum dots with titanium dioxide rearranges the band structure to accommodate the overall water splitting. Shen et al demonstrates a confined pyrolysis strategy for the synthesis of an integrated photothermal nanoreactor (IPR) with higher metal loading and dispersity compared with that of traditional supported metal catalysts. The newly developed IPR, characteristic of a unique core–satellite structure, achieves a dramatic synergy effect of the photothermal effects of large-sized plasmonic Co nanoparticles (nanoheaters) and great intrinsic catalytic performance of small-sized Co nanoparticles (nanoreactors).…”

“…Schematic illustration of the preparation process of Co@SiO 2 . Reproduced with permission from ref . Copyright 2022 Tianjin Daxue.…”

Photothermal Cocatalytic Carbonylation of Isobutyl Amine with CO2 over Bi2O3 Polymorphs under Visible-Light Irradiation

“…Hence, thermal activation is introduced to assist the excitation and migration of carriers and thus promote the desorption of products and (or) harmful species, finally fulfilling the "1 + 1 > 2" photothermal synergy for highly efficient CO 2 activation under relatively mild conditions. 21 Meanwhile, considering the fact that the kinetic control step of carbamate dehydration is a strong endothermic process in the carbonylation of amines with CO 2 to N,N′-dialkylurea, 22 we propose photothermal cocatalytic carbonylation of amines with CO 2 to N,N′-dialkylurea, in order to effectively ameliorate the defects of severe reaction conditions (e.g., high temperature and pressure) faced by current thermal catalytic activation, and thus to facilitate the industrialization of the technology of CO 2 capture and utilization by carbonylation of amines with CO 2 . Due to the thermodynamic stability and kinetic inertness of the feedstock CO 2 , it is essential to develop efficient photothermal synergistic catalysts in the carbonylation of CO 2 with amines to N,N′-dialkylurea.…”