Greenery-inspired nanoengineering of bamboo-like hierarchical porous nanotubes with spatially organized bifunctionalities for synergistic photothermal catalytic CO2 fixation. Issue 23 (27th May 2022)

• Record Type: Journal Article
• Authors: Guo, Yingchun; Chen, Weijia; Feng, Lei; Fan, Yanchen; Liang, Jinsheng; Wang, Xiaomei; Zhang, Xu
• Is Part Of: Journal of materials chemistry. Volume 10:Issue 23(2022)
• Page Start: 12418
• Page End: 12428
• Publication Date: 2022-05-27
• Subjects: Materials -- Research -- Periodicals; Chemistry, Analytic -- Periodicals; Environmental sciences -- Research -- Periodicals; 543.0284
• DOI: 10.1039/d2ta02885a
• Languages: English
• ISSNs: 2050-7488

Abstract

Abstract : The hollow tubular core–shell photocatalyst (Ni-BNCNTs@HMPs-NH2 ) exhibits superior activity and stability for the photothermal conversion of CO2 to cyclic carbonates under mild and co-catalyst/solvent-free conditions. Abstract : The fixation of CO2 and epoxides into cyclic carbonates is a promising strategy for the resourceful use of CO2 . However, halogen-based homogeneous co-catalysts are usually required for synergistic catalysis in most heterogeneous catalytic systems, which complicates the process of product separation and purification. Furthermore, CO2 cycloaddition usually requires heating to drive the reaction, making it a highly energy-consuming catalytic process. Herein, the hyper-cross-linked mesoporous poly(ionic liquid)s and nickel-based bamboo-like N-doped carbon nanotubes are spatially organized to construct a synergistic photothermal catalytic system for CO2 cycloaddition (denoted as Ni-BNCNTs@HMPs-NH2 ). The integrated bifunctional catalyst Ni-BNCNTs@HMPs-NH2 exhibits superior activity and stability for the conversion of CO2 to cyclic carbonates under mild and co-catalyst/solvent-free conditions. Specifically, when the light intensity is 0.4 W cm −2, the reaction temperature can reach 74.2 °C, the yield is 99%, and there is no significant activity loss after 10 cycles of catalysis. Various characterizations illustrate that atomically dispersed Ni–N–C sites and imidazolium-based poly(ionic liquid)s in the Ni-BNCNTs@HMPs-NH2 can act as Lewis acid sites and nucleophiles for synergistic catalytic CO2 cycloaddition, respectively. In addition, under light irradiation, bamboo-like carbon nanotubes and plasmonic Ni nanoparticles facilitate the photothermal conversion, and semiconductor Ni–N–C generates photogenerated electrons as well as accelerates the rate-limiting step of the CO2 cycloaddition. This work provides insights into low-energy photothermal-driven catalytic CO2 conversion.