4.7 Article

Surface-amino-induced boosting solar conversion of CO2 to CO over natural metal-free catalyst

Journal

JOURNAL OF CO2 UTILIZATION
Volume 54, Issue -, Pages -

Publisher

ELSEVIER SCI LTD
DOI: 10.1016/j.jcou.2021.101773

Keywords

Metal-free; Charge separation; CO2 reduction; Photocatalysis

Funding

  1. National Natural Science Foundation of China [22178149]
  2. Jiangsu Fund for Outstanding Youth Scientists [BK20211599]
  3. Jiangsu Distinguished Professor Program
  4. Funding for Scientific Research Startup of Jiangsu University [2020096]

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The synthesis of TRP-NH2 catalyst with heteroatoms doping and NH2 functionalization has effectively improved the efficiency of photocatalytic CO2 reduction. Experimental results demonstrate a significantly higher CO formation rate compared to traditional catalysts, indicating promising potential for applications in solar-driven CO2 reduction.
Design and construction of visible-light-responsive and low-cost catalyst to improve photocatalytic CO2 reduction efficiency are highly urgent due to rapid increment of CO2 emission. Herein, a facile but effective strategy is proposed to synthesize heteroatoms-doped porous treated rape pollen (TRP) and NH2-functionalized TRP for CO2 reduction. Heteroatoms doping can accelerate photoinduced charge transfer between neighboring carbon atom. The introduction of NH2- group offers effective sites to boost CO2 adsorption, which is beneficial to facilitate CO2to-CO conversion. The experimental results indicate that TRP-NH2 exhibits visible-light-driven CO formation rate of 1165.3 mu mol h-1 g-1 in the gas-solid reaction system without co-catalysts or sacrificial agents, which is 2.4 and 70.1 times than those of TRP (488.4 mu mol h-1 g-1) and g-C3N4 (16.6 mu mol h-1 g-1), and exceeds reported state-of-the-art carbon-based photocatalysts. The theoretical investigation shows that the incorporation of NH2group can improve its charge density and converge more electrons to adsorb CO2 molecules. In situ Fourier transform infrared (FT-IR) spectroscopy spectra disclose that the COOH* radical is the main intermediate. The findings reveal the correlation between surface NH2- group and photocatalytic CO2 reduction performance and can be extended to other sustainable metal-free based catalysts for solar-driven CO2 reduction.

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