Covalent triazine-based frameworks confining cobalt single atoms for photocatalytic CO2 reduction and hydrogen production

doi:10.1016/j.jmst.2021.11.035

Abstract

Abstract:

Single-atom catalysts (SACs) have emerged as an advanced frontier in heterogeneous catalysis due to their potential to maximize the atomic efficiency. Herein, covalent triazine-based frameworks (CTFs) confining cobalt single atoms (Co-SA/CTF) photocatalysts have been synthesized and used for efficient CO₂ reduction and hydrogen production under visible light irradiation. The resulted Co-SA/CTF demonstrate excellent photocatalytic activity, with the CO and H₂ evolution rates reaching 1665.74 µmol g^-1 h^-1 and 1293.18 µmol g^-1 h^-1, respectively, far surpassing those of Co nanoparticles anchored CTF and pure CTF. A variety of instrumental analyses collectively indicated that Co single atoms sites served as the reaction center for activating the adsorbed CO₂ molecules, which significantly improved the CO₂ reduction performance. Additionally, the introduction of Co single atoms could accelerate the separation/transfer of photogenerated charge carriers, thus boosting the photocatalytic performance. This study envisions a novel strategy for designing efficient photocatalysts for energy conversion and showcases the application of CTFs as attractive support for confining metal single atoms.

Key words: Covalent triazine-based frameworks, Co single atoms, Photocatalysis, CO₂ reduction, Hydrogen evolution

Guocheng Huang, Guiyun Lin, Qing Niu, Jinhong Bi, Ling Wu. Covalent triazine-based frameworks confining cobalt single atoms for photocatalytic CO₂ reduction and hydrogen production[J]. J. Mater. Sci. Technol., 2022, 116: 41-49.

Figures/Tables 8

Fig. 1. TEM images of (a) CTF-1 and (b) Co0.10-SA/CTF; and (c) HRTEM, (d) HAADF-STEM, (e) EDX mapping images of Co0.10-SA/CTF.

Fig. 2. (a) XPS survey spectra of CTF-1 and Co0.10-SA/CTF, and high resolution XPS spectra of (b) C 1 s and (c) N 1 s for CTF-1 and Co0.10-SA/CTF. (d) Co 2p spectra of Co0.10-SA/CTF and Co-Pc (phthalocyanine cobalt(Ⅱ)).

Fig. 3. (a) UV-vis DRS spectra of CTF-1, Co-NP/CTF and Cox-SA/CTF (x = 0.05, 0.10, 0.20, 0.30). (b) LSV curves of CTF-1 and Co0.10-SA/CTF in CO2 or Ar saturated Na2SO4 solution. (c) Transient photocurrent responses and (d) electrochemical impedance spectra of CTF-1, Co-NP/CTF and Cox-SA/CTF (x = 0.05, 0.10, 0.20, 0.30).

Fig. 4. Femtosecond time-resolved transient absorption decay kinetics of (a) CTF-1 and (b) Co0.10 SA/CTF at 600 nm probe (Black: experimental curves; Red: fitting curves).

Fig. 5. (a) CO2 physisorption isotherms (1 atm, 273 K) and (b) CO2-TPD profiles of CTF-1, Co-NP/CTF and Co0.10-SA/CTF.

Fig. 6. (a) Photocatalytic activities of the as-prepared samples. (b) Photocatalytic CO2 reduction performance of Co0.10-SA/CTF under various conditions. (c) GC-MS spectrum analysis of generated CO by Co0.10-SA/CTF with 13CO2 as carbon source. (d) Stability test of Co0.10-SA/CTF in four repeats of the photocatalytic CO2 reduction reactions and hydrogen evolution.

Fig. 7. In-situ FTIR spectra of Co0.10-SA/CTF in the absence of CO2 and H2O (black line) and in presence of CO2 and H2O along with increasing irradiation time.

Fig. 8. Schematic illustration of photocatalytic CO2 reduction of Co-SA/CTF.

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Covalent triazine-based frameworks confining cobalt single atoms for photocatalytic CO₂ reduction and hydrogen production

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