Efficient photoelectrochemical cell composed of Ni single atoms/P, N-doped amorphous NiFe2O4 as anode catalyst and Ag NPs@CuO/Cu2O nanocubes as cathode catalyst for microplastic oxidation and CO2 reduction

doi:10.1016/S1872-2067(25)64777-2

Abstract

Abstract:

Plastics are ubiquitous in human life and pose certain hazards to the environment and human body. The increasing amount of CO2 in the atmosphere will lead to the greenhouse effect. Therefore, it is urgent to treat microplastic waste and CO2 by using environmentally friendly and efficient technologies. In this work, we developed an efficient photoelectrocatalytic system composed of Ni single atoms (Ni SAs) supported by P, N-doped amorphous NiFe2O4 (Ni SAs/A-P-N-NFO) as anode and Ag nanoparticles (Ag NPs) supported by CuO/Cu2O nanocubes (Ag NPs@CuO/Cu2O NCs) as cathode for microplastic oxidation and CO2 reduction. The Ni SAs/A-P-N-NFO was synthesized by calcination-H2 reduction method, and it achieved a Faraday efficiency of 93% for the oxidation reaction of poly (ethylene terephthalate) (PET) solution under AM 1.5 G light. As a photocathode, the synthesized Ag NPs@CuO/Cu2O NCs was utilized to reduce CO2 to ethylene and CO at 1.5 V vs. RHE with selectivity of 42% and 55%, respectively. This work shows that the photoelectrocatalysis, as an environmentally friendly technology, is a feasible strategy for reducing the environmental and biological hazards of light plastics, as well as for efficient CO2 reduction.

Key words: Ni single atom, NiFe2O4, Photoelectrocatalysis, Poly (ethylene terephthalate) plastics, oxidation, CO2 reduction reaction

Hong-Rui Zhu, Xi-Lun Wang, Juan-Juan Zhao, Meng-Han Yin, Hui-Min Xu, Gao-Ren Li. Efficient photoelectrochemical cell composed of Ni single atoms/P, N-doped amorphous NiFe₂O₄ as anode catalyst and Ag NPs@CuO/Cu₂O nanocubes as cathode catalyst for microplastic oxidation and CO₂ reduction[J]. Chinese Journal of Catalysis, 2025, 76: 159-172.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(25)64777-2

https://www.cjcatal.com/EN/Y2025/V76/I9/159

Figures/Tables 8

Fig. 1. Schematic illustration of synthesis procedures of Ni SAs/A-P-N-NFO.

Fig. 2. TEM images (a) and AC-HAADF-STEM images (b) of Ni SAs/A-P-N-NFO. (c) Statistical analysis of Ni single-atoms in Ni SAs/A-P-N-NFO. (d) Magnified images from (b). (c,d) show the intensity profile marked by the yellow dashed circle, indicating the isolated arrangement of Ni atoms. XRD patterns (e) and EPR spectra (f) of Ni SAs/A-P-N-NFO, P-NFO and C-NFO. XANES spectra of the Ni-K edge (g), Ni-K edge EXAFS spectra (h), and the wavelet-transformed EXAFS spectra (i) of Ni SAs/A-P-N-NFO and P-NFO.

Fig. 3. Performance of Ni SAs/A-P-N-NFO electrode toward PET hydrolysate oxidation at the photoanode under dark conditions. (a) LSV curves of with different P contents of NFO samples and Ni SAs/A-P-N-NFO in 1 mol L-1 KOH solutions with 0.1 mol L-1 PET hydrolysate. (b) Tafel slopes from LSV curves. (c) Faradaic efficiency on Ni SAs/A-P-N-NFO at different potentials. Error bars correspond to the standard deviation of measurements. (d) EIS spectra of different samples. (e) LSV curves of different reaction conditions of Ni SAs/A-P-N-NFO. (f) 1H NMR spectra of products before and after electrolysis of PET hydrolysate, applied bias is 1.5V vs. RHE.

Fig. 4. UV-vis DRS (a), Tauc’s plots (b), and PL spectra (c) of Ni SAs/A-P0.09-N-NFO, P-NFO and C-NFO. ESR spectra of DMPO-·OH (d) and DMPO-·O2-(e) for Ni SAs/A-P0.09-N-NFO under AM 1.5G light irradiation. (f) LSV curves under dark and light reaction conditions of Ni SAs/A-P0.09-N-NFO. IR thermal images of Ni SAs/A-P0.09-N-NFO (g1-g4) and P-NFO (h1-h4) under 480 nm illumination with time keeping from 30 to 120 s, the intervals are 30 s.

Fig. 5. (a) ELF profile of (001) facet of Ni SAs/A-P-N-NFO, P-NFO and C-NFO (the color bar represents the degree of electronic localization). (b,c) The phonon density of state (PDOS) of Ni SAs/A-P-N-NFO, P-NFO and C-NFO for the active Ni and Fe sites, respectively. (d) Gibbs free energy diagrams for the electrooxidation of EG to formate on Ni SAs/A-P-N-NFO, P-NFO and C-NFO (0 V vs. RHE).

Fig. 6. (a) Schematic illustration of the Cu2O and Ag NPs@CuO/Cu2O NCs preparation process. SEM, TEM and HRTEM images of Cu2O (b-d) and Ag NPs@CuO/Cu2O NCs (e-f). (g) Atomic-resolution HAADF-STEM image of Ag NPs@CuO/Cu2O NCs. (h) STEM image and EDX mappings of Ag NPs@CuO/Cu2O.

Fig. 7. Photoelectrochemical performance of the Ag NPs@CuO/Cu2O NCs toward the CO2RR at the photocathode. (a) FEs of the Ag NPs@CuO/Cu2O NCs photocathode for the CO2RR at different potentials. (b) LSV curves of the Ag NPs@CuO/Cu2O NCs photocathode in CO2-saturated 1 mol L-1 NaHCO3 solutions. (c) The stability test for CO2RR over Ag NPs@CuO/Cu2O NCs photocathode. (d) Comparison of CO2RR product selectivity of dark and light conditions. (e) The free-energy diagram for the PEC CO2RR to C2H4 on Ag NPs@CuO/Cu2O NCs and Cu2O.

Fig. 8. (a) Digital photographs of Ni SAs/A-P-N-NFO||Ag NPs@CuO/Cu2O NCs PEC cells under AM 1.5G illumination imposed in the laboratory. Photoanode on the left is in PET hydrolysis solution and photocathode on the right is in NaHCO3 solution. (b) LSV curve of Ni SAs/A-P-N-NFO||Ag NPs@CuO/Cu2O NCs PEC cells under AM 1.5G illumination. (c) FEs of the products of CO2RR of the Ni SAs/A-P-N-NFO||Ag NPs@CuO/Cu2O NCs PEC cells under AM 1.5G illumination.

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Efficient photoelectrochemical cell composed of Ni single atoms/P, N-doped amorphous NiFe₂O₄ as anode catalyst and Ag NPs@CuO/Cu₂O nanocubes as cathode catalyst for microplastic oxidation and CO₂ reduction

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