Atomically dispersed Ni-N-C catalyst derived from NiZn layered double hydroxides for efficient electrochemical CO2 reduction

doi:10.1016/S1872-2067(22)64188-3

Abstract

Abstract:

Atomically dispersed catalytic metal sites anchored on N-doped carbon support catalysts (M-N-C) show great prospects for CO₂ electroreduction. Here, single-layer NiZn layered double hydroxides (NiZn-LDHs) was used as a sacrificial assistant to fabricate single-Ni atom anchored on ultrathin porous carbon catalyst. NiZn-LDHs were exfoliated to single-layer by polyhydroxy compounds which took as the carbon resource in Ni-N-C, and single layer NiZn LDHs taking as the Ni resource could avoid the agglomeration of Ni atoms during calcining. The CO Faradaic efficiency (FE_CO) of the synthesized Ni-N-C catalyst exceeded 90% at -0.6 to -1.0 V and a FE_CO of 95.2% with a current density of 24 mA cm^-2 at -0.9 V. This work not only provides a new method for preparing M-N-C catalysts, but also offers an effective and controllable strategy for large-scale production of high-performance single-atom catalysts.

Key words: NiZn-Layered double hydroxides, CO2 reduction, Ni-N-C Catalyst, Active site, Efficient preparation

Ping Zhang, Hao Chen, Lin Chen, Ying Xiong, Ziqi Sun, Haoyu Yang, Yingke Fu, Yaping Zhang, Ting Liao, Fei Li. Atomically dispersed Ni-N-C catalyst derived from NiZn layered double hydroxides for efficient electrochemical CO₂ reduction[J]. Chinese Journal of Catalysis, 2023, 45: 152-161.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(22)64188-3

https://www.cjcatal.com/EN/Y2023/V45/I2/152

Figures/Tables 6

Scheme 1. Schematic illustration of the synthesis of Ni-N-C.

Fig. 1. XRD patterns of NiZn-LDHs (a), NiZn-LDHs/PHC (b), and Ni-N-C and CN (c). (d) Raman spectra of CN and Ni-N-C.

Fig. 2. TEM images (a-c) and HR-TEM image (d) of Ni-N-C-1. (e) HAADF-TEM image and corresponding EDS element mapping of Ni-N-C-1. AFM image (f) and the height profile (i) of Ni-N-C-1. (g) BET surface area and (inset) pore-size distribution curve of Ni-N-C-1. (h) Aberration-corrected HAADF-STEM image of Ni-N-C-1.

Fig. 3. (a) Ni K-edge XANES spectra of Ni-N-C-1, Ni foil, NiO and NiPc shown in k2-weighted R space. The wavelet transform of Ni-N-C-1 (b). NiPc (d), and NiO (f). (c) Fourier transformation of EXAFS spectra Ni-N-C-1, Ni foil, and NiO. (e) Ni K-edge EXAFS fitting result of Ni-N-C-1 shown in k2-weighted R space and Ni-N4 coordination environment.

Fig. 4. (a) LSV in CO2-saturated. (b) FECO at different potentials. (c) CO current density. (d) Tafel plots. (e) Nyquist plots. (f) Charging current density differences plotted against scan rates of CN, Ni-N-C-1NPs, and Ni-N-C-1. FECO (g) and current densities (h) of CO of Ni-N-C-0.5, Ni-N-C-1, and Ni-N-C-2 at different potentials. (i) Durability of Ni-N-C-1 at ?0.8 V (vs. RHE).

Fig. 5. (a) Free-energy diagram of CO2RR reaction on Ni-N co-doped graphite and the schematic of the reaction steps of the electrocatalytic CO2 to CO reaction. (b) The charge density difference of NiN4 configurations. The isosurface is selected at 0.0025 e ?-3 and the yellow and cyan regions represent electron accumulation and depletion, respectively.

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Atomically dispersed Ni-N-C catalyst derived from NiZn layered double hydroxides for efficient electrochemical CO₂ reduction

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