High-efficiency electrochemical H2O2 synthesis by heteroatom-doped NiX/Ni nanocomposites with honeycomb-like porous carbon

doi:10.1016/S1872-2067(24)60121-X

Abstract

Abstract:

Transition metal Ni anchored in carbon material represents outstanding 2e^- oxygen reduction reaction (ORR) catalytic selectivity, but enhancing the adsorption strength of intermediate *OOH to promote its selectivity remains a major challenge. Herein, the NiX/Ni@NCHS composite catalyst with heteroatom doping (O,S) is modulated by controlling partial pyrolysis strategies on honeycomb-like porous carbon to manipulate the electronic structure of the metal Ni. With the synergistic effect of honeycomb structure and O atom, NiO/Ni@NCHS-700 exhibits an exceptional H₂O₂ selectivity of above 89.1% across a wide potential range from 0.1 to 0.6 V in an alkaline electrolyte, and an unexpected H₂O₂ production rate up to 1.47 mol g_cat^-1 h^-1@0.2 V, which outperforms most of the state-of-the-art catalyst. Meanwhile, NiS/Ni@NCHS exhibits excellent electrocatalytic performance, with 2e^- ORR selectivity of 91.3%, H₂O₂ yield of 1.85 mol g_cat^-1 h^-1@0.3 V. Density functional theory simulations and experiments results reveal that the heteroatom doping (O,S) method has been employed to regulate the adsorption strength of Ni atoms with *OOH, and combined with the self-sacrificing template-assisted pyrolysis approach to improve the microstructure of catalysts and optimize the active site. The heteroatom doping method in this work provides significant guidance for promoting 2e^- ORR electrocatalysis to produce H₂O₂.

Key words: NiX/Ni@NCHS composite catalyst, 2e^- oxygen reduction reaction, Honeycomb-like porous carbon, Density functional theory, Electrocatalysis

Mengran Liu, Canyu Liu, Tianfang Yang, Shixiang Hu, Siyun Li, Shizhe Liu, Yang Liu, Ye Chen, Bingcheng Ge, Shuyan Gao. High-efficiency electrochemical H₂O₂ synthesis by heteroatom-doped NiX/Ni nanocomposites with honeycomb-like porous carbon[J]. Chinese Journal of Catalysis, 2024, 66: 212-222.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(24)60121-X

https://www.cjcatal.com/EN/Y2024/V66/I11/212

Figures/Tables 6

Scheme 1. Schematic illustration for the synthesis of the NiO/Ni@NCHS-700 composite catalyst with a honeycomb structure (a) and the NCSS-700 catalyst with a solid structure (b).

Fig. 1. Compositions and morphologies of NiO/Ni@NCHS-700. (a,b) FESEM images; (c,d) TEM images; (e,f) HR-TEM images; (g) HAADF images, and corresponding EDS maps.

Fig. 2. N2 adsorption-desorption isotherms (a), pore size distributions by the DFT method (b), BET specific area and total pore volume information (c), XRD patterns (d), Raman spectra (e), and FT-IR spectra (f) of NiO/Ni@NCHS-700 and counterparts.

Fig. 3. (a) Full spectrum of NCHS-700, NCSS-700, NiO/Ni@NCHS-700, and NiO/Ni@NCSS-700. High-resolution XPS spectra of C 1s (b). (c) Element contents of different samples. N 1s (d), O 1s (e) and Ni 2p (f) spectra of catalysts XPS.

Fig. 4. LSV curves (a), limiting disk current density (jL) and onset potential (Eon) (b), H2O2 selectivity and electron transfer number (n) (c) of NCHS-700, NCSS-700, NiO/Ni@NCHS-700, and NiO/Ni@NCSS-700. (d) Performance comparison of electrochemical H2O2 production on NiO/Ni@NCHS-700 and other reported catalysts based on RRDE performance map of Eon and maximum H2O2 selectivity. (e) Tafel plots of NiO/Ni@NCHS-700. (f) The calculated H2O2 productivity and Faradaic efficiency of NiO/Ni@NCHS-700 at 0.2, 0.3, 0.4, 0.5, and 0.6 V vs. RHE, respectively (Error bars from three measurements at different potentials). (g) Stability measurement of NiO/Ni@NCHS-700. (h) Performance comparison of electrochemical H2O2 production on NiO/Ni@NCHS-700 and other recently reported catalysts performance map of jL and durability.

Fig. 5. (a) The ATR-FIIR spectra of NiO/Ni@NCHS for the 2e- ORR in the potentiostatic step. (b) In situ Raman spectra of NiO/Ni@NCHS. (c,d) Free energy diagram of the Ni@NCHS, NiO@NCHS, NiS6@NCHS, NiO/Ni@NCHS, and NiS6/Ni@NCHS. (e) PDOS for the d-orbitals. (f,g) Charge density differences of NiO/Ni@NCHS and NiS6/Ni@NCHS, where the electron accumulation and depletion regions are shown in yellow and green, respectively. (h) Volcano plot for 2e- ORR activity with the *OOH descriptor. (i) Schematic diagrams of NiO/Ni@NCHS reaction processes.

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High-efficiency electrochemical H₂O₂ synthesis by heteroatom-doped NiX/Ni nanocomposites with honeycomb-like porous carbon

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