Synergistic promotion of HER and OER by alloying ternary Zn-Co-Ni nanoparticles in N-doped carbon interfacial structures

doi:10.1016/S1872-2067(21)63938-4

Abstract

Abstract:

Catalytic water splitting potentially reduce the consumption of fossil fuels and has received intense research attention. Synergy effects in multi-element transition metal-based water splitting catalysts have evoked special interests. Studies on catalysts in interfacial structures are especially meaningful due to their pertinence in applications. In this study, we report the synergy effects in promoting catalytic power in the ternary transition metal Zn, Co, Ni alloy nanoparticles that embeds in the carbonized Ppy/CNT multilayered matrix. By comparison with a series of binary or single metal counterparts, the mechanism under the synergy effects are elucidated. Experimental and DFT calculation results indicate that the ternary transition metal catalysts in the N-doped carbon matrix present special electronic structure, which benefits the reversible transition-state adsorption in HER and OER and render the catalysts high conductivity in room temperature. We expect our findings inspire further development of efficient transition metal HER and OER catalysts.

Key words: Water splitting, Hydrogen evolution reaction, Oxygen evolution reaction, Diversity of elements, Electron modification

Limei Lu, Yihe Zhang, Zhensheng Chen, Feng Feng, Kaixuan Teng, Shuting Zhang, Jialin Zhuang, Qi An. Synergistic promotion of HER and OER by alloying ternary Zn-Co-Ni nanoparticles in N-doped carbon interfacial structures[J]. Chinese Journal of Catalysis, 2022, 43(5): 1316-1323.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63938-4

https://www.cjcatal.com/EN/Y2022/V43/I5/1316

Figures/Tables 6

Scheme 1. Schematic illustration of the preparation process of ZnCoNi/(Ppy/CNTs)4.

Fig. 1. (a) XRD patterns of the prepared series of catalysts; SEM (b,d), HRTEM (c) images, and corresponding elemental mapping images (e-j) of ZnCoNi/(Ppy/CNTs)4.

Fig. 2. High-resolution XPS spectra of Ni 2p (a), N 1s (b), Co 2p (c), Zn 2p (d) in samples as denoted in the images.

Fig. 3. LSV curves (a), Tafel plots (b), linear fitting of the capacitive currents (c), and Nyquist plots (d) of the series of samples as denoted in the images; (e) LSV curves of ZnCoNi/(Ppy/CNT)4 before and after CV; (f) Time dependent current density curves of ZnCoNi/(Ppy/CNTs)4.

Fig. 4. (a) DFT simulation of ΔGH* on the series of catalyst model structures as denoted as in (b-e), which presents models used in DFT calculations and optimized geometric configuration of H adsorption, (f-i) The charge density distribution illustrates the change in electron distribution: yellow area denotes obtaining electrons and blue color denotes loss of electrons, (j-m) Calculated DOS distribution of ZnCo/(Ppy/CNTs)4, ZnNi/(Ppy/CNTs)4, CoNi/(Ppy/CNTs)4 and ZnCoNi/(Ppy/CNTs)4, respectively.

Fig. 5. OER activities of the series of catalysts as denoted in the images in 1 mol/L KOH. (a) LSV curves; (b) Corresponding Tafel plots; (c) Free energy diagrams at the U of 1.23 V.

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