Improved nitrogen reduction electroactivity by unique MoS2-SnS2 heterogeneous nanoplates supported on poly(zwitterionic liquids) functionalized polypyrrole/graphene oxide

doi:10.1016/S1872-2067(21)63944-X

Abstract

Abstract:

Unique MoS₂-SnS₂ heterogeneous nanoplates have successfully in-situ grown on poly(3-(1-vinylimidazolium-3-yl)propane-1-sulfonate) functionalized polypyrrole/ graphene oxide (PVIPS/PPy/GO). PVIPS can attract heptamolybdate ion (Mo₇O₂₄^6-) and Sn⁴⁺ as the precursors by the ion-exchange, resulting in the simultaneous growth of 1T’-MoS₂ and the berndtite-2T-type hexagonal SnS₂ by the interfacial induced effect of PVIPS. The obtained MoS₂-SnS₂/ PVIPS/PPy/GO can serve as electrocatalysts, exhibiting good NRR performance by the synergistic effect. The semi-conducting SnS₂ would limit the surface electron accessibility for suppressing HER process of 1T’-MoS₂, while metallic 1T’-MoS₂ might efficiently improve the NRR electroactivity of SnS₂ by the creation of Mo-Sn-Sn trimer catalytic sites. Otherwise, the irreversible crystal phase transition has taken place during the NRR process. Partial 1T’-MoS₂ and SnS₂ have electrochemically reacted with N₂, and irreversibly converted into Mo₂N and Sn_xN_z due to the formation of Mo-N and Sn-N bonding, meanwhile, partial SnS₂ has been irreversibly evolved into SnS due to the reduction by the power source in the electrochemical system. It would put forward a new design idea for optimizing the preparation method and electrocatalytic activity of transition metal dichalcogenides.

Key words: MoS₂, SnS₂, Poly(3-(1-vinylimidazolium-3-yl)propane-1-sulfonate), functionalized polypyrrole/graphene oxide, Nitrogen reduction reaction, Irreversible crystal phase transition

Hui Mao, Haoran Yang, Jinchi Liu, Shuai Zhang, Daliang Liu, Qiong Wu, Wenping Sun, Xi-Ming Song, Tianyi Ma. Improved nitrogen reduction electroactivity by unique MoS₂-SnS₂ heterogeneous nanoplates supported on poly(zwitterionic liquids) functionalized polypyrrole/graphene oxide[J]. Chinese Journal of Catalysis, 2022, 43(5): 1341-1350.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63944-X

https://www.cjcatal.com/EN/Y2022/V43/I5/1341

Figures/Tables 8

Fig. 1. XRD patterns (a), EDS spectra (b), survey (c), Mo 3d (d), Sn 3d (e), and S 2p (f) XPS spectra of MoS2/PVIPS/PPy/GO (1), SnS2/PVIPS/PPy/GO (2), and MoS2-SnS2/PVIPS/PPy/GO (3).

Fig. 2. SEM (a), TEM (b), HRTEM (c), the SAED pattern (d) and high-angle annular dark field image (e) of MoS2-SnS2/PVIPS/PPy/GO, with the corresponding elemental mapping of C, N, O, Mo, Sn, S.

Fig. 3. The NH3 yield and FE of MoS2/PVIPS/PPy/GO (a), SnS2/PVIPS/PPy/GO (b), MoS2-SnS2/PVIPS/PPy/GO (c) for NRR under electrolysis for 2 h in 0.1 mol/L Na2SO4 at different potentials (vs. RHE); (d) The NH3 yield and FE obtained by different electrocatalysts at ?0.5 V (vs. RHE) under electrolysis for 2 h in 0.1 mol/L Na2SO4: (1) MoS2-SnS2, (2) MoS2-SnS2/GO, (3) MoS2-SnS2/PPy/GO, (4) MoS2/PVIPS/PPy/GO, (5) SnS2/PVIPS/PPy/GO and (6) MoS2-SnS2/PVIPS/PPy/GO.

Table 1 Different electrocatalysts synthesized by different supporters with their Mo and Sn content determined by ICP and calculated MoS2+SnS2 loading content.

Electrocatalyst	Mo content by ICP (wt%)	Sn content by ICP (wt%)	MoS₂+SnS₂ loading (wt%)
MoS₂-SnS₂	—	—	100.00
MoS₂-SnS₂/GO	7.97	13.22	33.63
MoS₂-SnS₂/PPy/GO	5.75	5.21	17.59
MoS₂/PVIPS/PPy/GO	17.46	0	29.10
SnS₂/PVIPS/PPy/GO	0	7.51	11.56
MoS₂-SnS₂/PVIPS/PPy/GO	5.16	6.03	17.88

Fig. 4. (a) Linear sweep voltammograms of MoS2-SnS2/PVIPS/PPy/GO under saturated Ar and N2 in 0.1 mol/L Na2SO4; (b) The NH3 yield and FE of MoS2-SnS2/PVIPS/PPy/GO with alternating 2 h cycles at ?0.5 V between Ar and N2 atmosphere; (c) Recycling test for MoS2-SnS2/PVIPS/PPy/GO at ?0.5 V under electrolysis for 2 h performed six times; (d) XRD patterns of MoS2-SnS2/PVIPS/PPy/GO before (1) and after (2) NRR for 30 h.

Fig. 5. SEM (a), TEM (b), HRTEM (c), the SAED pattern (d) and high-angle annular dark field image (e) of MoS2-SnS2/PVIPS/PPy/GO after NRR for 30 h, with the corresponding elemental mapping of C, N, O, Mo, Sn, S.

Fig. 6. XPS spectra of MoS2-SnS2/PVIPS/PPy/GO before (1) and after (2) electrocatalysis, performed by chronoamperometry for 30 h under saturated N2 in 0.1 mol/L Na2SO4. (a) C 1s; (b) O 1s; (c) N 1s; (d) Mo 3d; (e) Sn 3d; (f) S 2p.

Scheme 1. The irreversible crystal phase transition of MoS2-SnS2 heterogeneous nanoplates with the corresponding electrode reactions on MoS2-SnS2/PVIPS/PPy/GO in 0.1 mol/L Na2SO4 solution containing saturated N2.

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Improved nitrogen reduction electroactivity by unique MoS₂-SnS₂ heterogeneous nanoplates supported on poly(zwitterionic liquids) functionalized polypyrrole/graphene oxide

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