RuFe Nanoparticles Modified Sheet-like BiVO4 : High-efficient Synergistic Catalyst for Ammonia Borane Hydrolytic Dehydrogenation

doi:10.15541/jim20190502

Abstract

Abstract:

Developing highly efficient and low-cost catalysts is crucial in the field of clean energy economy, in which ammonia borane (AB) has attracted great attention due to its high hydrogen production through the catalytic hydrolysis. In this work, BiVO₄ nanosheet was firstly synthesized by a facile reflux method. And then bimetallic RuFe@BiVO₄ catalysts with different molar ratios of Ru/Fe were prepared via in situ impregnation-reduction techniques and their catalytic activities were also tested in the hydrogen generation from aqueous solution of AB at room temperature. Compared with the releasing hydrogen rates of catalysts of BiVO₄, Ru@BiVO₄, Fe@BiVO₄, RuFe NPs and RuFe@BiVO₄, respectively, Ru₁Fe_0.1@BiVO₄ exhibits the highest catalytic activity for the dehydrogenation of AB among all catalysts, the activation energy (E_a) and turnover frequency (TOF) are 43.7 kJ·mol^-1 and 205.4 mol_H2·mol_Ru·min^-1, respectively. The addition of non-noble Fe can significantly enhance the catalytic activity of Ru counterparts, which is closely related to the strong electronic effect between Ru and Fe NPs, bi-functional effect generated between the RuFe NPs and the support BiVO₄.

Key words: BiVO₄, RuFe nanoparticles, synergistic catalysis, ammonia borane, releasing hydrogen

CLC Number:

O643

ZHANG Yiqing,ZHANG Shujuan,WAN Zhengrui,MO Han,WANG Niangui,ZHOU Liqun. RuFe Nanoparticles Modified Sheet-like BiVO₄ : High-efficient Synergistic Catalyst for Ammonia Borane Hydrolytic Dehydrogenation[J]. Journal of Inorganic Materials, 2020, 35(7): 809-816.

Figures/Tables 10

Fig. 1 XRD patterns of BiVO4, Ru@BiVO4, Fe@BiVO4, Ru1Fe0.1@BiVO4 and Ru1Fe0.1@BiVO4 after five cycles

Fig. 2 TEM images of BiVO4 (A, B), Ru1Fe0.1@BiVO4 (C) and RuFe NPs (E); particle size distributions of Ru1Fe0.1@BiVO4 (D) and RuFe NPs (F)

Fig. 3 FESEM image (A); elemental mappings of Ru and Fe (B) and EDS pattern of Ru1Fe0.1@BiVO4 (C)

Fig. 4 XPS spectra of the Ru1Fe0.1@BiVO4 catalysts (A) Survey; (B) Ru3p; (C) Fe2p; (D) Bi4f; (E) V2p; (F) O1s

Fig. 5 FT-IR spectra of BiVO4, Ru1Fe0.1@BiVO4 and Ru1Fe0.1@BiVO4 after five cycles

Table 1 ICP-AES analyses results of RuFe@BiVO4 catalyst

Catalyst	Initial ratio of Ru : Fe	Actual ratio of Ru : Fe	Actual Ru loading/wt%
RuFe@BiVO₄	1 : 0.10	1 : 0.12	4.21

Fig. 6 Plots of n(H2)/n(AB) vs. time from the hydrolysis of AB (18.5 mg) (A) Catalysts with the same nanoparticles loadings; (B) Ru1Fex NPs; (C) Ru1Fex@BiVO4 ; (D) Catalysts with different supporters

Fig. 7 Mechanism of AB hydrolysis catalyzed by the Ru1Fe0.1@BiVO4 catalyst

Fig. 8 Plots of n(H2)/n(AB) vs. time for the hydrolysis of AB catalyzed by Ru1Fe0.1@BiVO4 at different temperatures(A) and corresponding Arrhenius plots (B), and cycling test for the Ru1Fe0.1@BiVO4 within five cycles (C)

Table 2 Catalytic activities of different Ru-based catalysts used for the hydrolytic dehydrogenation of AB

Catalyst	TOF/(mol_H2?mol_Ru?min^-1)	E_a/(kJ?mol^-1)	Ref.
Ru NPs	26.7	66.5	[30]
RuCu(1 : 1)/γ-Al₂O₃	16.4	52	[31]
RuCo(1 : 11)/γ-Al₂O₃	32.9	47.0	[31]
RuCuCo@MIL-101	241.2	48.0	[32]
Ru@g-C₃N₄	313.0	37.4	[33]
RuCu/graphene	135.0	30.6	[34]
Ru₁Fe_0.1@BiVO₄	205.4	43.7	This study

References 34

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RuFe Nanoparticles Modified Sheet-like BiVO₄ : High-efficient Synergistic Catalyst for Ammonia Borane Hydrolytic Dehydrogenation

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