Hydrolytic dehydrogenation of ammonia borane catalyzed by poly(amidoamine) dendrimers-modified reduced graphene oxide nanosheets supported Ag0.3Co0.7 nanoparticles

doi:10.1016/j.jmst.2018.06.003

Abstract

Abstract:

Poly(amidoamine) dendrimers-modified reduced graphene oxide nanosheets (PAMAM/rGO) composite was selected as a carrier of heterogeneous Ag_0.3Co_0.7 nanoparticles in order to obtain an excellent catalyst for ammonia borane (AB) hydrolysis. During the synthetic processes, GO could easily assembled with PAMAM by the electrostatic and hydrogen-bonding interactions. Structural characterization revealed that Ag_0.3Co_0.7 bimetallic nanoparticles with uniform size distribution of 5 nm are well dispersed on PAMAM/rGO composite architecture. Ag_0.3Co_0.7@PAMAM/rGO was found to be a highly active and reusable catalyst in hydrogen generation from the hydrolysis of AB with a turnover frequency value (TOF) of 19.79 mol_H2 min^-1 mol_M^-1 at 25.0 ± 0.1 °C and retained 75.4% of their initial activity with a complete release of hydrogen in five runs. The relatively high TOF value and low apparent activation energy (34.21 kJ mol^-1) make these Ag_0.3Co_0.7@PAMAM/rGO NPs as a high-efficient catalyst for catalytic dehydrogenation of AB facilitating the development of practically applicable energy storage materials.

Key words: Ammonia borane, Reduced graphene oxide, Ammonia borane, Ag_0.3Co_0.7 bimetallic nanoparticles, Hydrolytic dehydrogenation

Dandan Ke, Jin Wang, Hongming Zhang, Yuan Li, Lu Zhang, Xin Zhao, Shumin Han. Hydrolytic dehydrogenation of ammonia borane catalyzed by poly(amidoamine) dendrimers-modified reduced graphene oxide nanosheets supported Ag_0.3Co_0.7 nanoparticles[J]. J. Mater. Sci. Technol., 2018, 34(12): 2350-2358.

Figures/Tables 10

Fig. 1. (a) Schematic illustration of self-assembly of PAMAM/GO suspensions, followed by chemical reduction of Ag+ and Co2+ and (b) photographs of PAMAM dendrimers, GO dispersion, PAMAM/GO, and Ag0.3Co0.7@PAMAM/rGO suspensions; (c) Schematic illustration of the synthesized Ag-Co@PAMAM/rGO NPs applied for hydrolytic dehydrogenation of AB.

Fig. 2. TEM images of (a) Ag0.3Co0.7, (b) Ag0.3Co0.7@rGO, (c) Ag0.3Co0.7@PAMAM, (d) Ag0.3Co0.7@PAMAM/rGO, (e) the corresponding the selected-area electron diffraction (SAED) pattern and (f) EDAX of Ag0.3Co0.7@PAMAM/rGO.

Fig. 3. XRD patterns of GO, PAMAM/GO, Ag0.3Co0.7@PAMAM/rGO composite.

Fig. 4. FT-IR results of GO, PAMAM, PAMAM/GO composite and Ag0.3Co0.7@PAMAM/rGO NPs.

Fig. 5. (a) XPS survey of Ag0.3Co0.7@PAMAM/rGO; (b-e) high-resolution XPS spectrum of C1s, N1s, Ag3d5/2 and Co2p3/2 respectively; (f) high-resolution Co2p3/2XPS spectrum ofCo@PAMAM/rGO.

Fig. 6. (a) Hydrogen evolution plots and (b) the corresponding TOF values of the AB hydrolysis (1.5 mmol, 6 mL) in the presence of Ag0.3Co0.7, Co@rGO, Co@PAMAM/rGO, Ag0.3Co0.7/PAMAM, Ag0.3Co0.7@rGO, Ag0.3Co0.7@PAMAM/rGO catalysts.

Fig. 7. Kinetic studies of Ag0.3Co0.7@PAMAM/rGO catalyst towards hydrolysis of NH3·BH3 under different reaction parameters: (a) different NH3·BH3 concentrations; (b) plot of ln [AB] vs lnr; (c) different catalyst concentrations; (d) plot of ln [cat.] vs ln r; (e) effect of NaOH concentration from 0 to 0.25 M on NH3·BH3 hydrolysis reaction; (f) plot of ln [NaOH] vs ln r.

Fig. 8. Effect of temperature on the hydrolysis of AB solution without (a); (b) lnk versus 1/T (Arrhenius eq.); and (c) ln (k/T) versus 1/T (Eyring eq.), [0.25 M AB, 0.05 mmol Ag0.3Co0.7@PAMAM/rGO NPs].

Table 1 Catalytic activity of reported Ag- and/or Co- based catalysts applied for the hydrolysis of NH3·BH3.

Catalyst	TOF (total metal)	Ea (kJ mol^-1)	Ref.
Ag_0.3Co_0.7/PAMAM/rGO	19.79	34.21	This study
Ag_0.3Co_0.7/PAMAM	15.84	35.66	[8]
PSSA-co-MA stabilized Co(0) nanoclusters	25.7	34	[34]
PEI-capped Co	39.9	28.2	[30]
PEI-GO/Fe-Ni	4.4	-	[22]
Ag@Co/graphene	10.24	20.03	[12]
Ag@CoFe/graphene	8.29	32.79	[35]
graphene-CoNi	16.4	13.49	[36]
RuCo (1:1)/γ-Al₂O₃	16.4	47	[37]
Cryogel p(4-VP)-Co	-	34.98	[38]
Amorphous Co-B, Ultrasonic hydrolysis	21.8	47.50	[39]
Co/Pdop-o-MWCNT	-	50.41	[40]

Fig. 9. Hydrolysis of aqueous NH3·BH3 solution catalyzed by Ag0.3Co0.7@PAMAM/rGO catalyst from the 1st to 5th cycle, insert: dehydrogenation rate values after five cycles.

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