The formation and catalytic activity of silver nanoparticles in aqueous polyacrylate solutions

doi:10.1007/s11705-016-1584-0

Front. Chem. Sci. Eng.

2016, Vol. 10

Issue (3) : 432-439 https://doi.org/10.1007/s11705-016-1584-0

RESEARCH ARTICLE

The formation and catalytic activity of silver nanoparticles in aqueous polyacrylate solutions

Jie Wang¹,Jianjia Liu¹,Xuhong Guo^1,^*(

),Liang Yan²,Stephen F. Lincoln^2,^*(

)

¹. State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China
². Department of Chemistry, University of Adelaide, Adelaide, SA 5005, Australia

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Abstract

Silver nanoparticles (AgNPs) have been synthesized in the presence of polyacrylate through the reduction of silver nitrate by sodium borohydride in aqueous solution. The AgNO₃ and polyacrylate carboxylate group concentrations were kept constant at 2.0 × 10⁻⁴ and 1.0 × 10⁻² mol?L⁻¹, respectively, while the ratio of [NaBH₄]/[AgNO₃] was varied from 1 to 100. The ultra-violet-visible plasmon resonance spectra of these solutions were found to vary with time prior to stabilizing after 27 d, consistent with changes of AgNP size and distribution within the polyacrylate ensemble occurring. These observations, together with transmission electron microscopic results, show this rearrangement to be greatest among the samples at the lower ratios of [NaBH₄]/[AgNO₃] used in the preparation, whereas those at the higher ratios showed a more even distribution of smaller AgNP. All ten of the AgNP samples, upon a one thousand-fold dilution, catalyze the reduction of 4-nitrophenol to 4-aminophenol in the temperature range 283.2–303.2 K with a substantial induction time being observed at the lower temperatures.

Keywords silver nanoparticles polyacrylates catalysis mechanism sodium borohydride

PACS:

Fund:

Corresponding Author(s): Xuhong Guo,Stephen F. Lincoln

Just Accepted Date: 08 July 2016 Online First Date: 10 August 2016 Issue Date: 23 August 2016

Cite this article:

Jie Wang,Jianjia Liu,Xuhong Guo, et al. The formation and catalytic activity of silver nanoparticles in aqueous polyacrylate solutions[J]. Front. Chem. Sci. Eng., 2016, 10(3): 432-439.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-016-1584-0
https://academic.hep.com.cn/fcse/EN/Y2016/V10/I3/432

Fig.1 Schematic illustration of the formation of a AgNP through NaBH₄ reduction of Ag⁺ dispersed in a polyacrylate ensemble

Fig.2 UV-vis spectra of AgNP solutions in which the initial [NaBH₄]/[AgNO₃] decreases from 100 to 1 determined 1 d after preparation

Fig.3 Time dependence of the UV-vis spectra of a AgNP sample prepared with [NaBH₄]/[AgNO₃] = 2

Fig.4 Time dependence of the UV-vis spectrum of a AgNP sample prepared with [NaBH₄]/[AgNO₃] = 4

Fig.5 Time dependence of the UV-vis spectrum of a AgNP sample prepared with [NaBH₄]/[AgNO₃] = 100

Fig.6 Time dependence of absorbance at 400 nm as [NaBH₄]/[AgNO₃] varies from 1 to 100

Fig.7 TEM images and histograms of AgNPs and their size distribution: (a,b) Sample taken 1 day after preparation ([NaBH₄]/[AgNO₃] = 2); (c,d) Ag sample taken 27 d after preparation ([NaBH₄]/[AgNO₃] = 2); (e,f) Ag sample taken 27 d after preparation ([NaBH₄]/[AgNO₃] =10); (g,h) Ag sample taken 27 d after preparation ([NaBH₄]/[AgNO₃] = 100)

Fig.8 UV-vis absorbance changes at (a) 283. 2 K and (b) 303.2 K for the AgNP catalyzed reduction of 4-NP to 4-AP in the AgNP solutions with [NaBH₄]/[AgNO₃] = 30 and [AgNP] = 2.0 × 10⁻⁷ mol?L⁻¹ (calculated on the basis of single Ag atoms) after dilution. The initial concentrations of 4-NP and NaBH₄, were 5.39 × 10⁻⁵ and 1.08 × 10⁻² mol?L⁻¹, respectively; (c) Variation of induction time and ln(c_t/c₀) with time at five temperatures, where c_t and c₀ are [4-NP] mol?L⁻¹ at a time t and zero, respectively

Fig.9 The temperature variation of lnk for the Ag-NP/polyacrylate systems prepared at different [NaBH₄]/[AgNO₃] ratios

Tab.1 Kinetic parameters^a) derived for the catalytic reduction of 4-NP to 4-AP by AgNP in a polyacrylate ensemble in aqueous solution

Fig.10 The Langmuir-Hinshelwood mechanism proposed for the AgNP catalyzed reduction of 4-NP to 4-AP by BH₄⁻ in aqueous solution. Borohydride and 4-NP simultaneously adsorb reversibly to the AgNP. Borohydride is subsequently converted to B(OH)₄⁻ as it loses H^? as a consequence of the reduction of 4-NP. The rate determining step characterized by k_red, is the reduction of 4-NP to 4-AP which desorbs reversibly from the surface

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