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. 2022 Jul 14;12(14):2414.
doi: 10.3390/nano12142414.

Amine-Functionalized Natural Halloysite Nanotubes Supported Metallic (Pd, Au, Ag) Nanoparticles and Their Catalytic Performance for Dehydrogenation of Formic Acid

Limin Song  1 , Kaiyuan Tan  1 , Yingyue Ye  1 , Baolin Zhu  1   2 , Shoumin Zhang  1   2 , Weiping Huang  1   2
Affiliations

Amine-Functionalized Natural Halloysite Nanotubes Supported Metallic (Pd, Au, Ag) Nanoparticles and Their Catalytic Performance for Dehydrogenation of Formic Acid

Limin Song et al. Nanomaterials (Basel). .

Abstract

In today's age of resource scarcity, the low-cost development and utilization of renewable energy, e.g., hydrogen energy, have attracted much attention in the world. In this work, cheap natural halloysite nanotubes (HNTs) were modified with γ-aminopropyltriethoxysilane (APTES), and the functionalized HNTs were used as to support metal (Pd, Au, Ag) catalysts for dehydrogenation of formic acid (DFA). The supports and fabricated catalysts were characterized with ICP, FT-IR, XRD, XPS and TEM. The functional groups facilitate the anchoring of metal particles to the supports, which brings about the high dispersion of metallic particles in catalysts. The catalysts show high activity against DFA and exhibit selectivity of 100% toward H2 at room temperature or less. The interactions between active centers and supports were investigated by evaluation and comparison of the catalytic performances of Pd/NH2-HNTs, PdAg/NH2-HNTs and PdAu/NH2-HNTs for DFA.

Keywords: Pd; dehydrogenation; formic acid; halloysite nanotube; γ-aminopropyltriethoxysilane.

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Conflict of interest statement

The authors declare no conflict of interest.

Figures

Scheme 1
Scheme 1
Synthesis processes of Pd/NH2-HNTs.
Figure 1
Figure 1
The device for evaluating the performances of catalysts in DFA.
Figure 2
Figure 2
(a) XRD patterns; (b) FTIR spectra.
Figure 3
Figure 3
TEM images of (a) NH2-HNTs, (b,c) Pd/NH2-HNTs and (d) Pd/HNTs; (e) HAADF-STEM images of Pd/NH2-HNTs; (f) EDX mapping of Pd in Pd/NH2-HNTs; (g) HAADF-STEM images of PdAu/NH2-HNTs; (h) EDX mapping of Pd in PdAu/NH2-HNTs; (i) EDX mapping of Au in PdAu/NH2-HNTs.
Figure 4
Figure 4
XPS spectra. (a) Full spectra of HNTs, NH2-HNTs and Pd/NH2-HNTs; (b) Pd spectra of Pd/HNTs; (c) Pd spectra of Pd/NH2-HNTs; (d) Pd spectra of PdAg/NH2-HNTs; (e) PdAu spectra of Pd/NH2-HNTs.
Figure 5
Figure 5
(a) H2 volumes generated in DFA reactions of solution with FA/SF = 1 over catalysts at 298 K. (b) Hydrogen generation over the catalyst Pd/NH2-HNTs with FA/SF = 1 at 283, 298 and 313 K; (c) with different FA/SF molar ratios at 298 K. (d) Recyclability results of Pd/NH2-HNTs used in DFA.
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