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Enhanced Formic Acid Oxidation over SnO₂-decorated Pd Nanocubes.

ABSTRACT: The formic acid oxidation reaction (FAOR) is one of the key reactions that can be used at the anode of low-temperature liquid fuel cells. To allow the knowledge-driven development of improved catalysts, it is necessary to deeply understand the fundamental aspects of the FAOR, which can be ideally achieved by investigating highly active model catalysts. Here, we studied SnO₂-decorated Pd nanocubes (NCs) exhibiting excellent electrocatalytic performance for formic acid oxidation in acidic medium with a SnO₂ promotion that boosts the catalytic activity by a factor of 5.8, compared to pure Pd NCs, exhibiting values of 2.46 A mg^-1 _Pd for SnO₂@Pd NCs versus 0.42 A mg^-1 _Pd for the Pd NCs and a 100 mV lower peak potential. By using ex situ, quasi in situ, and operando spectroscopic and microscopic methods (namely, transmission electron microscopy, X-ray photoelectron spectroscopy, and X-ray absorption fine-structure spectroscopy), we identified that the initially well-defined SnO₂-decorated Pd nanocubes maintain their structure and composition throughout FAOR. In situ Fourier-transformed infrared spectroscopy revealed a weaker CO adsorption site in the case of the SnO₂-decorated Pd NCs, compared to the monometallic Pd NCs, enabling a bifunctional reaction mechanism. Therein, SnO₂ provides oxygen species to the Pd surface at low overpotentials, promoting the oxidation of the poisoning CO intermediate and, thus, improving the catalytic performance of Pd. Our SnO _x -decorated Pd nanocubes allowed deeper insight into the mechanism of FAOR and hold promise for possible applications in direct formic acid fuel cells.

SUBMITTER: Rettenmaier C

PROVIDER: S-EPMC7754515 | biostudies-literature | 2020 Dec

REPOSITORIES: biostudies-literature

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Enhanced Formic Acid Oxidation over SnO<sub>2</sub>-decorated Pd Nanocubes.

Rettenmaier Clara C Arán-Ais Rosa M RM Timoshenko Janis J Rizo Rubén R Jeon Hyo Sang HS Kühl Stefanie S Chee See Wee SW Bergmann Arno A Roldan Cuenya Beatriz B

ACS catalysis 20201125 24

The formic acid oxidation reaction (FAOR) is one of the key reactions that can be used at the anode of low-temperature liquid fuel cells. To allow the knowledge-driven development of improved catalysts, it is necessary to deeply understand the fundamental aspects of the FAOR, which can be ideally achieved by investigating highly active model catalysts. Here, we studied SnO<sub>2</sub>-decorated Pd nanocubes (NCs) exhibiting excellent electrocatalytic performance for formic acid oxidation in acid ...[more]

PMID: 33362944

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Project description:Recently, photo-electrooxidation of fuel using a noble metal-semiconductor junction has been one of the most promising approaches in fuel cell systems. Herein, we report the development of a Pd-supported Bi2MoO6-Bi2O2CO3-CuO novel ternary heterojunction for ethanol oxidation in alkali in the presence and absence of visible light. Various spectroscopic and microscopic characterization techniques confirm strong coupling between palladium nanoparticles and Bi2MoO6-Bi2O2CO3-CuO ternary heterojunction supports. The photo-electrocatalytic efficacy of the synthesized catalysts was inspected by cyclic voltammetry (CV), chronoamperometry (CA), and electrochemical impedance spectroscopy (EIS). The CV study reveals that the forward peak current density (in mA mg-1 of Pd) of the synthesized quaternary heterojunction was about 1482.5, which is 2.4, 4, and 4.6 times higher than that of Pd/CuO (608.3), Pd/Bi2MoO6-Bi2O2CO3 (368.3), and similarly synthesized Pd catalyst (321.5) under visible light radiation. The best heterojunction catalyst shows 2.21-fold higher peak current density in visible light compared to that in dark. CA study reveals that after operation for 6000 s, the current density of the quaternary electrode is 1.5 and 3.4 times greater than that of Pd/CuO and Pd/C catalysts, respectively. The greater photocurrent response, lower photoluminescence (PL) emission intensity, and smaller semicircle arc in the Nyquist plot of the quaternary catalyst demonstrate the efficient segregation and higher charge transfer conductance of photogenerated charges to facilitate the photo-electrooxidation process of ethanol. The stability test shows that the quaternary catalyst loses only 9.8 and 7.7% of its maximum current density after 500 cycles of CV operation in the dark and light, respectively, indicating that light energy is more beneficial in establishing high stability. The dramatic enhancement of the photo-electrocatalytic activity of the quaternary electrode is owing to the lower band gap, high ECSA, enhanced charge separation of photogenerated carriers (e--h+), and all cocatalytic support of Bi2MoO6, Bi2O2CO3, and CuO in Pd/ Bi2MoO6-Bi2O2CO3-CuO under visible light radiation. The morphology and structure of the used quaternary catalyst are tested using FESEM and PXRD. Finally, ex situ FTIR spectroscopy and HPLC techniques help understand the ethanol electrooxidation reaction mechanism.

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Enhanced Formic Acid Oxidation over SnO₂-decorated Pd Nanocubes.

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Enhanced Formic Acid Oxidation over SnO<sub>2</sub>-decorated Pd Nanocubes.

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Enhanced Formic Acid Oxidation over SnO2-decorated Pd Nanocubes.

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Enhanced Formic Acid Oxidation over SnO<sub>2</sub>-decorated Pd Nanocubes.

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Enhanced Formic Acid Oxidation over SnO₂-decorated Pd Nanocubes.