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Optimal Electrocatalytic Pd/MWNTs Nanocatalysts toward Formic Acid Oxidation.

ABSTRACT: The operating conditions such as composition of electrolyte and temperature can greatly influence the formic acid (HCOOH) oxidation reaction (FAOR). Palladium decorated multi-walled carbon nanotubes (Pd/MWNTs) were successfully synthesized and employed as nanocatalysts to explore the effects of formic acid, sulfuric acid (H2SO4) concentration and temperature on FAOR. Both the hydrogen adsorption in low potential range and the oxidation of poisoning species during the high potential range in cyclic voltammetry were demonstrated to contribute to the enhanced electroactivity of Pd/MWNTs. The as-synthesized Pd/MWNTs gave the best performance under a condition with balanced adsorptions of HCOOH and H2SO4 molecules. The dominant dehydrogenation pathway on Pd/MWNTs can be largely depressed by the increased dehydration pathway, leading to an increased charge transfer resistance (Rct ). Increasing HCOOH concentration could directly increase the dehydration process proportion and cause the production of COads species. H2SO4 as donor of H+ greatly facilitated the onset oxidation of HCOOH in the beginning process but it largely depressed the HCOOH oxidation with excess amount of H+. Enhanced ion mobility with increasing the temperature was mainly responsible for the increased current densities, improved tolerance stabilities and reduced Rct values, while dehydration process was also increased simultaneously.

SUBMITTER: Wang Y

PROVIDER: S-EPMC5881920 | biostudies-literature | 2015 Dec

REPOSITORIES: biostudies-literature

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Optimal Electrocatalytic Pd/MWNTs Nanocatalysts toward Formic Acid Oxidation.

Wang Yiran Y He Qingliang Q Wei Huige H Guo Jiang J Ding Keqiang K Wang Qiang Q Wang Zhe Z Wei Suying S Guo Zhanhu Z

Electrochimica acta 20151022

The operating conditions such as composition of electrolyte and temperature can greatly influence the formic acid (HCOOH) oxidation reaction (FAOR). Palladium decorated multi-walled carbon nanotubes (Pd/MWNTs) were successfully synthesized and employed as nanocatalysts to explore the effects of formic acid, sulfuric acid (H<sub>2</sub>SO<sub>4</sub>) concentration and temperature on FAOR. Both the hydrogen adsorption in low potential range and the oxidation of poisoning species during the high p ...[more]

PMID: 29622817

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Project description:Formic acid oxidation reaction (FAOR) at anode counterpart incurs at substantial high overpotential, limiting the power output efficiency of direct formic acid fuel cells (DFAFCs). Despite intense research, the lack of high-performance nanocatalysts (NCs) for FAOR remains a challenge in realizing DFAFC technologies. To surmount the overpotential losses, it is desirable to have NCs to trigger the FAOR as close to the reversible conditions (i.e. with over-potential loss as close to zero as possible). Herein, Pd-based binary and ternary NCs consisting of PdPt and PdRuPt have been synthesized via the polyol reduction method on the carbon support. As prepared PdPt and PdRuPt NCs were further subjected to heat treatment (annealed) in CO (namely PdPt-CO and PdRuPt-CO) and O2 (namely PdPt-O2 and PdRuPt-O2) atmosphere at 473?K temperature. By cross-referencing results of electron microscopy and X-ray spectroscopy together with electrochemical analysis, the effects of heat treatment under CO-reductive and O2-oxidative conditions towards FAOR were schematically elucidated. Of special relevance, the mass activity (MA) of PdPt-CO, PdPt-O2, PdRuPt-CO, and PdRuPt-O2 NCs is 1.7/2.0, 1.3/2.2, 1.1/5.5, and 0.9/4.7 Amg-1 in the anodic/cathodic scan, respectively, which is 2~4-folds improved comparative to of as-prepared PdPt (1.0/1.9 Amg-1 in anodic/cathodic scan, respectively) and PdRuPt (0.9/1.4 Amg-1 in anodic/cathodic scan, respectively) NCs. Meanwhile, after chronoamperometric (CA) stability test up to 2000 s, PdPt-CO (72 mAmg-1) and PdRuPt-CO (213 mAmg-1) NCs exhibit higher MA compared to as-prepared PdPt (54 mAmg-1) and PdRuPt (62 mAmg-1) NCs, which is attributed to the increase of surface Pt composition, especially for PdRuPt-CO NC. Besides, the stability of PdPt-O2 (15 mAmg-1) and PdRuPt-O2 (22 mAmg-1) NCs is deteriorated as compared to that of as-prepared NCs due to severe oxidation in O2 atmosphere. Of utmost importance, we developed a ternary PdRuPt catalyst with ultra-low Pt content (~2 wt.%) and significantly improved FAOR performance than pure Pt catalysts. Moreover, we demonstrated that the FAOR performance can be further enhanced by more than 30% via a unique CO annealing treatment.

Dataset Information

Optimal Electrocatalytic Pd/MWNTs Nanocatalysts toward Formic Acid Oxidation.

Publications

Optimal Electrocatalytic Pd/MWNTs Nanocatalysts toward Formic Acid Oxidation.

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