Formic acid as a natural biomass and a CO2 reduction product has attracted considerable interest in renewable energy exploitation, serving as both a promising candidate for chemical hydrogen storage material and a direct fuel for low temperature liquid fed fuel cells In addition to its chemical dehydrogenation, formic acid oxidation (FAO) is a model reaction in the study of electrocatalysis of C1 molecules and the anode reaction in direct formic acid fuel cells (DFAFCs) Thanks to a deeper mechanistic understanding of FAO on Pt and Pd surfaces brought about by recent advances in the fundamental investigations, the “synthesis-by-design” concept has become a mainstream idea to attain high-performance Pt- and Pd-based nanocatalysts As a result, a large number of efficient nanocatalysts have been obtained through different synthesis strategies by tailoring geometric and electronic structures of the two primary catalytic metals In this paper, we provide a brief overview of recent progress in the mechanistic studies of FAO, the synthesis of novel Pd- and Pt-based nanocatalysts as well as their practical applications in DFAFCs with a focus on discussing studies significantly contributing to these areas in the past five years

Electrocatalysis of formic acid on palladium and platinum surfaces: from fundamental mechanisms to fuel cell applications

The decomposition of HCOOH on Pd surfaces over a potential range of practical relevance to hydrogen production and fuel cell anode operation was probed by combining high-sensitivity in situ surface-enhanced IR spectroscopy with attenuated total reflection and thin-layer flow cell configurations. For the first time, concrete spectral evidence of COad formation has been obtained, and a new main pathway from HCOOH to COad involving the reduction of the dehydrogenation product of HCOOH (i.e., CO2) is proposed.

From HCOOH to CO at Pd electrodes: a surface-enhanced infrared spectroscopy study.

Highly dispersed boron-doped palladium nanoparticles supported on carbon black (Pd−B/C) with high Pd loading (ca. 40 wt % Pd) are synthesized through an aqueous process using dimethylamine borane as the reducing agent. The as-prepared Pd−B/C catalyst shows extraordinary activity toward formic acid electro-oxidation compared to that of a commercially available Pd/C catalyst and the one prepared by using NaBH4 as the reductant. Subsequent thermal treatment further enhances the durability of the electro-oxidation current on Pd−B/C, enabling this new material to be a promising anode catalyst for direct formic acid fuel cells. The superior performance of our Pd−B/C catalyst may arise from uniformly dispersed nanoparticles within optimal size ranges, the increase in surface-active sites, and the electronic modification effect of boron species.

Boron-Doped Palladium Nanoparticles on Carbon Black as a Superior Catalyst for Formic Acid Electro-oxidation

Preparation of carbon supported Pd–P catalyst with high content of element phosphorus and its electrocatalytic performance for formic acid oxidation

The electrocatalytic properties of palladium nanocubes towards the electrochemical oxidation of formic acid were studied in H2SO4 and HClO4 solutions and compared with those of spherical Pd nanoparticles. The spherical and cubic Pd nanoparticles were characterized by transmission electron microscopy (TEM) and X-ray diffraction (XRD). The intrinsic electrocatalytic properties of both nanoparticles were shown to be strongly dependent on the amount of metal deposited on the gold substrate. Thus, to properly compare the activity of both systems (spheres and nanocubes), the amount of sample has to be optimized to avoid problems due to a lower diffusion flux of reactants in the internal parts of the catalyst layer resulting in a lower apparent activity. Under the optimized conditions, the activity of the spheres and nanocubes was very similar between 0.1 and 0.35 V. From this potential value, the activity of the Pd nanocubes was remarkably higher. This enhanced electrocatalytic activity was attributed to the prevalence of Pd(100) facets in agreement with previous studies with Pd single crystal electrodes. The effect of HSO4−/SO42− desorption–adsorption was also evaluated. The activity found in HClO4 was significantly higher than that obtained in H2SO4 in the whole potential range.

Shape-dependent electrocatalysis: formic acid electrooxidation on cubic Pd nanoparticles

In situ and ex situ FTIR characterization of a cyanate adlayer on Cu(111)

Catalytic and electro-catalytic oxidation of formic acid on the pure and Cu-modified Pd(111)-surface

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In situ and ex situ FTIR characterization of a cyanate adlayer on Cu(111)

Catalytic and electro-catalytic oxidation of formic acid on the pure and Cu-modified Pd(111)-surface