Controllable H2 Generation by Formic Acid Decomposition on a Novel Pd/Templated Carbon Catalyst

Lucian Barbu-Tudoran,Mihaela D Lazar,Maria Mihet,Gabriela Blanita,Monica Dan

doi:10.3390/hydrogen1010003

Lucian Barbu-Tudoran, Mihaela D Lazar + Show 3 more

Open Access

https://doi.org/10.3390/hydrogen1010003

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Abstract

A novel Pd/templated carbon catalyst (Pd/TC) was developed, characterized, and tested in the dehydrogenation of formic acid (FA) under mild conditions, with the possibility to control the H2 generation rate, in the absence or presence of HCOONa (SF), by adjusting the Pd:FA and/or FA:SF ratios. The characterization results of the templated carbon obtained by the chemical vapor deposition of acetylene on NaY zeolite revealed different structural and morphological properties compared to other C-based supports. Therefore, it was expected to induce a different catalytic behavior for the Pd/TC catalyst. Indeed, the TC-supported Pd catalyst exhibited superior activity in the decomposition of FA, even at room temperature, with turnover frequencies (TOFs) of up to 143.7 and 218.8 h−1 at 60 °C. The H2 generation rate increased with an increasing temperature, while the H2 yield increased with a decreasing FA concentration. Constant generation of gaseous flow (H2 + CO2) was achieved for 11 days, by the complete dehydrogenation of FA at room temperature using a 2 M FA solution and Pd:FA = 1:2100. The presence of SF in the reaction medium significantly enhanced the H2 generation rate (535 h−1 for FA:SF = 3:1 and 60 °C).

Highlights

In the quest for environmentally friendly energy sources, hydrogen is regarded as the most promising energy carrier, considering that its combustion leads to the formation of the benign water molecule [1,2]
The aim of this paper is to report the synthesis of a novel Pd/templated carbon catalyst (Pd/TC)
The actual Pd concentration on the templated carbon catalyst determined by inductively coupled plasma mass spectrometry (ICP-MS) was 9.75 wt.%, very close to the target concentration

Summary

Introduction

In the quest for environmentally friendly energy sources, hydrogen is regarded as the most promising energy carrier, considering that its combustion leads to the formation of the benign water molecule [1,2] Issues such as efficient hydrogen production or effective hydrogen storage and safe transportation have to be addressed, in order to reach the goal of a hydrogen-based economy [2,3,4,5]. In this context, there is a tremendous research interest towards the development of appropriate storage solutions which can allow the controllable and efficient generation of hydrogen under mild conditions (near ambient temperatures and atmospheric pressure) [6,7]. Physical storage deals with the compression of molecular hydrogen at low temperatures and high pressures [1,2], or with its adsorption on high surface area materials, such as carbon-based materials [2,8], zeolites, or metal–organic frameworks [9,10,11].

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