Deciphering the role of amine in amino silane-functionalized Pd/rGO catalyst for formic acid decomposition at room tempe
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Bull Mater Sci (2020)43:302 https://doi.org/10.1007/s12034-020-02295-0
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Deciphering the role of amine in amino silane-functionalized Pd/rGO catalyst for formic acid decomposition at room temperature S SMITA BISWAS, M SRI TANDRAPADU, E ABINAYA and M ESWARAMOORTHY* Nanomaterials and Catalysis Laboratory, Chemistry and Physics of Materials Science, Jawaharlal Nehru Centre for Advanced Scientific Research, Bengaluru 560064, India *Author for correspondence ([email protected]) MS received 25 January 2020; accepted 27 July 2020 Abstract. Additive free, selective decomposition of formic acid to hydrogen and carbon dioxide at room temperature is still a challenging catalytic process which often requires noble metal catalyst (Pd, AuPd, AuPt) and sodium formate as an additive. Till date, catalyst design is targeted towards minimum noble metal usage along with incorporation of basic functionalities to produce in situ formate ion (key intermediate for dehydrogenation) from formic acid. In this work, we have studied the catalytic behaviour of amino silane-functionalized graphene oxide (GO) containing palladium nanoparticles for formic acid decomposition in ambient condition. By varying amine functionalization on GO and palladium content, the best performing catalyst was obtained with 5 wt% palladium loading. Additionally, it was observed for the first time that along with stability of a catalyst in reaction medium, its interaction with decomposed products, i.e., carbon dioxide with amine functional groups plays a crucial role in recyclability of a catalyst. Keywords.
1.
Formic acid; recyclability; graphene oxide; amino silane; palladium; dehydrogenation.
Introduction
Hydrogen being a CO2 neutral energy carrier and a clean alternative to fossil fuel is largely used in fuel cell-based technology. Although its gravimetric energy density is three times higher than gasoline, the low volumetric energy density (*10 kJ l-1 at ambient conditions) makes it illsuited for a large scale energy storage and transportation. As the production of hydrogen through renewable energy sources is gaining momentum, its efficient storage still remains a key challenge to realize a hydrogen-based energy economy [1]. Conventional physical methods of using high pressure and cryogenic containers to store hydrogen suffer from efficiency and safety problems [2]. The solid hydrogen carriers like zeolites, MOFs, porous carbons and metal hydrides (NaAlH4, MgH2, etc.), on the other hand, depend on high desorption temperature and/or very low adsorption and storage temperature restricting their wider usage [3–5]. The liquid organic hydrogen carriers (LOHC) for their convenience in transportation, refueling and handling are being considered as potential candidates for hydrogen storage and release. Nevertheless, toxicity, flammability and explosive nature, limits the usage of many LOHCs, such as
carbazole derivatives, hydrazine and methyl-cyclohexane [6–8]. Recently, formic acid, holding 4.4 wt% of H2, is re
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