Catalytic CO2 hydrogenation to formic acid over carbon nanotube-graphene supported PdNi alloy catalysts

Abstract

Pure formic acid was successfully produced via CO₂ hydrogenation for the first time over a heterogeneous catalyst of PdNi alloy on a carbon nanotube-graphene (CNT-GR) support in water as an eco-friendly solvent without a base additive. The highest formic acid yield obtained was 1.92 mmol with a turnover number of 6.4 and a turnover frequency of 1.2 × 10⁻⁴ s⁻¹ under mild reaction conditions of 40 °C and 50 bar. Alloying Pd with Ni brought a significant enhancement in catalytic activity compared to the monometallic Pd catalyst. In addition, the CNT-GR composite as a catalytic support improved the dispersion of Pd–Ni alloy particles, which exhibited good stability under the reaction conditions.