Ambient CO2 Hydrogenation to Formate Over NiPd Catalyst

Abstract

The urgent need for sustainable CO<inf>2</inf> management has driven the development of efficient catalytic systems capable of converting CO<inf>2</inf> into value-added chemicals under mild conditions. Herein, we report a Ni<inf>9</inf>Pd<inf>1</inf> catalyst with a low Pd content (Ni/Pd = 9:1) for the selective CO<inf>2</inf> hydrogenation to formate at low temperatures. Remarkably, this catalyst exhibits exceptional versatility, efficiently hydrogenating both aqueous (bi)carbonate and CO<inf>2</inf> captured from air (as carbonate) to formate. Moreover, this catalyst shows appreciable robustness by achieving cumulative formate yields of 770.5 mmol g<inf>Pd</inf>−1 (TON of 82, STY of 32.18 mmol<inf>formate</inf> g<inf>Pd</inf>−1h−1 at 28 °C) and 1371.9 mmol g<inf>Pd</inf>−1 (TON of 146, STY of 57.16 mmol<inf>formate</inf> g<inf>Pd</inf>−1h−1 at 80 °C) over multiple cycles. The synergistic Ni-to-Pd interaction in this catalyst leads to the efficient CO<inf>2</inf> activation and H<inf>2</inf> dissociation, enabling operation under mild conditions. This study demonstrates an integrated and sustainable approach where CO<inf>2</inf> captured from air can be hydrogenated to formate at low temperature. © 2025 Elsevier B.V., All rights reserved.