CO2 hydrogenation to HCOOH catalyzed by aqueous Pd needle assembly

Abstract

Carbon dioxide (CO₂) conversion to liquid fuels has attracted great attention due to the current environmental concerns and energy crisis. However, the selective conversion of CO₂ to target liquids is formidably challenging due to the chemical inertness of CO₂. We theoretically and experimentally confirm that the bending of Pd−Pd bond can breaks the asymmetric potential well and facilitate CO₂ adsorption. We have successfully synthesized a new class of Pd nanoneedles via a “close edges and open corners” process, with a magic angle of 60^o between the main trunk and branch, and realized the selective CO₂ hydrogenation to formic acid (HCOOH) at room temperature in water. Impressively, a HCOOH productivity of ~250 mmol g⁻¹ in 100 h while maintaining HCOOH selectivity over 99%. This work bridges nanostructure design and catalytic application, which may open a new avenue for selective CO₂ conversion in an elegant manner.