Dual function materials (DFMs) are key for the integrated capture of CO₂ from waste gas streams and its valorisation to valuable chemicals, such as syngas. To be able to function in commercial applications, DFMs require both high capture capacity and catalytic activity, achieved by optimising the synergistic interactions among the catalytic metals, support and adsorbent components. To obtain increased interaction, the dry milling process can be used as a sustainable, solvent free, green synthesis method. In this work, we report the performance of RuNi bimetallic DFMs supported on CeO₂-Al₂O₃ and promoted with CaO and Na₂O, synthesised by a mild-energy mechano-chemical process. The materials show superior capture capacity and increased activity in Reverse Water-Gas Shift reaction (RWGS) for CO production at 650 °C compared to their counterpart prepared by a conventional impregnation method. High activity and stability are also maintained when O₂ is present in the capture step, indicating potential for real exhaust-gases capture applications. Also, direct air capture of CO₂ is reported, further underlining the benefits of the dry milling approach for creating versatile DFMs.

Those are the data generated for our collaborative project with Italy. All the data are given in excel files except of two figures with png format. The uploaded data also include the data used in the supplementary information and those figures and table are denoted with an 'S' before the number. The data include the physiochemical characterisation of ten (or nine) different samples and their activity performance under ideal and realistic conditions.