Short talk 2

The scaling up of electrocatalytic CO₂ reduction for practical applications is still hindered by a few challenges: low selectivity, small current density to maintain a reasonable selectivity, and the cost of the catalytic materials. Here we report a facile synthesis of earth-abundant Ni single-atom catalysts on commercial carbon black, which were further employed in a gas-phase electrocatalytic reactor under ambient conditions. As a result, those single-atomic sites exhibit an extraordinary performance in reducing CO₂ to CO, yielding a current density above 100 mA cm^-
2, with nearly 100% selectivity for CO and around 1%toward the hydrogen evolution side reaction. By further scaling up the electrode into a 10 * 10 cm² modular cell, the overall current in one unit cell can easily ramp up to more than 8 A while maintaining an exclusive CO evolution with a generation rate of 3.34 L hr
^-1 per unit cell.

The utilization of photothermal catalysis enables the direct transformation from solar energy to chemical energy over the catalyst. The indium oxide with surface hydroxides has been considered as a special catalyst that able to conduct CO₂ hydrogenation with significant photo-enhancement. We confirmed the presence of surface frustrated Lewis pairs via various in-situ characterizations. We further utilized them in photo-assist thermal and photothermal CO₂ hydrogenation towards the production of CO and methanol under atmospheric pressure. 

Transition metal-based materials (TM) are easily designed to adsorb and activate the small molecules in the catalytic process due to their coordinated ability of 3d-orbital electrons. Regulating the surface state and catalytic site to control the catalytic properties becomes more and more critical. How to understand the interface reconstruction phenomenon is the core issue for declaring coordinated reaction on the real catalytic site. Meanwhile, tuning the coordination environment induces or controls the surface reconstruction resulting in the unsaturated coordination site, which is benefit for photocatalytic CO₂ adsorption, activation and conversion. Through the construction of active site and the exploration of electron transport path, we have realized the controllable operation of activity and selectivity, which provides a solid scientific research foundation for the coordination catalysis research caused by the interface reconstruction effect. Therefore, the regulation of orbital spin state involved in coordination chemistry will provide deep insight for CO₂ catalysis.

In the past two decades, atomically dispersed metal catalysts have emerged as newly advanced materials for heterogeneous catalysis. However, the unsaturated metal center may easily aggregate or decompose to undesired big nanoparticles, resulting in a loss of catalytic activity and selectivity. Although strong metal-support interactions are proposed to control the aggregation of metal centers, the types of support and the activity of metal are limited. Recently, we have developed many types of surface isolated metal complexes on porous supports. For instance, the covalently bonded Pt, Co, and Fe complexes were selectively deposited on the surface of oxides via the surface self-limiting reaction, and perform a high activity, selectivity of CO, and stability in CO₂ hydrogenation. The single molecular metal complex or clusters were also isolated on the surface many types of supports by the molecular sieve liked films through the area selective atomic layer deposition for high selectivity in chiral catalysis.