Synergism of Ultrasmall Pt Clusters and Basic La2O2CO3 Supports Boosts the Reverse Water Gas Reaction Efficiency. Issue 12 (20th January 2023) - Zhang, Rui
Abstract: The reverse water‐gas shift reaction (RWGS) has been regarded as a promising approach for fighting climate change caused by the excessive emission of the greenhouse gas CO2, but it still suffers from relatively poor low‐temperature reactivity. Herein, a high‐performance RWGS catalyst composed of ultrasmall Pt clusters (1.38 nm on average) anchored by La2 O2 CO3 support (PtNC /LOC), which possesses a record CO production rate of 2678 molCO molPt −1 h −1 with nearly 100% CO selectivity at 300 °C, is reported. The specific activity is nearly 1.5 and 7.9 fold higher than that of Pt single atoms and nanoparticles on La2 O2 CO3, respectively. More importantly, over 87.7% of the initial activity of PtNC /LOC remains after 80 h constant operation at 380 °C, firmly verifying the structural robustness. LOC support is essential, because of not only the moderate basicity that can boost the reaction efficiency but also the strong interaction with Pt species that can stabilize the ultrasmall particle size. Further investigations also point out the key role of the Pt clusters. The two key steps, CO2 adsorption, and CO desorption, individually prefer electron‐rich and electron‐deficient Pt species. Ultrasmall Pt clusters successfully integrate the unique surface states of single atoms and nanoparticles, thus achieving excellent low‐temperature RWGS performance. Abstract : A series of La2 O2 CO3 ‐based catalysts are developed and used as advanced catalysts for the reverse water‐gas shift reaction. Compared with their single atom and nanoparticle counterparts, the La2 O2 CO3 ‐supported Pt clusters achieve a better balance between CO2 adsorption and CO desorption, thus leading to an accelerated reaction rate.