the most promising routes of the artificial carbon cycle, has aroused widespread concern and paves a new way to sustainably produce fuels and fine chemicals, but a validated process is still lacking both conceptually and practically. [1a] As the most fundamental route of CO 2 hydrogenation, the reverse-water gas shift (RWGS) reaction offers a chance to overcome the challenges. [2] Despite the catalytic process being no longer mysterious, the specific reaction rate achieved currently is still far from the thermodynamic equilibrium, possibly owing to the difficulties in manipulating the surface state the of catalyst to simultaneously meet all the requirements of distinct steps involved. [3] The size of metal centers plays an essential role. [4] Conventional RWGS catalysts embedded with metal nanoparticles (NP) are favorable to the activation of CO 2 / H 2 reactants, contributing to an accelerated conversion rate, but it might also cause the problem of CO desorption, thus leading to over-hydrogenation. [5] In contrast, when scaling into a single atom (SA), besides the maximized metal utilization efficiency, the metal centers are commonly ionized, which can greatly weaken the adsorption strength of CO. [4a,c] However, single-atom metals without forming a complete crystal possess a poorer capacity of hydrogen dissociation compared with the nanoscale counterparts, which is unfavorable to activity. [6] That is because the active hydrogen species can not only directly involve in the catalysis, but also be responsible for creating oxygen vacancies (O V ) by reacting with the lattice oxygen of support, which is of great significance in CO 2 adsorption. [7] Therefore, it is eager to discover a new strategy for tailoring the surface state of catalysts aiming at achieving a better balance between CO 2 adsorption and CO desorption.Besides metal centers, the supports also give a considerable impact on RWGS performance. [8] Previous reports pointed out that basic oxides are favorable to CO 2 adsorption and metal dispersion compared with acidic and neutral oxides. [9] As a typical example, Nomura et al. demonstrated that a small amount of K 2 O can effectively improve the CO 2 conversion rate by accelerating CO 2 adsorption. [9c] However, the basicity of the catalyst cannot be too strong. Muroyama et al. revealed that Ni/ Y 2 O 3 exhibits more powerful capability in CO 2 to CH 4 conversion compared with Ni/La 2 O 3 . [10] That is because the key 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 CO 2 , 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 La 2 O 2 CO 3 support (Pt NC /LOC), which possesses a record CO production rate of 2678 mol CO mol Pt −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 tha...
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