Strain plays an important role in the catalytic mechanisms, especially in the transition state where catalyst and substrate interact. In biological systems, Strain Release Theory is a fundamental theory used to describe enzyme catalysis, where the enzymes or substrates undergo strain or distortion during the catalytic process to facilitate product generation. For heterogeneous catalysis, lattice strain, such as compression and tension, may be introduced into different catalysts to improve their catalytic performance. The two chief strategies to induce strain in heterogeneous catalysts are metal alloying, where heterometals are doped into the metal matrix to change lattice strength, and catalyst/substrate lattice mismatch, where substrate deformation is induced to modify the supported catalyst's lattice. Here we use the vapor-phase infiltration to create a metal active center that further demonstrated to be strained. The hybrid MOFs demonstrates superior CO<sub>2</sub> reduction reactivity compared with the same metal center created by the solution-phase synthesis (four times better conversion efficiency at -1.2 V and 200 mV reduced onset potential). This catalytic improvement is attributed to better interactions between the MOFs and the gas phase formed clusters. This gas phase infiltration method for synthesizing the metal active center is quite general and expected to have great potentials to create other metal active centers.<br/>

Metal-ligand catalytic site distortion induced by internal strain through vapor-phase infiltration

2019 Fall National Meeting

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