DOE OSTI · 3367235
Controlling Exsolution Dynamics in High‐Entropy Oxides for Highly Active and Selective Acetylene Semi‐Hydrogenation
Abstract
Exsolution-derived catalysts feature robust metal–support interactions that enhance catalytic performance; yet achieving precise control over exsolution dynamics in multicomponent oxides remains challenging. In this study, we demonstrate that exsolution behavior in high-entropy oxides (HEOs) can be rationally tuned through coupled lattice- and valence-engineering to create a highly active and selective catalyst for acetylene semi-hydrogenation. Incorporation of Li + into a rock salt-structured HEO (LiNiMgCuZnCoO x and LiHEO) induces local lattice distortion, generates oxygen vacancies, and partially oxidizes Co sites from Co 2+ to Co 3+ , collectively modulating local charge redistribution. This strategy enables facilitated Cu nanoparticle exsolution and alters the exsolution sequence from Cu 0 > Ni 0 > Co 0 in pristine HEO to Cu 0 > Co 0 > Ni 0 in the LiHEO. The resulting catalyst via controlled exsolution exhibits superior activity and ethylene selectivity, outperforming state-of-the-art transition metal systems. This work establishes entropy-enabled lattice and valence engineering as a facile route to programmable exsolution for enhanced catalysis.
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Yu, Hailing [Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division], Wang, Caiqi [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division] (ORCID:0000000198849990), Siniard, Kevin M. [Univ. of Tennessee, Knoxville, TN (United States)], Wang, Qingju [Univ. of Tennessee, Knoxville, TN (United States)], Zhang, Yuanpeng [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division] (ORCID:0000000342243361), Boscoboinik, J. Anibal [Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)] (ORCID:0000000250907079), Tong, Xiao [Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)] (ORCID:0000000255679677), Gomez, Eliseo Perez [Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)], Yuan, Shuai [Vanderbilt Univ., Nashville, TN (United States)], Asundi, Arun S. [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)], Mueller, Oliver [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)], Martins, Murillo Longo [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division], Cheng, Yongqiang [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division], Koehler, Michael Richard [Univ. of Tennessee, Knoxville, TN (United States)], Jiang, De‐en [Vanderbilt Univ., Nashville, TN (United States)] (ORCID:0000000151670731), Wu, Zili [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division] (ORCID:0000000244683240), Yang, Zhenzhen [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division] (ORCID:0000000202334747), Dai, Sheng [Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division] (ORCID:0000000280463931). 2026-05-15. Controlling Exsolution Dynamics in High‐Entropy Oxides for Highly Active and Selective Acetylene Semi‐Hydrogenation. https://doi.org/10.1002/anie.9920205
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