Ambient‐Pressure Polyolefin Upcycling With Earth‐Abundant Catalyst

ABSTRACT Polyolefin hydrogenolysis offers a promising route for the upcycling of plastic waste, yet is hindered by the high cost of noble‐metal catalysts and the safety concerns of high‐pressure H 2 . Current systems typically rely on Ru or Pt catalysts to mediate key elementary steps, including H 2 dissociation and C─C bond cleavage. However, achieving comparable performance with earth‐abundant metals under near‐ambient hydrogen pressure remains a significant challenge. Here, we present an elementary reaction kinetic matching strategy to enable efficient hydrogenolysis over a non‐noble metal catalyst. By tuning the electronic structure of Ni, the kinetics of H 2 activation, C─C bond cleavage, and hydrogenation are balanced, facilitating the rapid removal of CH x * intermediates and sustaining the dynamic exposure of catalytic active sites. As a result, the Ni‐based catalyst exhibited superior hydrogenolysis activity and selectivity toward waste polyolefins under low pressure, even at atmospheric pressure, surpassing the benchmark Ru and Pt catalysts. This study overturns the traditional perception of low efficiency in non‐noble metal‐catalyzed hydrogenolysis and provides new design principles for efficient catalysis under mild conditions.