The bimetallic Re-Pd catalysts for perchlorate reduction have evolved from the original ReOx-Pd/C to the 100-fold more active Re(hoz)2-Pd/C, demonstrating the power of tuning active site coordination chemistry with multifunctional catalyst structures. However, the immobilized Re(hoz)2 coordination structure is susceptible to decomposition when treating concentrated perchlorate solutions (e.g., 10 mM). After elucidating the decomposition mechanisms and screening different hydrogenation metals, we hybridized different metals with Re(hoz)2 to suppress complex decomposition and Re leaching. Alternatively, we tuned the coordination structure of the Re complex and discovered new candidates exhibiting higher stability than Re(hoz)2 when immobilized in Pd/C. The final combination of these new coordination complexes and new hydrogenation metal nanoparticles yielded a catalyst exhibiting excellent reactivity and negligible decomposition when treating concentrated perchlorate.

Evolution of heterogeneous catalysts for oxyanion reduction: Improved sustainability of biomimetic materials with rational design

251st National Meeting (2016)

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