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Single atom catalysts have been found to exhibit superior selectivity over nanoparticulate catalysts for catalytic reactions such as hydrogenation due to their single-site nature. However, improved selectively is often accompanied by loss of activity and slow kinetics. Here we demonstrate that neighboring Pd single atom catalysts retain the high selectivity merit of sparsely isolated single atom catalysts, while the cooperative interactions between neighboring atoms greatly enhance the activity for hydrogenation of carbon-halogen bonds. Experimental results and computational calculations suggest that neighboring Pd atoms work in synergy to lower the energy of key meta-stable reactions steps, i.e., initial water desorption and final hydrogenated product desorption. The placement of neighboring Pd atoms also contribute to nearly exclusive hydrogenation of carbon-chlorine bond without altering any other bonds in organohalogens. The promising hydrogenation performance achieved by neighboring single atoms sheds light on a new approach for manipulating the activity and selectivity of single atom catalysts that are increasingly studied in multiple applications. Single atom catalysts have exhibited high selectivity for hydrogenation, yet improved selectively is often accompanied by loss of activity. Here the authors report that synergistic interactions of neighboring Pd single atoms lead to both high activity and selectivity for hydrodehalogenation catalysis. [ABSTRACT FROM AUTHOR] more...

The demands for efficient and robust heterogeneous hydrogenation catalysts have triggered extensive research to optimize the structures of metal catalytic centers, but the potential of support construction for enhanced hydrogenation performance has been overlooked. This study introduces a hierarchically ordered porous poly(2,6‐diaminopyridine) (PDAP) as a Pd nanoparticle support for hydrogenation removal of recalcitrant pollutants in water purification. The PDAP support acts as a sorbent and microreactor to enhance the proximity of targeted water pollutants and reactive hydrogen atom species, achieving unprecedently high water purification efficiency. The PDAP support also acts as a catalyst in mediating peroxide‐activation for oxidative destruction of Pd poisons (e.g., reduced sulfur), achieving in situ regeneration of poisoned Pd catalysis centers. The high activity and in situ regenerativity achieved by rational construction of the support structure sheds light on a new approach for designing efficient and robust heterogeneous hydrogenation catalysts. [ABSTRACT FROM AUTHOR] more...

The PDAP support also acts as a catalyst in mediating peroxide-activation for oxidative destruction of Pd poisons. Keywords: hydrogenation; in situ regeneration; microreactors; support construction EN hydrogenation in situ regeneration microreactors support construction 1 1 1 05/28/21 20210526 NES 210526 In article number 2100971, Chiheng Chu and co-workers introduce hierarchically ordered porous poly(2,6-diaminopyridine) (PDAP) as a Pd nanoparticle support for hydrogenation removal of recalcitrant pollutants in water purification. Heterogeneous Hydrogenation Catalysts: Constructing the Support as a Microreactor and Regenerator for Highly Active and In Situ Regenerative Hydrogenation Catalyst (Adv. Funct. [Extracted from the article] more...