Sulfur poisoning and regeneration are global challenges for metal catalysts even at the ppm level. The sulfur poisoning of single-metal-site catalysts and their regeneration is worthy of further study. Herein, sulfur poisoning and self-recovery are first presented on an industrialized single-Rh-site catalyst (Rh /POPs). A decreased turnover frequency of Rh /POPs from 4317 h to 318 h was observed in a 1000 ppm H S co-feed for ethylene hydroformylation, but it self-recovered to 4527 h after withdrawal of H S, whereas the rhodium nanoparticles demonstrated poor activity and self-recovery ability. H S reduced the charge density of the single Rh atom and lowered its Gibbs free energy with the formation of inactive (SH)Rh(CO)(PPh -frame) , which could be regenerated to active HRh(CO)(PPh -frame) after withdrawing H S. The mechanism and the sulfur-related structure-activity relationship were highlighted. This work provides an understanding of heterogeneous ethylene hydroformylation and sulfur-poisoned regeneration in the science of single-atom catalysts.
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