MICROSCOPIE+CATREN:ING+TLN:PAF:FMO:JRO:MAO:LPIInternational audienceStimulated by recent advances in scanning transmission electron microscopy (STEM), single-atom catalysts (SACs) have become prominent materials in heterogeneous catalysis [1]. In spite of the numerous reports on promising catalytic performance and noble-metal saving, single-atom stabilization remains a challenge – in particular for noble metals on oxides [2,3]. In addition, single atoms are not necessarily more efficient than their cluster or nanoparticle counterparts [3,4]. In this communication, the previous issues will be illustrated for two prototypical catalytic systems: CO oxidation on Pt/Al2O3 and photocatalytic hydrogen evolution reaction over Pt/TiO2. The combined use of catalytic testing, STEM, operando X-ray and infrared absorption spectroscopies, and DFT calculations, reveals the influence of the reactive environment on Pt nuclearity and oxidation state (generally clustering and reduction), which in turn correlates to changes in catalytic activity [5–8]. From this knowledge, strategies can be suggested to stabilize the metals in an ultradispersed state. [1]R. Lang, X. Du, Y. Huang, X. Jiang, Q. Zhang, Y. Guo, K. Liu, B. Qiao, A. Wang, T. Zhang, Chem. Rev. 120 (2020) 11986[2]L. Piccolo, Catal. Today 373 (2021) 80[3] L. Liu, D.M. Meira, R. Arenal, P. Concepcion, A.V. Puga, A. Corma, ACS Catal. 9 (2019) 10626[4]A. Beniya, S. Higashi, Nat. Catal. 2 (2019) 590[5]C. Dessal, A. Sangnier, C. Chizallet, C. Dujardin, F. Morfin, J.-L. Rousset, M. Aouine, M. Bugnet, P. Afanasiev, L. Piccolo, Nanoscale 11 (2019) 6897[6]C. Dessal, T. Len, F. Morfin, J.-L. Rousset, M. Aouine, P. Afanasiev, L. Piccolo, ACS Catal. 9 (2019) 5752[7]C. Dessal, L. Martínez, C. Maheu, T. Len, F. Morfin, J.-L. Rousset, E. Puzenat, P. Afanasiev, M. Aouine, L. Soler, J. Llorca, L. Piccolo, J. Catal. 375 (2019) 155[8]L. Piccolo, P. Afanasiev, F. Morfin, T. Len, C. Dessal, J.L. Rousset, M. Aouine, F. Bourgain, A. Aguilar-Tapia, O. Proux, Y. Chen, L. Soler, J. Llorca, ACS Catal. 10 (2020) 1269