CoSe<sub>2</sub> supported single Pt site catalysts for hydrogen peroxide generation via two‐electron oxygen reduction
Xiaodong Zhu, Qian Zhang, Xiaoxuan Yang, Yingnan Wang, Jinting Wu, Jian Gao, Ji‐Jun Zou, Gang Wu, Yong‐Chao Zhang
Abstract
Abstract Electrocatalytic oxygen reduction reaction (ORR) to prepare H 2 O 2 in acidic medium has the advantages of green, safety, and portability, which shows broad development prospects. However, it still suffers from low catalyst activity, insufficient selectivity, and high cost. Herein, Pt 1 /CoSe 2 with ultralow 0.01 wt.% Pt atomic distribution was synthesized by a simple hydrothermal method. The Pt 1 /CoSe 2 with ultralow Pt content exhibits high activity, high selectivity, and long‐term stability for ORR to H 2 O 2 in O 2 ‐saturated 0.1 M HClO 4 . The onset potential is as low as 0.75 V versus reversible hydrogen electrode (RHE), H 2 O 2 selectivity is as high as 84% (0.4 V vs. RHE), and the electron transfer number is 2.3 (0.4 V vs. RHE). Moreover, the hydrogen peroxide yield using the flow cell testing is 110.02 mmol g cat. −1 h −1 with high Faradaic efficiency of 78% (0 V vs. RHE) at 0.1 M HClO 4 , and the catalyst did not deactivate significantly after 60 h stability testing. Mechanistic studies and in situ X‐ray photoelectron spectroscopy characterization confirm that the ultralow Pt content on CoSe 2 can effectively regulate the electronic structure of Co as the real active site around the Pt site, which gives a suitable ∆ dp value (the difference between the d‐band center of the active metal site and the p‐band center of the terminal oxygen in *OOH), provides an ideal *OOH binding energy, and inhibits the O–O bond breakage. This work successfully improves the intrinsic activity of the Co active sites around Pt in Pt 1 /CoSe 2 for acidic ORR to H 2 O 2 by constructing ultralow‐content Pt single atom.