Issue 10, 2023

Single-iron, cobalt, nickel, and copper-atom catalysts for the selective reduction of oxygen to H2O2

Abstract

The pursuit of hydrogen peroxide (H2O2) production via two-electron electrochemical oxygen reduction reaction (ORR) is hampered by the lack of high-performance electrocatalysts. In this work, a series of single metal (i.e., Fe, Co, Ni, and Cu) atom catalysts anchored into N-doped carbon nanosheets (NCNSs) are evaluated for H2O2 production at pH-universal electrolytes. The catalytic performance of the samples, including current density, H2O2 selectivity, turnover of frequency (TOF), and faradaic efficiency, are characterized by electrochemical measurements. The generation of H2O2 is monitored by a UV-vis spectrophotometer. Among the samples, Cu/NCNSs exhibits the best catalytic performance with a ring current density of 2.15 mA cm−2, TOF of 15.8 s−1 at 0.1 V vs. reversible hydrogen electrode, Tafel slope of 88 mV dec−1, and H2O2 selectivity of 100% at 0.57 V in alkaline media. Importantly, the Cu/NCNSs yields H2O2 selectivity of 81% at 0.05 V in acidic electrolytes. In contrast, Cu nanoparticles possess an inferior current density and much lower H2O2 selectivity via the 4e ORR pathway. Further quantitative analysis of H2O2 demonstrates that the Cu/NCNSs catalyst has an H2O2 production rate of 5.1 mol gcatalyst−1 L−1 h−1 in alkaline media at 0.4 V, which is larger than those in acidic media (3.2 mol gcatalyst−1 L−1 h−1) and neutral media (2.2 mol gcatalyst−1 L−1 h−1) at −0.2 V. Such performance of Cu/NCNSs renders it as one of the best catalysts for H2O2 production.

Graphical abstract: Single-iron, cobalt, nickel, and copper-atom catalysts for the selective reduction of oxygen to H2O2

Supplementary files

Article information

Article type
Paper
Submitted
04 mar 2023
Accepted
24 apr 2023
First published
26 apr 2023

Green Chem., 2023,25, 3931-3939

Single-iron, cobalt, nickel, and copper-atom catalysts for the selective reduction of oxygen to H2O2

C. Ye, Y. Zhou, H. Li and Y. Shen, Green Chem., 2023, 25, 3931 DOI: 10.1039/D3GC00737E

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