Halloysite nanotube@N-doped carbon electrocatalysts for highly efficient hydrogen peroxide cathode fuel electrosynthesis

•The HNTs@NC is fabricated by combining hydrothermal treatment and calcination.•The H2O2 selectivity of HNTs@NC is up to 93.3% due to the introduction of HNTs.•Degradation experiment verifies the H2O2 electrosynthesis ability of HNTs@NC.•The formation of Si-C and Si-N bonds of HNTs@NC promote long-term stability. Hydrogen peroxide (H2O2) fuel cells represent one type of promising energy conversion device to realize the application in airtight environments with replacing oxygen or air by high mass power density of liquid H2O2 as cathode fuel. However, H2O2 electrosynthesis as an efficient, green and economical technology is largely plagued by lacking catalyst owning high catalytic activity and selectivity simultaneously. Although nitrogen-doped carbon (NC) is considered as potential candidate for H2O2 electrosynthesis through two-electron oxygen reduction reaction (2e− ORR), it is still far away from commercial application. Herein, a regulation strategy is proposed, in which charged halloysite nanotubes (HNTs) are served as cores and with NC as shells, denoting as HNTs@NC. The introduction of HNTs can induce excessive electron accumulation in NC, promoting the adsorption of oxygen and intermediate species (OOH*) on HNTs@NC catalyst, inhibiting OOH* reaction, and thus improve the catalytic activity and H2O2 selectivity. Electrochemical degradation experiment using methyl blue (MB) and Rhodamine B (RhB) as representative simulated dyes further verify the H2O2 electrosynthesis ability of HNTs@NC catalyst. At the same time, the formation of Si-N and Si-C bonds between HNTs and NC also ensure the high stability in long-term application. This work proposes a novel strategy in designing H2O2 electrosynthesis catalyst by constructing core–shell structure to satisfy the development requirements of H2O2 fuel cells.