It remains great challenge to develop precious‐metal‐free electrocatalysts to implement high‐activity electrochemical conversion of O2 into value‐added hydroperoxide species (HO2−), which are vulnerable when exposed to various transition‐metal‐based catalysts. A strategy based on steric hindrance and layered nickel‐based layered double hydroxide (Ni‐LDH) induction has been developed for one‐pot inlaying high‐density ultrathin 2 D Ni‐LDH chips on in situ‐grown carbon nanosheets (Ni‐LDH C/CNSs). The resulting material exhibits high electrocatalytic selectivity with a faradaic efficiency up to 95 % for oxygen reduction into peroxide and attains a fairly high mass activity of approximately 22.2 A g−1, outperforming most metal‐based catalysts reported previously. Systematic studies demonstrate that the greatly increased defect concentration at Ni edge sites of Ni‐LDH chips results in more active sites, which contributes a favorable thermodynamically neutral adsorption of OOH* and adsorbed H2O2 molecules relatively weakly. Additionally, the modified CNSs effectively suppress H2O2 decomposition and avoid O−O bond cleavage to produce H2O by steric effects. The synergistic effect of CNSs and Ni‐LDH chips therefore leads to high activity and high selectivity in a two‐electron pathway. A proof‐of‐concept zinc–air fuel cell is proposed and set up to demonstrate the feasibility of green synthesis of peroxide, generating an impressive H2O2 production rate of 5239.67 mmol h−1 gcat.−1.
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Huang et al. (2019) studied this question.