Regulating N Species in N-Doped Carbon Electro-Catalysts for High-Efficiency Synthesis of Hydrogen Peroxide in Simulated Seawater

通过调控氮掺杂碳电催化剂中的氮物种,实现模拟海水中过氧化氢的高效合成

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Abstract

Electrochemical oxygen reduction reaction (ORR) is an attractive and alternative route for the on-site production of hydrogen peroxide (H(2) O(2) ). The electrochemical synthesis of H(2) O(2) in neutral electrolyte is in early studying stage and promising in ocean-energy application. Herein, N-doped carbon materials (N-C(x) ) with different N types are prepared through the pyrolysis of zeolitic imidazolate frameworks. The N-C(x) catalysts, especially N-C(800) , exhibit an attracting 2e(-) ORR catalytic activity, corresponding to a high H(2) O(2) selectivity (≈95%) and preferable stability in 0.5 m NaCl solution. Additionally, the N-C(800) possesses an attractive H(2) O(2) production amount up to 631.2 mmol g(-1)  h(-1) and high Faraday efficiency (79.8%) in H-type cell. The remarkable 2e(-) ORR electrocatalytic performance of N-C(x) catalysts is associated with the N species and N content in the materials. Density functional theory calculations suggest carbon atoms adjacent to graphitic N are the main catalytic sites and exhibit a smaller activation energy, which are more responsible than those in pyridinic N and pyrrolic N doped carbon materials. Furthermore, the N-C(800) catalyst demonstrates an effective antibacterial performance for marine bacteria in simulated seawater. This work provides a new insight for electro-generation of H(2) O(2) in neutral electrolyte and triggers a great promise in ocean-energy application.

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