Electrochemical Hydrogen Peroxide Production from Molecular Oxygen on Nitrogen-Doped Mesoporous Carbon Catalysts
Electrochemical Hydrogen Peroxide Production from Molecular Oxygen on Nitrogen-Doped Mesoporous Carbon Catalysts
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发表时间：
2018
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通讯作者：
Yanyan Sun;I. Sinev;W. Ju;A. Bergmann;Sören Dresp;S. Kühl;C. Spöri;Henrike Schmies;Huan Wang
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作者：
Yanyan Sun;I. Sinev;W. Ju;A. Bergmann;Sören Dresp;S. Kühl;C. Spöri;Henrike Schmies;Huan Wang
双电子氧还原电化学法生产过氧化氢(H_2O_2)是一种很有前途的替代已有工业生产工艺的方法。目前的挑战涉及寻找具有高电催化活性、稳定性和产物选择性的低成本电催化剂。在这里，我们探索了一些不同的氮掺杂介孔碳催化剂对H_2O_2产生的电催化活性和选择性，并报道了在酸性溶液中∼95−98%以前没有达到的H_2O_2选择性。为了解释我们的观察，我们将它们的结构、组成和其他物理化学性质与其电催化性能相关联，并发现过氧化氢产物的产率与比表面积和界面Zeta电位之间存在密切的关联。氮掺杂显著提高了过氧化氢的活性和选择性。计时安培过氧化氢电解证实了最佳的掺氮CMK-3样品在酸性、中性和碱性溶液中具有极高的过氧化氢产生率和巨大的过氧化氢法拉第选择性。在碱性条件下，催化H_2O_2产率进一步提高，其中H_2O_2-−阴离子的生成速率高达561.7 mmolg催化剂−1 h−-1，H_2O_2法拉第选择性大于70%。我们的工作为先进的碳基电催化剂的设计、合成和机理研究提供了指导。
Electrochemical hydrogen peroxide (H2O2) production by two-electron oxygen reduction is a promising alternative process to the established industrial anthraquinone process. Current challenges relate to finding cost-effective electrocatalysts with high electrocatalytic activity, stability, and product selectivity. Here, we explore the electrocatalytic activity and selectivity toward H2O2 production of a number of distinct nitrogen-doped mesoporous carbon catalysts and report a previously unachieved H2O2 selectivity of ∼95−98% in acidic solution. To explain our observations, we correlate their structural, compositional, and other physicochemical properties with their electrocatalytic performance and uncover a close correlation between the H2O2 product yield and the surface area and interfacial zeta potential. Nitrogen doping was found to sharply boost H2O2 activity and selectivity. Chronoamperometric H2O2 electrolysis confirms the exceptionally high H2O2 production rate and large H2O2 faradaic selectivity for the optimal nitrogen-doped CMK-3 sample in acidic, neutral, and alkaline solutions. In alkaline solution, the catalytic H2O2 yield increases further, where the production rate of the HO2 − anion reaches a value as high as 561.7 mmol gcatalyst −1 h−1 with H2O2 faradaic selectivity above 70%. Our work provides a guide for the design, synthesis, and mechanistic investigation of advanced carbon-based electrocatalysts for H2O2 production.