Electrochemical synthesis of hydrogen peroxide (H₂O₂) through 2e^– oxygen reduction reaction is an effective approach to replace anthraquinone process. However, most reported electrocatalysts work effectively in alkaline medium in which H₂O₂ will easily decompose into water. It is still of great challenge to develop cost-effective electrocatalysts with high activity and selectivity for electrocatalytic H₂O₂ production in acidic media. Herein, it is first theoretically demonstrated that the adsorption energy of OOH* intermediate on carbon can be optimized by embedding Co nanoparticles (Co NPs) and tuning oxygen-containing functional groups, ensuring high activity and selectivity. Guided by density functional theory calculations, highly porous open carbon nanocages with embedded Co NPs are designed and synthesized by template-engaged method. The pyrolysis temperature can effectively modulate the electronic and pore structure of carbon nanocages. Impressively, the optimized carbon nanocages synthesized at 700 °C (P-Co@C-700) with highest percentage of –C–O–C group and defects, largest specific surface area (1351 m² g^–1), and mesoporous structure exhibit high selectivity up to 94% toward H₂O₂ production in 0.1 m HClO₄. Furthermore, the P-Co@C-700 nanocages display promising application for efficient electro-Fenton degradation of model organic pollutant.

中文翻译：

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开放式碳纳米笼中的协同电子和孔结构调制能够在酸性介质中高效电催化生产 H2O2

通过2e-氧还原反应电化学合成过氧化氢（H ₂ O ₂ ^）是替代蒽醌法的有效途径。然而，大多数报道的电催化剂在H ₂ O ₂容易分解成水的碱性介质中有效工作。_{开发具有高活性和高选择性的电催化H 2} O ₂的高性价比电催化剂仍然是一个巨大的挑战在酸性介质中生产。在此，首先从理论上证明，OOH* 中间体在碳上的吸附能可以通过嵌入 Co 纳米粒子 (Co NPs) 和调整含氧官能团来优化，从而确保高活性和选择性。以密度泛函理论计算为指导，采用模板接合法设计并合成了嵌入Co NPs的高孔开放碳纳米笼。热解温度可以有效地调节碳纳米笼的电子和孔结构。令人印象深刻的是，在 700 °C 下合成的优化碳纳米笼 (P-Co@C-700) 具有最高百分比的 –C–O–C 基团和缺陷、最大的比表面积 (1351 m ²  g ^–1 ) 和介孔结构对 H 表现出高达 94% 的高选择性在 0.1  m HClO _4中产生2 O ₂。此外，P-Co@C-700 纳米笼在高效电芬顿降解模型有机污染物方面具有广阔的应用前景。