High Yield Electrosynthesis of Hydrogen Peroxide from Water Using Electrospun CaSnO3@Carbon Fiber Membrane Catalysts with Abundant Oxygen Vacancy
High Yield Electrosynthesis of Hydrogen Peroxide from Water Using Electrospun CaSnO3@Carbon Fiber Membrane Catalysts with Abundant Oxygen Vacancy
复制标题
富氧空位电纺CaSnO3@碳纤维膜催化剂从水中高产率电合成过氧化氢
DOI：
10.1002/adfm.202100099
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发表时间：
2021
影响因子：
19
通讯作者：
Yu Chengzhong
中科院分区：
文献类型：
--
作者：
Zhang Chaoqi;Lu Ruihu;Liu Chao;Yuan Ling;Wang Jing;Zhao Yan;Yu Chengzhong
通过电化学双电子水氧化反应（2 e-WOR）生产过氧化氢（H2 O2）是一种很有前途的方法，其中高性能的电催化剂起着关键作用。本文报道了在具有丰富氧空位（OV）的导电碳纤维膜中合成纳米结构CaSnO 3作为新一代2 e-WOR电催化剂。CaSnO3 @碳纤维膜可直接用作自立电极，表现出创纪录的39.8 µmol cm− 2 min − 1的H2 O2生产速率和90%的选择性（在2.9 V时，相对于可逆氢电极）。CaSnO3 @碳纤维膜设计不仅提高了催化剂的导电性和稳定性，还提高了CaSnO 3的固有活性。密度泛函理论计算进一步表明，OVin增加了与竞争性四电子水氧化反应途径相关的氧中间体的吸附自由能，从而提高了2 e-WOR的活性和选择性。该研究结果为水制氢电催化剂的合理设计提供了新的思路。
Hydrogen peroxide (H2O2) production by electrochemical two‐electron water oxidation reaction (2e‐WOR) is a promising approach, where high‐performance electrocatalysts play critical roles. Here, the synthesis of nanostructured CaSnO3confined in conductive carbon fiber membrane with abundant oxygen vacancy (OV) as a new generation of 2e‐WOR electrocatalyst is reported. The CaSnO3@carbon fiber membrane can be directly used as a self‐standing electrode, exhibiting a record‐high H2O2production rate of 39.8 µmol cm−2min−1and a selectivity of ≈90% (at 2.9 V vs reversible hydrogen electrode). The CaSnO3@carbon fiber membrane design improves not only the electrical conductivity and stability of catalysts but also the inherent activity of CaSnO3. Density functional theory calculation further indicates the crucial role of OVin increasing the adsorption free energy toward oxygen intermediates associated with the competitive four‐electron water oxidation reaction pathway, thus enhancing the activity and selectivity of 2e‐WOR. The findings pave a new avenue to the rational design of electrocatalysts for H2O2production from water.