电合成
催化作用
杂原子
电化学
共价键
电催化剂
金属
共价有机骨架
选择性
材料科学
金属有机骨架
解吸
无机化学
化学
电极
物理化学
有机化学
吸附
冶金
戒指(化学)
作者
Minghao Liu,Shuai Yang,Sijia Liu,Qiyang Miao,Xiubei Yang,Xuewen Li,Qing Xu,Gaofeng Zeng
出处
期刊:Small
[Wiley]
日期:2022-11-01
卷期号:18 (50): e2204757-e2204757
被引量:45
标识
DOI:10.1002/smll.202204757
摘要
Abstract Electrosynthesis of H 2 O 2 is a promising alternative to the anthraquinone oxidation process because of its low energy utilization and cost‐effectiveness. Heteroatom‐doped carbons‐based catalysts have been widely developed for H 2 O 2 synthesis. However, their doping degree, defective degree, and location of active sites are difficult to be preciously controlled at molecular level. Herein, a dioxin‐linked covalent organic framework (COF) is used as the template to preciously construct different metal‐N 2 sites along the porous walls for H 2 O 2 synthesis. By tuning the metal centers, the catalyst with Ca‐N 2 sites enables to catalyze H 2 O 2 production with selectivity over 95% from 0.2 to 0.6 V versus RHE, while the H 2 O 2 yields for Co sites or Ni sites are 20% and 60% in the same potential range. In addition, the turnover frequency (TOF) values for Ca‐N 2 sites are 11.63 e –1 site –1 s –1 , which are 58 and 20 times higher than those of Co and Ni sites (0.20 and 0.57 e –1 site –1 s –1 ). The theoretical calculations further reveal that the OOH* desorption on Ca sites is easier than those on Co or Ni sites, and thus catalyzes the oxygen reduction reaction in the 2e – pathway with high efficiency.
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