镍
光催化
金属有机骨架
催化作用
过氧化氢
水溶液
连接器
光化学
分解
制氢
材料科学
分解水
化学
有机化学
吸附
计算机科学
操作系统
作者
Yoshifumi Kondo,Kôtarô Honda,Yasutaka Kuwahara,Kohsuke Mori,Hisayoshi Kobayashi,Hiromi Yamashita
出处
期刊:ACS Catalysis
日期:2022-11-22
卷期号:12 (24): 14825-14835
被引量:24
标识
DOI:10.1021/acscatal.2c04940
摘要
Metal–organic frameworks (MOFs) are one of the most promising candidates for photocatalytic hydrogen peroxide (H2O2) production from dioxygen (O2) and water. However, MOF-driven H2O2 production from O2 and water remains a challenge because MOF photocatalysts need to exhibit high structural stability in aqueous reaction systems while suppressing H2O2 decomposition. In the present study, we demonstrate that a Hf-based UiO-66-NH2 with missing-linker defects and Ni single atoms dramatically promotes the photocatalytic production of H2O2 from O2 and water under visible-light (λ > 420 nm) irradiation. The acetate-capped missing-linker defects lead to suppression of the nonradiative relaxation of organic linkers and to the prevention of H2O2 decomposition, whereas the Ni single-atom cocatalysts promote the separation of photogenerated charges and selective two-electron oxidation of water to generate H2O2. The synergetic effect of missing-linker defects and Ni single atoms dramatically improves photocatalytic H2O2 production, resulting in a 6.3-fold increase in activity compared with that of pristine Hf-UiO-66-NH2. This study provides not only new insights into defect engineering in MOF photocatalysts but also an important strategy for achieving highly selective H2O2 production via O2 reduction and water oxidation.
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