Visible Light-Switchable Lattice Oxygen Sites for Selective C-H and C(O)-C Bond Electrooxidation
文献类型：期刊论文
| 作者 | Wang, Keping2; Huang, Jinshu2; Hu, Jinguang1; Wu, Mei2; Liao, Yuhe3; Yang, Song2; Li, Hu2 |
| 刊名 | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
 |
| 出版日期 | 2024-12-02 |
| 卷号 | 63期号:49页码:11 |
| 关键词 | Biomass conversion C(O)-C bond cleavage electrocatalytic oxidation lattice-oxygen selectivity control |
| ISSN号 | 1433-7851 |
| DOI | 10.1002/anie.202410555 |
| 通讯作者 | Hu, Jinguang(jinguang.hu@ucalgary.ca) ; Yang, Song(jhzx.msm@gmail.com) ; Li, Hu(hli13@gzu.edu.cn) |
| 英文摘要 | Lattice-oxygen is highly oxidizable, ideal for electrocatalytic C-H oxidation but insufficient alone for C(O)-C bond cleavage due to the non-removable nature of lattice sites. Here, we present a visible light-assisted electrochemical method of in situ formulating removable lattice-oxygen sites in a nickel-oxyhydroxide (ESE-NiOOH) electrocatalyst. This catalyst efficiently converts aromatic alcohols and carbonyls with C(O)-C fragments from lignin and plastics into benzoic acids (BAs) with high yields (83-99 %). Without light irradiation, ESE-NiOOH's intrinsic lattice-oxygen is non-removable and inert for C(O)-C bond cleavage. In situ characterizations show light-induced lattice-oxygen removal and regeneration via OH- refilling. Theoretical calculations identify the nucleophilic oxygen attack on ketone-derived carbanion as a rate-determining step, which can be remarkably facilitated by removable lattice-oxygen to activate alpha-C-H bonds. As a proof-of-concept, an "electrochemical funnel" strategy is developed for high-efficiency upgrading aromatic mixtures with C(O)-C moieties into BA with up to 94 % yield. This in situ removal-regeneration approach for lattice sites opens an avenue for the tailored design of interfacial electrocatalysts to selectively upcycle waste carbon sources into valuable products. |
| WOS关键词 | H-2 PRODUCTION ; OXIDATION ; EFFICIENT ; BIOMASS ; ACID ; VALORIZATION ; EVOLUTION ; CLEAVAGE ; ALCOHOLS ; CARBON |
| 资助项目 | National Natural Science Foundation of China ; Guizhou Provincial ST Project (GCC)[[2023]011] ; Guizhou Provincial ST Project (GCC)[ZK[2022]011] ; [22368014] ; [22478087] |
| WOS研究方向 | Chemistry |
| 语种 | 英语 |
| WOS记录号 | WOS:001357258400001 |
| 出版者 | WILEY-V C H VERLAG GMBH |
| 资助机构 | National Natural Science Foundation of China ; Guizhou Provincial ST Project (GCC) |
| 源URL | [http://ir.giec.ac.cn/handle/344007/43599]  |
| 专题 | 中国科学院广州能源研究所 |
| 通讯作者 | Hu, Jinguang; Yang, Song; Li, Hu |
| 作者单位 | 1.Univ Calgary, Dept Chem & Petr Engn, 2500 Univ Dr NW, Calgary, AB T2N 1N4, Canada 2.Guizhou Univ, Ctr R&D Fine Chem, State Key Lab Green Pesticide, Key Lab Green Pesticide & Agr Bioengn,Minist Educ, Guiyang 550025, Peoples R China 3.Chinese Acad Sci, Guangzhou Inst Energy Convers, Guangzhou 510640, Guangdong, Peoples R China |
| 推荐引用方式 GB/T 7714 | Wang, Keping,Huang, Jinshu,Hu, Jinguang,et al. Visible Light-Switchable Lattice Oxygen Sites for Selective C-H and C(O)-C Bond Electrooxidation[J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2024,63(49):11. |
| APA | Wang, Keping.,Huang, Jinshu.,Hu, Jinguang.,Wu, Mei.,Liao, Yuhe.,...&Li, Hu.(2024).Visible Light-Switchable Lattice Oxygen Sites for Selective C-H and C(O)-C Bond Electrooxidation.ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,63(49),11. |
| MLA | Wang, Keping,et al."Visible Light-Switchable Lattice Oxygen Sites for Selective C-H and C(O)-C Bond Electrooxidation".ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 63.49(2024):11. |
入库方式： OAI收割
来源：广州能源研究所
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