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Boosting CatalyticnPerformance of MOF-808(Zr) by DirectnGeneration of Rich Defective Zr Nodes via a Solvent-Free Approach 无溶剂法直接生成富缺陷Zr节点提高MOF-808（Zr）的催化性能

Figshare Pub Date : 2023-03-01 DOI: 10.1021/acs.inorgchem.2c04364.s001

Gan Ye (4479982), Lulu Wan (14701466), Qiuli Zhang (560871), Hu Liu (176964), Jun Zhou (6477), Lei Wu (202933), Xingye Zeng (4246105), Hanlu Wang (14701469), Xixi Chen (5749067), Jin Wang (29560)

{"title":"Boosting CatalyticnPerformance of MOF-808(Zr) by DirectnGeneration of Rich Defective Zr Nodes via a Solvent-Free Approach","authors":"Gan Ye (4479982), Lulu Wan (14701466), Qiuli Zhang (560871), Hu Liu (176964), Jun Zhou (6477), Lei Wu (202933), Xingye Zeng (4246105), Hanlu Wang (14701469), Xixi Chen (5749067), Jin Wang (29560)","doi":"10.1021/acs.inorgchem.2c04364.s001","DOIUrl":"https://doi.org/10.1021/acs.inorgchem.2c04364.s001","url":null,"abstract":"Creationnof rich open metal sites (defect) on the nodesnof metal–organicnframeworks (MOFs) is an efficient approach to enhance their catalyticnperformance in heterogeneous reactions; however, direct generationnof such defects remains challenging. In this contribution, we developednan in situ green route for rapid fabrication of defective MOF-808(Zr)nwith rich Zr-OH/OH2 sites (occupying 25% Zr coordinationnsites) and hierarchical porosity without the assistance of formicnacid and solvent. The optimal MOF-808(Zr) not only displayed superiornactivity in oxidative desulfurization (ODS) for removing 1000 ppmnsulfur at ambient temperature within 20 min but also could convertn3.8 mmol of benzaldehyde to (dimethoxymethyl)benzene within 90 s atn30 °C. The turnover frequencies reached 45.4 h–1 for ODS and 3451 h–1 for acetalization, outperformingnthe most reported MOF-based catalysts. Theoretical calculation andnexperimental results show that the formed Zr-OH/OH2 cannreact with H2O2 to generate peroxo-zirconiumnspecies, which readily oxidize the sulfur compound. Our work providesna new approach to the synthesis of defect-rich MOF-808(Zr) with thenaccessibility of active sites for target reactions.","PeriodicalId":522696,"journal":{"name":"Figshare","volume":"1 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147901909","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

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