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Controlled Assembly of Ru-Containing Polyoxometalates for Photocatalytic Activity of the Primary Amine Coupling Reaction
Inorganic Chemistry ( IF 4.6 ) Pub Date : 2022-06-16 , DOI: 10.1021/acs.inorgchem.2c00718 Huafeng Li 1 , Wenjing Chen 1 , Zelong Yuan 1 , Yuzhen Jin 1 , Yujie Zhao 1 , Pengtao Ma 1 , Jingyang Niu 1 , Jingping Wang 1
Inorganic Chemistry ( IF 4.6 ) Pub Date : 2022-06-16 , DOI: 10.1021/acs.inorgchem.2c00718 Huafeng Li 1 , Wenjing Chen 1 , Zelong Yuan 1 , Yuzhen Jin 1 , Yujie Zhao 1 , Pengtao Ma 1 , Jingyang Niu 1 , Jingping Wang 1
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Three Ru-induced structural interconversion polyoxometalates (POMs), Na13H5[Ru4(H2O)2(Cl)2(WO2)4(AsW9O33)4]·43H2O (1), K5Na9H8[Ru2(WO2)4(AsW9O33)4]·50H2O (2), and KNa13H14[(WO2)4(AsW9O33)4]·34H2O (3), were successfully synthesized and thoroughly characterized. Interconversion of structures was accomplished by changing the number of active sites for compounds 1–3. All three compounds contain one {As4W40O140} unit, showing similar structural characteristics except for the active center number (Ru). Interestingly, compound 1 [turnover number (TON)= 486; turnover frequency (TOF)= 20 h–1] showed highly efficient photocatalysis in achieving oxidative coupling of primary amines. Compound 2 (TON = 406, TOF = 17 h–1) was also found to promote the oxidative coupling with relatively poor efficiency; however, compound 3 (TON = 178; TOF = 7.4 h–1) had no obvious contribution to the coupling reaction system, and a chain of evidence indicates that the catalytic performances are strongly dependent on element contents of active sites. Furthermore, the Ru-containing POM-based photocatalysts are conveniently recyclable and reusable during the photocatalytic processes. This study demonstrates the possibility of tuning the catalytic efficiency and stability of POM-based photocatalysts by well designing and controlling their structures. The possible reaction mechanism for the photocatalysis synthesis of imine product is also proposed based on experimental studies.
中文翻译：
含钌多金属氧酸盐的可控组装用于伯胺偶联反应的光催化活性
三种Ru诱导的结构互变多金属氧酸盐（POM），Na 13 H 5 [Ru 4 (H 2 O) 2 (Cl) 2 (WO 2 ) 4 (AsW 9 O 33 ) 4 ]·43H 2 O ( 1 ), K 5 Na 9 H 8 [Ru 2 (WO 2 ) 4 (AsW 9 O 33 ) 4 ]·50H 2 O ( 2 )、KNa 13 H 14[(WO 2 ) 4 (AsW 9 O 33 ) 4 ]·34H 2 O ( 3 )成功合成并进行了全面表征。通过改变化合物1-3的活性位点的数量来实现结构的相互转换。所有三种化合物都含有一个{As 4 W 40 O 140 }单元，除了活性中心数（Ru）外，显示出相似的结构特征。有趣的是，化合物1 [营业额数 (TON)= 486；周转频率 (TOF)= 20 h –1] 在实现伯胺的氧化偶联方面表现出高效的光催化作用。还发现化合物2 (TON = 406, TOF = 17 h –1 ) 促进了氧化偶联，但效率相对较低；然而，化合物3 (TON = 178; TOF = 7.4 h –1) 对偶联反应体系没有明显贡献，一系列证据表明催化性能强烈依赖于活性位点的元素含量。此外，含Ru的POM基光催化剂在光催化过程中可方便地回收和重复使用。本研究证明了通过良好设计和控制其结构来调整 POM 基光催化剂的催化效率和稳定性的可能性。还基于实验研究提出了光催化合成亚胺产物的可能反应机理。
更新日期：2022-06-16
中文翻译：
含钌多金属氧酸盐的可控组装用于伯胺偶联反应的光催化活性
三种Ru诱导的结构互变多金属氧酸盐（POM），Na 13 H 5 [Ru 4 (H 2 O) 2 (Cl) 2 (WO 2 ) 4 (AsW 9 O 33 ) 4 ]·43H 2 O ( 1 ), K 5 Na 9 H 8 [Ru 2 (WO 2 ) 4 (AsW 9 O 33 ) 4 ]·50H 2 O ( 2 )、KNa 13 H 14[(WO 2 ) 4 (AsW 9 O 33 ) 4 ]·34H 2 O ( 3 )成功合成并进行了全面表征。通过改变化合物1-3的活性位点的数量来实现结构的相互转换。所有三种化合物都含有一个{As 4 W 40 O 140 }单元，除了活性中心数（Ru）外，显示出相似的结构特征。有趣的是，化合物1 [营业额数 (TON)= 486；周转频率 (TOF)= 20 h –1] 在实现伯胺的氧化偶联方面表现出高效的光催化作用。还发现化合物2 (TON = 406, TOF = 17 h –1 ) 促进了氧化偶联，但效率相对较低；然而，化合物3 (TON = 178; TOF = 7.4 h –1) 对偶联反应体系没有明显贡献，一系列证据表明催化性能强烈依赖于活性位点的元素含量。此外，含Ru的POM基光催化剂在光催化过程中可方便地回收和重复使用。本研究证明了通过良好设计和控制其结构来调整 POM 基光催化剂的催化效率和稳定性的可能性。还基于实验研究提出了光催化合成亚胺产物的可能反应机理。
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