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Metalloligand Hybrid Polyoxometalates for Efficient Selective Photocatalytic Oxidation of Sulfides to Sulfoxides under Visible-Light Irradiation
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2022-12-21 , DOI: 10.1021/acs.jpcc.2c07333 Kaihui Ji 1 , Yanan Liu 1 , Yinghua Luo 1 , Xue Zhang 1 , Yufan Bai 1 , Hailong Yue 1 , Pengtao Ma 1 , Jingyang Niu 1 , Jingping Wang 1
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2022-12-21 , DOI: 10.1021/acs.jpcc.2c07333 Kaihui Ji 1 , Yanan Liu 1 , Yinghua Luo 1 , Xue Zhang 1 , Yufan Bai 1 , Hailong Yue 1 , Pengtao Ma 1 , Jingyang Niu 1 , Jingping Wang 1
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The development of novel high-efficiency photocatalysts to solve the bottleneck problems of low efficiency and harsh conditions of organic oxidation reactions is of vital significance. In this paper, a novel hybrid polyoxometalate (POM) crystal, (C2H8N)6[SiW11CdO39][Ru(bpy)2(dcbpy)]·DMF·5.5H2O (RuCd–SiW), was synthesized by combining the metalloligand [Ru(bpy)2(dcbpy)] with the oxidation catalyst POM. The introduction of the metalloligand extended the light absorption range of RuCd–SiW to the visible region, while electrochemical measurements demonstrated its potential as an excellent photocatalyst. Under visible light (λ > 400 nm) irradiation with O2 as the sole oxidant, RuCd–SiW showed highly efficient photocatalytic activity for the selective oxidation of thioanisole to (methylsulfoxide)benzene with a yield of 99.5%, a turnover number of 497.5, and a turnover frequency of 103 h–1. Particularly, the yield of (methylsulfoxide)benzene was still higher than 99% after five rounds of recycling, demonstrating its high stability and recyclability.
中文翻译：
金属配体杂化多金属氧酸盐在可见光照射下高效选择性光催化氧化硫化物为亚砜
开发新型高效光催化剂，解决有机氧化反应效率低、条件苛刻等瓶颈问题具有重要意义。在本文中，一种新型杂化多金属氧酸盐 (POM) 晶体，(C 2 H 8 N) 6 [SiW 11 CdO 39 ][Ru(bpy) 2 (dcbpy)]·DMF·5.5H 2 O ( RuCd–SiW )，通过将金属配体 [Ru(bpy) 2 (dcbpy)] 与氧化催化剂 POM 结合合成。金属配体的引入扩展了RuCd–SiW的光吸收范围到可见区域，而电化学测量证明了它作为一种出色的光催化剂的潜力。在以 O 2作为唯一氧化剂的可见光（λ> 400 nm）照射下， RuCd-SiW表现出高效的光催化活性，可将苯甲硫醚选择性氧化为（甲基亚砜）苯，产率为 99.5%，转换数为 497.5，周转频率为 103 h –1。特别是（甲基亚砜）苯经过五轮循环后收率仍高于99%，表明其具有较高的稳定性和可循环性。
更新日期：2022-12-21
中文翻译：
金属配体杂化多金属氧酸盐在可见光照射下高效选择性光催化氧化硫化物为亚砜
开发新型高效光催化剂，解决有机氧化反应效率低、条件苛刻等瓶颈问题具有重要意义。在本文中，一种新型杂化多金属氧酸盐 (POM) 晶体，(C 2 H 8 N) 6 [SiW 11 CdO 39 ][Ru(bpy) 2 (dcbpy)]·DMF·5.5H 2 O ( RuCd–SiW )，通过将金属配体 [Ru(bpy) 2 (dcbpy)] 与氧化催化剂 POM 结合合成。金属配体的引入扩展了RuCd–SiW的光吸收范围到可见区域，而电化学测量证明了它作为一种出色的光催化剂的潜力。在以 O 2作为唯一氧化剂的可见光（λ> 400 nm）照射下， RuCd-SiW表现出高效的光催化活性，可将苯甲硫醚选择性氧化为（甲基亚砜）苯，产率为 99.5%，转换数为 497.5，周转频率为 103 h –1。特别是（甲基亚砜）苯经过五轮循环后收率仍高于99%，表明其具有较高的稳定性和可循环性。
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