Highly Crystalline K-Intercalated Polymeric Carbon Nitride for Visible-Light Photocatalytic Alkenes and Alkynes Deuterations

被引:95
作者
Qiu, Chuntian [1 ,2 ,3 ]
Xu, Yangsen [1 ,2 ]
Fan, Xin [1 ,2 ,4 ]
Xu, Dong [5 ]
Tandiana, Rika [1 ,2 ]
Ling, Xiang [1 ,2 ]
Jiang, Yanan [1 ,2 ]
Liu, Cuibo [1 ,2 ]
Yu, Lei [4 ]
Chen, Wei [6 ]
Su, Chenliang [1 ,2 ,3 ]
机构
[1] Shenzhen Univ, Coll Optoelect Engn, Minist Educ, SZU NUS Collaborat Ctr, Shenzhen 518060, Peoples R China
[2] Shenzhen Univ, Coll Optoelect Engn, Minist Educ, Int Collaborat Lab 2D Mat Optoelect Sci & Technol, Shenzhen 518060, Peoples R China
[3] Shenzhen Univ, Engn Technol Res Ctr 2D Mat Informat Funct Device, Shenzhen 518060, Peoples R China
[4] Yangzhou Univ, Sch Chem & Chem Engn, Yangzhou 225002, Jiangsu, Peoples R China
[5] Natl Univ Singapore, Dept Civil & Environm Engn, 1 Engn Dr 2, Singapore 117576, Singapore
[6] Natl Univ Singapore, Dept Chem, 3 Sci Dr 3, Singapore 117543, Singapore
基金
新加坡国家研究基金会;
关键词
alkene deuterations; crystalline KPCN; deuterated chemicals; hydrogen evolution; photocatalysis; SOLAR HYDROGEN-PRODUCTION; EXCITON DISSOCIATION; GENERATION; REDUCTION; CATALYSIS; WATER; TEMPERATURES; TRIAZINES; EVOLUTION; DEUTERIUM;
D O I
10.1002/advs.201801403
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
In addition to the significance of photocatalytic hydrogen evolution, the utilization of the in situ generated H/D (deuterium) active species from water splitting for artificial photosynthesis of high value-added chemicals is very attractive and promising. Herein, photocatalytic water splitting technology is utilized to generate D-active species (i.e., D-ad) that can be stabilized on anchored 2nd metal catalyst and are readily for tandem controllable deuterations of carbon-carbon multibonds to produce high value-added D-labeled chemicals/pharmaceuticals. A highly crystalline K cations intercalated polymeric carbon nitride (KPCN), rationally designed, and fabricated by a solid-template induced growth, is served as an ultraefficient photocatalyst, which shows a greater than 18-fold enhancement in the photocatalytic hydrogen evolution over the bulk PCN. The photocatalytic in situ generated D-species by superior KPCN are utilized for selective deuteration of a variety of alkenes and alkynes by anchored 2nd catalyst, Pd nanoparticles, to produce the corresponding D-labeled chemicals and pharmaceuticals with high yields and D-incorporation. This work highlights the great potential of developing photocatalytic water splitting technology for artificial photosynthesis of value-added chemicals instead of H-2 evolution.
引用
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页数:7
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