Water-Soluble Polymeric Carbon Nitride Colloidal Nanoparticles for Quasi-Homogeneous Photoredox Applications

Author(s):  
Dariusz Mitoraj ◽  
Igor Krivtsov ◽  
Radim Beranek
2019 ◽  
Vol 132 (1) ◽  
pp. 495-503 ◽  
Author(s):  
Igor Krivtsov ◽  
Dariusz Mitoraj ◽  
Christiane Adler ◽  
Marina Ilkaeva ◽  
Mariana Sardo ◽  
...  

2019 ◽  
Author(s):  
Igor Krivtsov ◽  
Dariusz Mitoraj ◽  
Marina Ilkaeva ◽  
Mariana Sardo ◽  
Luís Mafra ◽  
...  

Heptazine-based polymeric carbon nitrides (PCN) are well established as promising photocatalysts for light-driven redox transformations. However, the activity of these materials is hampered by their low surface area translating into low concentration of active sites accessible for reactants. Herein, we report, for the first time, a bottom-up preparation of PCN nanoparticles with a narrow size distribution (~10±3 nm), which are fully soluble in water showing no gelation or precipitation over several months, and allow carrying out photocatalysis under <i>quasi</i>-homogeneous conditions. The rate of selective (up to 100%) photooxidation of 4-methoxybenzyl alcohol to 4-methoxybenzaldehyde was enhanced by the factor of 6.5 as compared to conventional solid PCN and was accompanied by simultaneous H<sub>2</sub>O<sub>2</sub> production <i>via</i> reduction of oxygen. The dissolved photocatalyst can be easily recovered and re-dissolved by simple modulation of the ionic strength of the medium, without any loss of activity and selectivity. This work thus establishes a new paradigm of easily operable <i>quasi-</i>homogeneous photocatalysis with PCN, and opens up a route for other applications in which liquid aqueous operation or processing of PCN is required.


2019 ◽  
Author(s):  
Igor Krivtsov ◽  
Dariusz Mitoraj ◽  
Marina Ilkaeva ◽  
Mariana Sardo ◽  
Luís Mafra ◽  
...  

Heptazine-based polymeric carbon nitrides (PCN) are well established as promising photocatalysts for light-driven redox transformations. However, the activity of these materials is hampered by their low surface area translating into low concentration of active sites accessible for reactants. Herein, we report, for the first time, a bottom-up preparation of PCN nanoparticles with a narrow size distribution (~10±3 nm), which are fully soluble in water showing no gelation or precipitation over several months, and allow carrying out photocatalysis under <i>quasi</i>-homogeneous conditions. The rate of selective (up to 100%) photooxidation of 4-methoxybenzyl alcohol to 4-methoxybenzaldehyde was enhanced by the factor of 6.5 as compared to conventional solid PCN and was accompanied by simultaneous H<sub>2</sub>O<sub>2</sub> production <i>via</i> reduction of oxygen. The dissolved photocatalyst can be easily recovered and re-dissolved by simple modulation of the ionic strength of the medium, without any loss of activity and selectivity. This work thus establishes a new paradigm of easily operable <i>quasi-</i>homogeneous photocatalysis with PCN, and opens up a route for other applications in which liquid aqueous operation or processing of PCN is required.


2019 ◽  
Vol 59 (1) ◽  
pp. 487-495 ◽  
Author(s):  
Igor Krivtsov ◽  
Dariusz Mitoraj ◽  
Christiane Adler ◽  
Marina Ilkaeva ◽  
Mariana Sardo ◽  
...  

2018 ◽  
Author(s):  
Chaofeng Huang ◽  
Jing Wen ◽  
Yanfei Shen ◽  
Fei He ◽  
Li Mi ◽  
...  

<a></a><a>As a metal-free conjugated polymer, carbon nitride (CN) has attracted tremendous attention as heterogeneous (photo)catalysts. </a><a></a><a>By following prototype of enzymes, making all catalytic sites of accessible via homogeneous reactions is a promising approach toward maximizing CN activity, but hindered due to </a><a></a><a>the poor insolubility of CN</a>. Herein, we report the dissolution of CN in environment-friendly methane sulfonic acid and the homogeneous photocatalysis driven by CN for the first time with the activity boosted up to 10-times, comparing to the heterogeneous counterparts. Moreover, facile recycling and reusability, the <a>hallmark</a> of heterogeneous catalysts, were kept for the homogeneous CN photocatalyst via reversible precipitation using poor solvents. It opens new vista of CN in homogeneous catalysis and offers a successful example of polymeric catalysts in bridging gaps of homo/heterogeneous catalysis.


2019 ◽  
Author(s):  
Zhengyuan Jin ◽  
Xiantao Jiang ◽  
Qitao Zhang ◽  
Shaolong Huang ◽  
Luhong Zhang ◽  
...  

ChemSusChem ◽  
2020 ◽  
Vol 13 (14) ◽  
pp. 3605-3613 ◽  
Author(s):  
Qin Lei ◽  
Rongzhi Chen ◽  
Yurong Zhao ◽  
Huanyu Chen ◽  
Xinxin Long ◽  
...  

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