Dissolution and Performing Homogeneous Photocatalysis of Polymeric Carbon Nitride

2018 ◽  
Author(s):  
Chaofeng Huang ◽  
Jing Wen ◽  
Yanfei Shen ◽  
Fei He ◽  
Li Mi ◽  
...  
Keyword(s):  
Conjugated Polymer ◽  
Carbon Nitride ◽  
Heterogeneous Catalysts ◽  
Methane Sulfonic Acid ◽  
Environment Friendly ◽  
The Poor ◽  
Catalytic Sites ◽  
Homogeneous Photocatalysis ◽  
Polymeric Carbon ◽  
First Time

<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.

scholarly journals Dissolution and Performing Homogeneous Photocatalysis of Polymeric Carbon Nitride

2018 ◽  
Author(s):  
Chaofeng Huang ◽  
Jing Wen ◽  
Yanfei Shen ◽  
Fei He ◽  
Li Mi ◽  
...  
Keyword(s):  
Conjugated Polymer ◽  
Carbon Nitride ◽  
Heterogeneous Catalysts ◽  
Methane Sulfonic Acid ◽  
Environment Friendly ◽  
The Poor ◽  
Catalytic Sites ◽  
Homogeneous Photocatalysis ◽  
Polymeric Carbon ◽  
First Time

<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.

scholarly journals Dissolution and homogeneous photocatalysis of polymeric carbon nitride

2018 ◽  
Vol 9 (41) ◽  
pp. 7912-7915 ◽  
Author(s):  
Chaofeng Huang ◽  
Jing Wen ◽  
Yanfei Shen ◽  
Fei He ◽  
Li Mi ◽  
...  
Keyword(s):  
Carbon Nitride ◽  
Heterogeneous Catalysts ◽  
Homogeneous Photocatalysis ◽  
Polymeric Carbon

After dissolution, a homogeneous carbon nitride photocatalyst showed boosted activity; meanwhile, the hallmarks of heterogeneous catalysts (facile separation and recycling) were retained.

scholarly journals Water-Soluble Polymeric Carbon Nitride Colloidal Nanoparticles for Highly Selective Quasi-Homogeneous Photocatalysis

2019 ◽  
Author(s):  
Igor Krivtsov ◽  
Dariusz Mitoraj ◽  
Marina Ilkaeva ◽  
Mariana Sardo ◽  
Luís Mafra ◽  
...  
Keyword(s):  
Active Sites ◽  
Carbon Nitride ◽  
Water Soluble ◽  
Colloidal Nanoparticles ◽  
Narrow Size Distribution ◽  
New Paradigm ◽  
Redox Transformations ◽  
Homogeneous Photocatalysis ◽  
Polymeric Carbon ◽  
First Time

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.

scholarly journals Water-Soluble Polymeric Carbon Nitride Colloidal Nanoparticles for Highly Selective Quasi-Homogeneous Photocatalysis

2019 ◽  
Author(s):  
Igor Krivtsov ◽  
Dariusz Mitoraj ◽  
Marina Ilkaeva ◽  
Mariana Sardo ◽  
Luís Mafra ◽  
...  
Keyword(s):  
Active Sites ◽  
Carbon Nitride ◽  
Water Soluble ◽  
Colloidal Nanoparticles ◽  
Narrow Size Distribution ◽  
New Paradigm ◽  
Redox Transformations ◽  
Homogeneous Photocatalysis ◽  
Polymeric Carbon ◽  
First Time

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.

scholarly journals Water‐Soluble Polymeric Carbon Nitride Colloidal Nanoparticles for Highly Selective Quasi‐Homogeneous Photocatalysis

2019 ◽  
Vol 132 (1) ◽  
pp. 495-503 ◽  
Author(s):  
Igor Krivtsov ◽  
Dariusz Mitoraj ◽  
Christiane Adler ◽  
Marina Ilkaeva ◽  
Mariana Sardo ◽  
...  
Keyword(s):  
Carbon Nitride ◽  
Water Soluble ◽  
Colloidal Nanoparticles ◽  
Homogeneous Photocatalysis ◽  
Polymeric Carbon

scholarly journals NIR-Responsive Carbon Nitride of Five-Membered Rings (C3N2) for Photoelectrochemical Biosensing

2020 ◽  
Author(s):  
Hong Yang ◽  
Qing Zhou ◽  
Zhengzou Fang ◽  
Lufang Zhao ◽  
Jin Ma ◽  
...  
Keyword(s):  
Density Functional ◽  
Carbon Nitride ◽  
Density Functional Theory Calculations ◽  
Electronic Band ◽  
Functional Theory ◽  
Hard Materials ◽  
Polymeric Carbon ◽  
First Time ◽  
Electronic Transition Energy

Polymeric carbon nitrides (pCN) have garnered immense attention, ranging from super-hard materials to artificial photosynthesis, due to their exceptional chemical and optoelectronic properties. The most studied C<sub>3</sub>N<sub>4</sub> along with other stoichiometric pCN, such as C<sub>3</sub>N, C<sub>2</sub>N and C<sub>3</sub>N<sub>5</sub>, commonly employed a six-membered ring as the basic units; while the five-membered rings are also popular in a myriad of natural and artificial molecules with a more polarized framework and intriguing functionalities. Here, we report a facile synthesis of C<sub>3</sub>N<sub>2</sub> with a topological structure of five-membered rings, endowing by far the narrowest the first electronic transition energy (0.81 eV) in pCN family. The basic imidazole unit with dangling bonds, resulting in an unusual electronic band of p-π conjugation and split molecular orbitals, was revealed in C<sub>3</sub>N<sub>2</sub> by both experiments and density functional theory calculations. Moreover, a NIR-responsive photoelectrochemical (PEC) biosensor for non-transparent biosamples was constructed for the first time using C<sub>3</sub>N<sub>2</sub> with outstanding performance. This work would not only open a new vista of pCN with different topological structures but also broaden the horizon of their application, such as prospective <i>in vivo</i> PEC bioassay.

scholarly journals NIR-Responsive Carbon Nitride of Five-Membered Rings (C3N2) for Photoelectrochemical Biosensing

2020 ◽  
Author(s):  
Hong Yang ◽  
Qing Zhou ◽  
Zhengzou Fang ◽  
Lufang Zhao ◽  
Jin Ma ◽  
...  
Keyword(s):  
Density Functional ◽  
Carbon Nitride ◽  
Density Functional Theory Calculations ◽  
Electronic Band ◽  
Functional Theory ◽  
Hard Materials ◽  
Polymeric Carbon ◽  
First Time ◽  
Electronic Transition Energy

Polymeric carbon nitrides (pCN) have garnered immense attention, ranging from super-hard materials to artificial photosynthesis, due to their exceptional chemical and optoelectronic properties. The most studied C<sub>3</sub>N<sub>4</sub> along with other stoichiometric pCN, such as C<sub>3</sub>N, C<sub>2</sub>N and C<sub>3</sub>N<sub>5</sub>, commonly employed a six-membered ring as the basic units; while the five-membered rings are also popular in a myriad of natural and artificial molecules with a more polarized framework and intriguing functionalities. Here, we report a facile synthesis of C<sub>3</sub>N<sub>2</sub> with a topological structure of five-membered rings, endowing by far the narrowest the first electronic transition energy (0.81 eV) in pCN family. The basic imidazole unit with dangling bonds, resulting in an unusual electronic band of p-π conjugation and split molecular orbitals, was revealed in C<sub>3</sub>N<sub>2</sub> by both experiments and density functional theory calculations. Moreover, a NIR-responsive photoelectrochemical (PEC) biosensor for non-transparent biosamples was constructed for the first time using C<sub>3</sub>N<sub>2</sub> with outstanding performance. This work would not only open a new vista of pCN with different topological structures but also broaden the horizon of their application, such as prospective <i>in vivo</i> PEC bioassay.

Environment-friendly preparation of porous graphite-phase polymeric carbon nitride using calcium carbonate as templates, and enhanced photoelectrochemical activity

2015 ◽  
Vol 3 (9) ◽  
pp. 5126-5131 ◽  
Author(s):  
Jianhai Wang ◽  
Cheng Zhang ◽  
Yanfei Shen ◽  
Zhixin Zhou ◽  
Jiachao Yu ◽  
...  
Keyword(s):  
Calcium Carbonate ◽  
Silica Nanoparticles ◽  
Porous Carbon ◽  
Carbon Nitride ◽  
Photoelectrochemical Activity ◽  
Graphite Phase ◽  
Environment Friendly ◽  
Porous Graphite ◽  
Polymeric Carbon

Superior to silica nanoparticles, the easily accessible and removable CaCO3 particles produced porous carbon nitride with photocurrents 7.5-times that of the bulk one.

The true liquid crystal phases of 2D polymeric carbon nitride and macroscopic assembled fibers

2019 ◽  
Vol 6 (8) ◽  
pp. 1726-1732 ◽  
Author(s):  
Ji-Yoon Song ◽  
Hui-Ju Kang ◽  
Jong Chan Won ◽  
Yun Ho Kim ◽  
Young-Si Jun ◽  
...  
Keyword(s):  
Liquid Crystal ◽  
Sulfuric Acid ◽  
Aspect Ratio ◽  
Liquid Crystalline ◽  
Carbon Nitride ◽  
Interlayer Spacing ◽  
Concentrated Sulfuric Acid ◽  
Crystal Phases ◽  
Polymeric Carbon ◽  
First Time

We report that controlled graphitic carbon nitride (g-CN) which has high aspect ratio and expanded interlayer spacing can exhibit lyotropic liquid crystalline (LC) phase in concentrated sulfuric acid. By utilizing its LC phase, a g-CN fiber for the first time was successfully fabricated.

Facile synthesis of tin-doped polymeric carbon nitride with a hole-trapping center for efficient charge separation and photocatalytic hydrogen evolution

2019 ◽  
Vol 7 (45) ◽  
pp. 25824-25829 ◽  
Author(s):  
Zhiwei Liang ◽  
Yuguo Xia ◽  
Guiming Ba ◽  
Haiping Li ◽  
Quanhua Deng ◽  
...  
Keyword(s):  
Hydrogen Evolution ◽  
Charge Separation ◽  
Carbon Nitride ◽  
Facile Synthesis ◽  
Photocatalytic Hydrogen Evolution ◽  
Hole Capture ◽  
Hole Trapping ◽  
Efficient Charge ◽  
Polymeric Carbon ◽  
First Time

For the first time, Sn-doped polymeric carbon nitride was synthesized with N–Sn bonds working as hole-capture centers for enhanced photocatalytic hydrogen evolution.

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