scholarly journals Sol−Gel Processing of Water‐Soluble Carbon Nitride Enables High‐Performance Photoanodes**

ChemSusChem ◽  
2021 ◽  
Author(s):  
Christiane Adler ◽  
Igor Krivtsov ◽  
Dariusz Mitoraj ◽  
Lucía Santos‐Gómez ◽  
Santiago García‐Granda ◽  
...  

ChemSusChem ◽  
2021 ◽  
Author(s):  
Christiane Adler ◽  
Igor Krivtsov ◽  
Dariusz Mitoraj ◽  
Lucía Santos‐Gómez ◽  
Santiago García‐Granda ◽  
...  


2020 ◽  
Author(s):  
Christiane Adler ◽  
Igor Krivtsov ◽  
Dariusz Mitoraj ◽  
Lucía dos Santos-Gómez ◽  
Santiago García-Granda ◽  
...  

In spite of the enormous promise that polymeric carbon nitride (PCN) materials hold for photoelectrochemical (PEC) applications, the fabrication of high-quality PCN photoelectrodes has been a largely elusive goal to date. Here we tackle this challenge by devising, for the first time, a sol–gel approach that enables facile preparation of photoanodes based on poly(heptazine imide) (PHI), a polymer belonging to the PCN family. The sol–gel process capitalizes on the use of a water-soluble PHI precursor composed of nanosized (~10 nm) particles that allows formation of a non-covalent hydrogel. The hydrogel can be deposited on a conductive substrate resulting in formation of mechanically stable porous polymeric thin layers (~400 nm), in contrast to the commonly obtained loosely attached thick particulate coatings. The resulting photoanodes exhibit unprecedented PEC performance in methanol reforming in neutral pH electrolytes with photocurrents of up to 177±27 mA cm<sup>-2</sup> (1 sun illumination) and 320±40 mA cm<sup>-2</sup> (2 sun illumination) at 1.23 V vs. RHE, maintaining such high photocurrents even down to ~0 V vs. RHE. These parameters permit effective operation even without any external electric bias, as demonstrated by bias-free photoreforming of methanol and glycerol, and highly selective (~100%) photooxidation of 4-methoxybenzyl alcohol (4-MBA). The robust binder-free films derived from sol–gel processing of water-soluble PCN thus represent a new paradigm for high-performance ‘soft-matter’ photoelectrocatalytic systems, and pave the way for further applications in which high-quality PCN films are required.



2020 ◽  
Author(s):  
Christiane Adler ◽  
Igor Krivtsov ◽  
Dariusz Mitoraj ◽  
Lucía dos Santos-Gómez ◽  
Santiago García-Granda ◽  
...  

In spite of the enormous promise that polymeric carbon nitride (PCN) materials hold for various applications, the fabrication of high-quality, binder-free PCN films and electrodes has been a largely elusive goal to date. Here we tackle this challenge by devising, for the first time, a sol–gel approach that enables facile preparation of thin films based on poly(heptazine imide) (PHI), a polymer belonging to the PCN family. The sol–gel process capitalizes on the use of a water-soluble PHI precursor that allows formation of a non-covalent hydrogel. The hydrogel can be deposited on conductive substrates resulting in formation of mechanically stable polymeric thin layers. The resulting photoanodes exhibit unprecedented PEC performance in alcohol reforming and selective (~100%) conversions with very high photocurrents down to ~0 V vs. RHE, which enables even effective operation under bias-free conditions. The robust binder-free films derived from sol–gel processing of water-soluble PCN thus represent a new paradigm for high-performance ‘soft-matter’ photoelectrocatalytic systems, and pave the way for further applications in which high-quality PCN films are required.



2020 ◽  
Author(s):  
Christiane Adler ◽  
Igor Krivtsov ◽  
Dariusz Mitoraj ◽  
Lucía dos Santos-Gómez ◽  
Santiago García-Granda ◽  
...  

In spite of the enormous promise that polymeric carbon nitride (PCN) materials hold for various applications, the fabrication of high-quality, binder-free PCN films and electrodes has been a largely elusive goal to date. Here we tackle this challenge by devising, for the first time, a sol–gel approach that enables facile preparation of thin films based on poly(heptazine imide) (PHI), a polymer belonging to the PCN family. The sol–gel process capitalizes on the use of a water-soluble PHI precursor that allows formation of a non-covalent hydrogel. The hydrogel can be deposited on conductive substrates resulting in formation of mechanically stable polymeric thin layers. The resulting photoanodes exhibit unprecedented PEC performance in alcohol reforming and selective (~100%) conversions with very high photocurrents down to ~0 V vs. RHE, which enables even effective operation under bias-free conditions. The robust binder-free films derived from sol–gel processing of water-soluble PCN thus represent a new paradigm for high-performance ‘soft-matter’ photoelectrocatalytic systems, and pave the way for further applications in which high-quality PCN films are required.



2020 ◽  
Author(s):  
Christiane Adler ◽  
Igor Krivtsov ◽  
Dariusz Mitoraj ◽  
Lucía dos Santos-Gómez ◽  
Santiago García-Granda ◽  
...  

In spite of the enormous promise that polymeric carbon nitride (PCN) materials hold for photoelectrochemical (PEC) applications, the fabrication of highly stable and photoactive PCN photoelectrodes has been a largely elusive goal to date. Here we tackle this challenge by devising, for the first time, a sol–gel approach that enables facile preparation of photoanodes based on poly(heptazine imide) (PHI), a polymer belonging to the PCN family. The sol–gel process capitalizes on the use of a water-soluble PHI precursor composed of nanosized (~10 nm) particles that allows formation of a non-covalent hydrogel. The hydrogel can be deposited on a conductive substrate resulting in formation of mechanically stable porous polymeric thin layers (~400 nm), in contrast to the commonly obtained loosely attached thick particulate coatings. The resulting photoanodes exhibit unprecedented PEC performance in methanol reforming in neutral pH electrolytes with very high photocurrents of 177±27 mA (1 sun illumination) cm<sup>-2</sup> and 320±40 mA cm<sup>-2</sup> (2 sun illumination) at 1.23 V vs. RHE, with very high photocurrents down to ~0 V vs. RHE. These parameters permit effective operation even without any external electric bias, as demonstrated by zero-bias photoreforming of methanol and glycerol, and highly selective (~100%) photooxidation of 4-methoxybenzyl alcohol (4-MBA). The robust binder-free films derived from sol–gel processing of water-soluble PCN thus represent a new paradigm for high-performance ‘soft-matter’ photoelectrocatalytic systems based on PCN.



ChemSusChem ◽  
2021 ◽  
Vol 14 (7) ◽  
pp. 1728-1736
Author(s):  
Chunyu Li ◽  
Elisabeth Hofmeister ◽  
Igor Krivtsov ◽  
Dariusz Mitoraj ◽  
Christiane Adler ◽  
...  


2015 ◽  
Vol 3 (27) ◽  
pp. 5490-5500 ◽  
Author(s):  
T. G. Khonina ◽  
A. P. Safronov ◽  
M. V. Ivanenko ◽  
E. V. Shadrina ◽  
O. N. Chupakhin

The formation of organic/inorganic hydrogels based on silicon and titanium polyethylene glycolates, new biocompatible water-soluble precursors in sol–gel processing, was investigated.



2015 ◽  
Vol 51 (49) ◽  
pp. 9932-9935 ◽  
Author(s):  
Mai Nishibayashi ◽  
Hiroyuki Yoshida ◽  
Masamoto Uenishi ◽  
Masakoto Kanezashi ◽  
Hiroki Nagasawa ◽  
...  

Silsesquioxane (SQ) membranes derived from 3-methacryloxypropyltrimethoxysilane and bis(trimethoxysilyl)ethane were successfully fabricated at low temperature via photo-induced sol–gel processing.





MRS Bulletin ◽  
1990 ◽  
Vol 15 (1) ◽  
pp. 18-25 ◽  
Author(s):  
J. Livage ◽  
M. Henry ◽  
J.P. Jolivet ◽  
C. Sanchez

Interest in the synthesis of submicron monodispersed powders is increasing. Such powders find applications in the ceramic industry when high performance materials are required. Sintering time and temperature can be significantly reduced with powders of narrow particle-size distribution. Fine colloidal particles can be made by a variety of methods, from the vapor phase or the liquid phase.The sol gel process offers new approaches to the synthesis of fine powders. Starting from molecular precursors, such as metal alkoxides or aqueous solutions, an oxide network is obtained via inorganic polymerization reactions. These reactions occur in solution, and the term “sol-gel processing” is often used to describe the synthesis of inorganic oxides by wet chemical methods. It offers many advantages compared to the conventional powder route. One unique advantage is the ability to go all the way from the molecular precursor to the solid material, permitting better control of the entire process and allowing synthesis of “tailor-made” powders.



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