Correction: Phosphorescent bio-based resin for digital light processing (DLP) 3D-printing

Correction for 'Phosphorescent bio-based resin for digital light processing (DLP) 3D-printing' by Mirko Maturi et al., Green Chem., 2020, 22, 6212–6224, DOI: 10.1039/D0GC01983F

Rational Design of Carbon Nitride Photoelectrodes with High Activity Toward Organic Oxidations

Carbon nitride (CNx) is a light-absorber with excellent performance in photocatalytic suspension systems, but the activity of CNx photoelectrodes has remained low. Here, cyanamide-functionalized CNx (NCNCNx) was co-deposited with ITO nanoparticles on a 1.8 Å thick alumina-coated FTO electrode. Transient absorption spectroscopy and impedance measurements support that ITO acts as a conductive binder and improves electron extraction from the NCNCNx, whilst the alumina underlayer reduces recombination losses between the ITO and the FTO glass. The Al2O3|ITO : NCNCNx film displays a benchmark performance for CNx-based photoanodes with an onset of −0.4 V vs a reversible hydrogen electrode (RHE), and 1.4±0.2 mA cm−2 at 1.23 V vs RHE during AM1.5G irradiation for the selective oxidation of 4-methylbenzyl alcohol. This assembly strategy will improve the exploration of CNx in fundamental and applied photoelectrochemical (PEC) studies.The authors thank Dr. Carla Casadevall, Dr. Motiar Rahaman, and Dr. Mark Bajada (University of Cambridge) for helpful discussions. This work was funded by the European Union's Horizon 2020 project SOLAR2CHEM (Marie Skłodowska-Curie Actions with Grant Agreement No. 861151, C.P., E.R.) and Methasol (Grant Agreement No. 101022649, S.A.J.H., J.D.), the EPSRC (NanoDTC, EP/L015978/1, and EP/S022953, T.U., E.R.), Generalitat Valenciana (APOSTD/2021/251 fellowship, C.A.M.), and the project PID2020-116093RB-C41 by MCIN/AEI/10.13039/501100011033/ (S.G.). The authors acknowledge the use of the Cambridge XPS System, which is part of Sir Henry Royce Institute - Cambridge Equipment, EPSRC grant EP/P024947/1, and the EPSRC Underpinning Multi-User Equipment Call (EP/P030467/1) for the Talos F200X G2 TEM

Research data supporting: "Electrostatic [FeFe]-hydrogenase–carbon nitride assemblies for efficient solar hydrogen production"

Manuscript folder - contains Fig.1-5: schematics, photocatalysis, QCM, PEIS, IMVS, and TPC (as PNG, XLSX files) Electronic Supplementary Information (ESI) folder - contains Fig.S1-S24: SEM, FTIR, PL, UV–vis, Zeta potential, NMR, HPLC, photograph, photocatalysis, PEIS (as EPS, PDF, TIF, PNG, XLSX files) Please see Readme file

Rational Design of Carbon Nitride Photoelectrodes with High Activity Toward Organic Oxidations.

Carbon nitride (CNx) is a scalable polymeric light-absorber with excellent performance in photocatalytic suspension systems, but the activity of CNx photoelectrodes has remained low. Here, cyanamide-functionalized CNx (NCNCNx) has been co-deposited with ITO nanoparticles on a 1.8 Å thick alumina-coated FTO-glass electrode. Transient spectroscopy and impedance measurements support that ITO acts as conductive binder and improves the electron extraction from the NCNCNx, whilst the alumina underlayer reduces the electrical resistance between the ITO and the FTO-coated electrode. The Al2O3|ITO:NCNCNx electrode displays a new benchmark performance for CNx-based photoanodes with a remarkably low onset of -0.4 V vs the reversible hydrogen electrode (RHE) and an outstanding 1.4 ± 0.2 mA cm-2 at 1.23 V vs RHE for the selective oxidation of 4-methylbenzyl alcohol to the corresponding aldehyde. This facile assembly will enable the exploration of CNx in fundamental and applied PEC studies, paving the way for the development of high-performance photoelectrodes using other semiconductor powders

Dataset for "Rational Design of Carbon Nitride Photoelectrodes with High Activity Toward Organic Oxidations"

The dataset contains the raw data that support the findings of the study “Rational Design of Carbon Nitride Photoelectrodes with High Activity Toward Organic Oxidations”. Data was collected using the instrumentation described in the Methods section of the study. Please see documentation included in dataset for more detailed information

Heterostructured PHI-PTI/Li+Cl- Carbon Nitrides for Multiple Photocatalytic Applications

[EN] Two series of novel carbon nitride photocatalysts, Rho-CN ("rhodizonate-doped carbon nitride") and Rho-CN-TC (Rho-CN treated in potassium thiocyanate melt), are synthesized in a multistep fashion via copolymerization of cyanamide with potassium rhodizonate. The formed ionic carbon nitrides are composed of poly(triazine imide) (PTI/Li+Cl-) and potassium poly(heptazine imide) (K-PHI) phases and provide a broad absorption range up to 800 nm. The photocatalysts are characterized by several techniques (including diffuse reflectance ultraviolet-visible, powder X-ray diffraction, Fourier transform infrared, scanning electron microscopy, and electrochemical methods) and studied in a series of photocatalytic reactions, including red light-promoted benzylamine oxidation, dual photoredox/nickel C-N cross-coupling, and hydrogen peroxide evolution. The optimal ratio of rhodizonate dopant in its mixture with cyanamide is found to be 0.5 mol%. The performance of the newly synthesized materials is comparable to the activities of the benchmark catalysts K-PHI and CN-OA-m (defective poly(heptazine imide) doped with oxamide), while not requiring more expensive nitrogen sources for preparation, like 5-aminotetrazole, or multiple oven cycles.This project has received funding from the European Union's Horizon 2020 research and innovation program under the Marie Sklodowska-Curie grant agreement no. 861151 Solar2Chem. The material presented and views expressed here are the responsibility of the authors only. The EU Commission takes no responsibility for any use made of the information set out. J.A.S. also thanks the Spanish Ministry of Science and Innovation for a Ramon y Cajal research associate contract (RYC2021-031006-I). A.G. and C.P. would like to thank Dr. Camilo A. Mesa (Institute of Advanced Materials (INAM), Universitat Jaume I (UJI)) for help with impedance data processing. Michael Born (electric workshop of the MPICI) is acknowledged for his contribution to this project.Open Access funding enabled and organized by Projekt DEAL.Galushchinski, A.; Pulignani, C.; Szalad, H.; Reisner, E.; Albero-Sancho, J.; Tarakina, NV.; Pelicano, CM.... (2023). Heterostructured PHI-PTI/Li+Cl- Carbon Nitrides for Multiple Photocatalytic Applications. Solar RRL. 7(14). https://doi.org/10.1002/solr.20230007771

Electrostatic [FeFe]-Hydrogenase–Carbon Nitride Assemblies for Efficient Solar Hydrogen Production

The assembly of semiconductors as light absorbers and enzymes as redox catalysts offers a promising approach for sustainable chemical synthesis driven by light. However, achieving the rational design of such semi-artificial systems requires a comprehensive understanding of the abiotic-biotic interface, which poses significant challenges. In this study, we demonstrate an electrostatic interaction strategy to interface negatively charged cyanamide modified graphitic carbon nitride (NCNCNX) with an [FeFe]-hydrogenase possessing a positive surface charge around the distal FeS cluster responsible for electron uptake into the enzyme. The strong electrostatic attraction enables efficient solar hydrogen (H2) production via direct interfacial electron transfer (DET), achieving a turnover frequency (TOF) of 18,669 h–1 (4 h) and a turnover number (TON) of 198,125 (24 h). Interfacial characterizations, including quartz crystal microbalance (QCM) and photoelectrochemical impedance spectroscopy (PEIS), have been conducted for the first time on a carbon nitride-enzyme to provide a comprehensive understanding for the future development of photocatalytic hybrid assemblies

Rational Design of Carbon Nitride Photoelectrodes with High Activity Toward Organic Oxidations

Carbon nitride (CN x ) is a light‐absorber with excellent performance in photocatalytic suspension systems, but the activity of CN x photoelectrodes has remained low. Here, cyanamide‐functionalized CN x (NCNCN x ) was co‐deposited with ITO nanoparticles on a 1.8 Å thick alumina‐coated FTO electrode. Transient absorption spectroscopy and impedance measurements support that ITO acts as a conductive binder and improves electron extraction from the NCNCN x , whilst the alumina underlayer reduces recombination losses between the ITO and the FTO glass. The Al2O3|ITO : NCNCN x film displays a benchmark performance for CN x ‐based photoanodes with an onset of −0.4 V vs a reversible hydrogen electrode (RHE), and 1.4±0.2 mA cm−2 at 1.23 V vs RHE during AM1.5G irradiation for the selective oxidation of 4‐methylbenzyl alcohol. This assembly strategy will improve the exploration of CN x in fundamental and applied photoelectrochemical (PEC) studies

Rational Design of Carbon Nitride Photoelectrodes with High Activity Toward Organic Oxidations.

Carbon nitride (CNx ) is a light-absorber with excellent performance in photocatalytic suspension systems, but the activity of CNx photoelectrodes has remained low. Here, cyanamide-functionalized CNx (NCN CNx ) was co-deposited with ITO nanoparticles on a 1.8 Å thick alumina-coated FTO electrode. Transient absorption spectroscopy and impedance measurements support that ITO acts as a conductive binder and improves electron extraction from the NCN CNx , whilst the alumina underlayer reduces recombination losses between the ITO and the FTO glass. The Al2 O3 |ITO : NCN CNx film displays a benchmark performance for CNx -based photoanodes with an onset of -0.4 V vs a reversible hydrogen electrode (RHE), and 1.4±0.2 mA cm-2 at 1.23 V vs RHE during AM1.5G irradiation for the selective oxidation of 4-methylbenzyl alcohol. This assembly strategy will improve the exploration of CNx in fundamental and applied photoelectrochemical (PEC) studies

Electrostatic [FeFe]-hydrogenase–carbon nitride assemblies for efficient solar hydrogen production

The assembly of semiconductors as light absorbers and enzymes as redox catalysts offers a promising approach for sustainable chemical synthesis driven by light. However, achieving the rational design of such...</jats:p