TY - JOUR
T1 - Photoelectrochemical alcohols oxidation over polymeric carbon nitride photoanodes with simultaneous H2 production
AU - Karjule, Neeta
AU - Phatake, Ravindra S.
AU - Barzilai, Shmuel
AU - Mondal, Biswajit
AU - Azoulay, Adi
AU - Shames, Alexander I.
AU - Volokh, Michael
AU - Albero, Josep
AU - García, Hermenegildo
AU - Shalom, Menny
N1 - Funding Information:
This project has received funding from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation programme (grant agreement No. [849068]). This work was also partially supported by the joint Israel Science Foundation-National Science Foundation of China (ISF-NSFC), grant No. 2969/19, the ISF grant No.601/21, and by the Pazy Foundation (grant No. 119-2020). J.A. and H.G. gratefully acknowledge financial support by the Spanish Ministry of Science and Innovation (RTI2018-98237-CO2-1) and Generalitat Valenciana (Prometeo 2021/038). The authors thank Liel Abisdris, Jonathan Tzadikov, Ayelet Tashakory, and Rotem Geva for help with material characterization. We thank Dr Chabanne for fruitful discussion.
Funding Information:
This project has received funding from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation programme (grant agreement No. [849068]). This work was also partially supported by the joint Israel Science Foundation–National Science Foundation of China (ISF–NSFC), grant No. 2969/19, the ISF grant No.601/21, and by the Pazy Foundation (grant No. 119-2020). J.A. and H.G. gratefully acknowledge financial support by the Spanish Ministry of Science and Innovation (RTI2018-98237-CO2-1) and Generalitat Valenciana (Prometeo 2021/038). The authors thank Liel Abisdris, Jonathan Tzadikov, Ayelet Tashakory, and Rotem Geva for help with material characterization. We thank Dr Chabanne for fruitful discussion.
Publisher Copyright:
© 2022 The Royal Society of Chemistry.
PY - 2022/7/25
Y1 - 2022/7/25
N2 - The photoelectrochemical oxidation of organic molecules into valuable chemicals is a promising technology, but its development is hampered by the poor stability of photoanodic materials in aqueous solutions, low faradaic efficiency, low product selectivity, and a narrow working pH range. Here, we demonstrate the synthesis of value-added aldehydes and carboxylic acids with clean hydrogen (H2) production in water using a photoelectrochemical cell based solely on polymeric carbon nitride (CN) as the photoanode. Isotope labeling measurements and DFT calculations reveal a preferential adsorption of benzyl alcohol and molecular oxygen to the CN layer, enabling fast proton abstraction and oxygen reduction, which leads to the synthesis of an aldehyde at the first step. Further oxidation affords the corresponding acid. The CN photoanode exhibits excellent stability (>40 h) and activity for the oxidation of a wide range of substituted benzyl alcohols with high yield, selectivity (up to 99%), and faradaic efficiency (>90%).
AB - The photoelectrochemical oxidation of organic molecules into valuable chemicals is a promising technology, but its development is hampered by the poor stability of photoanodic materials in aqueous solutions, low faradaic efficiency, low product selectivity, and a narrow working pH range. Here, we demonstrate the synthesis of value-added aldehydes and carboxylic acids with clean hydrogen (H2) production in water using a photoelectrochemical cell based solely on polymeric carbon nitride (CN) as the photoanode. Isotope labeling measurements and DFT calculations reveal a preferential adsorption of benzyl alcohol and molecular oxygen to the CN layer, enabling fast proton abstraction and oxygen reduction, which leads to the synthesis of an aldehyde at the first step. Further oxidation affords the corresponding acid. The CN photoanode exhibits excellent stability (>40 h) and activity for the oxidation of a wide range of substituted benzyl alcohols with high yield, selectivity (up to 99%), and faradaic efficiency (>90%).
UR - http://www.scopus.com/inward/record.url?scp=85135342801&partnerID=8YFLogxK
U2 - 10.1039/d2ta03660f
DO - 10.1039/d2ta03660f
M3 - Article
C2 - 36091884
AN - SCOPUS:85135342801
SN - 2050-7488
VL - 10
SP - 16585
EP - 16594
JO - Journal of Materials Chemistry A
JF - Journal of Materials Chemistry A
IS - 31
ER -
