Nanostructure Engineering via Intramolecular Construction of Carbon Nitride as Efficient Photocatalyst for CO2 Reduction

Muhammad Sohail; Tariq Altalhi; Abdullah G Al-Sehemi; Taha Abdel Mohaymen Taha; Karam S El-Nasser; Ahmed A Al-Ghamdi; Mahnoor Boukhari; Arkom Palamanit; Asif Hayat; Mohammed A Amin; Wan Izhan Nawawi Bin Wan Ismail

doi:10.3390/nano11123245

Nanostructure Engineering via Intramolecular Construction of Carbon Nitride as Efficient Photocatalyst for CO₂ Reduction

Nanomaterials (Basel). 2021 Nov 29;11(12):3245. doi: 10.3390/nano11123245.

Authors

Affiliations

¹ Yangtze Delta Region Institute (Huzhou), University of Electronic Science and Technology of China, Huzhou 313001, China.
² Department of Chemistry, College of Science, Taif University, P.O. Box 11099, Taif 21944, Saudi Arabia.
³ Department of Chemistry, Faculty of Science, Research Center for Advanced Materials Science (RCAMS), King Khalid University, P.O. Box 9004, Abha 61413, Saudi Arabia.
⁴ Physics Department, College of Science, Jouf University, Sakaka 75471, Saudi Arabia.
⁵ Physics and Engineering Mathematics Department, Faculty of Electronic Engineering, Menoufia University, Menouf 32952, Egypt.
⁶ Chemistry Department, College of Science and Arts, Jouf University, Al-Gurayyat 77447, Saudi Arabia.
⁷ Chemistry Department, Faculty of Science, Al-Azhar University, Assiut 71524, Egypt.
⁸ Department of Physics, Faculty of Science, King Abdulaziz University, Jeddah 21589, Saudi Arabia.
⁹ College of Material Science & Engineering, Beijing University of Technology, Beijing 100081, China.
¹⁰ Energy Technology Program, Department of Specialized Engineering, Faculty of Engineering, Prince of Songkla University, 15 Karnjanavanich Rd., Hat Yai, Songkhla 90110, Thailand.
¹¹ State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou 350116, China.
¹² Faculty of Applied Sciences, Universiti Teknologi MARA, Cawangan Perlis, Arau Perlis 02600, Malaysia.

Abstract

Light-driven heterogeneous photocatalysis has gained great significance for generating solar fuel; the challenging charge separation process and sluggish surface catalytic reactions significantly restrict the progress of solar energy conversion using a semiconductor photocatalyst. Herein, we propose a novel and feasible strategy to incorporate dihydroxy benzene (DHB) as a conjugated monomer within the framework of urea containing CN (CNU-DHBx) to tune the electronic conductivity and charge separation due to the aromaticity of the benzene ring, which acts as an electron-donating species. Systematic characterizations such as SPV, PL, XPS, DRS, and TRPL demonstrated that the incorporation of the DHB monomer greatly enhanced the photocatalytic CO₂ reduction of CN due to the enhanced charge separation and modulation of the ionic mobility. The significantly enhanced photocatalytic activity of CNU-DHB_15.0 in comparison with parental CN was 85 µmol/h for CO and 19.92 µmol/h of the H₂ source. It can be attributed to the electron-hole pair separation and enhance the optical adsorption due to the presence of DHB. Furthermore, this remarkable modification affected the chemical composition, bandgap, and surface area, encouraging the controlled detachment of light-produced photons and making it the ideal choice for CO₂ photoreduction. Our research findings potentially offer a solution for tuning complex charge separation and catalytic reactions in photocatalysis that could practically lead to the generation of artificial photocatalysts for efficient solar energy into chemical energy conversion.

Keywords: CO2 reduction; carbon nitride (CN); copolymerization; dihydroxy benzene (DHB); photocatalysis.

Abstract

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