An efficient visible-light photocatalyst for CO 2 reduction fabricated by cobalt porphyrin and graphitic carbon nitride
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An efficient visible-light photocatalyst for CO2 reduction fabricated by cobalt porphyrin and graphitic carbon nitride via covalent bonding Shufang Tian1, Sudi Chen1, Xitong Ren1, Yaoqing Hu1, Haiyan Hu1, and Jiajie Sun2 (), and Feng Bai1 () Key Laboratory for Special Functional Materials of Ministry of Education, National & Local Joint Engineering Research Center for Highefficiency Display and Lighting Technology, School of Materials Science and Engineering, and Collaborative Innovation Center of Nano Functional Materials and Applications, Henan University, Kaifeng 475004, China 2 School of Physics and Electronics, Henan University, Kaifeng 475004, China 1
© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2020 Received: 21 May 2020 / Revised: 28 May 2020 / Accepted: 29 May 2020
ABSTRACT Nanoparticle photosensitizers possess technical advantages for photocatalytic reactions due to enhanced light harvesting and efficient charge transport. Here we report synthesis of semiconductor nanoparticles through covalent coupling and assembly of metalloporphyrin with condensed carbon nitride. The resultant nanoparticles consist of light harvesting component from the condensed carbon nitride and photocatalytic sites from the metalloporphyrins. This synergetic particle system effectively initiates efficient charge separation and transport and exhibits excellent photocatalytic activity for CO2 reduction. The CO production rate can reach up to 57 μmol/(g·h) with a selectivity of 79% over competing H2 evolution. Controlled experiments demonstrate that the combination of light harvesting with photocatalytic activity via covalent assembly is crucial for the high photocatalytic activity. Due to effective charge separation and transfer, the resultant nanoparticle photocatalysts show exceptional photo stability against photo-corrosion under light irradiation, enabling for long-term utilization. This research opens a new way for the development of stable, effective nanoparticle photocatalysts using naturally abundant porphyrin pigments.
KEYWORDS photocatalysis, CO2 reduction, carbon nitride, porphyrin, two-dimensional nanosheets, function integrated, covalent bonding
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Introduction
Solar-driven conversion of carbon dioxide (CO2) into storable chemical fuels is an attractive way to alleviate the energy and environment tensions [1–9]. Numerous attempts have been applied to develop different kinds of visible-light photocatalysts to fulfil this vision [10–16]. Owing to the high thermodynamic stability of CO2 that the photocatalytic reduction process involves multiple electron and proton transfer, the development of catalysts to lower the CO2 activation barriers and the multielectron related kinetic barriers is critical to promote the catalytic efficiency [17]. Metal-complexes (e.g., Ru, Ir and Re) have been well demonstrated as homogeneous molecular photo catalysts for CO2 reduction with high activity and selectivity [18–21]. Their electron structure and redox property can be easily tuned by changi
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