Selective Photocatalytic CO₂ Reduction to CH₄ on Tri-s-triazine-Based Carbon Nitride via Defects and Crystal Regulation: Synergistic Effect of Thermodynamics and Kinetics

Zhiguo Liu; Shiqun Wu; Mingyang Li; Jinlong Zhang

doi:10.1021/acsami.2c03913

journal article·2022-06-08

Selective Photocatalytic CO₂ Reduction to CH₄ on Tri-s-triazine-Based Carbon Nitride via Defects and Crystal Regulation: Synergistic Effect of Thermodynamics and Kinetics

Zhiguo Liu, Shiqun Wu, Mingyang Li, Jinlong Zhang

ACS Applied Materials & Interfaces· Volume 14· Issue 22

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Source abstract

Abstract

Realizing the high selectivity of CH4 from the photocatalytic CO2 reduction reaction (CO2 RR) remains a great challenge owing to the lower efficiency of multi-electron transfer and the similar thermodynamic properties of CH4 and CO. Herein, nitrogen-deficient carbon nitride two-dimensional (2D) nanosheets were prepared via the high-temperature crystalline phase transformation process. Optimizing crystallinity enhances the in-plane polarization along the a-axis. Owing to the increased electron density of the N defect, the kinetic possibilities of CH4 production have increased. Furthermore, the potential energy of the mid-gap states introduced by the N defect favors the thermodynamics of CH4 production. The selectivity values of CH4 based on yield and electrons are 87.1 and 96.4%. This work unravels the mechanism to selectively produce CH4 from CO2 photoreduction through the crystalline phase and defect regulation and provides significant guidance for the rational design of CO2 reduction photocatalysts for selective CH4 production.

Source: openalex_inverted_index · Quality: baseline

Research context

Nanomaterials Catalysis & surfaces

OpenAlex topics: Advanced Photocatalysis Techniques · CO2 Reduction Techniques and Catalysts · Covalent Organic Framework Applications

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Shanghai Engineering Research Center for Multi-Media Environmental Catalysis and Resource Utilization, Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Frontiers Science Center for Materiobiology and Dynamic Chemistry, School of Chemistry and Molecular Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai 200237, P. R. China

School of Chemistry & Chemical Engineering, Yancheng Institute of Technology, Yancheng 224051, China

Funding

Ministry of Science and Technology of the People's Republic of China · Central University Basic Research Fund of China · Shanghai Municipal Education Commission · Science and Technology Commission of Shanghai Municipality · National Natural Science Foundation of China · Higher Education Discipline Innovation Project

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