Affiliation:
1. School of Materials Science and Engineering China University of Petroleum (East China) Qingdao 266580 China
2. College of Chemical Engineering China University of Petroleum (East China) Qingdao 266580 China
3. College of New Energy China University of Petroleum (East China) Qingdao 266580 China
4. Global Zero Emission Research Center National Institute of Advanced Industrial Science and Technology Tsukuba Ibaraki 305–8569 Japan
Abstract
AbstractCovalent triazine frameworks (CTFs) are emerging as a promising molecular platform for photocatalysis. Nevertheless, the construction of highly effective charge transfer pathways in CTFs for oriented delivery of photoexcited electrons to enhance photocatalytic performance remains highly challenging. Herein, a molecular engineering strategy is presented to achieve highly efficient charge separation and transport in both the lateral and vertical directions for solar‐to‐formate conversion. Specifically, a large π‐delocalized and π‐stacked Schottky junction (Ru‐Th‐CTF/RGO) that synergistically knits a rebuilt extended π‐delocalized network of the D–A1–A2 system (multiple donor or acceptor units, Ru‐Th‐CTF) with reduced graphene oxide (RGO) is developed. It is verified that the single‐site Ru units in Ru‐Th‐CTF/RGO act as effective secondary electron acceptors in the lateral direction for multistage charge separation/transport. Simultaneously, the π‐stacked and covalently bonded graphene is regarded as a hole extraction layer, accelerating the separation/transport of the photogenerated charges in the vertical direction over the Ru‐Th‐CTF/RGO Schottky junction with full use of photogenerated electrons for the reduction reaction. Thus, the obtained photocatalyst has an excellent CO2‐to‐formate conversion rate (≈11050 µmol g−1 h−1) and selectivity (≈99%), producing a state‐of‐the‐art catalyst for the heterogeneous conversion of CO2 to formate without an extra photosensitizer.
Funder
National Natural Science Foundation of China
Taishan Scholar Project of Shandong Province
Fundamental Research Funds for the Central Universities
Subject
Mechanical Engineering,Mechanics of Materials,General Materials Science
Cited by
1 articles.
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