Design of iron atom modified thiophene-linked metalloporphyrin 2D conjugated microporous polymer as CO2 reduction photocatalyst

文献信息

发布日期 2018-03-12
DOI 10.1039/C8CP00974K
影响因子 3.676
作者

Chongyang Chen, Chao Tang, Weiwei Xu, Youyong Li, Lai Xu


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摘要

Herein, by means of density functional theory (DFT) calculations, we designed a new type of thiophene-linked porphyrin unit and incorporated it into an extended 2D conjugated microporous polymer (CMP) to serve as a CO2 reduction catalyst. This newly designed catalyst combines the advantages of molecular catalysis, heterogeneous catalysis, high structural stability and tunable electronic properties. A series of metal atoms (Fe, Mg, Mn, and Cu) were introduced into the center of the porphyrin ring to modify its capacity for reducing CO2. Our transition state (TS) search calculations revealed that the Fe-modified CMP possessed the highest catalytic activity toward CO2 reduction. The plausible reduction pathway was also determined. The band structure and frontier orbital distribution calculations further demonstrated its semimetallic property and higher stimulated transition probability, both of which are critical factors for photocatalytic performance. We hope that our design could provide meaningful guidance for other relevant CO2 catalytic reactions.

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来源期刊

Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
自引率: 10.3%
年发文量: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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