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Band Structure Engineering of Schiff‐Base Microporous Organic Polymers for Enhanced Visible‐Light Photocatalytic Performance
Author(s) -
Xiao Zhichang,
Huang Xiaoxiong,
Zhao Kun,
Song Qi,
Guo Ruiying,
Zhang Xinghao,
Zhou Shanke,
Kong Debin,
Wagner Manfred,
Müllen Klaus,
Zhi Linjie
Publication year - 2019
Publication title -
small
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 3.785
H-Index - 236
eISSN - 1613-6829
pISSN - 1613-6810
DOI - 10.1002/smll.201900244
Subject(s) - photocatalysis , microporous material , materials science , electronic band structure , polymer , melamine , nanotechnology , semiconductor , chemical engineering , optoelectronics , catalysis , chemistry , organic chemistry , composite material , physics , quantum mechanics , engineering
Schiff‐base networks (SBNs), as typical examples of nitrogen‐doped microporous organic polymers (MOPs), exhibit promising application prospects owing to their stable properties and tunable chemical structures. However, their band structure engineering, which plays a key role in optical properties, remains elusive due to the complicated mechanisms behind energy level adjustment. In this work, a series of SBNs are fabricated by tailoring the ratio of p‐phthalaldehyde and o‐phthalaldehyde in the Schiff‐base chemistry reaction with melamine, resulting in a straightforward as well as continuous tuning of their band gaps ranging from 4.4 to 1.4 eV. Consequently, SBNs can be successfully used as photocatalysts with excellent visible‐light photocatalytic activity even under metal‐free conditions. Significantly, electronic structures of SBNs are systematically studied by electrochemical and spectroscopic characterizations, demonstrating that the enhanced performance is ascribed to proper band structure and improved charge separation ability. More importantly, in combination with theoretical calculations, the band structure regulation mechanism and band structure‐photocatalytic property relationship are deeply disclosed. The results obtained from this study will not only furnish SBN materials with excellent performance for solar energy conversion, but also open up elegant protocols for the molecular engineering of MOPs with desirable band structures.