Lead(II)-Based Coordination Polymer Exhibiting Reversible Color Switching and Selective CO2 Photoreduction Properties

被引:3
作者
Suppaso, Chomponoot [1 ]
Akiyoshi, Ryohei [2 ]
Yamada, Hiroki [3 ]
Kamakura, Yoshinobu [1 ]
Ishiwari, Fumitaka [4 ,5 ,6 ]
Ogasawara, Kazuyoshi [2 ]
Saeki, Akinori [4 ,5 ]
Tanaka, Daisuke [2 ]
Maeda, Kazuhiko [1 ,7 ]
机构
[1] Tokyo Inst Technol, Sch Sci, Dept Chem, Tokyo 1528550, Japan
[2] Kwansei Gakuin Univ, Sch Sci, Dept Chem, Sanda, Hyogo 6691337, Japan
[3] Japan Synchrotron Radiat Res Inst JASRI, Sayo, Hyogo 6795198, Japan
[4] Osaka Univ, Grad Sch Engn, Dept Appl Chem, Suita, Osaka 5650871, Japan
[5] Osaka Univ, Inst Open & Transdisciplinary Res Initiat ICS OTRI, Innovat Catalysis Sci Div, Suita, Osaka 5650871, Japan
[6] PRESTO Japan Sci & Technol Agcy JST, Kawaguchi, Saitama 3320012, Japan
[7] Tokyo Inst Technol, Res Ctr Autonomous Syst Mat ASMat, Yokohama, Kanagawa 2268501, Japan
基金
日本科学技术振兴机构;
关键词
METAL-ORGANIC FRAMEWORKS; CRYSTAL; REDUCTION; EFFICIENT; EXCHANGE; MOBILITY;
D O I
10.1021/acs.inorgchem.4c01883
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
Herein, we report a new photofunctional Pb-S-based coordination polymer (CP) with the formula [Pb(ATAT)(OAc)](n) (ATAT = 3-amino-5-mercapto-1,2,4-triazole, OAc = acetate, CP1). Apart from its photoactive one-dimensional (1D) (-Pb-S-)(n) chain, CP1 is also composed of another 1D (-Pb-O-)(n) chain that originates from the coordination with acetate. The coordinated acetate can be exchanged with water (H2O) or dimethyl sulfoxide (DMSO), leading to the formation of a CP1-H2O or CP1-DMSO structure that exhibits a distinct change in optical properties, including a white-to-yellow color change. The structural transformation of CP1 to CP1-H2O and CP1-DMSO, and its subsequent recovery to the original CP1 structure could be controlled by the presence or absence of acetic acid vapor; the transformation was completely reversible. CP1 absorbed light with wavelengths shorter than 390 nm, with an estimated bandgap of 3.18 eV. Density functional theory calculations indicated that the valence band of CP1 is mainly formed by N and S orbitals originating from the ATAT unit, whereas the conduction band is composed of the Pb orbitals. Even without any modification, such as the incorporation of a molecular catalyst, CP1 reduced CO2 into formate under UV light with >99% selectivity.
引用
收藏
页码:13644 / 13652
页数:9
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