Structure-Activity Relationships in Bulk Polymeric and Sol-Gel-Derived Carbon Nitrides during Photocatalytic Hydrogen Production

被引：96

作者：

Hollmann, Dirk ^{[1
]}

Karnahl, Michael ^{[1
]}

Tschierlei, Stefanie ^{[2
]}

Kailasam, Kamalakannan ^{[3
]}

Schneider, Matthias ^{[1
]}

Radnik, Joerg ^{[1
]}

Grabow, Kathleen ^{[1
]}

Bentrup, Ursula ^{[1
]}

Junge, Henrik ^{[1
]}

Beller, Matthias ^{[1
]}

Lochbrunner, Stefan ^{[2
]}

Thomas, Arne ^{[3
]}

Brueckner, Angelika ^{[1
]}

机构：

[1] Univ Rostock, Leibniz Inst Catalysis, Albert Einstein Str 29A, D-18059 Rostock, Germany

[2] Univ Rostock, Inst Phys, D-18055 Rostock, Germany

[3] Tech Univ Berlin, Inst Chem, Fak 2, D-10623 Berlin, Germany

来源：

CHEMISTRY OF MATERIALS | 2014年 / 26卷 / 04期

关键词：

VISIBLE-LIGHT IRRADIATION; METAL-FREE CATALYSTS; ARTIFICIAL PHOTOSYNTHESIS; THERMAL CONDENSATION; WATER REDUCTION; MELAMINE; EVOLUTION; G-C3N4; PHOTODEGRADATION; POLYANILINE;

D O I：

10.1021/cm500034p

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Photocatalytic hydrogen evolution rates and structural properties as well as charge separation, electron transfer, and stabilization have been analyzed in advanced sol-gel-derived carbon nitrides (SG-CN) pyrolyzed at different temperatures (350-600 degrees C) and in bulk polymeric carbon nitride reference samples (CN) by XRD, XPS, FTIR, UV-vis, Raman, and photoluminescence as well as by in situ EPR spectroscopy. SG-CN samples show about 20 times higher H-2 production rates than bulk CN. This is due to their porous structure, partial disorder, and high surface area which favor short travel distances and fast trapping of separated electrons on the surface where they are available for reaction with protons. In contrast, most of the excited electrons in bulk polymeric CN return quickly to the valence band upon undesired emission of light, which is responsible for their low catalytic activity.

引用

页码：1727 / 1733

页数：7

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