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Copolymerization Approach to Improving Ru(II)-Complex/C3N4 Hybrid Photocatalysts for Visible-Light CO2 Reduction
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2018-10-16 00:00:00 , DOI: 10.1021/acssuschemeng.8b03782 Constantine Tsounis 1 , Ryo Kuriki 2, 3 , Kengo Shibata 2 , Junie Jhon M. Vequizo 4 , Daling Lu 5 , Akira Yamakata 4 , Osamu Ishitani 2 , Rose Amal 1 , Kazuhiko Maeda 2
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2018-10-16 00:00:00 , DOI: 10.1021/acssuschemeng.8b03782 Constantine Tsounis 1 , Ryo Kuriki 2, 3 , Kengo Shibata 2 , Junie Jhon M. Vequizo 4 , Daling Lu 5 , Akira Yamakata 4 , Osamu Ishitani 2 , Rose Amal 1 , Kazuhiko Maeda 2
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Copolymerized carbon nitride nanosheets (NS-C3N4) were used as a light absorbing unit while paired with a Ru(II) complex that served as a catalyst for CO2 reduction, forming a hybrid photocatalytic system. Copolymerization with urea and phenylurea in air at 823 K resulted in a carbon nitride material that had wide visible light absorption extending to 650 nm, significantly red-shifted compared to the absorption edge of pristine NS-C3N4, an analogue prepared with only urea (ca. 435 nm). While a hybrid system consisting of pristine NS-C3N4 was found to be inactive under longer wavelength visible light (λ > 500 nm) due to its large band gap, the copolymerized material was able to catalytically convert CO2 to HCOOH under λ > 500 nm irradiation. Furthermore, its activity toward HCOOH production is doubled under λ > 400 nm irradiation after 5 h compared to pristine NS-C3N4. Transient absorption spectroscopy clearly showed improved lifetime of photogenerated free (and/or shallowly trapped) electrons, which should be the key to enhancing the photocatalytic activity of this hybrid system even under shorter wavelength visible light.
中文翻译：
改善Ru（II）-Complex / C 3 N 4杂化光催化剂用于可见光CO 2还原的共聚方法
将共聚的氮化碳纳米片（NS-C 3 N 4）用作光吸收单元，同时与用作CO 2还原催化剂的Ru（II）配合物配对，形成混合光催化体系。在空气中以823 K与尿素和苯脲共聚，生成的氮化碳材料的可见光吸收范围宽至650 nm，与原始NS-C 3 N 4的吸收边相比，红光显着红移，而NS-C 3 N 4仅用尿素（约435 nm）。而由原始NS-C 3 N 4组成的混合系统已知由于其较大的带隙，在较长波长的可见光（λ> 500 nm）下无活性，共聚的材料能够在λ> 500 nm的辐射下将CO 2催化转化为HCOOH。此外，与原始NS-C 3 N 4相比，在5 h后的λ> 400 nm辐射下，其对HCOOH产生的活性增加了一倍。瞬态吸收光谱法清楚地显示了光生自由（和/或浅陷）电子的寿命延长，即使在较短波长的可见光下，这也应该是增强该杂化系统光催化活性的关键。
更新日期：2018-10-16
中文翻译：
改善Ru（II）-Complex / C 3 N 4杂化光催化剂用于可见光CO 2还原的共聚方法
将共聚的氮化碳纳米片（NS-C 3 N 4）用作光吸收单元，同时与用作CO 2还原催化剂的Ru（II）配合物配对，形成混合光催化体系。在空气中以823 K与尿素和苯脲共聚，生成的氮化碳材料的可见光吸收范围宽至650 nm，与原始NS-C 3 N 4的吸收边相比，红光显着红移，而NS-C 3 N 4仅用尿素（约435 nm）。而由原始NS-C 3 N 4组成的混合系统已知由于其较大的带隙，在较长波长的可见光（λ> 500 nm）下无活性，共聚的材料能够在λ> 500 nm的辐射下将CO 2催化转化为HCOOH。此外，与原始NS-C 3 N 4相比，在5 h后的λ> 400 nm辐射下，其对HCOOH产生的活性增加了一倍。瞬态吸收光谱法清楚地显示了光生自由（和/或浅陷）电子的寿命延长，即使在较短波长的可见光下，这也应该是增强该杂化系统光催化活性的关键。
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