Highly Robust Hybrid Photocatalyst for Carbon Dioxide Reduction: Tuning and Optimization of Catalytic Activities of Dye/TiO2/Re(I) Organic–Inorganic Ternary Systems,Journal of the American Chemical Society

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Highly Robust Hybrid Photocatalyst for Carbon Dioxide Reduction: Tuning and Optimization of Catalytic Activities of Dye/TiO2/Re(I) Organic–Inorganic Ternary Systems
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2015-10-16 , DOI: 10.1021/jacs.5b08890
Dong-Il Won ₁ , Jong-Su Lee ₁ , Jung-Min Ji ₁ , Won-Jo Jung ₁ , Ho-Jin Son ₁ , Chyongjin Pac ₁ , Sang Ook Kang ₁

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Herein we report a detailed investigation of a highly robust hybrid system (sensitizer/TiO2/catalyst) for the visible-light reduction of CO2 to CO; the system comprises 5'-(4-[bis(4-methoxymethylphenyl)amino]phenyl-2,2'-dithiophen-5-yl)cyanoacrylic acid as the sensitizer and (4,4'-bis(methylphosphonic acid)-2,2'-bipyridine)Re(I)(CO)3Cl as the catalyst, both of which have been anchored on three different types of TiO2 particles (s-TiO2, h-TiO2, d-TiO2). It was found that remarkable enhancements in the CO2 conversion activity of the hybrid photocatalytic system can be achieved by addition of water or such other additives as Li(+), Na(+), and TEOA. The photocatalytic CO2 reduction efficiency was enhanced by approximately 300% upon addition of 3% (v/v) H2O, giving a turnover number of ≥570 for 30 h. A series of Mott-Schottky (MS) analyses on nanoparticle TiO2 films demonstrated that the flat-band potential (V(fb)) of TiO2 in dry DMF is substantially negative but positively shifts to considerable degrees in the presence of water or Li(+), indicating that the enhancement effects of the additives on the catalytic activity should mainly arise from optimal alignment of the TiO2 V(fb) with respect to the excited-state oxidation potential of the sensitizer and the reduction potential of the catalyst in our ternary system. The present results confirm that the TiO2 semiconductor in our heterogeneous hybrid system is an essential component that can effectively work as an electron reservoir and as an electron transporting mediator to play essential roles in the persistent photocatalysis activity of the hybrid system in the selective reduction of CO2 to CO.

中文翻译：

用于二氧化碳还原的高强度杂化光催化剂：染料/TiO2/Re(I) 有机-无机三元体系催化活性的调整和优化

在此，我们报告了对用于将 CO2 可见光还原为 CO 的高度稳健的混合系统（敏化剂/TiO2/催化剂）的详细研究；该体系包含5'-(4-[双(4-甲氧基甲基苯基)氨基]苯基-2,2'-二噻吩-5-基)氰基丙烯酸作为敏化剂和(4,4'-双(甲基膦酸)-2 ,2'-联吡啶)Re(I)(CO)3Cl 作为催化剂，两者都锚定在三种不同类型的 TiO2 颗粒（s-TiO2、h-TiO2、d-TiO2）上。研究发现，通过添加水或 Li(+)、Na(+) 和 TEOA 等其他添加剂，可以显着提高混合光催化系统的 CO2 转化活性。添加 3% (v/v) H2O 后，光催化 CO2 还原效率提高了约 300%，30 小时内的周转数≥570。

更新日期：2015-10-16

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