化学
光催化
氮化碳
可见光谱
六价铬
催化作用
太阳能燃料
量子产额
光化学
电子转移
石墨氮化碳
铬
无机化学
有机化学
荧光
物理
光电子学
材料科学
量子力学
作者
Sujeong Kim,Gun‐hee Moon,Hye-Jin Kim,Yeongdong Mun,Peng Zhang,Jun Young Lee,Wonyong Choi
标识
DOI:10.1016/j.jcat.2017.10.002
摘要
Photochemical production of H2O2 through O2 reduction has been proposed as an alternative method of solar energy storage. A carbon nitride (CN) photocatalyst was selected for this purpose. The incorporation of KPF6 into the CN structure greatly enhanced the apparent quantum yield (AQY) of H2O2 production in the UV and visible light region. The AQY of KPF6-modified CN was measured to be 35.9% and 24.3% under monochromatic irradiation at 370 and 420 nm, respectively, which are 8.3 and 26.1 times higher than for bare CN. The KPF6-enhanced activity is ascribed to several factors including (i) enhanced absorption of UV and visible light, (ii) higher charge carrier density, (iii) retarded radiative recombination of charge pairs, (iv) highly selective two-electron transfer to O2, and (v) hindered photodecomposition of in-situ generated H2O2. The markedly high selectivity of KPF6-modified CN toward the two-electron reduction of O2 (leading to H2O2) was demonstrated in comparision with other photoreductive conversions such as the reduction of polyoxometalate (POM → POM−), hexavalent chromium (CrVI → CrIII), CCl4 (dechlorination), and protons (H2 production). This study developed a simple method of efficient production of H2O2 using visible light, which could be utilized for a variety of applications that employ H2O2 as a solar fuel or a green oxidant.
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