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Humidity-Independent Photocatalytic Toluene Mineralization Benefits from the Utilization of Edge Hydroxyls in Layered Double Hydroxides (LDHs): A Combined Operando and Theoretical Investigation
ACS Catalysis ( IF 11.3 ) Pub Date : 2021-06-18 , DOI: 10.1021/acscatal.1c01599 Xing’an Dong 1, 2 , Zhihao Cui 3 , Yanjuan Sun 2 , Fan Dong 1, 2, 4
ACS Catalysis ( IF 11.3 ) Pub Date : 2021-06-18 , DOI: 10.1021/acscatal.1c01599 Xing’an Dong 1, 2 , Zhihao Cui 3 , Yanjuan Sun 2 , Fan Dong 1, 2, 4
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Water vapor (humidity) has been known as one of the important enhancement factors in the photocatalytic degradation of volatile organic compounds (VOCs). In this study, a composite structure of TiO2/Mg–Al layered double hydroxides (LDHs) has been constructed, which displays unique humidity-independent photocatalytic activity. Optimized structure has shown toluene degradation efficiency values as high as 74.3% under a completely dry atmosphere and the degradation efficiency ranges between 73.2% to 84.3% as the humidity increases from 0 to 90%. The origin of humidity-independent photocatalytic activity is investigated by in situ attenuated total reflection (ATR) Fourier transform infrared (FT-IR) spectroscopy, which can distinguish H2O and hydroxyl via different adsorption modes. We found that the OH– would lose electrons and be oxidized into hydroxyl radicals at the edge of LDH to participate in toluene mineralization reaction under light irradiation. The surface structure of the sample can be recovered when the surface hydroxyl is consumed, because of the existence of water vapor. Density functional theory (DFT) theoretical calculations verify that H2O molecules are more likely to dissociate and adsorb through the isolated hydrogen-terminated hydroxyl group (OHT) on LDH surface to generate hydroxyl radicals to participate in toluene photocatalytic degradation under harsh conditions, compared with the case on TiO2 surface. This work introduces a new strategy to promote the efficiency of the photocatalytic degradation of VOCs under a wide range of relative humidity.
中文翻译：
在层状双氢氧化物 (LDH) 中利用边缘羟基使不依赖湿度的光催化甲苯矿化受益：结合操作和理论研究
众所周知，水蒸气（湿度）是挥发性有机化合物（VOCs）光催化降解的重要促进因素之一。在本研究中，构建了 TiO 2 /Mg-Al 层状双氢氧化物 (LDHs) 的复合结构，该结构显示出独特的与湿度无关的光催化活性。优化的结构在完全干燥的气氛下显示出高达74.3%的甲苯降解效率值，当湿度从0增加到90%时，降解效率在73.2%到84.3%之间。通过原位衰减全反射 (ATR) 傅立叶变换红外 (FT-IR) 光谱研究了与湿度无关的光催化活性的起源，该光谱可以区分 H 2O 和羟基通过不同的吸附模式。我们发现，OH -将失去电子，且LDH的边缘被氧化成羟基自由基参与光照射下甲苯矿化反应。由于水蒸气的存在，当表面羟基被消耗时，样品的表面结构可以恢复。密度泛函理论（DFT）理论计算证实，H 2 O分子更容易通过LDH表面孤立的氢端羟基（OH T）解离和吸附，生成羟基自由基参与苛刻条件下的甲苯光催化降解，与 TiO 2的情况相比表面。这项工作引入了一种新策略，可在较宽的相对湿度范围内提高光催化降解 VOC 的效率。
更新日期：2021-07-02
中文翻译：
在层状双氢氧化物 (LDH) 中利用边缘羟基使不依赖湿度的光催化甲苯矿化受益：结合操作和理论研究
众所周知，水蒸气（湿度）是挥发性有机化合物（VOCs）光催化降解的重要促进因素之一。在本研究中，构建了 TiO 2 /Mg-Al 层状双氢氧化物 (LDHs) 的复合结构，该结构显示出独特的与湿度无关的光催化活性。优化的结构在完全干燥的气氛下显示出高达74.3%的甲苯降解效率值，当湿度从0增加到90%时，降解效率在73.2%到84.3%之间。通过原位衰减全反射 (ATR) 傅立叶变换红外 (FT-IR) 光谱研究了与湿度无关的光催化活性的起源，该光谱可以区分 H 2O 和羟基通过不同的吸附模式。我们发现，OH -将失去电子，且LDH的边缘被氧化成羟基自由基参与光照射下甲苯矿化反应。由于水蒸气的存在，当表面羟基被消耗时，样品的表面结构可以恢复。密度泛函理论（DFT）理论计算证实，H 2 O分子更容易通过LDH表面孤立的氢端羟基（OH T）解离和吸附，生成羟基自由基参与苛刻条件下的甲苯光催化降解，与 TiO 2的情况相比表面。这项工作引入了一种新策略，可在较宽的相对湿度范围内提高光催化降解 VOC 的效率。
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