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Nonoxidative coupling of ethane with gold loaded photocatalysts

机译:乙烷与金载的光催化剂的非氧化偶联

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Direct and continuous conversion of ethane to yield n-butane and hydrogen at near room temperature (ca. 320 K) was examined with gold loaded gallium oxide and titanium dioxide photocatalysts without the aid of any oxidant in a flow reactor. A Ga2O3 photocatalyst produced n-butane and ethene as well as hydrogen with an almost stoichiometric ratio of products from ethane. Loading Au on the Ga2O3 sample gave a 12 times higher production rate of n-butane such as 0.65 μmol h−1 with a high selectivity of 89%. Although a bare TiO2 sample showed very low yield due to poor reduction resistance, the addition of an Au cocatalyst drastically improved the photocatalytic performance of the TiO2 sample, i.e., the Au(0.2)/TiO2 sample produced n-butane and ethene continuously at least for 5 h, where the production rate of n-butane, the n-butane selectivity, and the apparent quantum efficiency (AQE) for n-butane formation were 0.92 μmol h−1, 92%, and 0.02%, respectively. The reaction mechanism of n-butane formation as the main reaction was proposed to be the photocatalytic nonoxidative coupling of ethane (NOCE), which is similar to the photocatalytic nonoxidative coupling of methane (NOCM).
机译:乙烷在近室温度(大约320 K)下向乙烷的直接转化为N-丁烷和氢,并使用金氧化韧带和二氧化钛光催化剂检查,而无需在流动反应器中任何氧化剂。 GA2O3光催化剂产生了N-丁烷和乙烯以及乙烷产物几乎化学计量比的氢。在GA2O3样品上加载AU的N-丁烷的生产速率高12倍,例如0.65μmolH-1,高选择性为89%。尽管裸露的TiO2样品由于耐药性降低而显示出非常低的产量,但添加Au cocatalyst可极大地改善TiO2样品的光催化性能,即Au(0.2)/TiO2样品,至少会连续产生N-丁烯和乙烯在5小时内,N-丁烷的生产速率,N-丁烷选择性和N-丁烷形成的明显量子效率(AQE)分别为0.92μmolH-1、92%和0.02%。提议N-丁烷形成为主要反应的反应机理是乙烷的光催化非氧化偶联(NOCE),该偶联与甲烷(NOCM)的光催化非氧化偶联相似。

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