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Insights into the Relationship of the Heterojunction Structure and Excellent Activity: Photo-Oxidative Coupling of Benzylamine on CeO2-rod/g-C3N4 Hybrid under Mild Reaction Conditions
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2018-07-05 00:00:00 , DOI: 10.1021/acssuschemeng.8b01865 Yuanyuan Chai 1 , Lu Zhang 1 , Qianqian Liu 1 , Fengli Yang 1 , Wei-Lin Dai 1
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2018-07-05 00:00:00 , DOI: 10.1021/acssuschemeng.8b01865 Yuanyuan Chai 1 , Lu Zhang 1 , Qianqian Liu 1 , Fengli Yang 1 , Wei-Lin Dai 1
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Oxidation of amines to imines under light irradiation has been widely studied in the field of heterogeneous catalysis. For the first time, we demonstrate a facile mixing calcination approach for the preparation of CeO2/g-C3N4-x as a heterojunction catalyst for the photo-oxidative coupling of benzylamine under the irradiation of a 300 W Xe arc lamp at 308 K with the air balloon. It was found that the rate constant of CeR/CN-66% was 3 times as high as that of pure CeO2 or g-C3N4. All kinds of structural characterizations suggested the formation of heterojunction between the CeO2 and g-C3N4, serving as a tunnel for the transfer of photoinduced charge, which may contribute to the improvement of photoactivity. Moreover, the Ce3+ ions and oxygen vacancy significantly promoted the adsorption and activation of substrate or molecular O2. Therefore, the efficient separation of the charges, the prolonged photoinduced electron lifetime, and the abundant defect structure (increased content of Ce3+ ions or the oxygen vacancy) were considered as the main factors for the higher photo-oxidation efficiency of the CeR/CN-66%. Another striking observation that was noticed was that the CeR/CN-66% was recycled up to five cycles under the same condition and was found to be highly efficient without any obvious decrease in the activity or selectivity due to the outstanding stability of the defect structure. Thus, highly efficient CeR/CN-x heterojunction catalyst was synthesized in this work by a simple approach for the photo-oxidation of benzylamine under mild reaction conditions, and this finding may provide wide applications in other photocatalysis areas.
中文翻译：
深入了解异质结结构与优异活性之间的关系：在轻度反应条件下，苄胺在CeO 2 -rod / g -C 3 N 4杂化物上的光氧化偶联
在非均相催化领域中，在光照射下将胺氧化为亚胺已被广泛研究。首次，我们展示了一种简便的混合煅烧方法，该方法用于制备CeO 2 / g -C 3 N 4 - x作为异质结催化剂，用于在300 W Xe弧光灯照射下苄胺的光氧化偶联。带有气球的308K。发现CeR / CN-66％的速率常数是纯CeO 2或g -C 3 N 4的速率常数的3倍。各种结构特征均表明CeO 2之间形成异质结和g -C 3 N 4，用作光致电荷转移的隧道，这可能有助于光活性的提高。此外，Ce 3+离子和氧空位显着促进了底物或分子O 2的吸附和活化。因此，电荷的有效分离，延长的光诱导电子寿命和丰富的缺陷结构（增加了Ce 3+的含量）离子或氧空位）被认为是CeR / CN-66％较高的光氧化效率的主要因素。另一个引人注目的观察结果是，在相同条件下，CeR / CN-66％可循环使用多达五个周期，并且由于缺陷结构的出色稳定性，发现其效率很高，而活性或选择性没有任何明显下降。 。因此，在这项工作中，通过一种简单的方法在温和的反应条件下对苄胺进行光氧化，合成了高效的CeR / CN- x异质结催化剂，这一发现可能会在其他光催化领域中提供广泛的应用。
更新日期：2018-07-05
中文翻译：
深入了解异质结结构与优异活性之间的关系：在轻度反应条件下，苄胺在CeO 2 -rod / g -C 3 N 4杂化物上的光氧化偶联
在非均相催化领域中，在光照射下将胺氧化为亚胺已被广泛研究。首次，我们展示了一种简便的混合煅烧方法，该方法用于制备CeO 2 / g -C 3 N 4 - x作为异质结催化剂，用于在300 W Xe弧光灯照射下苄胺的光氧化偶联。带有气球的308K。发现CeR / CN-66％的速率常数是纯CeO 2或g -C 3 N 4的速率常数的3倍。各种结构特征均表明CeO 2之间形成异质结和g -C 3 N 4，用作光致电荷转移的隧道，这可能有助于光活性的提高。此外，Ce 3+离子和氧空位显着促进了底物或分子O 2的吸附和活化。因此，电荷的有效分离，延长的光诱导电子寿命和丰富的缺陷结构（增加了Ce 3+的含量）离子或氧空位）被认为是CeR / CN-66％较高的光氧化效率的主要因素。另一个引人注目的观察结果是，在相同条件下，CeR / CN-66％可循环使用多达五个周期，并且由于缺陷结构的出色稳定性，发现其效率很高，而活性或选择性没有任何明显下降。 。因此，在这项工作中，通过一种简单的方法在温和的反应条件下对苄胺进行光氧化，合成了高效的CeR / CN- x异质结催化剂，这一发现可能会在其他光催化领域中提供广泛的应用。
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