钨酸铋担载钯纳米粒子光催化甲苯及其衍生物到醛的氧化反应

doi:10.1016/S1872-2067(17)62757-8

催化学报 ›› 2017, Vol. 38 ›› Issue (3): 440-446.DOI: 10.1016/S1872-2067(17)62757-8

• 能源与环境新型催化剂专栏 • 上一篇下一篇

钨酸铋担载钯纳米粒子光催化甲苯及其衍生物到醛的氧化反应

袁博^a,b, 张宝^a,b, 王志亮^a,b, 卢胜梅^a, 李军^a, 刘龑^a, 李灿^a

a 中国科学院大连化学物理研究所, 辽宁大连 116023;
b 中国科学院大学, 北京 100049

收稿日期:2016-10-27 修回日期:2016-11-20 出版日期:2017-03-18 发布日期:2017-03-22
通讯作者: Yan Liu, Can Li
基金资助:
国家自然科学基金（21322202，21472187）；国家重点基础研究发展计划（2010CB833300）.

Photocatalytic aerobic oxidation of toluene and its derivatives to aldehydes on Pd/Bi₂WO₆

Bo Yuan^a,b, Bao Zhang^a,b, Zhiliang Wang^a,b, Shengmei Lu^a, Jun Li^a, Yan Liu^a, Can Li^a

a State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China;
b University of Chinese Academy of Sciences, Beijing 100049, China

Received:2016-10-27 Revised:2016-11-20 Online:2017-03-18 Published:2017-03-22
Supported by:
This work was supported by the National Natural Science Foundation of China (21322202, 21472187) and the National Basic Research Program of China (2010CB833300).

摘要/Abstract

摘要：

甲苯及其衍生物的选择性氧化是化学工业中重要的一环.氧化产物醛、酮和酸类化合物是各种农药、染料、防腐剂、阻燃剂、香料、塑料的合成中间体.在传统的化工过程中，通常在苛刻的条件下，如高温、高压以及酸性溶剂中进行甲苯的选择性氧化.光催化有机合成作为一种“绿色”的合成方法受到越来越多的关注.我们发现钨酸铋作为可见光响应的光催化剂，可以利用氧气作为氧化剂，对甲苯及其衍生物进行催化氧化反应.通过调节水热法合成钨酸铋的酸碱条件，控制其成核生长过程，改变其形貌，发现在pH值为0.49时，得到花状钨酸铋粉末活性最高.X射线衍射、扫描电镜、紫外可见吸收光谱和比表面测定结果发现，花状钨酸铋粉末表现出最佳的甲苯氧化活性很可能是与它最大的比表面积有关系.为了进一步提高催化的活性，我们将助催化剂担载在钨酸铋粉末上，发现Pd的担载量为0.1 wt%时甲苯氧化反应活性最高.将邻、间、对位甲基取代以及对位甲氧基和氯取代的甲苯衍生物进行反应，发现均可高选择性地得到目标产物.在加入电子牺牲剂硝酸银和空穴牺牲剂草酸铵到反应体系后，发现反应被完全禁阻，说明在甲苯氧化反应过程中电子和空穴都起到了相应的作用.通过电化学测试发现，钯作为助催化剂担载在钨酸铋表面后，产生更强的氧化和还原信号，说明其在电子和空穴发生反应的过程中都起到了相应的促进作用.由此推测，在甲苯的氧化反应中，钨酸铋材料表面吸收可见光，产生光生电子和空穴，而钯的担载则促进了电子和空穴进行氧气还原和甲苯氧化的过程.

关键词: 花状钨酸铋, 甲苯氧化, 苯甲醛, 助催化剂, 钯纳米粒子

Abstract:

The selective oxidation of toluene and its derivatives is extremely important in the chemical industry.The use of photocatalysis in organic synthesis has attracted considerable attention among synthetic chemists because of its “green” environmental characteristics. In this study, nanoscale Bi₂WO₆ with a flower-like morphology was found to be a highly efficient photocatalyst in the catalytic oxidation of toluene and its derivatives using O₂ as the oxidant. The loading of Pd nanoparticles as a cocatalyst onto the flower-like Bi₂WO₆ was found to produce a significant enhancement in the catalytic activity. Mechanistic investigation showed that the superior performance of Pd/Bi₂WO₆ could be attributed to the improvement of both the reductive and oxidative abilities of Bi₂WO₆by the loading of the cocatalyst.

Key words: Flower-like Bi₂WO₆, Toluene oxidation, Benzaldehyde, Cocatalyst, Palladium nanoparticle

袁博, 张宝, 王志亮, 卢胜梅, 李军, 刘龑, 李灿. 钨酸铋担载钯纳米粒子光催化甲苯及其衍生物到醛的氧化反应[J]. 催化学报, 2017, 38(3): 440-446.

Bo Yuan, Bao Zhang, Zhiliang Wang, Shengmei Lu, Jun Li, Yan Liu, Can Li. Photocatalytic aerobic oxidation of toluene and its derivatives to aldehydes on Pd/Bi₂WO₆[J]. Chinese Journal of Catalysis, 2017, 38(3): 440-446.

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钨酸铋担载钯纳米粒子光催化甲苯及其衍生物到醛的氧化反应

Photocatalytic aerobic oxidation of toluene and its derivatives to aldehydes on Pd/Bi₂WO₆

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钨酸铋担载钯纳米粒子光催化甲苯及其衍生物到醛的氧化反应

Photocatalytic aerobic oxidation of toluene and its derivatives to aldehydes on Pd/Bi2WO6

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Photocatalytic aerobic oxidation of toluene and its derivatives to aldehydes on Pd/Bi₂WO₆