Pd/PbTiO<sub>3</sub>表面的热电效应增强光催化Suzuki偶联反应

引用本文: 闻洁雅, 凌丽丽, 陈瑶, 卞振锋. Pd/PbTiO₃表面的热电效应增强光催化Suzuki偶联反应[J]. 催化学报, 2020, 41(10): 1674-1681. doi: 10.1016/S1872-2067(20)63581-1 shu

Citation: Jieya Wen, Lili Ling, Yao Chen, Zhenfeng Bian. Pyroelectricity effect on photoactivating palladium nanoparticles in PbTiO₃ for Suzuki coupling reaction[J]. Chinese Journal of Catalysis, 2020, 41(10): 1674-1681. doi: 10.1016/S1872-2067(20)63581-1 shu

Pd/PbTiO₃表面的热电效应增强光催化Suzuki偶联反应

a 上海师范大学, 资源化学教育部重点实验室, 稀土功能材料上海重点实验室, 上海 200234;
b 上海电力大学, 上海 201303
基金项目:
国家自然科学基金（21876114，217611142011，51572174）和上海市科委（19160712900），资源化学国际合作联合实验室（IJLRC），教育部（PCSIRT_IRT_16R49）.上海市特聘教授（东方学者）和上海市曙光学者.上海绿色能源化工工程研究中心（18DZ2254200）.

摘要: 发展绿色化学技术是21世纪化学研究的一个重要方向，其主要目标是取代那些对环境有害的耗能过程，其中新能源尤其是太阳能开发利用的重要性愈加突显.光催化作为一种低能耗、高效、无二次污染的技术，以其反应条件温和、能直接利用太阳能转化为化学能的优势而备受科研人员关注.光催化技术是利用半导体材料作为催化剂的光催化过程，当能量高于半导体禁带宽度的光子照射半导体材料时，半导体材料上的价带电子发生带间跃迁，从价带跃迁到导带，从而产生带正电荷的光致空穴和带负电荷的光生电子.光致空穴的强氧化能力和光生电子的还原能力导致半导体光催化剂引发一系列光催化反应的发生.光催化选择性氧化还原体系的出现和应用极大地满足了人们对能源和环境的要求.在光催化选择性氧化还原体系中，反应发生所需要的条件比传统催化温和，同时它也避免了一些危险的强氧化剂和还原性物质的使用.但是在一些过程中，催化反应常常需要在高温下进行.传统加热是由外部热源通过热辐射由表及里的热传导的方式进行的，并且为了达到催化温度，需使催化剂床层整体升温.而微波诱导的催化方法与常规不同，微波不仅加热速度快、能源利用率高，而且加热均匀、温度梯度小，因此微波化学作为一门新兴的前沿交叉学科，已在广泛的实际应用中显示出强大的生命力.将光催化技术与微波联用可能会取得意想不到的成果.
微波与光催化系统相结合是抑制光生电子-空穴复合并增强光催化反应性能的一种有效方法.本文通过简单的水热反应制备了单晶PbTiO₃纳米片.由XRD谱可以看出，所有衍射峰均归属于四方钙钛矿相PbTiO₃，紫外-可见漫反射光谱表明单晶PbTiO₃在紫外光区域有强吸收，在400-450nm处还存在微弱的可见光吸收.另外，负载了Pd纳米颗粒之后，在可见光区域吸收明显增强.这说明我们成功制备了一种既能利用微波又能利用光催化的Pd/PbTiO₃催化剂.利用PbTiO₃晶体的热释电效应在微波场下与紫外光协同促进以溴苯引导的Suzuki偶联反应发生，反应速度和选择性显著提高.在微波场和紫外光的协同作用下，PbTiO₃晶体的热电效应可以将热能转换为电能，产生正电荷和负电荷（q⁺和q^-），而Pd纳米粒子则显著提高了光催化过程的量子效率.光催化技术协同微波场可以直接作用于有机化学反应，以独特的方式促进甚至改变各种化学反应过程.

关键词:

English

Pyroelectricity effect on photoactivating palladium nanoparticles in PbTiO₃ for Suzuki coupling reaction

a The Education Ministry Key Laboratory of Resource Chemistry and Shanghai Key Laboratory of Rare Earth Functional Materials, Shanghai Normal University, Shanghai 200234, China;
b Shanghai University of Electric Power, Shanghai 201303, China
Received Date: 21 February 2020
Revised Date: 25 March 2020
Fund Project:
This work was supported by the National Natural Science Foundation of China (21876114, 21761142011, 51572174), Shanghai Government (19160712900), International Joint Laboratory on Resource Chemistry (IJLRC), and Ministry of Education of China (PCSIRT_IRT_16R49). Research is also supported by The Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning and Shuguang Research Program of Shanghai Education Committee. Shanghai Engineering Research Center of Green Energy Chemical Engineering (18DZ2254200).

Abstract: Combining microwave radiation with photocatalytic systems is a promising method to inhibit photogenerated electron-hole recombination and enhance the photocatalytic reaction performance. In this study, we have designed Pd/PbTiO₃ catalysts that can use both microwave fields and photocatalysis. Benefiting from the synergistic effect of microwave field and UV light, the PbTiO₃ crystals convert thermal energy into electrical energy via the pyroelectricity effect, generating positive and negative charges (q⁺ and q^-), while Pd nanoparticles significantly improve the quantum efficiency of the photocatalytic process. The composite catalyst significantly enhances the reaction rate and selectivity of the model Suzuki coupling reaction performed with bromobenzene. Microwave fields can directly act on chemical systems, promoting or changing various chemical reactions in unique ways.

Key words:

1. [1] E. Menachem, W. A. Phillip, Science, 2011, 333, 712-717.
2. [2] J. Fu, Y. L. Tian, B. B. Chang, F. N. Xi, J. Mater. Chem., 2012, 22, 21159-21166.
3. [3] Y. Chen, X. M. Deng, J. Y. Wen, J. Zhu, Z. F. Bian, Appl. Catal. B, 2019, 258, 118024.
4. [4] L. L. Ling, L. F. Liu, Y. W. Feng, J. Zhu, Z. F. Bian, Chin. J. Catal., 2018, 39, 639-645.
5. [5] G. Palmisano, V. Augugliaro, M. Pagliaro, L. Palmisano, Chem. Commun., 2007, 33, 3425-3437.
6. [6] X. M. Deng, Y. Chen, J. Y. Wen, Y. Xu, J. Zhu, Z. F. Bian, Sci. Bull., 2020, 65, 105-112.
7. [7] A. Fujishima, T. N. Rao, D. A. Tryk, J. Photochem. Photobiol. C, 2000, 1, 1-21.
8. [8] N. Hoffmann, ChemSusChem, 2012, 5, 352-371.
9. [9] Y. X. Zhang, M. J. Xu, H. X. Li, H. Ge, Z. F. Bian, Appl. Catal. B, 2018, 226, 213-219.
10. [10] M. J. Xu, Y. Chen, J. T. Qin, Y. W. Feng, W. Li, W. Chen, J. Zhu, H. X. Li, Z. F. Bian, Environ. Sci. Technol., 2018, 52, 13879-13886.
11. [11] H. Frank, T. Andreas, S. Frank, M. T. Reetz, Angew. Chem. Int. Ed., 2010, 46, 2903-2906.
12. [12] H. Shimizu, S. Onitsuka, H. Egami, T. Katsuki, J. Am. Chem. Soc., 2005, 127, 5396-5413.
13. [13] A. Dhakshinamoorthy, H. Garcia, Chem. Soc. Rev., 2014, 43, 5750-5765.
14. [14] Z. M. Xu, R. Zheng, Y. Chen, J. Zhu, Z. F. Bian, Chin. J. Catal., 2019, 40, 631-637.
15. [15] N. Hoffmann, Aust. J. Chem., 2015, 68, 1621-1639.
16. [16] Z. Wu, F. Xiong, Z. Wang, W. Huang, Chin. Chem. Lett., 2018, 29, 752-756.
17. [17] Y. Feng, H. Li, Ling, S. Yan, D. L. Pan, H. Ge, H. X. Li, Z. F. Bian, Environ. Sci. Technol., 2018, 52, 7842-7848.
18. [18] Y. W. Feng, L. L. Ling, J. Nie, K. Han, X. Chen, Z. F. Bian, H. X. Li, Z. L. Wang, ACS Nano, 2017, 11, 12411-12418.
19. [19] L. L. Ling, Y. W. Feng, H. Li, Y. Chen, J. Y. Wen, J. Zhu, Z. F. Bian, Appl. Surf. Sci., 2019, 483, 772-778.
20. [20] W. Zhang, X. Wang, X. Fu, Chem. Commun., 2003, 9, 2196-2197.
21. [21] S. Horikoshi, H. Tsutsumi, H. Matsuzaki, A. Furube, A. V. Emeline, N. Serpone, J. Mater. Chem. C, 2015, 3, 5958-5969.
22. [22] D. Z. Li, Acta Phys.-Chim. Sin., 2002, 18, 332-335.
23. [23] W. Liao, T. Zheng, P. Wang, S. Tu, W. Pan, J. Environ. Sci. 2010, 22, 1800-1806.
24. [24] Y. L. Zi, L. Lin, J. Wang, S. H. Wang, J. Chen, X. Fan, P.-K. Yang, F. Yi, Z. L. Wang, Adv. Mater., 2015, 27, 2340-2347.
25. [25] R. A. Arndt, A. C. Damask, J. Chem. Phys., 1966, 45, 4627-4633.
26. [26] S. B. Lang, Br. Ceram. Trans., 2004, 103, 65-70.
27. [27] N. Guarrotxena, N. Vella, A. Toureille, J. L. Millán, Macromol. Chem. Phys., 1997, 198, 457-469.
28. [28] B. S. Kang, S. K. Choi, C. H. Park, J. Appl. Phys., 2003, 94, 1904-1911.
29. [29] J. F. Nye, Physical Properties of Crystals, Clarendon Press, Oxford, 1957.
30. [30] S. Bauer, S. B. Lang, IEEE Trans. Dielectr. Electr. Insul., 1996, 3, 647-676.
31. [31] Y. Yang, J. H. Jung, B. K. Yun, F. Zhang, K. C. Pradel, W. X. Guo, Z. L. Wang, Advanced Materials, 2012, 24, 5357-5362.
32. [32] M. A. Green, S. P. Bremner, Nat. Mater., 2016, 16, 23-34.
33. [33] C. Pavithra, W. Madhuri, J. Sol-Gel Sci. Technol., 2018, 85, 437-445.
34. [34] E. P. Smirnova, G. Yu. Sotnikova, N. V. Zaitseva, G. A. Gavrilov, A. V. Sotnikov, Phys. Solid State, 2019, 10, 1766-1771.
35. [35] Z. H. Dai, J. L. Xie, W. G. Liu, S. B. Ge, M. X. Fang, D. B. Lin, L. X. Pang, H. F. Ji, S. Zhou, X. B. Ren, Mater. Lett., 2019, 241, 55-59.
36. [36] D. Zekria, A. M. Glazer, V. Shuvaeva, J. Appl. Crystallogr., 2010, 37, 551-554.
37. [37] G. Xu, X. Huang, V. Krstic, S. Chen, X. Yang, C. Chao, G. Shen, G. Han, CrystEngComm, 2014, 16, 4373-4376.
38. [38] Y. F. Li, Z. P. Liu, J. Am. Chem. Soc., 2011, 133, 15743-15752.
39. [39] P. Dong, Y. Wang, H. Li, H. Li, X. Ma, L. Han, J. Mater. Chem. A, 2013, 1, 4651-4656.
40. [40] X. Meng, H. Qin, Z. Zhang, J. Colloid Interface Sci., 2018, 513, 877-890.
41. [41] M. Kurasawa, P. C. McLntyre, J. Appl. Phys., 2005, 97, 104110.

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Pd/PbTiO₃表面的热电效应增强光催化Suzuki偶联反应

English

Pyroelectricity effect on photoactivating palladium nanoparticles in PbTiO₃ for Suzuki coupling reaction

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Pd/PbTiO3表面的热电效应增强光催化Suzuki偶联反应

English

Pyroelectricity effect on photoactivating palladium nanoparticles in PbTiO3 for Suzuki coupling reaction

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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中国化学会秘书处

Pd/PbTiO₃表面的热电效应增强光催化Suzuki偶联反应

Pyroelectricity effect on photoactivating palladium nanoparticles in PbTiO₃ for Suzuki coupling reaction

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs