化工学报 ›› 2021, Vol. 72 ›› Issue (8): 4166-4176.doi: 10.11949/0438-1157.20210172

• 催化、动力学与反应器 • 上一篇    下一篇

构建Bi2O2CO3/g-C3N4异质结光催化完全氧化苯甲醇至苯甲醛

李燕1(),蹇亮1,茅沁怡1,潘成思1,蒋平平1,朱永法2,董玉明1()   

  1. 1.江南大学化学与材料工程学院,光响应功能分子材料国家级国际联合研究中心,江苏 无锡 214122
    2.清华大学化学系,北京 100084
  • 收稿日期:2021-01-26 修回日期:2021-05-07 出版日期:2021-08-05 发布日期:2021-08-05
  • 通讯作者: 董玉明 E-mail:1911428406@qq.com;dongym@jiangnan.edu.cn
  • 作者简介:李燕(1996—),女,硕士研究生,1911428406@qq.com
  • 基金资助:
    国家自然科学基金项目(21676123);江苏省自然科学基金项目(BK20161127)

Construction of Bi2O2CO3/g-C3N4 heterojunction photocatalytic complete oxidation of benzyl alcohol to benzaldehyde

Yan LI1(),Liang JIAN1,Qinyi MAO1,Chengsi PAN1,Pingping JIANG1,Yongfa ZHU2,Yuming DONG1()   

  1. 1.School of Chemical and Material Engineering, Jiangnan University, International Joint Research Center for Photoresponsive Molecules and Materials, Wuxi 214122, Jiangsu, China
    2.Department of Chemistry, Tsinghua University, Beijing 100084, China
  • Received:2021-01-26 Revised:2021-05-07 Published:2021-08-05 Online:2021-08-05
  • Contact: Yuming DONG E-mail:1911428406@qq.com;dongym@jiangnan.edu.cn

摘要:

在保证选择性的前提下高效光催化氧化苯甲醇为苯甲醛仍然是当下面临的一个巨大挑战。g-C3N4的价带位置适中,具有温和的氧化能力,已被开发用来光催化氧化苯甲醇以保证反应的选择性,但由于其电子空穴复合率高导致反应的转化率难以提升。由于Bi2O2CO3的超薄片层结构不仅可以增加催化剂的比表面积形成更多的活性中心,同时可以形成局部电场,更有效地分离光生电子-空穴对,因此通过构建Bi2O2CO3/g-C3N4异质结来加快光生载流子分离进而提升反应速率。其中最优的催化剂可以在反应9 h后使苯甲醇完全氧化为苯甲醛,降低了分离成本。

关键词: 异质结, 氧化, 光化学, 醇, 苯甲醛

Abstract:

Under the premise of ensuring selectivity, high-efficiency photocatalytic oxidation of benzyl alcohol to benzaldehyde is still a huge challenge. g-C3N4 has a moderate valence band position and mild oxidation ability. It has been developed for photocatalytic oxidation of benzyl alcohol to ensure the selectivity of the reaction, but the high electron-hole recombination rate makes it difficult to increase the conversion rate of the reaction. In this work, alternate Bi2O22+ and CO32- orthogonal symbiotic layer within Bi2O2CO3 can not only increase the specific surface area of catalyst to form more active center, but also can construct local electric field to separate electronic-hole pair more efficiently. Therefore, we build the Bi2O2CO3/g-C3N4 heterojunction structure to speed up the carrier separation to enhance the reaction rate. The best photocatalyst can achieve both 100% selectivity and conversion after 9 h reaction, which reduces the cost of separation and has a huge development prospect. In this paper, the in-situ construction of the heterojunction accelerates the charge separation to promote the reaction. Its preparation method, reaction mechanism, energy level structure, etc., all have a certain guiding role in organic conversion reactions.

Key words: heterojunction, oxidation, photochemistry, alcohol, benzaldehyde

中图分类号: 

  • O 643

图1

催化剂形貌表征(a),(b) 1.5-Bi2O2CO3/g-C3N4 的SEM图;(c)~(e) g-C3N4、Bi2O2CO3、1.5-Bi2O2CO3/g-C3N4 的TEM图; (f) 1.5-Bi2O2CO3/g-C3N4 的高分辨透射电镜图"

图2

g-C3N4与1.5-Bi2O2CO3/g-C3N4的N2吸附-解吸等温线(a)和相应的孔径分布曲线(b)"

图3

g-C3N4、Bi2O2CO3、x-Bi2O2CO3/g-C3N4 (x=0.5、1.5、2.5、3.5)的XRD谱图"

图4

1.5-Bi2O2CO3/g-C3N4 中 C 1s (a)、 N 1s (b)、 O 1s (c)、 Bi 4f (d)的高分辨率XPS光谱图"

图5

Bi2O2CO3、g-C3N4及1.5-Bi2O2CO3/g-C3N4的紫外-可见漫反射吸收光谱图(a); Bi2O2CO3、g-C3N4的Tauc曲线 (b); g-C3N4 (c)和 Bi2O2CO3 (d) 的Mott-Schottky图"

图6

g-C3N4、Bi2O2CO3、x-Bi2O2CO3/g-C3N4 (x=0.5、1.5、2.5、3.5)反应活性对比[测试条件:30 mg催化剂,300 W氙灯(AM 1.5G),光照时间4 h](a); 1.5-Bi2O2CO3/g-C3N4在相同条件下的延长反应时间转化率(b); 1.5-Bi2O2CO3/g-C3N4的稳定性测试[测试条件:30 mg催化剂,300 W氙灯(AM 1.5G),光照时间4 h](c); 1.5-Bi2O2CO3/g-C3N4在反应过程中的自由基捕获实验 (d)"

表1

选择性光催化苯甲醇氧化的相关文献"

序号催化剂反应条件选择性/%转化率/%文献
1TiO2@COFwhite light LED, 30 h99.992.5[12]
2Au-Pd/ZnIn2S4λ> 420 nm, 10 h>9990.6[45]
3NH2-MIL-125(Ti)white light LED, 40 h>9988[46]
4N-vacancy-g-C3N4AM 1.5, 9 h>9968.3[20]
5CdS@SnO2;λ> 420 nm, 8 h9878[47]
6Au-BiOCl-OVλ> 420 nm, 8 h>9975.6[19]
7Bi4O5Br2blue LED, 24 h>9999.1[48]
8Bi2O2CO3/g-C3N4AM 1.5, 9 h>99.9>99.9本工作

图7

g-C3N4、Bi2O2CO3及1.5-Bi2O2CO3/g-C3N4光催化剂的稳态荧光光谱(a)、时间分辨荧光光谱(b)、瞬态光电流谱图(c)和阻抗谱图(d)"

图8

光催化氧化苯甲醇反应机理"

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