ZIF-8衍生的具有可控氧空位的ZnO对光催化去除NO的增强及毒性NO2形成的抑制

doi:10.1016/S1872-2067(20)63592-6

催化学报 ›› 2021, Vol. 42 ›› Issue (1): 175-183.DOI: 10.1016/S1872-2067(20)63592-6

ZIF-8衍生的具有可控氧空位的ZnO对光催化去除NO的增强及毒性NO₂形成的抑制

朱鹏飞^a^,^#(), 尹晓荷^a, 高新华^b, 董国辉^a, 徐景坤^c, 王传义^a^,^c^,^*()

^a陕西科技大学环境科学与工程学院, 陕西西安710021
^b宁夏大学省部共建煤炭高效利用与绿色化工国家重点实验室, 宁夏银川750021
^c江西科技师范大学柔性电子创新研究院, 江西南昌330013

收稿日期:2020-02-29 接受日期:2020-04-21 出版日期:2021-01-18 发布日期:2021-01-18
通讯作者: 朱鹏飞,王传义
基金资助:
中华人民共和国国家外专局高端外国专家项目(#G20190241013);德国洪堡基金会研究小组联动计划;陕西省教育厅专项科研计划项目(17JK0094);陕西科技大学博士启动基金(2016BJ-20);煤炭高效利用与绿色化工国家重点实验室开放课题(2018-K26)

Enhanced photocatalytic NO removal and toxic NO₂ production inhibition over ZIF-8-derived ZnO nanoparticles with controllable amount of oxygen vacancies

Pengfei Zhu^a^,^#(), Xiaohe Yin^a, Xinhua Gao^b, Guohui Dong^a, Jingkun Xu^c, Chuanyi Wang^a^,^c^,^*()

^aSchool of Environmental Science and Engineering, Shaanxi University of Science and Technology, Xi’an 710021, Shaanxi, China
^bState Key Laboratory of High-Eﬃciency Utilization of Coal and Green Chemical Engineering, College of Chemistry & Chemical Engineering, Ningxia University, Yinchuan 750021, Ningxia, China
^cFlexible Electronics Innovation Institute (FEII), Jiangxi Science & Technology Normal University, Nanchang 330013, Jiangxi, China

Received:2020-02-29 Accepted:2020-04-21 Online:2021-01-18 Published:2021-01-18
Contact: Pengfei Zhu,Chuanyi Wang
About author:^#E-mail: zhupengfei@sust.edu.cn
^*Tel: +86-13299131206; E-mail: wangchuanyi@sust.edu.cn;
Supported by:
SAFEA of China (High-end foreign expert project)(#G20190241013);Research Group Linkage Program of the Alexander von Humboldt Foundation of Germany;Scientific Research Program Funded by Shaanxi Provincial Education Department(17JK0094);Doctoral Starting up Foundation of Shaanxi University of Science and Technology(2016BJ-20);Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering(2018-K26)

摘要/Abstract

摘要：

氧化锌作为一种半导体材料, 具有合适的能带结构位置, 高催化效率, 低成本和环境可持续性, 因而广泛用于光催化领域. 然而, 由于氧化锌的宽带隙, 可见光吸收能力差以及光生电子-空穴对的快速复合, 极大地影响了其光催化效率. 通过引入氧空位调控光催化剂的结构被证明是一种可以改善光生载流子的分离, 从而提高光催化性能的有效方法.
本文以ZIF-8为前驱体, 采用两步煅烧法合成了具有不同浓度氧空位分布的ZnO纳米光催化剂, 通过X射线衍射(XRD)、扫描电镜(SEM)、透射电镜(TEM)、紫外-可见漫反射光谱(UV-Vis DRS)、X射线光电子能谱(XPS)、电子顺磁共振(EPR)、荧光光谱仪(PL)等手段系统地分析了合成的光催化剂的理化性质, 并评价了它们在可见光下光催化氧化去除NO反应性能.
EPR结果表明, 样品中氧空位的浓度取决于温度处理的过程. 通过两步煅烧法得到氧化锌中氧空位的含量高于一步直接煅烧法所得的样品. 此外, 随着煅烧温度升高, 合成的氧化锌晶格越完好, 其氧空位含量越少. UV-Vis DRS结果表明, 两步煅烧法合成的ZnO与商业的ZnO及一步法直接煅烧合成的ZnO相比, 其吸光范围从紫外光拓展到了可见光, 表现出了更加优异的吸光性能. 光催化反应结果表明, 与商业氧化锌和一步直接煅烧法所得样品相比, 两步煅烧法合成的样品表现出了更优异的光催化去除NO性能, 并抑制了中间产物毒性NO₂的产生, 促进了NO的深度氧化. 具体反应路径为: 在光照过程中, 光生电子很容易被氧空位俘获, 与O₂反应产生更多的超氧自由基(∙O₂^-), 从而将NO氧化成最终的产物硝酸盐. 尤其有趣的是, 先在350 ^oC煅烧2小时再400 ^oC煅烧1小时的两步法样品Z 350-400的NO去除效率分别比一步法样品Z 400(400 ^oC煅烧)和商用ZnO高出1.5和4.6倍. 这表明以MOF材料衍生的具有适当量氧空位的金属氧化物为一种高效去除NO的光催化剂具有很好的应用前景.

关键词: 光催化去除NO, ZIF-8, 氧化锌, 氧空位, 温度处理

Abstract:

The controlled introduction of oxygen vacancies (OVs) in photocatalysts has been demonstrated to be an efficient approach for improving the separation of photogenerated charge carriers, and thus, for enhancing the photocatalytic performance of photocatalysts. In this study, a two-step calcination method where ZIF-8 was used as the precursor was explored for the synthesis of ZIF-8-derived ZnO nanoparticles with gradient distribution of OVs. Electron paramagnetic resonance measurements indicated that the concentration of OVs in the samples depended on the temperature treatment process. Ultraviolet-visible spectra supported that the two-step calcined samples presented excellent light-harvesting ability in the ultraviolet-to-visible light range. Moreover, it was determined that the two-step calcined samples presented superior photocatalytic performance for the removal of NO, and inhibited the generation of NO₂. These properties could be attributed to the contribution of the OVs present in the two-step calcined samples to their photocatalytic performance. The electrons confined by the OVs could be transferred to O₂ to generate superoxide radicals, which could oxidize NO to the final product, nitrate. In particular, the NO removal efficiency of Z 350-400 (which was a sample first calcined at 350 °C for 2 h, then at 400 °C for 1 h) was 1.5 and 4.6 times higher than that of Z 400 (which was one-step directly calcined at 400 °C) and commercial ZnO, respectively. These findings suggested that OV-containing metal oxides that derived from metal-organic framework materials hold great promise as highly efficient photocatalysts for the removal of NO.

Key words: Photocatalytic NO removal, ZIF-8, Zinc oxide, Oxygen vacancies, Temperature treatment

朱鹏飞, 尹晓荷, 高新华, 董国辉, 徐景坤, 王传义. ZIF-8衍生的具有可控氧空位的ZnO对光催化去除NO的增强及毒性NO₂形成的抑制[J]. 催化学报, 2021, 42(1): 175-183.

Pengfei Zhu, Xiaohe Yin, Xinhua Gao, Guohui Dong, Jingkun Xu, Chuanyi Wang. Enhanced photocatalytic NO removal and toxic NO₂ production inhibition over ZIF-8-derived ZnO nanoparticles with controllable amount of oxygen vacancies[J]. Chinese Journal of Catalysis, 2021, 42(1): 175-183.

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https://www.cjcatal.com/CN/Y2021/V42/I1/175

图/表 11

Fig. 1. (a) Photocatalytic performance of different photocatalyst samples for removal of NO under visible light irradiation; (b) corresponding amount of NO2 generated over different photocatalyst samples; (c) NO removal performance of different photocatalyst samples.

Fig. 2. XRD patterns of different samples.

Fig. 3. SEM (a-c) and TEM (d-f) images of ZIF-8 (a, d), Z 400 (b, e) and Z 350-400 (c, f).

Fig. 4. HRTEM images of Z 350-400 (a) and Z 400 (b).

Fig. 5. XPS profiles of Z 400 and Z 350-400. (a) Full scan; (b) O 1s; (c) Zn 2p.

Fig. 6. EPR signals of analyzed photocatalysts.

Fig. 7. PL spectra of P-ZnO, Z 400, and Z 350-400.

Fig. 8. UV-vis DRS spectra (a) and energy band gaps (Eg) (b) of samples.

Fig. 9. Photocurrent responses under Xe lamp irradiation (a) and EIS (b) measurements of ZIF-8, P-ZnO, Z 400, and Z 350-400.

Fig. 10. Possible photocatalytic removal mechanism of NO over Z 350-400.

Fig. 11. Trapping experiments using Z 350-400.

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ZIF-8衍生的具有可控氧空位的ZnO对光催化去除NO的增强及毒性NO₂形成的抑制

Enhanced photocatalytic NO removal and toxic NO₂ production inhibition over ZIF-8-derived ZnO nanoparticles with controllable amount of oxygen vacancies

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