Fe增强Ni2(CO3)(OH)2臭氧分解抗湿性与催化性能

doi:10.15541/jim20210127

无机材料学报 ›› 2022, Vol. 37 ›› Issue (1): 45-50.DOI: 10.15541/jim20210127

• 专栏: CO ₂ 绿色转化(特邀编辑: 欧阳述昕, 王文中) • 上一篇下一篇

Fe增强Ni₂(CO₃)(OH)₂臭氧分解抗湿性与催化性能

黎邦鑫¹^,²(), 张骞²(), 肖杰², 肖文艳², 周莹¹^,²

1.西南石油大学油气藏地质及开发工程国家重点实验室, 成都 610500
2.西南石油大学材料科学与工程学院新能源材料及技术研究中心, 成都 610500

收稿日期:2021-03-04 修回日期:2021-05-01 出版日期:2022-01-20 网络出版日期:2021-05-25
通讯作者: 张骞, 副教授. E-mail: zhangqian@swpu.edu.cn
作者简介:黎邦鑫(1995-), 男, 硕士研究生. E-mail: 1449569638@qq.com
基金资助:
四川省重大科技专项(2020ZDZX0008);四川省重点研发项目(2021YFSY0046)

Iron-doping Enhanced Basic Nickel Carbonate for Moisture Resistance and Catalytic Performance of Ozone Decomposition

LI Bangxin¹^,²(), ZHANG Qian²(), XIAO Jie², XIAO Wenyan², ZHOU Ying¹^,²

1. The Center of New Energy Materials and Technology, School of Materials Science and Engineering, Southwest Petroleum University, Chengdu 610500, China
2. State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation, Southwest Petroleum University, Chengdu 610500, China

Received:2021-03-04 Revised:2021-05-01 Published:2022-01-20 Online:2021-05-25
Contact: ZHANG Qian, associate professor. E-mail: zhangqian@swpu.edu.cn
About author:LI Bangxin(1995-), male, Master candidate. E-mail: 1449569638@qq.com
Supported by:
Science and Technology Major Projects Sichuan(2020ZDZX0008);Key R&D Program of Sichuan(2021YFSY0046)

摘要/Abstract

摘要：

臭氧污染已成为我国继PM2.5之后的主要污染物, 传统的臭氧分解催化材料在湿润环境中性能不稳定。本工作采用水热法制备了一种铁掺杂改性的碱式碳酸镍催化剂(NiCH-Fe), 该催化剂可在60%相对湿度下稳定分解2.14 μg/L臭氧12 h, 去除率达99%。水分子吸附质量检测结果表明, NiCH-Fe表面的水分子吸附量比纯NiCH明显减少, 表面水分子吸脱附可逆; 密度泛函理论结果证明, Fe原子是新的代替Ni原子的臭氧吸附位点, 并且Fe原子对臭氧分子的吸附能力更强。此外, XPS表明作为活性位点的Fe元素在反应前后保持稳定。掺杂Fe后的催化材料具有优异的抗湿性与长效稳定性。本研究表明通过金属离子掺杂, 改变催化材料的表面性质, 可获得具有良好抗湿性能的臭氧催化分解材料, 这为进一步开发兼具高抗湿性和高活性的臭氧催化分解材料, 提供了有效的技术方法。

关键词: 碱式碳酸镍, 掺杂, 臭氧催化分解, 抗湿性

Abstract:

Ozone pollution is taking more dominant position in China than PM2.5, traditional ozonolysis catalytic materials have limited performance in humid conditions. In this study, an iron-doped basic nickel carbonate catalyst (NiCH-Fe) was successfully fabricated via a facile hydrothermal method, which could stably decompose 2.14 μg/L ozone at 60% relative humidity for 12 h with nearly 100% removal ratio. The result of the Quartz Crystal Microbalance test showed that the water molecules adsorbed on the surface of NiCH-Fe were significantly reduced as compared with that adsorbed on pure NiCH, which were favorable for the competitive adsorption of ozone. Density functional theory results proved that Fe atoms were new sites instead of Ni atoms and had stronger adsorption capacity for ozone molecules. In addition, the XPS results demonstrated that the iron atoms serving as active sites were substantially stable in the reaction. Therefore, material doped with Fe provided excellent moisture resistance and long-term stability. This work provides an effective technical method for the development of materials with high moisture resistance ability for efficient ozone catalytic decomposition.

Key words: basic nickel carbonate, doping, ozone decomposition, moisture resistance

中图分类号:

TQ174

黎邦鑫, 张骞, 肖杰, 肖文艳, 周莹. Fe增强Ni₂(CO₃)(OH)₂臭氧分解抗湿性与催化性能[J]. 无机材料学报, 2022, 37(1): 45-50.

LI Bangxin, ZHANG Qian, XIAO Jie, XIAO Wenyan, ZHOU Ying. Iron-doping Enhanced Basic Nickel Carbonate for Moisture Resistance and Catalytic Performance of Ozone Decomposition[J]. Journal of Inorganic Materials, 2022, 37(1): 45-50.

图/表 9

图1 NiCH与NiCH-Fe的XRD图谱

Fig. 1 XRD patterns of NiCH and NiCH-Fe

图2 NiCH-Fe5%样品的(a)SEM照片及其上Ni(b)、Fe(c)元素的EDS分布; (d) NiCH和(e) NiCH-Fe5%的TEM照片; (f) NiCH-Fe5%的HRTEM照片

Fig. 2 (a) SEM image of NiCH-Fe5% and corresponding EDS mappings of (b) Ni and (c) Fe elements, TEM images of (d) NiCH and (e) NiCH-Fe5%, and (f) HRTEM image of NiCH-Fe5%

图3 NiCH、NiCH-Fe、FeCH的(a)氮气吸脱附等温曲线与(b)孔径分布图

Fig. 3 (a) Nitrogen adsorption-desorption isotherms and (b) pore size distributions of NiCH, NiCH-Fe and FeCH

图4 (a)不同铁掺杂量的NiCH-Fe在60%相对湿度下与(b)NiCH-Fe5%材料在60%、70%、80%相对湿度下的臭氧去除率

Fig. 4 Ozone removal rates of (a) NiCH-Fe with different Fe dopants at 60%RH and (b) NiCH-Fe5% at 60%, 70%, 80%RH

图5 NiCH-Fe5%与MnO2的长时间臭氧分解性能测试

Fig. 5 Long time ozone removal tests of NiCH-Fe5% and MnO2

图6 NiCH-Fe5%反应前后的(a)Ni2p3/2和(b)Fe2p的XPS图谱

Fig. 6 XPS spectra of (a) Ni2p3/2 and (b) Fe2p of NiCH-Fe5% before and after reaction

图7 NiCH与NiCH-Fe5%材料表面水分子吸附曲线

Fig. 7 Surface water adsorption curves of NiCH and NiCH- Fe5%

图8 单层的NiCH-Fe的模型

Fig. 8 Single-layer structure of NiCH-Fe

表1 NiCH与NiCH-Fe上不同位点臭氧与水分子的吸附能

Table 1 Adsorption energy of ozone and H2O on different sites of NiCH and NiCH-Fe5%

Molecule	Site	NiCH	NiCH-Fe
O₃	Ni	-0.36 eV	-0.57 eV
	Fe(Ni)	-0.02 eV(Ni)	-1.93eV(Fe)
	O1	-0.28 eV	-0.61 eV
	O2	-0.69 eV	-0.46 eV
H₂O	Ni	-0.15 eV	-0.41 eV
H₂O	Fe(Ni)	-0.24 eV(Ni)	-0.55 eV(Fe)

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Fe增强Ni₂(CO₃)(OH)₂臭氧分解抗湿性与催化性能

Iron-doping Enhanced Basic Nickel Carbonate for Moisture Resistance and Catalytic Performance of Ozone Decomposition

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