缺陷型金属氧化物脱除气体污染物研究进展

doi:10.11949/0438-1157.20241244

化工学报 ›› 2025, Vol. 76 ›› Issue (6): 2469-2482.DOI: 10.11949/0438-1157.20241244

缺陷型金属氧化物脱除气体污染物研究进展

杨盛华¹^,²(), 孙阳杰¹^,², 薛晓君¹^,², 米杰¹^,², 王建成²^,³, 冯宇¹^,²()

^1.太原理工大学省部共建煤基能源清洁高效利用国家重点实验室，山西太原 030024
^2.太原理工大学煤科学与技术教育部重点实验室，山西太原 030024
^3.太原理工大学环境与生态工程学院，山西晋中 030600

收稿日期:2024-11-02 修回日期:2024-12-16 出版日期:2025-06-25 发布日期:2025-07-09
通讯作者: 冯宇
作者简介:杨盛华（2001—），男，硕士研究生，1427143069@qq.com
基金资助:
国家自然科学基金项目(22378292);国家自然科学基金项目(21908156)

Research progress on gas pollutants removal by defective metal oxides

Shenghua YANG¹^,²(), Yangjie SUN¹^,², Xiaojun XUE¹^,², Jie MI¹^,², Jiancheng WANG²^,³, Yu FENG¹^,²()

^1.State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan 030024, Shanxi, China
^2.Key Laboratory of Coal Science and Technology, Ministry of Education, Taiyuan University of Technology, Taiyuan 030024, Shanxi, China
^3.College of Environmental and Ecological Engineering, Taiyuan University of Technology, Jinzhong 030600, Shanxi, China

Received:2024-11-02 Revised:2024-12-16 Online:2025-06-25 Published:2025-07-09
Contact: Yu FENG

摘要/Abstract

摘要：

金属氧化物因具有结构可调、易于改性、成本低廉等特性，广泛应用于气体净化领域。但未引入缺陷结构的金属氧化物对气体污染物的反应活性较低，且选择性仍有待提高。在金属氧化物中引入晶体缺陷后，能改变其晶体结构和物化性质，进而显著提高其对气体的吸附活性和选择性。但在气体脱除反应中，缺陷的促进作用机制极为复杂，这导致探究金属氧化物与气体反应中的缺陷作用机理变得十分困难，也使得将反应机理的研究成果应用于指导缺陷的策略性引入极具挑战性。首先概述了金属氧化物中的缺陷类型，其次对缺陷引入方法进行了分类概括，并总结了近年来缺陷型金属氧化物在气体净化领域的应用现状。最后，对金属氧化物缺陷工程的改进方法和未来研究方向进行了展望，以期为后续金属氧化物缺陷工程构筑及缺陷促进反应机制研究提供参考。

关键词: 金属氧化物, 缺陷, 气体净化, 制备, 吸附, 催化

Abstract:

Metal oxides are widely used in the field of gas purification because of their adjustable structure, easy modification and low cost. However, the reaction activity of metal oxides without defective structures to gaseous pollutants is low, and the selectivity still needs to be improved. After introducing crystal defects into metal oxides, their crystal structure and physicochemical properties can be changed, thereby significantly improving their adsorption activity and selectivity to gases. Nevertheless, in gas removal reactions, the promoting mechanism of defects is extremely complex, which makes it difficult to explore the mechanism of defects in the reaction between metal oxides and gases, and also makes it challenging to apply the research results of reaction mechanism to guide the strategic introduction of defects. In this review, the types of defects in metal oxides are summarized, and then the methods of introducing defects are classified and summarized, and the application status of defect metal oxides in gas purification field in recent years is summarized. Finally, the improvement methods and future research directions of metal oxide defect engineering are prospected, in order to provide reference for the subsequent research on the construction of metal oxide defect engineering and the reaction mechanism of defect promotion.

Key words: metal oxide, defects, gas purification, preparation, adsorption, catalysis

中图分类号:

X 511

杨盛华, 孙阳杰, 薛晓君, 米杰, 王建成, 冯宇. 缺陷型金属氧化物脱除气体污染物研究进展[J]. 化工学报, 2025, 76(6): 2469-2482.

Shenghua YANG, Yangjie SUN, Xiaojun XUE, Jie MI, Jiancheng WANG, Yu FENG. Research progress on gas pollutants removal by defective metal oxides[J]. CIESC Journal, 2025, 76(6): 2469-2482.

图/表 9

图1 缺陷型金属氧化物的缺陷种类、制备方法及应用

Fig.1 Defect types, preparation methods and applications of defective metal oxides

图2 CeNiO3-δ 的HAADF-扫描透射电子显微镜图(a)和CO2吸附模型示意图(b)[13]

Fig.2 HAADF-scanning transmission electron microscopy image (a) and schematic diagram of CO2 adsorption model (b) of CeNiO3-δ[13]

图3 Bi2MoO6(VMo)的高分辨率TEM图(a)，原子分辨率HAADF-STEM图(b)，晶体结构示意图(c)[17]

Fig.3 High-resolution TEM images (a), atomic resolution HAADF-STEM image and the contour line (b) and schematic crystal structure (c) of Bi2MoO6(VMo) [17]

图4 (a)Er(Mn,Ti)O3的HAADF-STEM图(1 Å=0.1 nm)；(b)模拟Er(Mn,Ti)O3的位错结构；(c)锂镧钛氧化物（LLTO）化学计量晶界的原子结构[19-20]

Fig.4 (a) HAADF-STEM map of Er(Mn,Ti)O3; (b) Simulated dislocation structure of Er(Mn,Ti)O3; (c) Atomic structure of lithium lanthanum titanium oxide (LLTO) stoichiometric grain boundaries[19-20]

图5 不同α-Fe2O3(0001)表面的优化结构（顶视图和侧视图）[35]

Fig.5 Optimized structures of different α-Fe2O3 (0001) surfaces(top and side views)[35]

图6 (a)ZnO形成表面氧缺陷示意图；(b)含缺陷ZnO通过增强载流子和缺陷诱导的分子氧活化促进光催化NO转化[39]

Fig.6 (a) Schematic representation of ZnO forming surface oxygen defects; (b) Defect-containing ZnO promotes photocatalytic NO conversion by enhancing carrier and defect-induced molecular oxygen activation[39]

图7 含缺陷ON-CuO的二氧化碳还原反应示意图(a)、TEM图(b)和(c)模拟晶格结构(b)[44]

Fig.7 Schematic representation of the carbon dioxide reduction reaction (a), TEM image (b) and simulated lattice structures (c) of defective ON-CuO-containing[44]

图8 (a)(Co,Mn)2O4原子分辨率球差校正高角度环形暗场扫描TEM图；(b)CoMnO x 原子分辨率球差校正高角度环形暗场扫描TEM图；(c)阳离子缺陷的CoMnO x 尖晶石的催化反应机理图[46]

Fig.8 (a) Atomic-resolution spherical aberration corrected high-angle annular dark-field scanning TEM images of (Co,Mn)2O4; (b) Atomic-resolution spherical aberration-corrected high-angle annular dark-field scanning TEM image of CoMnO x; (c) Mechanism of the catalytic reaction of cation-deficient CoMnO x spinel[46]

表1 不同合成方法制备的含缺陷金属氧化物及其应用

Table 1 Defect-containing metal oxides prepared by different synthetic methods and their applications

金属氧化物种类	缺陷类型	制备方法	应用	性能	文献
UO₂	氧空位	还原法	含硫气体	—	[48]
Ce_1-_x Zr _x O₂	氧空位	离子掺杂	含硫气体	—	[49]
Cu₂O	氧空位	还原法	含硫气体	—	[37]
Au/CeO₂	氧空位	离子掺杂	含硫气体	—	[50]
NiO/ACF	阳离子空位	热处理	含硫气体	23.65 mg_s/g脱硫剂	[51]
Mn-TiO₂	氧空位	还原法	含硫气体	0.40 ± 0.05（相对浓度）	[52]
ZnO	氧空位	热处理	NO _x	36.7%	[53]
TiO₂	氧空位	热处理	NO _x	—	[54]
Zn₂SnO₄	氧空位	离子掺杂	NO _x	62%	[55]
Ce-SnO₂	氧空位	离子掺杂	NO _x	5.001 μmol/(g·h)	[56]
MnFeO _x /TiO₂	氧空位	还原法	NO _x	> 80%	[57]
Bi₂WO₆	氧空位	离子掺杂	NO _x	64%	[58]
ZnO	氧空位	热处理	NO _x	55.45%	[59]
Cu₂O	氧空位	还原法	CO₂	35.4%（法拉第效率）	[60]
TiO₂-Cu _x O	氧空位、阳离子空位	离子掺杂	CO₂	—	[61]
Bi₄Ti₃O₁₂	氧空位、阳离子空位	还原法	CO₂	4.90 μmol/(g·h)	[62]
ON-CuO	氧空位、面缺陷	离子掺杂	CO₂	56%（法拉第效率）	[44]
Cu/Co₃O₄	氧空位	离子掺杂	CO₂	99%	[63]
TiO₂	氧空位	热处理	CO₂	20.2%	[64]
Cu₂O	线缺陷、面缺陷	还原法	CO₂	48.3%（法拉第效率）	[65]
CeO₂-MgO	氧空位	热处理	VOCs	90%	[66]
MnO _x	氧空位	热处理	VOCs	T₉₀ = 167℃	[67]
Ag-MnO _x	氧空位、阳离子空位	离子掺杂	VOCs	T₉₀ = 216℃	[68]
Fe-CeO₂	氧空位	离子掺杂	VOCs	> 98%	[69]
Co₃O₄-ZrO₂	氧空位	离子掺杂	VOCs	90%	[70]
MnO _x	氧空位	热处理	VOCs	95%	[71]

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缺陷型金属氧化物脱除气体污染物研究进展

Research progress on gas pollutants removal by defective metal oxides

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