半导体材料在光催化低浓度氮氧化物的研究进展

doi:10.11949/0438-1157.20201018

摘要/Abstract

摘要：

氮氧化物（NO_x）是一类有害的空气污染物，会引发酸雨、雾霾、光化学烟雾等严重的环境问题。目前，如何有效地去除空气中低浓度的NO_x（十亿分之一）是研究的热点和难点。半导体光催化氧化法可以将空气中低浓度NO_x氧化成无毒的硝酸盐，是一种经济有效的净化技术之一。本文主要围绕二氧化钛（TiO₂），氮化碳（g-C₃N₄）和Bi系三类半导体光催化材料，对近年来包括本课题组在内的国内外对光催化去除低浓度NO_x研究进行了简要概述。其中，通过代表性的工作介绍了贵金属沉积、元素掺杂、构建异质结和表面空位缺陷工程等改性策略，以提高半导体材料在去除低浓度NO_x的光催化活性和性能。此外，对半导体材料在光净化低浓度NO_x的未来发展进行了展望，以期待为高性能半导体光催化剂的理性设计和制备以及催化机理的探索等方面的研究提供思路。

关键词: 半导体材料, 光催化, 低浓度, 氮氧化物

Abstract:

Nitrogen oxides (NO_x) are a type of harmful air pollutants that can cause serious environmental problems such as acid rain, haze, and photochemical smog. At present, how to effectively remove the low concentration of NO_x in the air (ppb level: one part per billion) is a research hotspot and difficulty. The semiconductor photocatalytic oxidation method can oxidize low concentration NO_x in the air into non-toxic nitrate, which is one of the economic and effective purification technologies. This review article mainly focuses on three types of semiconductor photocatalytic materials, such as titanium dioxide (TiO₂), carbon nitride (g-C₃N₄) and Bi-based semiconductors, and provides a brief overview of their research on the photocatalytic removal of low-concentration NO_x in recent years. Meanwhile, various representative works introduce the modification strategies of noble metal deposition, element doping, semiconductor combination and surface vacancy defect engineering to improve the photocatalytic performance of semiconductor materials in removing low concentrations NO_x. In order to provide ideas for the rational design and preparation of high-performance semiconductor photocatalysts and the exploration of catalytic mechanisms, the future development of semiconductor materials in photocatalytic low concentration NO_x is finally prospected.

Key words: semiconductor materials, photocatalysis, low concentration, nitrogen oxides

中图分类号:

TQ 09

张顾平, 王贝贝, 周舟, 陈冬赟, 路建美. 半导体材料在光催化低浓度氮氧化物的研究进展[J]. 化工学报, 2021, 72(1): 259-275.

ZHANG Guping, WANG Beibei, ZHOU Zhou, CHEN Dongyun, LU Jianmei. Research progress of semiconductor materials for photocatalytic low concentration nitrogen oxides[J]. CIESC Journal, 2021, 72(1): 259-275.

图/表 13

图1 半导体材料在光催化低浓度氮氧化物的整体内容的简要说明

Fig.1 A brief description of the overall content of semiconductor materials for photocatalytic low concentration nitrogen oxides

图2 Bi2O2CO3对NO的吸附以及光催化氧化过程[36]

Fig.2 Proposed processes of NO adsorption and photocatalytic NO oxidation on Bi2O2CO3 [36]

图3 Ag-TiO2可见光诱导的光催化去除NO的合理机理[44]

Fig.3 A plausible mechanism for visible light induced photocatalytic NO removal on Ag-TiO2[44]

图4 可见光照射下材料光催化降解NO (a)；NO去除效率和NO2转化效率 (b)[46]

Fig.4 NO photocatalytic degradation of materials under visible light irradiation (a); NO removal efficiency and NO2 conversion efficiency (b)[46]

图5 叶绿体结构的CNTs-TiO2的光催化去除一氧化氮机理[47]

Fig.5 The photocatalytic NO removal mechanism of chloroplast structured CNTs-TiO2[47]

图6 TiO2-OV和TiO2的光催化去除NO (a)；相应生成NO2 (b)[48]

Fig.6 Photocatalytic NO removal over the TiO2-OV and TiO2 (a); the corresponding generation of NO2 (b)[48]

图7 N-g-C3N4和P-g-C3N4样品的紫外可见吸收光谱 (a)；变换的漫反射光谱 (b)[57]

Fig.7 UV-Vis absorption (a), transformed diffuse reflectance (b) spectra of N-g-C3N4 and P-g-C3N4 samples[57]

图8 所制备样品去除NO的光催化活性(插图是NO2生成率) (a)；DFT计算的g-C3N4 (b)和CNB-0.10 (c)上主要中间吸附物种的吸附能和键长，长度以?表示[59]

Fig.8 Photocatalytic activities for NO removal and the inset is the NO2 production rate of the as-prepared samples (a); DFT calculated adsorption energies and bond lengths of the major intermediate adsorption species on g-C3N4 (b) and CNB-0.10 (c), the lengths are given in ?[59]

图9 Sb2WO6/g-C3N4纳米复合材料在可见光照射下的S型光催化机理[65]

Fig.9 S-Scheme photocatalytic mechanism for Sb2WO6/g-C3N4 nanocomposite under visible-light irradiation[65]

图10 块状g-C3N4、HCNS、HCN/rGO和CNCF样品的可见光催化去除NO的性能 (a)；CNCF样品的多次光催化循环反应 (b)[66]

Fig.10 Visible-light photocatalytic performance of bulk-g-C3N4, HCNS, HCNS/rGO, and CNCF samples for the removal NO (a); multiple runs of photocatalytic reactions for CNCF (b)[66]

图11 CNQDs/GO-InVO4气凝胶的合成示意图[73]

Fig.11 Schematic diagram of the synthesis of CNQDs/GO-InVO4 aerogel[73]

图12 BOC-MoS2-CNF的合成示意图 (a)，CNF、BOC、BOC-CNF以及BOC-MoS2-CNF样品的可见光光催化去除NO的活性 (b) [82]

Fig.12 Schematic illustration of the fabrication of BOC-MoS2-CNFs (a); visible-light photocatalytic activities of CNFs, BOC, BOC-CNFs and BOC-MoS2-CNFs samples for NO removal (b)[82]

图13 BP/MBWO异质结的合成示意图 (a)；用于去除NO的光催化剂的性能 (b)；12% BP/MBWO样品的多次光催化循环 (c) [84]

Fig.13 Illustration of the fabrication of the BP/MBWO heterojunction (a); performance of the photocatalysts for NO removal (b); multiple cycles of photocatalytic reactions over 12% BP/MBWO (c)[84]

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