Band-Gap Modulation for Enhancing NO Photocatalytic Oxidation over Hollow ZnCdS: A Combined Experimental and Theoretical Investigation
Band-Gap Modulation for Enhancing NO Photocatalytic Oxidation over Hollow ZnCdS: A Combined Experimental and Theoretical Investigation
复制标题
带隙调制增强空心 ZnCdS 上 NO 光催化氧化：实验与理论相结合的研究
DOI：
10.1021/acs.jpcc.1c10182
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发表时间：
2022-02
期刊：
影响因子：
--
通讯作者：
Xinbo Wang
中科院分区：
文献类型：
--
作者：
Wanyuan Wang;Jing Guan;Jingxin Tan;Daoyuan Zheng;Junjie Bian;Xinbo Wang
光催化处理ppm浓度的NO对环境和人类健康的保护引起了学术界和工业界越来越大的兴趣。在此基础上，制备了不同Cd掺杂的中空硫化锌纳米笼催化剂，并将其用于可见光下脱除NO，脱除效率高达85%。密度泛函理论计算和实验表明，Cd离子能有效地将硫化锌的带隙调制到可见光吸收范围(2.69 eV)。具有空腔结构的Zn0.5Cd0.5S具有良好的光电响应和较低的电子-空穴复合几率。在瞬时吸收光谱中检测到高达2.33μ的S弛豫信号，表明光激发载流子具有较长的寿命。此外，还利用漫反射红外傅里叶变换光谱(DRIFTS)对NO的光催化氧化过程进行了动态监测。结果表明，在黑暗条件下，吸附在表面的NO迅速转化为二聚体(N2O_2)，并在光照后促进NO通过中间体亚硝酸盐(N_2O_2、→、NO、→、NO_3~-)转化为硝酸盐。该催化剂具有较高的活性和稳定性，在可见光下催化氧化NO具有很大的应用潜力。
The photocatalytic treatment of NO at ppm-level concentrations for the environment and human health protection has attracted ever-increasing interest in academia and industry. Here, hollow ZnCdS nanocage catalysts with different Cd dopings were prepared and used to remove NO under visible light, and a high removal rate of 85% was achieved. Density functional theory (DFT) theoretical calculations and experiments showed that Cd ions could effectively modulate the band gap of ZnS into the visible-light-absorbing range (2.69 eV). Zn0.5Cd0.5S with a cavity structure has an excellent photoelectric response and low electron–hole recombination probability. A relaxation signal of up to 2.33 μs was detected in the transient absorption spectrum, indicating the long lifetime of the photoexcited carriers. Furthermore, the photocatalytic oxidation process of NO was dynamically monitored byin situdiffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). It is found that NO adsorbed on the surface of Zn0.5Cd0.5S rapidly transformed into dimers (N2O2) under dark and facilitated NO conversion to nitrateviaintermediates such as nitrite after illumination (N2O2→ NO → NO3–). The high activity and stability of Zn0.5Cd0.5S present a high potential for scale-up application of the catalyst for NO oxidation under visible light.
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DOI：
10.1088/1757-899x/231/1/012111
发表时间：
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期刊：
IOP Conference Series: Materials Science and Engineering
影响因子：
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作者：
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影响因子：
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