Light intensity responsive changes of products in photocatalytic reduction of nitrous acid on a Cu-doped covalent triazine framework/TiO2 hybrid.
Light intensity responsive changes of products in photocatalytic reduction of nitrous acid on a Cu-doped covalent triazine framework/TiO2 hybrid.
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DOI：
10.1002/cssc.202000687
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发表时间：
2020-04
期刊：
影响因子：
8.4
通讯作者：
K. Kamiya;R. Sugimoto;Tomomi Tatebe;T. Harada;Shuji Nakanishi
中科院分区：
文献类型：
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作者：
K. Kamiya;R. Sugimoto;Tomomi Tatebe;T. Harada;Shuji Nakanishi
在太阳能转换电化学系统的设计中，重要的是要考虑到自然光的波动。以亚硝酸光还原为例，本工作表明，反应路径和反应产物对光强的变化有动态响应。在光照下，甲醇在二氧化钛上的光氧化反应和铜修饰的共价三嗪骨架(CuCTF)上的HNO2还原反应是电耦合的，这导致了HNO2在没有外加偏压的情况下被光还原。随着光照强度的增加，主要反应产物由N2O转变为NH4+。当光强增大(或减小)时，工作电位也发生负移(或正移)。这些结果表明，在不同的光强下，CuCTF催化剂的工作电位发生了变化，从而引发了反应路径的变化。在使用光响应电极并可以获得多种产物的系统中，这种依赖于光强度的反应路径的变化特别重要，例如太阳能驱动的二氧化碳和氮氧化物的减少。
In the design of solar-energy conversion electrochemical systems, it is important to consider that natural sunlight fluctuates. By taking nitrous acid photoreduction as an example, the present work has shown that the reaction pathway, and hence the reaction products, dynamically responded to the variation of light intensity. Under irradiation, the photooxidation of methanol (as sacrificial agent) on TiO 2 and the reduction of HNO 2 on Cu-modified covalent triazine framework (Cu-CTF) were electrically coupled, which led to the photoreduction of HNO 2 without an external bias. The dominant reaction product changes from N 2 O to NH 4 + with an increase in the light intensity. The operating potential also shifted negatively (or positively) when the light intensity was increased (or decreased). These results indicate that a change of the reaction pathway was triggered by a change of the operating potential of the Cu-CTF catalysts under varying light intensity. Such a light-intensity dependent change of the reaction pathway is particularly important in systems that use photoresponsive electrodes and where multiple products can be obtained, such as the solar-driven reduction of carbon dioxide and nitrogen oxides.