Light-tuned selective photosynthesis of azo- and azoxy-aromatics using graphitic C(3)N(4).

Light-tuned selective photosynthesis of azo- and azoxy-aromatics using graphitic C(3)N(4).
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使用石墨 C3N4 进行光调节偶氮和氧化偶氮芳香族化合物的选择性光合作用

DOI:
10.1038/s41467-017-02527-8
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发表时间:
2018-01-04
影响因子:
16.6
通讯作者:
Su R
Su R
中科院分区:
综合性期刊1区
文献类型:
--
作者:
Dai Y;Li C;Shen Y;Lim T;Xu J;Li Y;Niemantsverdriet H;Besenbacher F;Lock N;Su R

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太阳能驱动的光催化在水分解、二氧化碳还原和有机合成等方面引起了广泛的关注。利用负载型等离子体金属纳米颗粒在高温(≥90℃)下,通过选择性光还原硝基芳香族化合物,合成了有价值的偶氮和偶氮氧芳香族染料;但其成本高、效率低、室温下选择性差等缺点限制了其应用。在此,我们证明了廉价的石墨c3n4是一种有效的光催化剂,在紫色(410 nm)或蓝色(450 nm)激发下,由相应的硝基芳烃选择性合成一系列偶氮和偶氧芳烃化合物。对偶氮和偶氮芳香族化合物的高效和高选择性可归因于弱结合的光生成表面吸附h原子和有利的N-N偶联反应。结果揭示了光催化大规模生产有价化学品的经济和环境潜力。
Solar-driven photocatalysis has attracted significant attention in water splitting, CO2reduction and organic synthesis. The syntheses of valuable azo- and azoxyaromatic dyes via selective photoreduction of nitroaromatic compounds have been realised using supported plasmonic metal nanoparticles at elevated temperatures (≥90 °C); however, the high cost, low efficiency and poor selectivity of such catalyst systems at room temperature limit their application. Here we demonstrate that the inexpensive graphitic C3N4is an efficient photocatalyst for selective syntheses of a series of azo- and azoxy-aromatic compounds from their corresponding nitroaromatics under either purple (410 nm) or blue light (450 nm) excitation. The high efficiency and high selectivity towards azo- and azoxy-aromatic compounds can be attributed to the weakly bound photogenerated surface adsorbed H-atoms and a favourable N-N coupling reaction. The results reveal financial and environmental potential of photocatalysis for mass production of valuable chemicals.
DOI: 10.1021/sc5000545
发表时间: 2014-04-01
影响因子: 8.4
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期刊: Science (New York, N.Y.)
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