Adjusting effect of additives on decatungstate-photocatalyzed HMF oxidation with molecular oxygen under visible light illumination
Adjusting effect of additives on decatungstate-photocatalyzed HMF oxidation with molecular oxygen under visible light illumination
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可见光照射下添加剂对十钨酸盐光催化分子氧氧化HMF的调节作用
DOI：
10.1016/j.cej.2020.125345
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发表时间：
2020-09
影响因子：
15.1
通讯作者：
Liu Yachun
中科院分区：
文献类型：
--
作者：
Yang Bo;Hu Wenwei;Wan Feifei;Zhang Chao;Fu Zaihui;Su Anqun;Chen Mengke;Liu Yachun
以乙腈为溶剂，十聚钨酸盐（DT）为催化剂，在可见光引发下，能有效地催化氧气氧化5-羟甲基糠醛（HMF），生成2，5-二甲酰基呋喃（DFF）和2，5-呋喃二甲酸（FDCA）。DT阴离子的光催化效率取决于其抗衡阳离子调节的合成质量，并受添加剂的显著调节。在所考察的添加剂中，NaBr、DMSO和[Bimi]Cl对HMF光催化聚合有抑制作用，可明显提高光催化氧化的碳平衡产率（CBY）。水，特别是强酸溶液对光催化氧化起着积极的调节作用，最佳添加剂HBr可获得67.1%的DFF和5.8%的FDCA产率以及87.7%的CBY。一系列的表征表明，DT与HMF或HBr的给体-受体（D-A）相互作用也受到其抗衡阳离子的调节，并通过改善DT的光物理和光化学性质而有助于光催化氧化。值得注意的是，HBr具有比HMF更强的与DT的D-A相互作用，并且可以被光激发的DT优先氧化以形成Br原子自由基，后者因此在提高DFF产率方面起主导作用，如一系列控制和淬灭测试所支持的。
This paper discloses that decatungstate (DT) can efficiently catalyze the visible light-triggered oxidation of 5-hydroxymethylfurfural (HMF) with O2in MeCN under normal temperature and pressure, affording 2,5-diformylfuran (DFF) and 2,5-furandicarboxylicacid (FDCA) as the oxygenated products. The photo-catalytic efficiency of DT anion depends on its counter cations-regulated synthetic quality and is adjusted significantly by the additives. Among the additives examined, NaBr, DMSO and [Bimi]Cl may obviously improve the carbon balance yield (CBY) of this photo-catalytic oxidation owing to their restraining effect on the light-induced HMF polymerization. Water and especially some strong acid solutions play a positive adjusting effect on this photo-catalytic oxidation and the best additive HBr can achieve 67.1% DFF and 5.8% FDCA yields as well as 87.7% CBY. A series of characterizations indicate that the donor-acceptor (D-A) interaction of DT with HMF or HBr is also regulated by its counter cations and contributes to photo-catalytic oxidation by improving the photo-physical and photo-chemical properties of DT. Notably, HBr has a stronger D-A interaction with DT than HMF and can be preferentially oxidized by the photo-excited DT to form a Br atom free radical, the latter thus plays a leading role in improving DFF yield, as supported by a series of control and quenching tests.
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影响因子：
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