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Self-supported hierarchical crystalline carbon nitride arrays with triazine-heptazine heterojunctions for highly efficient photoredox catalysis
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2022-01-29 , DOI: 10.1016/j.cej.2022.134865
Zongzhao Sun 1 , Haozhe Dong 2 , Qi Yuan 3 , Yueyang Tan 1 , Wu Wang 4 , Yabin Jiang 1 , Jianyong Wan 1 , Jiangwei Wen 2 , Jianjing Yang 2 , Jiaqing He 4 , Tao Cheng 3 , Limin Huang 1
Affiliation  

Self-supported hierarchical crystalline carbon nitride arrays (MA-rod array), which show the excellent properties of photocatalytic hydrogen evolution and oxidative organic synthesis, were synthesized by molten salt-assisted pyrolysis of rod-like supramolecular precursors from the hydrolysis of melamine. On the nanoscale, the highly crystalline MA-rod array has an omasum-like architecture with combined advantages of rapid electrolyte diffusion, efficient gas evolution, fast electronic transmission, and lower interface resistance. At the molecular level, the triazine-heptazine heterojunctions remarkably improve charge carrier transfer and separation. In the tests of photoredox catalysis, the MA-rod array exhibited 51-fold higher hydrogen production rate (11720 μmol h−1 gcat-1) than the reference with a high apparent quantum yield (AQY) of 60% at 420 nm. Furthermore, the oxidation of aromatic hydrocarbons to aldehydes or ketones can be obtained under single wavelength (460 nm) irradiation with milligram yields (e.g., the isolated yield of benzaldehyde is 34.5 mg with the conversion rate of 1805.6 μmol h−1 gcat-1), surpassing other photocatalysts so far.



中文翻译:

用于高效光氧化还原催化的具有三嗪-庚嗪异质结的自支撑分级结晶氮化碳阵列

通过熔融盐辅助热解三聚氰胺水解产生的棒状超分子前体,合成了具有光催化析氢和氧化有机合成优异性能的自支撑分级结晶氮化碳阵列(MA-棒阵列)。在纳米尺度上,高度结晶的 MA 棒阵列具有类似 omasum 的结构,具有快速电解质扩散、高效气体析出、快速电子传输和较低界面电阻的综合优势。在分子水平上,三嗪-庚嗪异质结显着改善了电荷载流子的转移和分离。在光氧化还原催化测试中,MA 棒阵列的产氢率提高了 51 倍(11720 μmol h -1 g cat -1) 比在 420 nm 处具有 60% 的高表观量子产率 (AQY) 的参考。此外,在单波长(460 nm)辐照下,芳香烃氧化成醛或酮,产率为毫克(例如,苯甲醛的分离产率为34.5 mg,转化率为1805.6 μmol h -1 g cat -1 ),迄今为止超过了其他光催化剂。

更新日期:2022-02-03
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