Ultrathin Porous Carbon Nitride Bundles with an Adjustable Energy Band Structure toward Simultaneous Solar Photocatalytic Water Splitting and Selective Phenylcarbinol Oxidation,Angewandte Chemie International Edition

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Ultrathin Porous Carbon Nitride Bundles with an Adjustable Energy Band Structure toward Simultaneous Solar Photocatalytic Water Splitting and Selective Phenylcarbinol Oxidation
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2020-11-03 , DOI: 10.1002/anie.202013753
Baogang Wu ₁ , Liping Zhang ₂ , Baojiang Jiang ₁ , Qi Li ₁ , Chungui Tian ₁ , Ying Xie ₁ , Weizuo Li ₁ , Honggang Fu ₁

Affiliation

Actiniae‐like carbon nitride (ACN) bundles were synthesized by the pyrolysis of an asymmetric supramolecular precursor prepared from L‐arginine (L‐Arg) and melamine. ACN has adjustable band gaps (2.25 eV–2.75 eV) and hollow microtubes with ultrathin pore walls, which enrich reaction sites, improve visible‐light absorption and enhance charge separation. In the presence of phenylcarbinol, ACN exhibited excellent water‐splitting ability (95.3 μmol h⁻¹) and in the meanwhile phenylcarbinol was selectively oxidized to benzaldehyde (conversion of 90.9 %, selectivity of 99.7 %) under solar irradiation. For the concurrent reactions, ²D isotope labeling, separation, and detection were conducted to confirm that the proton source of released hydrogen is water. The mechanism of water splitting and phenylcarbinol oxidation was also investigated.

中文翻译：

具有可调节能带结构的超薄多孔氮化碳束，可同时实现太阳能光催化水分解和选择性苯甲醇氧化

通过热解由L-精氨酸（L-Arg）和三聚氰胺制备的不对称超分子前体，合成了类似猕猴桃的氮化碳（ACN）束。ACN具有可调节的带隙（2.25 eV–2.75 eV）和带有超薄孔壁的中空微管，可丰富反应部位，改善可见光吸收并增强电荷分离。在苯甲醇存在下，ACN表现出优异的水分解能力（95.3μmolh ^-1），同时在阳光照射下苯甲醇被选择性氧化为苯甲醛（转化率为90.9％，选择性为99.7％）。对于并发反应，²进行D同位素标记，分离和检测以确认释放的氢的质子来源是水。还研究了水分解和苯甲醇氧化的机理。

更新日期：2020-11-03

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