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Bandgap engineering of polymetric carbon nitride copolymerized by 2,5,8-triamino-tri-s-triazine (melem) and barbituric acid for efficient nonsacrificial photocatalytic H2O2 production
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2020-03-25 , DOI: 10.1016/j.apcatb.2020.118917
Zhenyuan Teng , Wenan Cai , Sixiao Liu , Chengyin Wang , Qitao Zhang , Su Chenliang , Teruhisa Ohno

Photocatalytic production of H2O2 from water and oxygen utilizing polymetric carbon nitride (PCN) is a promising alternative to the energy-consuming anthraquinone method. However, insufficient oxidation potential and limited light-absorption have restricted its further improvement. Herein, PCN with sufficient oxidation potential and improved visible-light usage (up to 550 nm) was prepared by co-polymerization of 2,5,8-triamino-tri-s-triazine (melem) and barbituric acid (BA). With the loading of Na2CoP2O7 as a water-oxidation co-catalyst, this novel PCN system showed a record-high apparent quantum efficiency (420 nm) of 8.0 % and a solar-to-chemical conversion efficiency of 0.30 % for H2O2 production. This improvement is attributed to the introduced O 2p states by CO groups remained in the PCN matrix, leading to a positive valence band maximum of 1.85 eV (vs. SHE). The co-polymerization of BA and melem combined with Na2CoP2O7 loading also suppressed the charge recombination, resulting in a rapid stepwise one-electron to one-electron reaction for efficient H2O2 production.



中文翻译:

2,5,8-三氨基-三-s-三嗪(蜜em)和巴比妥酸共聚的多尺度氮化碳的带隙工程用于高效非牺牲性光催化H 2 O 2的生产

利用多尺度氮化碳(PCN)从水和氧气中光催化生产H 2 O 2是一种耗能的蒽醌方法的有前途的替代方法。然而,不足的氧化电位和有限的光吸收限制了其进一步的改进。在此,通过2,5,8-三氨基-三-s-三嗪(蜜胺)和巴比妥酸(BA)的共聚制备具有足够的氧化电位和改善的可见光使用率(至多550 nm)的PCN。通过负载Na 2 CoP 2 O 7作为水氧化助催化剂,该新型PCN系统的表观量子效率(420 nm)达到了创纪录的8.0%,日光化学转化效率为0.30%对于H 2O 2生产。这种改善归因于PCN矩阵中保留的C O基团引入的O 2p状态,从而导致最大价带为1.85 eV(相对于SHE)。BA和melem的共聚以及Na 2 CoP 2 O 7的加入也抑制了电荷的重组,导致快速的单电子到单电子的逐步反应,以有效地生产H 2 O 2

更新日期:2020-03-26
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