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

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
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2,5,8-三氨基-三均三嗪(蜜勒姆)和巴比妥酸共聚聚合氮化碳的带隙工程,用于高效非牺牲光催化 H2O2 生产

DOI:
10.1016/j.apcatb.2020.118917
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发表时间:
2020-08
期刊:
Applied Catalysis B: Environmental
影响因子:
--
通讯作者:
Ohno Teruhisa
Ohno Teruhisa
中科院分区:
其他
文献类型:
--
作者:
Teng Zhenyuan;Cai Wenan;Liu Sixiao;Wang Chengyin;Zhang Qitao;Su Chenliang;Ohno Teruhisa

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利用聚碳氮化碳(PCN)从水和氧气中光催化制备过氧化氢是一种很有前途的替代耗能的蒽醌方法的方法。然而,氧化电位不足和光吸收有限限制了其进一步的改进。本论文通过2,5,8-三氨基-三-S-三嗪(MELEM)与巴比妥酸(BA)的共聚反应,制备了氧化电位高、可见光利用率高(达550 nm)的PCN。当负载量为Na_2CoP_2O_7作为水氧化助剂时,该体系的表观量子效率(420 nm)达到了创纪录的8.0%,光化学转化效率达到了0.30%。这一改善归因于保留在PCN基质中的C双键引入的O2p态,导致正价带最大值为1.85 eV(vs.Se)。BA和甜蜜素的共聚以及Na2CoP2O7的负载也抑制了电荷复合,导致快速的一电子对一电子反应,从而有效地产生了H_2O_2。
Photocatalytic production of H2O2from 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 Na2CoP2O7as 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 H2O2production. This improvement is attributed to the introduced O 2p states by Cdouble bondO 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 Na2CoP2O7loading also suppressed the charge recombination, resulting in a rapid stepwise one-electron to one-electron reaction for efficient H2O2production.
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