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Efficient visible-light-driven selective oxygen reduction to hydrogen peroxide by oxygen-enriched graphitic carbon nitride polymers†
Energy & Environmental Science ( IF 32.5 ) Pub Date : 2018-06-20 00:00:00 , DOI: 10.1039/c8ee01316k
Zhen Wei 1, 2, 3, 4 , Meili Liu 4, 5, 6, 7 , Zijian Zhang 1, 2, 3, 4 , Wenqing Yao 1, 2, 3, 4 , Hongwei Tan 4, 5, 6, 7 , Yongfa Zhu 1, 2, 3, 4
Affiliation  

H2O2 is a green, environmentally friendly potential energy source. The photocatalytic reduction of molecular oxygen to synthesise H2O2 is an eco-friendly strategy compared with the anthraquinone method and H2/O2 direct synthesis. We proposed oxygen-enriched carbon nitride polymer (OCN) models, which were proven to more easily produce 1,4-endoperoxide species and have a high selectivity for molecular oxygen reduction to H2O2, rather than superoxide radicals, through theoretical calculations and experiments. The apparent quantum yield for H2O2 production by OCNs reached 10.2% at 420 nm under an O2 atmosphere, which was 3.5 times higher than that of g-C3N4 and the activity did not decay over 20 h. OCN has a better oxygen reducibility and electron–hole separation efficiency than g-C3N4 and is more prone to 2-electron reduction in the ORR. This work promotes understanding of the mechanism of photocatalytic oxygen reduction and provides a new idea for the design and synthesis of new materials for the preparation of H2O2.

中文翻译:

富氧的石墨氮化碳聚合物有效地将可见光驱动的选择性氧气还原为过氧化氢

H 2 O 2是绿色,环保的潜在能源。与蒽醌法和H 2 / O 2直接合成相比,光催化还原分子氧来合成H 2 O 2是一种环保策略。我们提出了富氧氮化碳聚合物(OCN)模型,通过理论计算和分析,事实证明,该模型更易于产生1,4-内过氧化物,并且对分子氧还原为H 2 O 2而不是超氧自由基具有较高的选择性。实验。H 2 O 2的表观量子产率生产由OCNS的O下达到在420nm处为10.2%2气氛中,这比GC的3.5倍3 Ñ 4和活性没有衰减超过20小时。与gC 3 N 4相比,OCN具有更好的氧还原性和电子-空穴分离效率,并且ORR中更易于2电子还原。这项工作促进了对光催化氧还原机理的理解,为设计和合成用于制备H 2 O 2的新材料提供了新的思路。
更新日期:2018-06-20
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