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Solid-Solution-Like o-C3N4/Ag2SO4 Nanocomposite as a Direct Z-Scheme Photocatalytic System for Photosynthesis of Active Oxygen Species
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2018-07-06 00:00:00 , DOI: 10.1021/acssuschemeng.8b02241
Chuanbao Xiong 1 , Shujuan Jiang 1, 2 , Shaoqing Song 1, 2 , Xi Wu 1, 2 , Jinghua Li 3 , Zhanggao Le 1
Affiliation  

Efficient photosynthesis of active oxygen species (e.g., •OH, •O2, and H2O2) is of cardinal significance for environmental science and biochemistry. We report a system of o-C3N4/Ag2SO4 with solid-solution-like structure synthesized by coordinating the 5s orbit of Ag+ with surface 2p lone electrons of o-C3N4. The as-synthesized o-C3N4/Ag2SO4 demonstrates a unique electronic structure, as illuminated high light absorption, perfect redox potentials, large BET specific area, abundant active sites, and efficient interfacial charge transfer. Electron paramagnetic resonance spectra and Mott–Schottky measurements confirm that o-C3N4/Ag2SO4 photocatalysts demonstrate highly efficient activity for yielding •OH, •O2, and H2O2 species with the Z-scheme photocatalytic principle. Experimental and DFT calculation reveal that the transferred electrons on the conduction band (CB) made up of Ag 5s were favorably shifted into the valence band (VB) composed of N 2p with the formed coordination under irradiation, greatly promoting electron transportation in the Z-scheme photocatalytic system. (o-C3N4)2/(Ag2SO4)1 with the mass ratio of 2 to 1 possesses the highest photocatalytic rate of •OH (45 μmol L–1 h–1), •O2 (87 μmol L–1 h–1), and H2O2 (480 μmol L–1 h–1). The work provides a new approach to design advanced photocatalysts to efficiently yield active oxygen species for environmental purification.

中文翻译:

类似于O -C 3 N 4 / Ag 2 SO 4纳米固溶体的直接Z型光催化体系,用于活性氧的光合作用

活性氧的光合作用效率(例如,OH•,•Ø 2 -和H 2 Ø 2)是环境科学与生物化学根本意义。我们报告了一个o- C 3 N 4 / Ag 2 SO 4系统,该系统具有通过将Ag +的5s轨道与o- C 3 N 4的表面2p孤电子配位而合成的固溶体状结构。合成后的o -C 3 N 4 / Ag 2 SO 4展示了独特的电子结构,如照明的高光吸收,完美的氧化还原电势,大的BET比表面积,丰富的活性位点和有效的界面电荷转移。电子顺磁共振光谱和莫特肖特基测量确认ø -C 3 Ñ 4 /银2 SO 4层的光催化剂演示了高产高效活性•OH,•Ø 2 - ,和H 2 ö 2具有Z方案光催化原理的物种。实验和DFT计算表明,由Ag 5s构成的导带(CB)上的转移电子在辐照下能良好地转移到由N 2p组成的价带(VB)中,形成了配位配位,极大地促进了Z-中电子的传输。方案光催化体系。质量比为2到1的(o -C 3 N 42 /(Ag 2 SO 41具有•OH(45μmolL –1 h –1),•O 2 (87 )的最高光催化速率。μmolL –1 h –1)和H2 O 2(480μmolL –1 h –1)。这项工作为设计先进的光催化剂提供了一种新方法,可以有效地产生用于环境净化的活性氧。
更新日期:2018-07-06
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