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首页> 外文期刊>Environmental Science & Technology >Enhanced Photoreduction of U(Ⅵ) on C_3N_4 by Cr(Ⅵ) and Bisphenol A: ESR, XPS, and EXAFS Investigation
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Enhanced Photoreduction of U(Ⅵ) on C_3N_4 by Cr(Ⅵ) and Bisphenol A: ESR, XPS, and EXAFS Investigation

机译:Cr(Ⅵ)和双酚A增强C_3N_4上U(Ⅵ)的光还原:ESR,XPS和EXAFS研究

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摘要

The effect of Cr(VI) and bisphenol A (BPA) on U(VI) photoreduction by C3N4 photocatalyst was demonstrated by the batch experiments, electron spin resonance (ESR), X-ray photoelectron spectroscopy (XPS), X-ray absorption near edge structure (XANES), and extended X-ray absorption fine structure (EXAFS) techniques. The batch experiments manifested that Cr(VI) and BPA enhanced the photocatalytic activity of C3N4 for U(VI) photoreduction, whereas U(VI) photoreduction was significantly diminished with increased pH from 4.0 to 8.0. According to radical scavengers and ESR analysis, U(VI) was photoreduced to U(IV) by photogenerated electrons of conduction band edge, whereas Cr(VI) was reduced to Gr(III) by H2O2. BPA and its products such as organic acid and alcohols can capture photoinduced holes, which resulted in the enhancement of U(VI) photoreduction to U(IV). XPS and XANES analyses demonstrated that U(VI) was gradually photoreduced to U(IV) by C3N4 within irradiation 60 min, whereas U(IV) was reoxidized to U(VI) with increasing irradiation time. EXAFS analysis determined that the dominant interaction mechanisms of U(VI) on C3N4 after irradiation for 240 min were reductive precipitation and inner-sphere surface complexation. This work highlights the synergistic removal of radionuclides, heavy metals, and persistent organic pollutants by C3N4, which is crucial for the design and application of a high-performance photocatalyst in actual environmental cleanup.
机译:通过分批实验,电子自旋共振(ESR),X射线光电子能谱(XPS),近X射线吸收证明了Cr(VI)和双酚A(BPA)对C3N4光催化剂光还原U(VI)的影响。边缘结构(XANES)和扩展的X射线吸收精细结构(EXAFS)技术。批处理实验表明,Cr(VI)和BPA增强了C3N4对U(VI)光还原的光催化活性,而U(VI)光还原则随着pH从4.0增加到8.0显着降低。根据自由基清除剂和ESR分析,U(VI)被导带边缘的光生电子光还原为U(IV),而Cr(VI)被H2O2还原为Gr(III)。 BPA及其产品(例如有机酸和醇)可以捕获光致空穴,从而导致U(VI)光还原为U(IV)。 XPS和XANES分析表明,U(VI)在60分钟内被C3N4逐渐光还原为U(IV),而U(IV)随着照射时间的增加而被重新氧化为U(VI)。 EXAFS分析确定,辐照240分钟后U(VI)在C3N4上的主要相互作用机理是还原性沉淀和内球表面络合。这项工作强调了C3N4协同去除放射性核素,重金属和持久性有机污染物的能力,这对于在实际环境清洁中设计和应用高性能光催化剂至关重要。

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  • 来源
    《Environmental Science & Technology》 |2019年第11期|6454-6461|共8页
  • 作者单位

    North China Elect Power Univ, Coll Environm Sci & Engn, MOE Key Lab Resources & Environm Syst Optimizat, Beijing 102206, Peoples R China|Soochow Univ, Sch Radiol & Interdisciplinary Sci, Suzhou 215123, Peoples R China|Jiangsu Higher Educ Inst, Collaborat Innovat Ctr Radiat Med, Suzhou 215123, Peoples R China|Shaoxing Univ, Sch Life Sci, Huancheng West Rd 508, Shaoxing 312000, Peoples R China;

    North China Elect Power Univ, Coll Environm Sci & Engn, MOE Key Lab Resources & Environm Syst Optimizat, Beijing 102206, Peoples R China;

    North China Elect Power Univ, Coll Environm Sci & Engn, MOE Key Lab Resources & Environm Syst Optimizat, Beijing 102206, Peoples R China;

    North China Elect Power Univ, Coll Environm Sci & Engn, MOE Key Lab Resources & Environm Syst Optimizat, Beijing 102206, Peoples R China;

    Shaoxing Univ, Sch Life Sci, Huancheng West Rd 508, Shaoxing 312000, Peoples R China;

    North China Elect Power Univ, Coll Environm Sci & Engn, MOE Key Lab Resources & Environm Syst Optimizat, Beijing 102206, Peoples R China|Soochow Univ, Sch Radiol & Interdisciplinary Sci, Suzhou 215123, Peoples R China|Jiangsu Higher Educ Inst, Collaborat Innovat Ctr Radiat Med, Suzhou 215123, Peoples R China;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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