Ling Wang, Minghui Tang, Hongxian Li, Jiamin Ding, Juan Qiu, Shengyong Lu
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The V/T-1%NHPC catalyst could achieve expectant low-temperature performances with 50% furan conversion at 150 °C and a complete conversion at 200 °C, which decreased 23 °C and 40 °C compared to the V/T catalyst respectively. Moreover, the addition of NHPC presented lifting chemical stability during long-time test. The addition of NHPC in V/T catalysts decreased the formation of crystalline V<sub>2</sub>O<sub>5</sub> and increased the percentages of V<sup>5+</sup> and O<sub>lat</sub>, which improved the utilization of vanadium ions and the catalytic activity. Simultaneously, the higher binding energy shift of O<sub>lat</sub> implied more reaction possibility with other oxidise reactants. Importantly, this work proved the lifting catalytic activity by the interaction between catalysts and NHPC, and proposed the promoting effects of the N element. The results showed that the content of the pyridinic N and graphitic N in NHPC changed after combining with V/T catalyst, which played crucial roles in the excellent catalytic performance. Overall, this work provides comprehensive research of the V/T-1%NHPC catalyst toward furan oxidation at low temperature and explain the effects of N-doped biomass carbon in catalytic activity clearly, which gave a new thought to design low-temperature catalysts in PCDD/Fs degradation. 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引用次数: 0
摘要
多氯二苯并对二恶英和多氯二苯并呋喃(PCDD/Fs)因其剧毒性而受到广泛关注,其在实验室中的操作难度也使研究过程变得艰难。因此,在我们的工作中,由于呋喃具有相同的中心含氧环结构,因此被选为模型化合物。虽然催化氧化法被认为是一种有效且适用的多氯二苯并对二恶英/多氯二苯并呋喃减排方法,但在实际应用中,低温催化剂的合成仍然是一个具有挑战性的问题。考虑到这一情况,我们通过湿法浸渍制备了一种新型 V2O5/TiO2 催化剂,并用掺杂 N 的分层多孔碳(NHPC)对其进行了修饰。V/T-1%NHPC 催化剂可实现预期的低温性能,在 150 °C 时呋喃转化率为 50%,在 200 °C 时完全转化,与 V/T 催化剂相比分别降低了 23 °C 和 40 °C。此外,NHPC 的添加在长期试验中表现出了较高的化学稳定性。在 V/T 催化剂中添加 NHPC 可减少结晶 V2O5 的形成,增加 V5+ 和 Olat 的比例,从而提高钒离子的利用率和催化活性。同时,Olat 较高的结合能转移意味着与其他氧化反应物发生反应的可能性更大。重要的是,这项工作证明了催化剂与 NHPC 之间的相互作用可提高催化活性,并提出了 N 元素的促进作用。结果表明,NHPC 与 V/T 催化剂结合后,NHPC 中吡啶 N 和石墨 N 的含量发生了变化,这对催化剂的优异催化性能起到了关键作用。总之,本研究对 V/T-1%NHPC 催化剂在低温下的呋喃氧化作用进行了全面研究,清楚地解释了掺杂 N 的生物质碳对催化活性的影响,为设计低温降解 PCDD/Fs 的催化剂提供了新思路。此外,N物种的内部功能机理也值得在今后的研究中进一步探讨。
Enhancing mechanisms of N-doped biomass carbon on the vanadium-based catalyst for furan degradation at low temperature
Polychlorinated dibenzo-p-dioxins and polychlorinated dibenzofurans (PCDD/Fs) have attracted widespread concern due to their high toxicity, and their difficult manipulation in laboratories has made the research process tough. Thus, in our work, furan is selected as the model compound owing to the same structure of a central oxygenate ring. Although catalytic oxidation is regarded as an effective and applicable method for the abatement of PCDD/Fs, the synthesis of low-temperature catalysts is still a challenging problem in practical applications. Considering this situation, we prepared a novel V2O5/TiO2 catalyst modified with N-doped hierarchical porous carbon (NHPC) via a wet impregnation method. The V/T-1%NHPC catalyst could achieve expectant low-temperature performances with 50% furan conversion at 150 °C and a complete conversion at 200 °C, which decreased 23 °C and 40 °C compared to the V/T catalyst respectively. Moreover, the addition of NHPC presented lifting chemical stability during long-time test. The addition of NHPC in V/T catalysts decreased the formation of crystalline V2O5 and increased the percentages of V5+ and Olat, which improved the utilization of vanadium ions and the catalytic activity. Simultaneously, the higher binding energy shift of Olat implied more reaction possibility with other oxidise reactants. Importantly, this work proved the lifting catalytic activity by the interaction between catalysts and NHPC, and proposed the promoting effects of the N element. The results showed that the content of the pyridinic N and graphitic N in NHPC changed after combining with V/T catalyst, which played crucial roles in the excellent catalytic performance. Overall, this work provides comprehensive research of the V/T-1%NHPC catalyst toward furan oxidation at low temperature and explain the effects of N-doped biomass carbon in catalytic activity clearly, which gave a new thought to design low-temperature catalysts in PCDD/Fs degradation. Besides, the internal functional mechanisms of N species are worth further exploration in future studies.