中文标题：W-Nb-O固体酸的合成并应用于低浓度一氯苯废气的催化燃烧治理
英文标题：Synthesis of W-Nb-O solid acid for catalytic combustion of low-concentration monochlorobenzene
期刊名称及期号、页码：Chemical Engineering Journal，2020，382，123045
作者姓名（中文）：陶红雨，李静，马谦益，陈振杨，张秀文，全益侥，杨鹏*，齐陈泽
作者姓名（英文）：Hongyu Tao, Jing Li, Qianyi Ma, Zhenyang Chen, Xiuwen Zhang, Yirao Quan, Peng Yang*, Chenze Qi
摘要（英文） ：WO3-Nb2O5 mixed oxides were prepared by citric acid based sol-gel method, and were tested for catalytic combustion of 1000 ppmv monochlorobenzene (MCB), as a typical chlorinated aromatic hydrocarbon in air pollution. Research results for the structure-function relationship revealed that the physicochemical properties of WO3-Nb2O5 were notably promoted than single component metal oxide, due to the strong electron interaction between W, Nb and O elements, which were confirmed by the techniques of H2-TPR, positron lifetime spectra and XPS characterization. WO3-Nb2O5 were amorphous, in which W and Nb elements were homogeneous dispersed. The functionalized materials contributed to the improvement of adsorption, activation, cracking and deep oxidation of MCB on the catalyst surface, and only non-negligible production of CO byproduct was detected. Both the acid property and oxidative property played important roles in the catalytic degradation process, and their cooperative catalytic effect could be optimized by the catalyst composition and preparation process. 2W1Nb (W/Nb = 2:1, molar ratio) displayed the largest acid amount and the best redox property, and thus it displayed the highest catalytic degradation performance, and 50% conversion of MCB was achieved at 280 °C with the GHSV of 9000 mL gcat−1 h−1. Besides, in the 120 h continuous reaction, only slight decrease (from 91% to 86%) for the catalytic activity of 2W1Nb was observed in initial 7 h, showing that it was desired towards the demanding conditions (such as resistance to water adsorption, chlorine poison and carbon deposition). Moreover, the WO3-Nb2O5 materials also satisfied the environment-friendly and low-cost needs for environmental catalysis, which could be a promising alternative for traditional V2O5-WO3/TiO2 catalyst system.
摘要（中文）：本文通过基于柠檬酸的溶胶-凝胶法制备了单组分金属氧化物和WO3-Nb2O5复合氧化物，并测试了其对1000 ppmv一氯苯（简称为MCB，是空气污染物中的典型氯化芳烃之一）的催化燃烧效果。结构-功能关系的研究结果表明，WO3-Nb2O5的物理化学性质（如介孔结构，表面元素分布，酸性和氧化性）明显优于单组分金属氧化物，这是由于W、Nb、O原子之间存在着强烈的电子相互作用，这些结论可通过H2-TPR技术、正电子寿命谱和XPS表征证实。 WO3-Nb2O5是无定形的，在该种氧化物中W和Nb元素是均匀分散的。WO3-Nb2O5多功能材料可以改善催化剂表面对模型分子MCB的吸附、活化、裂解和深度氧化。催化剂的酸性和氧化性均在催化降解过程中起重要作用，其组成和制备过程都可以优化其协同催化效果。2W1Nb（W / Nb = 2：1，摩尔比）显示出最佳的酸性和氧化性，因此在这些催化剂中表现出最佳的催化降解性能，并且在反应温度为280℃，GHSV为9000 mL gcat-1h-1的条件下实现了50％的MCB转化率。此外，在120小时连续反应中，在最初的7小时内观察到2W1Nb的催化活性仅略微下降（转化率从91％降到86％），这表明催化剂可以在苛刻的条件下运行（例如可以抵抗水吸附、氯毒和碳沉积）。此外，WO3-Nb2O5材料还满足环境友好和低成本的要求，这可能是传统V2O5-WO3 / TiO2催化剂体系的最有前途的替代品。
创新点：该研究工作引入了新的表征方法，发现WO3-Nb2O5复合氧化物材料具有较好的表面酸性质和氧化还原性能，可在较低的反应温度时实现对典型有机分子的深度氧化，有望取代目前工业上焚烧垃圾时使用的V2O5-WO3/TiO2传统催化剂，避免使用具有较高毒性的V元素。近年来，该课题组利用工业催化、环境催化学科的研究方法，发展了系列固体酸催化剂并应用在VOCs治理领域，在研究我国铌矿、稀土元素的深层次加工和利用领域取得了一系列成果。
全文链接：
https://www.sciencedirect.com/science/article/abs/pii/S138589471932457X
