Yao Dongwei, Hu Xiaohan, Wu Feng, Li Xingwen, Li Yuxi
College of Energy Engineering, Zhejiang University, Hangzhou310027, China.
Key Laboratory of Smart Thermal Management Science & Technology for Vehicles of Zhejiang Province, Taizhou317200, China.
ACS Omega. 2023 Jan 2;8(2):2421-2434. doi: 10.1021/acsomega.2c06902. eCollection 2023 Jan 17.
Based on the activity evaluation and characterization test, we explored the hydrothermal aging mechanism of a vanadium-based SCR catalyst and constructed a dual-site hydrothermal aging kinetic model in this study. The vanadium-based catalyst contains Brønsted acidic sites and Lewis acidic sites, which show different sensitivities to hydrothermal aging, and the reduction of active sites is the main reason for the NO conversion efficiency reduction after hydrothermal aging. The ammonia storage capacities of both sites have a high correlation coefficient with the NO conversion efficiency. Based on the method of NH-TPD curve peak resolution, we quantified the transformations of the two active sites and established the relationship between the site density, the aging temperature, and the duration to determine the aging factor. Then, a hydrothermal aging kinetic model was constructed, and the parameter identification and verification of the model were carried out through flow reactor experiments. The results show that the model constructed in this study can accurately reflect the catalyst activity after hydrothermal aging.
基于活性评价和表征测试,本研究探索了钒基选择性催化还原(SCR)催化剂的水热老化机理,并构建了双位点水热老化动力学模型。钒基催化剂含有布朗斯特酸性位点和路易斯酸性位点,它们对水热老化表现出不同的敏感性,活性位点的减少是水热老化后NO转化效率降低的主要原因。两个位点的氨存储容量与NO转化效率具有较高的相关系数。基于NH-TPD曲线峰解析方法,我们量化了两个活性位点的转变,并建立了位点密度、老化温度和持续时间之间的关系以确定老化因子。然后,构建了水热老化动力学模型,并通过流动反应器实验对模型进行了参数识别和验证。结果表明,本研究构建的模型能够准确反映水热老化后的催化剂活性。