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Nature Identification of Cu Active Sites in Sulfur-Fouled Cu/SAPO-34 Regeneration
Industrial & Engineering Chemistry Research ( IF 4.2 ) Pub Date : 2018-03-01 00:00:00 , DOI: 10.1021/acs.iecr.7b05053
Meiqing Shen 1, 2, 3 , Xinhua Li 1 , Jianqiang Wang 1 , Chen Wang 4 , Jun Wang 1
Affiliation  

In order to probe the nature of regeneraion on the sulfated Cu/SAPO-34 selective catalytic reduction catalysts, CHA structure, copper species, and NOx conversion were investigated. A sulfated Cu/SAPO-34 catalyst was treated at different temperatures and times. The ammonia-sulfate species was removed at 500 °C, and copper sulfate was completely decompose at 750 °C. The NOx conversion of sulfated catalyst gradually recovers with the degree of regeneration increasing. XRD and ex situ DRIFTs results show that thermal treatment presents no effect on the framework structure of Cu/SAPO-34. The TPR and EPR results suggest that thermal treatment has an influence on the number of isolated Cu2+ and CuO instead of coordination environment and redox ability. However, the apparent activation energy of fresh, sulfated, and regenerated catalysts for SCR reaction remains the same, and turnover frequencies are also identical. The study reveals that the activity recovery is attributed to the increased number of active sites by sulfate species decomposition and migration effect.

中文翻译:

硫污染的Cu / SAPO-34再生过程中Cu活性位点的性质鉴定

为了探讨在硫酸化的Cu / SAPO-34选择性催化还原催化剂上再生的性质,研究了CHA结构,铜种类和NO x转化率。在不同的温度和时间对硫酸化的Cu / SAPO-34催化剂进行了处理。在500°C时除去硫酸氨,在750°C时硫酸铜完全分解。使NO X的硫酸化催化剂逐渐恢复时的转化率随着再生的增加的程度。XRD和异位DRIFTs结果表明,热处理对Cu / SAPO-34的骨架结构没有影响。TPR和EPR结果表明热处理对分离出的Cu 2+的数量有影响。而CuO代替了协调环境和氧化还原能力。然而,新鲜的,硫酸化的和再生的用于SCR反应的催化剂的表观活化能保持不变,并且周转频率也相同。研究表明,活性恢复归因于硫酸盐类物质分解和迁移作用增加了活性位点的数量。
更新日期:2018-03-01
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