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具焙烧服役史钛白粉对新制脱硝催化剂活性影响机制研究
引用本文:李柯志,罗河,赵冉,韩帅,任靖,张新军,孟凡立.具焙烧服役史钛白粉对新制脱硝催化剂活性影响机制研究[J].分子催化,2020,34(5):415-424.
作者姓名:李柯志  罗河  赵冉  韩帅  任靖  张新军  孟凡立
作者单位:中国石化催化剂有限公司工程技术研究院,中国石化催化剂有限公司长岭分公司,中石化催化剂(北京)有限公司,中国石化催化剂有限公司工程技术研究院,中国石化催化剂有限公司工程技术研究院,中石化催化剂(北京)有限公司,中石化催化剂(北京)有限公司
基金项目:中国石化催化剂有限公司科学技术研究开发项目(19-FGS-23)
摘    要:市场上废剂回收再生钛白粉以及催化剂生产企业产生的废料逐渐成为两类广泛使用的廉价钛白粉来源以降低成本。为探究两类具有焙烧服役史物料回用制备新催化剂的可能性及其对催化剂性能影响的微观作用机制,本工作将两类料按不同比例混掺制备出新催化剂样品,进行了脱硝活性测试。并结合拉曼光谱(Raman)、NH3程序升温脱附(NH3-TPD)、氢气程序升温还原(H2-TPR)、原位红外(in situ-FTIR)等手段对催化剂进行分析,探究焙烧服役史对催化剂活性的潜在影响。结果表明:具有焙烧服役史钛白粉混掺量过高则成品活性有所下降,性能下降与比表面积变化、酸性位点等均无密切联系,其根本原因是混掺料残存V2O5发生了过烧团聚,由单分散向结晶态转变,氧化还原性得到一定程度损失。在酸性无显著变化前提下,由于氧化还原受影响,从而抑制了其活性。这启示了未来应用具有焙烧服役史物料,除了考虑比表面积影响,还应着重考虑V物种高温服役烧结带来的氧化还原性能损失。

关 键 词:脱硝  选择性催化还原  焙烧  氧化还原性  团聚
收稿时间:2020/8/12 0:00:00
修稿时间:2020/8/24 0:00:00

Research on the Influence of Calcined Titanium Dioxide to the Newly-Produced Selective Catalytic Reduction Catalyst and the Mechanism
LI Ke-zhi,LUO He,ZHAO Ran,HAN Shuai,REN Jing,ZHANG Xin-jun and MENG Fan-li.Research on the Influence of Calcined Titanium Dioxide to the Newly-Produced Selective Catalytic Reduction Catalyst and the Mechanism[J].Journal of Molecular Catalysis (China),2020,34(5):415-424.
Authors:LI Ke-zhi  LUO He  ZHAO Ran  HAN Shuai  REN Jing  ZHANG Xin-jun and MENG Fan-li
Institution:Institute of Engineering Technology, Sinopec Catalyst Co., Ltd.,Changling Branch of Sinopec Catalyst Co., Ltd.,Sinopec Catalyst Beijing Co., Ltd.,Institute of Engineering Technology, Sinopec Catalyst Co., Ltd.,Institute of Engineering Technology, Sinopec Catalyst Co., Ltd.,Sinopec Catalyst Beijing Co., Ltd.,Sinopec Catalyst Beijing Co., Ltd.
Abstract:The titanium oxide from regenerated waste catalyst and from waste materials in catalyst production are gradually becoming two of the major sources of cheap replacement which could be widely obtained to decrease cost. To investigate the possibility of the use of these two sources in producing fresh catalysts and to disclose the influence mechanism from the micro-perspective, this work mixed these two titanium oxides with fresh material to produce catalyst, and the activity was evaluated. Raman spectroscopy, NH3-temperature programmed desorption (NH3-TPD), H2-temperature programmed reduction, in situ-FTIR, and other methods were combined to evaluate the catalysts, in order to analyze the possible influence of the history of calcination of these reused materials. It shows that the catalysts produced with over-added calcined titanium oxide show worse activity. The specific surface area and acid sites have less influence on the activity. The major reason is the remnant V2O5 in the calcined titanium oxide was over-sintered, to transform from isolated form to crystalized form. Thus, on the condition that the acid sites were merely changed, the redox property was suppressed, which was the reason for activity loss. This work would cast a new insight in thinking about the use of materials with calcination history in the future, that the status of V-species after sintering should be taken into consideration on the influence of activity of the catalysts besides with specific surface area.
Keywords:DeNOx  Selective catalytic reduction  Calcination  Redox  Sintering
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