【摘要】 为消除氮氧化物对人类健康和生态环境的危害,以甲烷为还原剂进行选择性催化脱硝（CH₄-SCR）得到了普遍的关注。研发高活性的CH₄-SCR脱硝催化剂成为该技术的研究重点。采用浸渍法制备了Co（x）/ZRP催化剂,考察了钴负载量对Co（x）/ZRP催化剂CH₄-SCR脱硝性能的影响。利用X射线衍射仪（XRD）、H₂程序升温还原（H₂-TPR）、吡啶吸附红外光谱（Py-IR）、NH₃程序升温脱附（NH₃-TPD）和NO程序升温脱附（NO-TPD）等对Co（x）/ZRP催化剂的理化性质进行了表征,在常压固定床微型反应器上评价了Co（x）/ZRP催化剂的CH₄-SCR脱硝性能。结果表明:Co（x）/ZRP催化剂中钴物种为Co₃O₄,钴负载量增加,Co₃O₄晶粒变大,催化剂的氧化还原能力和NO的吸脱附性能均得到改善。随着钴负载量的增加,Co（x）/ZRP催化剂的CH₄-SCR脱硝活性先增强后降低,与催化剂中的中强酸量在总酸中的变化规律基本一致。其中Co（20）/ZRP催化剂的中强酸量较多,CH₄-SCR脱硝性能较好,T_m为342℃,X_No^max为39.2%。催化剂表面的L酸位以及中强酸量对催化剂的CH₄-SCR催化脱硝活性具有重要作用。更多还原

【Abstract】 To eliminate the harm of nitrogen oxides to human health and ecological environment,selective catalytic denitrification using methane as a reducing agent （CH₄-SCR） has received widespread attention.Developing highly active CH4-SCR denitrification catalysts has become a research focus of this technology.In this article,Co（x）/ZRP catalysts were prepared by impregnation method,and the effects of Co（x）/ZRP catalysts with different cobalt loading amounts on the denitrification performance of CH4-SCR were investigated.The physicochemical properties of Co （x）/ZRP catalysts were characterized using XRD,H₂-TPR,Py-IR,NH₃-TPD and NO-TPDmethods.The CH₄-SCR denitrification performance of Co（x）/ZRP catalysts was evaluated on fixed bed micro-reactor under atmospheric pressure.The results showed that the cobalt species in the Co（x）/ZRP catalyst were Co₃O₄.With the increase of cobalt loading,the Co₃O₄ grains became larger,the redox ability and NO adsorption and desorption performance of the catalyst were improved.With the increase of cobalt loading,the denitrification activity of Co（x）/ZRP catalyst first increased and then decreased,which was consistent with the variation of medium strong acid amount in the total acid of the catalyst.Among them,the Co（20）/ZRP catalyst had a higher amount of medium strong acid,and the CH₄-SCR denitrification performance was good,with T_m of 342℃,X^max_Noof 39.2%.The L-acid and medium strong acid content of the catalyst played an important role in the CH4-SCR catalytic denitrification activity of the catalyst.更多还原