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沉淀剂对Co3O4催化分解N2O的性能影响OA北大核心CSTPCD

Effect of precipitating agent on the performance of Co3O4-catalyzed decomposition of N2O

中文摘要英文摘要

以乙酸钴为钴源采用水热法制备了Co3O4催化剂,通过X射线衍射仪、傅里叶变换红外光谱仪、透射电子显微镜、扫描电子显微镜、N2物理吸附脱附测试、H2程序升温还原、氧的程序升温脱附和X射线光电子能谱等表征手段对Co3O4催化剂的物理化学性质进行表征,在固定床微型反应器中评价催化剂催化分解N2O活性,考察了不同沉淀剂(氢氧化钠、碳酸钠、碳酸氢钠、尿素、碳酸铵、氨水)对催化剂催化分解N2O的性能影响.结果表明,水热法制备的Co3O4催化剂均为尖晶石结构,不同沉淀剂影响催化剂形貌、氧化还原性能和催化分解N2O活性;含有钠离子沉淀剂制备而得的催化剂活性高于其他催化剂,其促进了 Co3+到Co2+的还原过程,影响了钴离子化学环境,提高了给电子能力,弱化了催化剂中的Co—O键,加快了反应过程中氧空位的再生,进而提高了自身的催化活性;其中含少量Na离子的Co3O4-NaOH催化剂具有较强的氧化还原性,Oads/Olatt较大,表面吸附氧数量多,N2O分解温度较低,在反应气体组成为0.88%O2、0.65%N2O,N2为平衡气的(流量为80mL/min)条件下,T10和 T95分别为 330℃和470℃.

The Co3O4 composite metal oxides were prepared by the hydrothermal method using cobalt acetate as the cobalt source.The physicochemical properties of the catalysts were characterized by XRD,FTIR,TEM,SEM,BET,H2-TPR,O2-TPD and XPS.The catalyst catalytic decomposition activity of N2O was evaluated in a fixed-bed microreactor,and the effect of precipitants(NaOH、Na2CO3、NaHCO3、H2NCONH2、CH8N2O3、NH3·H2O)on the catalytic decomposition performance of N2O was investigated.The results showed that the Co3O4 catalysts prepared by the hydrothermal method were all of spinel structure,and different precipitating agents affected the catalyst morphology,redox performance and catalytic decomposition N2O activity.The activity of the catalysts prepared with sodium precipitant was higher than that of other catalysts because it promoted the reduction process of Co3+to Co2+,influenced the chemical environment of cobalt ions,improved the electron donating capability,weakened the Co—O bond in the catalyst,and accelerated the regeneration of oxygen vacancies during the catalytic reaction.The Co3O4-NaOH catalyst,which contained a small amount of Na ions,had a strong redox ability,a large Oads/Olatt ratio,resulting in a large amount of oxygen adsorbed on the surface,and a low N2O decomposition temperature.Under the conditions of the reaction gas composition of 0.88%O2,0.65%N2O,and N2 as equilibrium gas(flow rate of 80mL/min),T10 and T95 were 330℃ and 470℃,respectively.

孙巾茹;宋傲磊;赵明新;赵田田;王虹;柯明

中国石油大学(北京)重质油全国重点实验室,北京 102249||北京石油化工学院燃料清洁化及高效催化减排技术北京市重点实验室,北京 102617北京石油化工学院燃料清洁化及高效催化减排技术北京市重点实验室,北京 102617中国石油大学(北京)重质油全国重点实验室,北京 102249

化学工程

沉淀剂氧化亚氮四氧化三钴钠离子氧空位

precipitating agentnitrous oxidetricobalt tetraoxidesodium ionoxygen vacancy

《化工进展》 2024 (004)

1823-1831 / 9

国家自然科学基金(2167329).

10.16085/j.issn.1000-6613.2023-0579

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