双金属有机骨架材料衍生CuO-Cu_(1.5)Mn_(1.5)O_(4)复合氧化物的丙烷催化燃烧性能  

SYNTHESIS OF CuO-Cu_(1.5)Mn_(1.5)O_(4) COMPOSITE OXIDE BY USING A BIMETALLIC ORGANIC FRAMEWORK FOR CATALYTIC PROPANE TOTAL OXIDATION

作　　者：冯超 熊高燕 汪云霞 潘原 柳云骐[1] FENG Chao;XIONG Gaoyan;WANG Yunxia;PAN Yuan;LIU Yunqi(Collge of Chemical Engineering,China University of Petroleum(East China),Qingdae 266580,China)

机构地区：[1]中国石油大学(华东)化学工程学院,山东青岛266580

出　　处：《环境工程》2022年第8期69-77,共9页Environmental Engineering

基　　金：国家自然科学基金(21878334);山东省泰山学者青年专家人才项目(tsqn201909065)。

摘　　要：采用气相辅助的离子置换法,合成了Cu、Mn双金属有机骨架(MOF)材料,通过控制煅烧条件制备了一系列CuO-Cu_(1.5)Mn_(1.5)O_(4)复合氧化物,研究了不同n(Mn)/n(Cu)对丙烷催化燃烧性能的影响。结果表明:随着n(Mn)/n(Cu)提高,CuO-Cu_(1.5)Mn_(1.5)O_(4)催化丙烷燃烧能力增强,当n(Mn)/n(Cu)为31∶69时,催化剂对丙烷的完全燃烧温度(T_(90))仅为309.8℃,催化活性远高于CuO和Mn_(2)O_(3)。表征和密度泛函理论(DFT)计算结果表明,由于Mn和Cu的相互作用,复合氧化物表面具有更高的n(Mn^(4+))/n(Mn^(3+))和n(Cu^(+))/n(Cu^(2+)),从而增强了催化剂的低温还原性能。并且n(Cu^(+))/n(Cu^(2+))提高导致催化剂中氧空位浓度升高,更容易吸附活化O_(2)、丙烷分子,增强了催化剂的丙烷燃烧性能。In the paper,Cu and Mn bimetallic organic framework materials were prepared using the gas-assisted ion replacement method.A series of CuO-Cu_(1.5)Mn_(1.5)O_(4) composite oxides were prepared through controlled calcination,and the effect of various n(Mn)/n(Cu)on the catalytic performance of propane total oxidation was studied.The results revealed that with an increase in the n(Mn)/n(Cu),CuO-Cu_(1.5)Mn_(1.5)O_(4) catalysts showed enhanced propane total oxidation catalytic activities.When n(Mn)/n(Cu)was 31∶69,the complete combustion temperature(T_(90))of propane was just 309.8℃,signifying that the activity was much higher than that of CuO and Mn_(2)O_(3).The experimental and density functional theory(DFT)calculation results revealed that the synergetic effect of Mn and Cu increased the n(Mn^(4+))/n(Mn^(3+))and n(Cu^(+))/n(Cu^(2+))on the surface,which enhanced the redox ability at low-temperature.Meanwhile,the increase of n(Cu^(+))/n(Cu^(2+))led to a higher concentration of oxygen vacancies,and made it easier to adsorb and activate oxygen and propane molecules on the surface,thereby boosted the propane catalytic oxidation performance.

关 键 词：CuO-Cu_(1.5)Mn_(1.5)O_(4)复合氧化物 丙烷催化燃烧 氧化还原性能 MOF材料 协同作用 

分 类 号：TQ426[化学工程] X701[环境科学与工程—环境工程]