(1. 中南大學(xué) 冶金與環(huán)境學(xué)院,長沙 410083;
2. 武漢科技大學(xué) 國家環(huán)境保護(hù)礦冶資源利用與污染控制重點(diǎn)實(shí)驗(yàn)室,武漢 430081;
3. 安徽工業(yè)大學(xué) 冶金減排與資源綜合利用教育部重點(diǎn)實(shí)驗(yàn)室,馬鞍山 243002;
4. 長沙瑞熙環(huán)保設(shè)備制造有限公司,長沙 410201)
摘 要: 低溫催化劑是CO選擇性催化還原(CO-SCR)的關(guān)鍵。本文通過一步溶劑熱法成功合成Cu1/6-MOF-5催化劑,利用X射線衍射儀(XRD)、掃描電子顯微鏡(SEM)、傅里葉紅外光譜(FTIR)、拉曼光譜(Raman)、X射線光電子能譜(XPS)對(duì)催化劑的結(jié)構(gòu)進(jìn)行表征。結(jié)果表明:摻雜的Cu元素具有Cu+、Cu2+兩種價(jià)態(tài),且部分取代了MOF-5中的Zn位形成雙金屬有機(jī)骨架Cu1/6-MOF-5。同時(shí),Cu的摻雜增加了氧空位的濃度,從而使得催化劑擁有更高的催化活性,Cu1/6-MOF-5的脫硝率在160 ℃時(shí)達(dá)到89%,在200 ℃時(shí)達(dá)到95%,分別比相應(yīng)溫度下MOF-5的脫硝率高57%和25%;即使在含硫環(huán)境中,其在200 ℃時(shí)的脫硝率仍大于87%。
關(guān)鍵字: MOF-5;Cu摻雜;CO-SCR;脫硝機(jī)理
(1. School of Metallurgy and Environment, Central South University, Changsha 410083, China;
2. National Key Laboratory of Environmental Protection Mining and Metallurgy Resources Utilization and Pollution Control, Wuhan University of Science and Technology, Wuhan 430081, China;
3. Key Laboratory of Metallurgical Emission Reduction & Resources Recycling, Ministry of Education, Anhui University of Technology, Ma’anshan 243002, China;
4. Changsha Ruixi Environmental Protection Equipment Manufacturing Co., Ltd., Changsha 410201, China)
Abstract:Low-temperature catalyst is the key to CO-selective catalytic reduction (CO-SCR). Cu1/6-MOF-5 catalyst was successfully synthesized by one-step solvothermal method. X-ray diffractometer (XRD), scanning electron microscope (SEM), Fourier transform infrared spectroscopy (FTIR), Raman spectroscopy (Raman) and X-ray photoelectron spectroscopy (XPS) were used to characterize the structure of the catalysts. The results show that the doped Cu exists in +1 and +2 valence states and partially replaces the Zn site in MOF-5 to form the bimetallic organic framework Cu1/6-MOF-5. At the same time, the Cu doping increases the concentration of oxygen vacancies, so that the catalyst has higher catalytic activity. Specifically, the denitrification rate of Cu1/6-mof-5 catalyst increases from 32% to 89% at 160 ℃ and from 70% to 95 % at 200 ℃. Even in the sulfur-containing environment, the NO conversion rate can still reach 87% at 200 ℃.
Key words: MOF-5; Cu doping; CO-SCR; denitration mechanism


