燃料化学学报（中英文）2025，Vol.53Issue(4)：527-537,11.DOI:10.3724/2097-213X.2024.JFCT.0015
Cu-Nix-BTC催化剂的C3H6-SCR脱硝特性的实验研究
Experimental study on C3H6-SCR activity over Cu-Nix-BTC catalysts
摘要
Abstract
Nitrogen oxides(NOx)emissions resulting from the burning of fossil fuels have detrimental effects on both human health and the environment.Therefore,it is necessary to reduce the release of NOx into the atmosphere.Selective catalytic reduction of NO with C3H6(C3H6-SCR)shows great potential because C3H6,as a reducing gas,not only reduces the expenses,but also offers enhanced safety and convenience,as compared to NH3.Low-temperature denitrification process is considered to be cost-saving and energy-efficient.Improving the low-temperature denitrification activity of the catalyst is the key point and a hot topic.Cu-BTC catalyst has the advantages of an adjustable metal site,uniform pore structure and high specific surface area and shows excellent low-temperature catalytic activity in SCR of NO using NH3(NH3-SCR),however,it has poor low-temperature activity when applied to C3H6-SCR.To overcome this limitation,in the present study,an additional metal,Ni,was introduced to Cu-BTC to enhance its low-temperature denitrification activity through intermetallic synergies effect.One-step hydrothermal technique was used to synthesize the Ni-doped Cu-Nix-BTC catalyst.The basic chemical physical properties of the catalysts were characterized by scanning electron microscopy(SEM),X-ray diffraction(XRD),N2 adsorption-desorption,X-ray photoelectron spectroscopy(XPS),temperature-programmed reduction of hydrogen(H2-TPR)and pyridine adsorption-Fourier transform infrared spectroscopy(Py-FTIR),etc.The C3H6-SCR reactivity was evaluated in a fixed bed reactor with flue gas consisting 0.05%NO,0.1%C3H6,5%O2.The results demonstrated that the introduction of Ni improved the catalytic activity of Cu-BTC.The Cu-Ni1/2-BTC catalyst achieved a NO conversion rate of 100%and N2 selectivity of 98.3%at 250-275℃,and the C3H6 conversion rate of Cu-Ni1/2-BTC is higher at the same temperature,and the C3H6 conversion temperature moves to low temperature.The resistance to SO2 of Cu-Ni1/2-BTC catalyst was tested.Results showed,when there was 0.02%SO2 in the simulated flue gas,the NO conversion rate of Cu-Ni1/2-BTC decreased to 89.2%at 275℃because of the formation of sulfate on the catalyst surface.Characterization results demonstrated that Ni was effectively doped into the catalyst framework structure and evenly distributed over the catalyst surface.Results from XRD patterns and SEM images demonstrated that Cu-Nix-BTC retained the characteristics peaks and basic morphology of Cu-BTC.The XPS spectra showed that the doped Ni existed as Ni2+and Ni3+,and that once Ni was doped,the Cu+content in the catalysts increased,suggesting that there was strong electron transfer between Ni and Cu.As the Ni content increased,the specific surface area and pore volume of the catalysts progressively decreased,while the pore size initially increased and then decreased.The H2-TPR data proved that when Ni was doped,the reduction peaks of the catalysts shifted to a lower temperature and exhibited a higher reduction capacity.Results showed that Cu-Nix-BTC possessed better redox properties at low temperatures,more surface-adsorbed oxygen,more Cu+ions,and more Lewis acid than Cu-BTC,all of which contributed to its increased catalytic activity.关键词
氮氧化物还原/C3H6-SCR/催化剂/Cu-Nix-BTC/一步水热法Key words
NOx reduction/C3H6-SCR/catalyst/Cu-Nix-BTC/one-step hydrothermal technique分类
资源环境引用本文复制引用
张津威,李炬星,宁淑英,张艳梅,苏亚欣..Cu-Nix-BTC催化剂的C3H6-SCR脱硝特性的实验研究[J].燃料化学学报（中英文）,2025,53(4):527-537,11.基金项目
The project was supported by the National Natural Science Foundation of China(52276103).国家自然科学基金(52276103)资助 （52276103）
