摘要
采用原位合成法将Ni单原子限域的Ni-N掺杂碳纳米管(NCNT)结构架构建到活性炭(AC)表面制备了Ni-NCNT/AC载体,再利用浸渍法制备了负载金属Ru催化剂(Ru@Ni-NCNT/AC),然后评价了其在催化湿式氧化乙酸过程中总有机碳的去除率。通过SEM、TEM、X射线吸收精细结构光谱(XAFS)、XPS、H_(2)-TPR和一氧化碳-漫反射傅里叶变换红外光谱(CO-DRIFTS)对样品的形貌、结构、元素价态、表面吸附和化学性质进行了表征和分析。此外,采用密度泛函理论计算了O_(2)和乙酸分子在催化剂表面的吸附构型及吸附能。结果表明,Ni单原子作为催化助剂能通过改变基底材料的电子特性促进表面贵金属发挥更高的催化氧化乙酸的活性。在温度250℃、压力6.5 MPa条件下,连续运行240h,乙酸的去除率持续稳定在95%以上,催化剂具有较高活性和良好的稳定性。
Ni-NCNT/AC carrier was firstly synthesized by in-situ growth of single atom Ni confined Ni-N doped carbon nanotubes(NCNT)on activated carbon(AC)surface,and then was impregnated with Ru to prepare catalyst Ru@Ni-NCNT/AC,whose catalytic activity in wet oxidation of acetic acid was evaluated by measuring the removal rate of total organic carbon.The morphology,structure,element valence,surface adsorption and chemical properties of the catalyst samples were characterized and analyzed respectively by SEM,TEM,X ray absorption fine structure spectroscopy(XAFS),XPS,H_(2)-TPR and carbon monoxide diffuse reflectance infrared Fourier transform spectroscopy(CO-DRIFTS).Moreover,the adsorption configurations as well as energies of O_(2) and acetic acid on catalyst surface were computed by density functional theory.The results showed that single atom Ni was promoter,by changing the electronic properties of the substrate material to increase the catalytic performance of surface precious metals for the oxidation of acetic acid.After continuous operation for 240 h at 250℃ and 6.5 MPa,the removal rate of acetic acid remained stable above 95% while the catalyst retained high activity and good stability.
作者
张立涛
安路阳
尹健博
裴振
靳承煜
卫皇曌
ZHANG Litao;AN Luyang;YIN Jianbo;PEI Zhen;JIN Chengyu;WEI Huangzhao(Engineering Research Center of Iron and Steel Industry Wastewater Advanced Treatment Technology of Liaoning Province,Sinosteel Anshan Research Institute of Thermo-Energy Co.,Ltd.,Ltd,Anshan 114044,Liaoning,China;Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian116023,Liaoning,China)
出处
《精细化工》
EI
CAS
CSCD
北大核心
2022年第7期1426-1433,共8页
Fine Chemicals
基金
辽宁省自然科学基金(2019-ZD-0894)。
关键词
碳纳米管
限域单原子
湿式氧化
助剂
催化技术
carbon nanotubes
confined single-atom
wet oxidation
promoter
catalytic technology
