Doping Pd 2+into Ni n CeO x nanofibers promotes low-temperature CO 2 methanation

被引:3
作者
Zhang, Mengyuan [1 ,2 ]
Ye, Jian [1 ]
Lu, Nana [1 ]
Lu, Xiaoyan [1 ]
Luo, Kongliang [1 ]
Dong, Jiali [1 ]
Niu, Qiang [3 ]
Zhang, Pengfei [1 ,2 ]
Dai, Sheng [4 ]
机构
[1] Ningxia Univ, Coll Chem & Chem Engn, State Key Lab High Efficiency Utilizat Coal & Gree, Yinchuan 750021, Peoples R China
[2] Shanghai Jiao Tong Univ, Sch Chem & Chem Engn, Shanghai 200240, Peoples R China
[3] Inner Mongolia Erdos Elect Power & Met Grp Co Ltd, Natl Enterprise Technol Ctr, Ordos 016064, Inner Mongolia, Peoples R China
[4] Oak Ridge Natl Lab, Chem Sci Div, Oak Ridge, TN 37830 USA
基金
中国国家自然科学基金;
关键词
Low-temperature; Nanofiber; CO2; methanation; In situ DRIFTS; DFT calculations; OXYGEN VACANCIES; CATALYST; NANOPARTICLES; HYDROGENATION; PERFORMANCE; ROLES;
D O I
10.1016/j.jcat.2024.115535
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
CO 2 methanation at low temperatures is still a challenge. Herein, Ni n CeO x (n = 1 - 3) and Ni 2.5 Pd 0.1 CeO x nanofibers by electrospinning is reported. The main advantage of this method is to obtain the highly dispersed precursor of palladium, nickel, and cerium, overcoming the difficulty of uniform mixing in conventional preparation methods. The Ni 2.5 Pd 0.1 CeO x nanofiber catalyst exhibited outstanding catalytic performance at low temperatures (CO 2 conversion rate = 90.4 %, CH 4 selectivity = 99.6 % at 230 degrees C) along with exceptional stability over 300 h. EPR, Raman, and O 1s XPS confirmed that Pd 2+ doping increased oxygen vacancy concentration. Insitu infrared spectroscopy indicated that CO 2 methanation on Ni 2.5 CeO x and Ni 2.5 Pd 0.1 CeO x catalysts followed the formate pathways. Pd 2+ doping increased the number of surface oxygen vacancies and hydroxyl groups, thus increasing the amount of bicarbonates and formates. DFT calculations suggested that Pd 2+ doping increased CO 2 adsorption energy, and confirmed surface hydroxyl groups and bicarbonate being beneficial for CO 2 methanation, consequently enhancing the activity of Ni 2.5 Pd 0.1 CeO x catalyst especially at low temperatures.
引用
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页数:15
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