CO2 Hydrogenation to Methanol over PdZnZr Solid Solution: Effects of the PdZn Alloy and Oxygen Vacancy

被引:51
作者
Huang, Chaojie [1 ,2 ]
Wu, Zhaoxuan [1 ]
Luo, Hu [1 ]
Zhang, Shunan [1 ,2 ]
Shao, Zilong [1 ,2 ]
Wang, Hui [1 ]
Sun, Yuhan [1 ,3 ]
机构
[1] Chinese Acad Sci, CAS Key Lab Low Carbon Convers Sci & Engn, Shanghai Adv Res Inst, Shanghai 201210, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[3] Shanghai Tech Univ, Sch Phys Sci & Technol, Shanghai 201203, Peoples R China
基金
中国国家自然科学基金;
关键词
CO2; hydrogenation; methanol; solid solution catalyst; PdZn alloy; oxygen vacancy; CATALYSTS; AROMATICS; DRIFTS; PD/ZNO; SITES; GAS; ZNO;
D O I
10.1021/acsaem.1c01502
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
Utilization of CO2 with renewable hydrogen to produce value-added chemicals is highly desirable to reduce the dependence on fossil fuels. Methanol is a key intermediate for hydrocarbon products as they require a high methanol selectivity at high temperature to connect the methanol-to-olefin and methanol-to-aromatic processes. To improve the performance of CO2 hydrogenation at a higher temperature, this study prepared a 0.1% Pd/ZnZr catalyst using the coprecipitation method, which showed an 87% methanol selectivity and a space time yield of 735 g(methanol) kg(cat)(-1) h(-1) at 320 degrees C, significantly higher than that of the binary ZnZr solid solution (434 g(methanol) kg(cat)(-1) h(-1)). The characterization of the catalyst revealed that Pd2+ species formed a PdZn alloy from the ZrO2 lattice. More oxygen vacancies were generated on the surface, which enhanced the CO2 adsorption and activation capacity and then led to the formation of a higher amount of *HCOO species and better catalytic performance.
引用
收藏
页码:9258 / 9266
页数:9
相关论文
共 42 条
[1]   Catalytic enrichment of plasma with hydroxyl radicals in the aqueous phase at room temperature [J].
Audemar, Maite ;
Vallcorba, Oriol ;
Peral, Inma ;
Thomann, Jean-Sebastien ;
Przekora, Agata ;
Pawlat, Joanna ;
Canal, Cristina ;
Ginalska, Grazyna ;
Kwiatkowski, Michal ;
Duday, David ;
Hermans, Sophie .
CATALYSIS SCIENCE & TECHNOLOGY, 2021, 11 (04) :1430-1442
[2]   Pd/ZnO catalysts for direct CO2 hydrogenation to methanol [J].
Bahruji, Hasliza ;
Bowker, Michael ;
Hutchings, Graham ;
Dimitratos, Nikolaos ;
Wells, Peter ;
Gibson, Emma ;
Jones, Wilm ;
Brookes, Catherine ;
Morgan, David ;
Lalev, Georgi .
JOURNAL OF CATALYSIS, 2016, 343 :133-146
[3]   A DRIFTS STUDY OF THE MORPHOLOGY AND SURFACE ADSORBATE COMPOSITION OF AN OPERATING METHANOL SYNTHESIS CATALYST [J].
BAILEY, S ;
FROMENT, GF ;
SNOECK, JW ;
WAUGH, KC .
CATALYSIS LETTERS, 1995, 30 (1-4) :99-111
[4]  
Behrens M, 2012, SCIENCE, V336, P893, DOI [10.1126/science.1219831, 10.1126/science.12198331]
[5]   Observational determination of surface radiative forcing by CO2 from 2000 to 2010 [J].
Feldman, D. R. ;
Collins, W. D. ;
Gero, P. J. ;
Torn, M. S. ;
Mlawer, E. J. ;
Shippert, T. R. .
NATURE, 2015, 519 (7543) :339-+
[6]   In-situ infrared study of methanol synthesis from H-2/CO2 over Cu/SiO2 and Cu/ZrO2/SiO2 [J].
Fisher, IA ;
Bell, AT .
JOURNAL OF CATALYSIS, 1997, 172 (01) :222-237
[7]   Atomic-scale engineering of indium oxide promotion by palladium for methanol production via CO2 hydrogenation [J].
Frei, Matthias S. ;
Mondelli, Cecilia ;
Garcia-Muelas, Rodrigo ;
Kley, Klara S. ;
Puertolas, Begona ;
Lopez, Nuria ;
Safonova, Olga, V ;
Stewart, Joseph A. ;
Ferre, Daniel Curulla ;
Perez-Ramirez, Javier .
NATURE COMMUNICATIONS, 2019, 10 (1)
[8]   Iron-Based Fischer-Tropsch Synthesis for the Efficient Conversion of Carbon Dioxide into Isoparaffins [J].
Geng, Shunshun ;
Jiang, Feng ;
Xu, Yuebing ;
Liu, Xiaohao .
CHEMCATCHEM, 2016, 8 (07) :1303-1307
[9]   Methanol-to-olefins process technology: current status and future prospects [J].
Gogate, Makarand R. .
PETROLEUM SCIENCE AND TECHNOLOGY, 2019, 37 (05) :559-565
[10]   Highly active copper-ceria and copper-ceria-titania catalysts for methanol synthesis from CO2 [J].
Graciani, Jesus ;
Mudiyanselage, Kumudu ;
Xu, Fang ;
Baber, Ashleigh E. ;
Evans, Jaime ;
Senanayake, Sanjaya D. ;
Stacchiola, Dario J. ;
Liu, Ping ;
Hrbek, Jan ;
Fernandez Sanz, Javier ;
Rodriguez, Jose A. .
SCIENCE, 2014, 345 (6196) :546-550