Rh promoted In2O3 as a highly active catalyst for CO2 hydrogenation to methanol

被引:76
作者
Dostagir, Nazmul Hasan M. D. [1 ,2 ]
Thompson, Coogan [3 ]
Kobayashi, Hirokazu [1 ]
Karim, Ayman M. [3 ]
Fukuoka, Atsushi [1 ]
Shrotri, Abhijit [1 ]
机构
[1] Hokkaido Univ, Inst Catalysis, Kita Ku, Kita 21 Nishi 10, Sapporo, Hokkaido 0010021, Japan
[2] Hokkaido Univ, Grad Sch Chem Sci & Engn, Kita Ku, Kita 13 Nishi 8, Sapporo, Hokkaido 0608628, Japan
[3] Virginia Polytech Inst & State Univ, Dept Chem Engn, Blacksburg, VA 24060 USA
关键词
SINGLE-ATOM CATALYST; PERFORMANCE; OXIDE; DFT; PD;
D O I
10.1039/d0cy01789b
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
Synthesis of methanol with high selectivity and productivity through hydrogenation of CO2 is highly attractive. This work uses a Rh doped In2O3 catalyst to achieve a high methanol productivity of 1.0 g(MeOH) h(-1) g(cat)(-1) while maintaining the intrinsic high selectivity of pure In2O3. Rh facilitated the dissociation of H-2 leading to creation of oxygen vacancies over the In2O3 surface. In addition, Rh atoms also participated in the activation of CO2 to produce formate species with a low activation barrier as evidenced by DFT calculation. Rh species were atomically dispersed in the In2O3 matrix and were stable during a long term reaction. Under reaction conditions, the surface Rh atoms were reduced and were stabilized by charge transfer from neighbouring In atoms. Our results show that incorporation of atomic Rh species in In2O3 can lead to high methanol productivity by creation of oxygen vacancies as well as Rh centred active sites for CO2 activation.
引用
收藏
页码:8196 / 8202
页数:8
相关论文
共 24 条
[1]   Turning a Methanation Co Catalyst into an In-Co Methanol Producer [J].
Bavykina, Anastasiya ;
Yarulina, Irina ;
Al Abdulghani, Abdullah J. ;
Gevers, Lieven ;
Hedhili, Mohamed Nejib ;
Miao, Xiaohe ;
Galilea, Adrian Ramirez ;
Pustovarenko, Alexey ;
Dikhtiarenko, Alla ;
Cadiau, Amandine ;
Aguilar-Tapia, Antonio ;
Hazemann, Jean-Louis ;
Kozlov, Sergey M. ;
Oud-Chikh, Samy ;
Cavallo, Luigi ;
Gascon, Jorge .
ACS CATALYSIS, 2019, 9 (08) :6910-6918
[2]   The Structure and Properties of Amorphous Indium Oxide [J].
Buchholz, D. Bruce ;
Ma, Qing ;
Alducin, Diego ;
Ponce, Arturo ;
Jose-Yacaman, Miguel ;
Khanal, Rabi ;
Medvedeva, Julia E. ;
Chang, Robert P. H. .
CHEMISTRY OF MATERIALS, 2014, 26 (18) :5401-5411
[3]   Stabilization of active Rh2O3 species for catalytic decomposition of N2O on La-, Pr-doped CeO2 [J].
Bueno-Lopez, A. ;
Such-Basanez, I. ;
Salinas-Martinez de Lecea, C. .
JOURNAL OF CATALYSIS, 2006, 244 (01) :102-112
[4]   Direct conversion of CO2 into methanol over promoted indium oxide-based catalysts [J].
Chou, Chen-Yu ;
Lobo, Raul F. .
APPLIED CATALYSIS A-GENERAL, 2019, 583
[5]   Kinetics of deactivation on Cu/ZnO/Al2O3 methanol synthesis catalysts [J].
Fichtl, Matthias B. ;
Schlereth, David ;
Jacobsen, Nikolas ;
Kasatkin, Igor ;
Schumann, Julia ;
Behrens, Malte ;
Schloegl, Robert ;
Hinrichsen, Olaf .
APPLIED CATALYSIS A-GENERAL, 2015, 502 :262-270
[6]   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)
[7]  
Gao P, 2017, NAT CHEM, V9, P1019, DOI [10.1038/NCHEM.2794, 10.1038/nchem.2794]
[8]   Probing the local structure of crystalline ZITO: In2-2xSnxZnxO3 (x ≤ 0.4) [J].
Hoel, Cathleen A. ;
Gaillard, Jean-Francois ;
Poeppelmeier, Kenneth R. .
JOURNAL OF SOLID STATE CHEMISTRY, 2010, 183 (04) :761-768
[9]   Selective Activation of Methane on Single-Atom Catalyst of Rhodium Dispersed on Zirconia for Direct Conversion [J].
Kwon, Yongwoo ;
Kim, Tae Yong ;
Kwon, Gihun ;
Yi, Jongheop ;
Lee, Hyunjoo .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2017, 139 (48) :17694-17699
[10]   Hydroformylation of Olefins by a Rhodium Single-Atom Catalyst with Activity Comparable to RhCl(PPh3)3 [J].
Lang, Rui ;
Li, Tianbo ;
Matsumura, Daiju ;
Miao, Shu ;
Ren, Yujing ;
Cui, Yi-Tao ;
Tan, Yuan ;
Qiao, Botao ;
Li, Lin ;
Wang, Aiqin ;
Wang, Xiaodong ;
Zhang, Tao .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2016, 55 (52) :16054-16058