Enhanced CH3OH selectivity in CO2hydrogenation using Cu-based catalysts generated via SOMC from GaIII single-sites

被引：46

作者：

Lam, Erwin ^{[1
]}

Noh, Gina ^{[1
]}

Chan, Ka Wing ^{[1
]}

Larmier, Kim ^{[1
]}

Lebedev, Dmitry ^{[1
]}

Searles, Keith ^{[1
]}

Wolf, Patrick ^{[1
]}

Safonova, Olga, V ^{[2
]}

Coperet, Christophe ^{[1
]}

机构：

[1] Swiss Fed Inst Technol, Dept Chem & Appl Biosci, Vladimir Prelog Weg 2, CH-8093 Zurich, Switzerland

[2] Paul Scherrer Inst, CH-5232 Villigen, Switzerland

来源：

CHEMICAL SCIENCE | 2020年 / 11卷 / 29期

关键词：

CONTACT QUANTIFICATION MODEL; COPPER-BASED CATALYSTS; METHANOL SYNTHESIS; CO2; HYDROGENATION; ACTIVE-SITE; INFRARED-SPECTROSCOPY; ZNO SYNERGY; CONVERSION; PROMOTION; ADSORPTION;

D O I：

10.1039/d0sc00465k

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Small and narrowly distributed nanoparticles of copper alloyed with gallium supported on silica containing residual Ga(III)sites can be obtainedviasurface organometallic chemistry in a two-step process: (i) formation of isolated Ga(III)surface sites on SiO(2)and (ii) subsequent grafting of a Cu(I)precursor, [Cu((OBu)-Bu-t)](4), followed by a treatment under H(2)to generate CuGa(x)alloys. This material is highly active and selective for CO(2)hydrogenation to CH3OH.In situX-ray absorption spectroscopy shows that gallium is oxidized under reaction conditions while copper remains as Cu-0. This CuGa material only stabilizes methoxy surface species while no formate is detected according toex situinfrared and solid-state nuclear magnetic resonance spectroscopy.

引用

页码：7593 / 7598

页数：6

共 45 条

[1] Challenges in the Greener Production of Formates/Formic Acid, Methanol, and DME by Heterogeneously Catalyzed CO2 Hydrogenation Processes [J].

Alvarez, Andrea ;

Bansode, Atul ;

Urakawa, Atsushi ;

Bavykina, Anastasiya V. ;

Wezendonk, Tim A. ;

Makkee, Michiel ;

Gascon, Jorge ;

Kapteijn, Freek .

CHEMICAL REVIEWS, 2017, 117 (14) :9804-9838

[2] Solid-state interactions, adsorption sites and functionality of Cu-ZnO/ZrO2 catalysts in the CO2 hydrogenation to CH3OH [J].

Arena, Francesco ;

Italiano, Giuseppe ;

Barbera, Katia ;

Bordiga, Silvia ;

Bonura, Giuseppe ;

Spadaro, Lorenzo ;

Frusteri, Francesco .

APPLIED CATALYSIS A-GENERAL, 2008, 350 (01) :16-23

[3] Sustainable Conversion of Carbon Dioxide: An Integrated Review of Catalysis and Life Cycle Assessment [J].

Artz, Jens ;

Mueller, Thomas E. ;

Thenert, Katharina ;

Kleinekorte, Johanna ;

Meys, Raoul ;

Sternberg, Andre ;

Bardow, Andre ;

Leitner, Walter .

CHEMICAL REVIEWS, 2018, 118 (02) :434-504

[4]

BAIKER A, 1993, STUD SURF SCI CATAL, V75, P1257

[5]

Behrens M, 2012, SCIENCE, V336, P893, DOI [10.1126/science.1219831, 10.1126/science.12198331]

[6] Adsorption of gases in multimolecular layers [J].

Brunauer, S ;

Emmett, PH ;

Teller, E .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1938, 60 :309-319

[7] Fuels and energy carriers from single-site catalysts prepared via surface organometallic chemistry [J].

Coperet, Christophe .

NATURE ENERGY, 2019, 4 (12) :1018-1024

[8] Single-Sites and Nanoparticles at Tailored Interfaces Prepared via Surface Organometallic Chemistry from Thermolytic Molecular Precursors [J].

Coperet, Christophe .

ACCOUNTS OF CHEMICAL RESEARCH, 2019, 52 (06) :1697-1708

[9] Surface Organometallic and Coordination Chemistry toward Single-Site Heterogeneous Catalysts: Strategies, Methods, Structures, and Activities [J].

Coperet, Christophe ;

Comas-Vives, Aleix ;

Conley, Matthew P. ;

Estes, Deven P. ;

Fedorov, Alexey ;

Mougel, Victor ;

Nagae, Haruki ;

Nunez-Zarur, Francisco ;

Zhizhko, Pavel A. .

CHEMICAL REVIEWS, 2016, 116 (02) :323-421

[10] Ga[OSi(OtBu)3]3•THF, a thermolytic molecular precursor for high surface area gallium-containing silica materials of controlled dispersion and stoichiometry [J].

Dombrowski, James P. ;

Johnson, Gregory R. ;

Bell, Alexis T. ;

Tilley, T. Don .

DALTON TRANSACTIONS, 2016, 45 (27) :11025-11034

← 1 2 3 4 5 →