CO2 hydrogenation to methanol over Cu-In intermetallic catalysts: Effect of reduction temperature

Shi, Zhisheng; Tan, Qing‐Qing; Tian, Chao; Pan, Yunzhi; Sun, Xuewei; Zhang, Jinxin; Wu, Dongfang

doi:10.1016/j.jcat.2019.09.024

Cited by 118 publications

(82 citation statements)

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“…4a and Figure S17a), which con rmed that isolated Cu 1 -O 3 active sites in Cu/ZrO 2 were really stable. However, the local Cu particles with 0.21nm spacing for Cu (111) planes 15,48,50,51 detected in used CAZ-15 by HRTEM (Fig. 4b, Figure S17b) revealed that Cu species were partially aggregated and reduced during the catalytic process, consistent with the XPS results (Fig.…”

Section: Resultssupporting

confidence: 82%

“…3. In comparison to the CAZ-15, the absence of Cu 2p satellite peaks between 940eV and 945eV implied that no Cu 2+ species exited in the fresh and used CAZ-1 catalysts 15,44 . Identical peaks situated at 932.9eV between Cu 0 (932.4eV) and Cu 2+ (934.6eV) were observed in CAZ-1 and CAZ-1-U (U: used), indicating the Cu species were at cationic Cu δ+ state 31,45 .…”

Section: Resultsmentioning

confidence: 97%

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The Role of Cu1-O3 Species in Single-Atom Cu Catalyst for Directional Methanol Synthesis from CO2 Hydrogenation

Zhao

et al. 2021

Preprint

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Cu-based catalysts have attracted much interest in CO2 hydrogenation to methanol because of their high activity. However, the effect of interface, coordination structure, particle size and other underlying factors existed in heterogeneous catalysts render to complex active sites on its surface, therefore it is difficult to study the real active sites for methanol synthesis. Here, we report a novel Cu-based catalyst with isolated Cu active sites (Cu1-O3 units) for highly selective hydrogenating CO2 to methanol at low temperature (100% selectivity for methanol at 180 oC). Experimental and theoretical results reveal that the single-atom Cu-Zr catalyst with Cu1-O3 units is only contributed to synthesize methanol at 180 oC, but the Cu clusters or nanoparticles with Cu-Cu or Cu-O-Cu active sites will promote the process of reverse water gas shift (RWGS) side reaction to form undesirable byproducts CO. Furthermore, the Cu1-O3 units with tetrahedral structure could gradually migrate to the catalyst surface for accelerating CO2 hydrogenation reaction during catalytic process. The high activity isolated Cu-based catalyst with legible structure will be helpful to understand the real active sites of Cu-based catalysts for methanol synthesis from CO2 hydrogenation, thereby guiding further design the Cu catalyst with high performance to meet the industrial demand, at the same time as extending the horizontal of single atom catalyst for application in the thermal catalytic process of CO2 hydrogenation.

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Section: Resultssupporting

confidence: 82%

Section: Resultsmentioning

confidence: 97%

The Role of Cu1-O3 Species in Single-Atom Cu Catalyst for Directional Methanol Synthesis from CO2 Hydrogenation

Zhao

et al. 2021

Preprint

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“…89 Shi et al found that the Cu 11 In 9 phase is formed by controlled reduction of CuO-In 2 O 3 mixed oxides, and the synergy between Cu 11 In 9 and In 2 O 3 gives a CH 3 OH STY of 0.2 g MeOH g cat –1 h –1 with a selectivity of 80.5% at CO 2 conversion of 11.4% under 280 °C, 3.0 MPa, 7500 mL g –1 h –1 , and H 2 /CO 2 = 3. 69 Bavykina et al combined Co and In 2 O 3 to prepare In@Co catalysts, which significantly enhanced methanol productivity due to the formation of Co-supported In 2 O 3– x films. The CH 3 OH STY is as high as 0.86 g MeOH g cat –1 h –1 with above 80% selectivity and ∼12% conversion at 300 °C, 5.0 MPa, 27 500 mL g –1 h –1 , and H 2 /CO 2 = 4.…”

Section: Co 2 Hydrogenation To Methanolmentioning

confidence: 99%

Novel Heterogeneous Catalysts for CO₂ Hydrogenation to Liquid Fuels

et al. 2020

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Carbon dioxide (CO 2 ) hydrogenation to liquid fuels including gasoline, jet fuel, diesel, methanol, ethanol, and other higher alcohols via heterogeneous catalysis, using renewable energy, not only effectively alleviates environmental problems caused by massive CO 2 emissions, but also reduces our excessive dependence on fossil fuels. In this Outlook, we review the latest development in the design of novel and very promising heterogeneous catalysts for direct CO 2 hydrogenation to methanol, liquid hydrocarbons, and higher alcohols. Compared with methanol production, the synthesis of products with two or more carbons (C 2+ ) faces greater challenges. Highly efficient synthesis of C 2+ products from CO 2 hydrogenation can be achieved by a reaction coupling strategy that first converts CO 2 to carbon monoxide or methanol and then conducts a C–C coupling reaction over a bifunctional/multifunctional catalyst. Apart from the catalytic performance, unique catalyst design ideas, and structure–performance relationship, we also discuss current challenges in catalyst development and perspectives for industrial applications.

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“…[261][262][263] The production of H 2 O enhances also the sintering of the catalyst. [70][71][72][73][74]263 To overcome these challenges, different support materials, which can promote structural and electronic properties and stabilize smaller Cu particles, 264 were investigated, including ZrO 2 , 265,266 La 2 O 3 , 267 MoC 2 , 267 CeO 2 , 268 and La 2 O 2 CO 3 (ref. 267) and ZnO-ZrO 2 .…”

Section: Co 2 Hydrogenation To Methanolmentioning

confidence: 99%

Mechanistic and multiscale aspects of thermo-catalytic CO₂conversion to C₁products

Alam

Cheula

Moroni

et al. 2021

Catal. Sci. Technol.

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CO2 hydrogenation to methanol over Cu-In intermetallic catalysts: Effect of reduction temperature

Cited by 118 publications

References 50 publications

The Role of Cu1-O3 Species in Single-Atom Cu Catalyst for Directional Methanol Synthesis from CO2 Hydrogenation

The Role of Cu1-O3 Species in Single-Atom Cu Catalyst for Directional Methanol Synthesis from CO2 Hydrogenation

Novel Heterogeneous Catalysts for CO₂ Hydrogenation to Liquid Fuels

Mechanistic and multiscale aspects of thermo-catalytic CO₂conversion to C₁products

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CO2 hydrogenation to methanol over Cu-In intermetallic catalysts: Effect of reduction temperature

Cited by 118 publications

References 50 publications

The Role of Cu1-O3 Species in Single-Atom Cu Catalyst for Directional Methanol Synthesis from CO2 Hydrogenation

The Role of Cu1-O3 Species in Single-Atom Cu Catalyst for Directional Methanol Synthesis from CO2 Hydrogenation

Novel Heterogeneous Catalysts for CO2 Hydrogenation to Liquid Fuels

Mechanistic and multiscale aspects of thermo-catalytic CO2conversion to C1products

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Product

Resources

About

Novel Heterogeneous Catalysts for CO₂ Hydrogenation to Liquid Fuels

Mechanistic and multiscale aspects of thermo-catalytic CO₂conversion to C₁products