Intermetallic PdIn catalyst for CO<sub>2</sub> hydrogenation to methanol: mechanistic studies with a combined DFT and microkinetic modeling method

Wu, Panpan; Yang, Bo

doi:10.1039/c9cy01242g

Cited by 49 publications

(39 citation statements)

References 77 publications

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“…No activation of the CO 2 molecule is compulsory on PdZn, in contrast to what has been proposed by Zhang et al on Pd, starting from activated CO 2 , adsorbed in a bidendate configuration ( E ads Pd > 0) to make the formate pathway achievable. Comparable trends have been calculated by alloying Pd with other metals, whether the considered active surface presents a similar surface structure ( E act PdIn(110) = 0.05 eV) or not ( E act PdCu(111) = 0.62 eV) . Once HCOO is formed, several steps can be considered (Figure S6, Table S5).…”

mentioning

confidence: 86%

Tuning Adsorption Energies and Reaction Pathways by Alloying: PdZn versus Pd for CO₂ Hydrogenation to Methanol

Brix

Desbuis

Piccolo

et al. 2020

J. Phys. Chem. Lett.

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The tunability offered by alloying different elements is useful to design catalysts with greater activity, selectivity, and stability than single metals. By comparing the Pd(111) and PdZn(111) model catalysts for CO 2 hydrogenation to methanol, we show that intermetallic alloying is a possible strategy to control the reaction pathway from the tuning of adsorbate binding energies. In comparison to Pd, the strong electron-donor character of PdZn weakens the adsorption of carbon-bound species and strengthens the binding of oxygen-bound species. As a consequence, the first step of CO 2 hydrogenation more likely leads to the formate intermediate on PdZn, while the carboxyl intermediate is preferentially formed on Pd. This results in the opening of a pathway from carbon dioxide to methanol on PdZn similar to that previously proposed on Cu. These findings rationalize the superiority of PdZn over Pd for CO 2 conversion into methanol and suggest guidance for designing more efficient catalysts by promoting the proper reaction intermediates.

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mentioning

confidence: 86%

Tuning Adsorption Energies and Reaction Pathways by Alloying: PdZn versus Pd for CO₂ Hydrogenation to Methanol

Brix

Desbuis

Piccolo

et al. 2020

J. Phys. Chem. Lett.

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“…Various bimetallic materials including Pd–Cu, − Pd–Ga, , Pd–In, − Pd–Zn, Ni–Ga, − In–Rh, In–Cu, , In–Co, In–Ni, , and Ni–Cu , have also been examined for methanol production from CO 2 hydrogenation. Among these catalysts, some non-noble metal-based bimetallics were designed for efficient CO 2 hydrogenation to CH 3 OH at low pressure.…”

Section: Co2 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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“…Noble metals have been studied to improve the activity of indium-based catalysts. DFT and microkinetic studies have found that the pathway for methanol formation on Pd-In intermetallic surfaces is comparable to that over Cu surfaces (Wu and Yang 2019). Furthermore, it has been shown that methanol is a more favorable product than CO. Rui et al (2017) prepared a Pd/In 2 O 3 catalyst by mixing In 2 O 3 powder with a Pd/peptide composite.…”

Section: Indium-based Catalystsmentioning

confidence: 97%

CO2 hydrogenation to methanol: the structure–activity relationships of different catalyst systems

Stangeland

2020

Energ. Ecol. Environ.

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CO 2 hydrogenation to methanol is a promising environmental-friendly route for combatting CO 2 emissions. Methanol can be used to produce a variety of chemicals and is also an alternative fuel. The CO 2-tomethanol process is mostly studied over multi-component catalysts in which both metal and oxide phases are present. The difficulty in elucidating the influence of the different phases on the catalytic performance has led to intense debate about the nature of the active site. Consequently, the main stumbling blocks in developing rational design strategies are the complexity of the multi-component catalytic systems and challenges in elucidating the active sites. In this paper, we reviewed the most promising catalyst systems for the industrial CO 2-to-methanol processes. Firstly, the copper-based catalysts are discussed. The focus is on the debate regarding the promotional effect of zinc, as well as other metal oxides typically employed to enhance the performance of copper-based catalysts. Other catalytic systems are then covered, which are mainly based on palladium and indium. Alloying and metal-metal oxide interaction also play a significant role in the hydrogenation of CO 2 to methanol over these catalysts. The purpose of this work is to give insight into these complex catalytic systems that can be utilized for advanced catalyst synthesis for the industrial CO 2-to-methanol process.

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Intermetallic PdIn catalyst for CO₂ hydrogenation to methanol: mechanistic studies with a combined DFT and microkinetic modeling method

Abstract: Reaction pathways of methanol and carbon monoxide formation from CO2 hydrogenation over PdIn(110) and (211) with a combined density functional theory and microkinetic modeling approach.

Cited by 49 publications

References 77 publications

Tuning Adsorption Energies and Reaction Pathways by Alloying: PdZn versus Pd for CO₂ Hydrogenation to Methanol

Tuning Adsorption Energies and Reaction Pathways by Alloying: PdZn versus Pd for CO₂ Hydrogenation to Methanol

Novel Heterogeneous Catalysts for CO₂ Hydrogenation to Liquid Fuels

CO2 hydrogenation to methanol: the structure–activity relationships of different catalyst systems

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Intermetallic PdIn catalyst for CO2 hydrogenation to methanol: mechanistic studies with a combined DFT and microkinetic modeling method

Abstract: Reaction pathways of methanol and carbon monoxide formation from CO2 hydrogenation over PdIn(110) and (211) with a combined density functional theory and microkinetic modeling approach.

Cited by 49 publications

References 77 publications

Tuning Adsorption Energies and Reaction Pathways by Alloying: PdZn versus Pd for CO2 Hydrogenation to Methanol

Tuning Adsorption Energies and Reaction Pathways by Alloying: PdZn versus Pd for CO2 Hydrogenation to Methanol

Novel Heterogeneous Catalysts for CO2 Hydrogenation to Liquid Fuels

CO2 hydrogenation to methanol: the structure–activity relationships of different catalyst systems

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Product

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Intermetallic PdIn catalyst for CO₂ hydrogenation to methanol: mechanistic studies with a combined DFT and microkinetic modeling method

Tuning Adsorption Energies and Reaction Pathways by Alloying: PdZn versus Pd for CO₂ Hydrogenation to Methanol

Tuning Adsorption Energies and Reaction Pathways by Alloying: PdZn versus Pd for CO₂ Hydrogenation to Methanol

Novel Heterogeneous Catalysts for CO₂ Hydrogenation to Liquid Fuels