Mechanistic Insights into Catalytic Ethanol Steam Reforming Using Isotope‐Labeled Reactants

Crowley, Stephen; Castaldi, Marco J.

doi:10.1002/anie.201604388

Cited by 13 publications

(16 citation statements)

References 37 publications

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“…Dominant peaks of 13 C-C 2 H 4 (m/z = 30), 13 C-EtOH (m/z = 47), and 13 C-acetic acid (m/z = 62) were observed ( Supplementary Figs. 22-24) [45][46][47] . The evidence confirms that the evolved reduction products derive from the CO electrolysis over Cu-SA/Ti 3 C 2 T x .…”

Section: Synthesis and Characterization Of Cu-sa/ti 3 C 2 Tmentioning

confidence: 99%

Isolated copper single sites for high-performance electroreduction of carbon monoxide to multicarbon products

et al. 2021

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Electrochemical carbon monoxide reduction is a promising strategy for the production of value-added multicarbon compounds, albeit yielding diverse products with low selectivities and Faradaic efficiencies. Here, copper single atoms anchored to Ti3C2Tx MXene nanosheets are firstly demonstrated as effective and robust catalysts for electrochemical carbon monoxide reduction, achieving an ultrahigh selectivity of 98% for the formation of multicarbon products. Particularly, it exhibits a high Faradaic efficiency of 71% towards ethylene at −0.7 V versus the reversible hydrogen electrode, superior to the previously reported copper-based catalysts. Besides, it shows a stable activity during the 68-h electrolysis. Theoretical simulations reveal that atomically dispersed Cu–O3 sites favor the C–C coupling of carbon monoxide molecules to generate the key *CO-CHO species, and then induce the decreased free energy barrier of the potential-determining step, thus accounting for the high activity and selectivity of copper single atoms for carbon monoxide reduction.

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Section: Synthesis and Characterization Of Cu-sa/ti 3 C 2 Tmentioning

confidence: 99%

Isolated copper single sites for high-performance electroreduction of carbon monoxide to multicarbon products

et al. 2021

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“…The isotope labeling strategy such as the deuterated ethanol and deuterium water allowed an unprecedented level visualizing and tracking the dominant reaction pathways, which the reaction products changed dynamically as a function of reaction temperature. [59,61] Based on the experimental and theoretical analysis, a general reaction pathway of ESR on supported metal catalysts is presented in Scheme 1. [25,[38][39][40][41] At lower reaction temperature, the ethanol molecule first undergoes cleavage of OÀ H bond to form ethoxy species with lower energy barrier.…”

Section: Reaction Pathways Of Ethanol Steam Reformingmentioning

confidence: 99%

Recent Status in Catalyst Modification Strategies for Hydrogen Production from Ethanol Steam Reforming

2023

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Hydrogen as the most promising alternative energy vector to fossil stands out due to its highly energy density and zero pollution. Extending the hydrogen feedstock from hydrocarbons (e. g., methane) to biomass derived oxygen‐containing compounds (CH3OH, C2H5OH etc.) provides the opportunity for low environmental pollution as well as a promising sustainable energy economy. Recently, ethanol with less toxic and high calorific value than traditional fossil energy (coal, oil and natural gas) has garnered significant attention for ethanol steam reforming (ESR) to produce hydrogen, a key component in fuel cell cogeneration system. This paper reviews recent advances on the catalyst developing strategies including structural constitution control, oxide supports modification, surface topography control and bimetallic interactions, and further discusses the catalytic mechanisms, anti‐carbon deposition and sintering resistance strategies on the ethanol steam reforming (ESR) processes. Finally, the challenges and possible strategies for the development of high‐performance catalysts in terms of fundamental research have been discussed.

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“…The isotope labeling method is particularly effective in mechanistic research with multiple competing reaction processes due to its ability to track the reactants’ atomic partitionings into the products. For example, isotope-labeled reactants have been used to explore the mechanisms of catalytic ethanol steam reforming . By using both isotope-labeled ethanol [1- 13 C] and water [ 18 O], all non-H atoms can be distinguished from one another, thus allowing for atom origin differentiation.…”

Section: Advanced Technology For Exploring the Chemical Looping React...mentioning

confidence: 99%

Review on Migration and Transformation of Lattice Oxygen during Chemical Looping Conversion: Advances and Perspectives

Song

Lin

et al. 2023

Energy Fuels

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Chemical looping technology is one of the most promising approaches in the fields of fuel conversion, pollution removal, energy conservation, and carbon dioxide capture and utilization and has been extensively investigated for more than two decades. A majority of the chemical looping process is achieved through the migration and transformation of lattice oxygen. Thus, exploring the migration and transformation of lattice oxygen is critical to clarify chemical looping’s reaction rules to allow for further control of reaction selectivity and yield. Herein, recent advances in the exploration of lattice oxygen’s migration mechanism are systematically reviewed, with a focus on structure–activity relationships. The great roles that characterization techniques perform to address the challenges in exploring the migration mechanism of lattice oxygen activities are discussed first. We then outline the categories of oxygen carrier materials and the migration mechanism of lattice oxygen. Lastly, the most promising research directions that design high-performance oxygen carriers with well-regulated lattice oxygen activity through the redox reaction mechanism are overviewed. We infer that the research on the relationship between lattice oxygen activity and target products is challenging but essentialit is a direction worthy of our efforts in the future.

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Mechanistic Insights into Catalytic Ethanol Steam Reforming Using Isotope‐Labeled Reactants

Cited by 13 publications

References 37 publications

Isolated copper single sites for high-performance electroreduction of carbon monoxide to multicarbon products

Isolated copper single sites for high-performance electroreduction of carbon monoxide to multicarbon products

Recent Status in Catalyst Modification Strategies for Hydrogen Production from Ethanol Steam Reforming

Review on Migration and Transformation of Lattice Oxygen during Chemical Looping Conversion: Advances and Perspectives

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