Hydrogen Production by Ethanol Steam Reforming (ESR) over CeO2 Supported Transition Metal (Fe, Co, Ni, Cu) Catalysts: Insight into the Structure-Activity Relationship

Konsolakis, Michalis; Ioakimidis, Zisis; Kraia, Tzouliana; Marnellos, George

doi:10.3390/catal6030039

Cited by 76 publications

(46 citation statements)

References 95 publications

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“…The superior activity of CeO 2 -based support can be linked to the good metals particles dispersion and the prevention of sintering phenomena; moreover, their capability to add and remove oxygen in a reversible manner facilitates carbon gasification [26]. Mobile oxygen of ceria can also activate water, with regard to the formation of hydroxyl groups, resulting in higher ESR efficiency [27]. In particular, ceria was shown to accelerate the reaction of steam and absorbed species at the metal-support interface, giving place to -O and -HO species, which are transferred to the surface carbon, thus promoting coke conversion to gaseous products (CO, H 2 , and CO 2 ) [28,29].…”

Section: Introductionmentioning

confidence: 99%

Influence of Catalytic Formulation and Operative Conditions on Coke Deposition over CeO2-SiO2 Based Catalysts for Ethanol Reforming

et al. 2017

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Abstract:In this work, a series of CeO 2 -SiO 2 (30 wt % of ceria)-based catalysts was prepared by the wetness impregnation method and tested for ESR (ethanol steam reforming) at 450-500 • C, atmospheric pressure and a water/ethanol ratio increasing from 4 to 6 (the ethanol concentration being fixed to 10 vol %); after every test, coke gasification measurements were performed at the same water partial pressure, and the temperature of the test and the gasified carbon was measured from the areas under the CO and CO 2 profiles. Finally, oxidation measurements under a 5% O 2 /N 2 stream made it possible to calculate the total carbon deposited. In an attempt to improve the coke resistance of a Pt-Ni/CeO 2 -SiO 2 catalyst, the effect of support basification by alkali addition (K and Cs), as well as Pt substitution by Rh was investigated. The novel catalysts, especially those containing Rh, displayed a lowering in the carbon formation rate; however, a faster reduction of ethanol conversion with time-on-stream and lessened hydrogen selectivities were recorded. In addition, no significant gain in terms of coke gasification rates was observed. The most active catalyst (Pt-Ni/CeO 2 -SiO 2 ) was also tested under different operative conditions, in order to study the effect of temperature and water/ethanol ratio on carbon formation and gasification. The increase in the water content resulted in an enhanced reactor-plugging time due to reduced carbonaceous deposits formation; however, no effect of steam concentration on the carbon gasification rate were recorded. On the other hand, the increase in temperature from 450-500 • C lowered the coke selectivity by almost one order of magnitude improving, at the same time, the contribution of the gasification reactions.

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Section: Introductionmentioning

confidence: 99%

Influence of Catalytic Formulation and Operative Conditions on Coke Deposition over CeO2-SiO2 Based Catalysts for Ethanol Reforming

et al. 2017

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“…SR is a strong endothermic process and requires an external heat sources [1,6], while auto-thermal reforming (ATR) with endothermic steaming reforming (SR) and exothermic partial oxidation reaction …”

Section: Introductionmentioning

confidence: 99%

Dolomite-Derived Ni-Based Catalysts with Fe Modification for Hydrogen Production via Auto-Thermal Reforming of Acetic Acid

et al. 2016

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Bio-oil can be obtained via fast pyrolysis of biomass, and typically contains acetic acid (~30 mass %). The acetic acid has often been tested as a model compound for hydrogen production via reforming bio-oil, in which catalysts are a key factor for stable hydrogen production. However, deactivation of catalysts by coking and oxidation hinders the application of the reforming process. Dolomite-derived Ni-based catalysts with Fe additive, MgNi 0.2 Ca 0.8´x Fe x O 2˘δ (x = 0-0.8), were successfully synthesized by the hydrothermal synthesis method, and then tested in auto-thermal reforming (ATR) of acetic acid (AC). The MgNi 0.2 Ca 0.5 Fe 0.3 O 2˘δ catalyst performed a stable reactivity in ATR: the conversion of AC reached 100%, and the H 2 yield remained stable around 2.6 mol-H 2 /mol-AC. The catalysts were characterized by X-ray diffraction (XRD), N 2 physisorption, X-ray photoelectron spectra (XPS), H 2 -temperature-programmed reduction (TPR), inductively coupled plasma-atomic emission spectroscopy (ICP-AES) and Thermogravimetry (TG); the results show that a periclase-like solid solution of Mg(Ni,Fe)O and lime were formed via the precursors of dolomite and hydrotalcite, and then transformed into Fe-rich Ni-Fe alloy with basic support of MgO-CaO after reduction. The stable Ni 0 spices with basic support can explain the stability and resistance to coking during ATR of AC.

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“…Scarabello et al [46] reported that the O-vacancy in Rh/Ce-ZrO 2 promotes the oxidation of CO to CO 2 by the reaction in Equation (15) and the dissociation of water, increasing H 2 production (Equation (16) …”

Section: Effect Of the Rh-pt Ratio On The Catalytic Performancementioning

confidence: 99%

“…However, the use of ethanol/gasoline mixtures in Base metals, such as Ni [15], Co [16], and Fe [17], and noble metals, such as Pd [18], Rh [18,19], Pt [7,20], and Ir [21], supported on metals oxides to catalyze SRE have been widely studied. The nature of the catalyst and operational conditions directly affect its performance in SRE [15,22]. Ni is a widely studied catalyst due to its low cost [10].…”

Section: Introductionmentioning

confidence: 99%

Response Surface Methodology and Aspen Plus Integration for the Simulation of the Catalytic Steam Reforming of Ethanol

2017

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Abstract:The steam reforming of ethanol (SRE) on a bimetallic RhPt/CeO 2 catalyst was evaluated by the integration of Response Surface Methodology (RSM) and Aspen Plus (version 9.0, Aspen Tech, Burlington, MA, USA, 2016). First, the effect of the Rh-Pt weight ratio (1:0, 3:1, 1:1, 1:3, and 0:1) on the performance of SRE on RhPt/CeO 2 was assessed between 400 to 700 • C with a stoichiometric steam/ethanol molar ratio of 3. RSM enabled modeling of the system and identification of a maximum of 4.2 mol H 2 /mol EtOH (700 • C) with the Rh 0.4 Pt 0.4 /CeO 2 catalyst. The mathematical models were integrated into Aspen Plus through Excel in order to simulate a process involving SRE, H 2 purification, and electricity production in a fuel cell (FC). An energy sensitivity analysis of the process was performed in Aspen Plus, and the information obtained was used to generate new response surfaces. The response surfaces demonstrated that an increase in H 2 production requires more energy consumption in the steam reforming of ethanol. However, increasing H 2 production rebounds in more energy production in the fuel cell, which increases the overall efficiency of the system. The minimum H 2 yield needed to make the system energetically sustainable was identified as 1.2 mol H 2 /mol EtOH. According to the results of the integration of RSM models into Aspen Plus, the system using Rh 0.4 Pt 0.4 /CeO 2 can produce a maximum net energy of 742 kJ/mol H 2 , of which 40% could be converted into electricity in the FC (297 kJ/mol H 2 produced). The remaining energy can be recovered as heat.

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Hydrogen Production by Ethanol Steam Reforming (ESR) over CeO2 Supported Transition Metal (Fe, Co, Ni, Cu) Catalysts: Insight into the Structure-Activity Relationship

Cited by 76 publications

References 95 publications

Influence of Catalytic Formulation and Operative Conditions on Coke Deposition over CeO2-SiO2 Based Catalysts for Ethanol Reforming

Influence of Catalytic Formulation and Operative Conditions on Coke Deposition over CeO2-SiO2 Based Catalysts for Ethanol Reforming

Dolomite-Derived Ni-Based Catalysts with Fe Modification for Hydrogen Production via Auto-Thermal Reforming of Acetic Acid

Response Surface Methodology and Aspen Plus Integration for the Simulation of the Catalytic Steam Reforming of Ethanol

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