Recycling Strategy for Bioaqueous Phase via Catalytic Wet Air Oxidation to Biobased Acetic Acid Solution

He, Shan; Bijl, Anton; Barana, Patryk Kamil; Lefferts, Leon; Kersten, Sascha R.A.; Brem, Gerrit

doi:10.1021/acssuschemeng.0c05946

Cited by 8 publications

(9 citation statements)

References 44 publications

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“…Wet Oxidation Followed by Extractive Distillation. An alternative use of the aqueous phase of bio-oil (identified herein as aqueous extract) is acetic acid production via wet oxidation as proposed by He et al 39 In their work, several conditions were tested using different reaction gases and catalysts. Pt/ZrO 2 showed the highest efficiency in converting the organic compounds into acetic acid.…”

Section: Started With the Liquid−liquid Extraction Of Pyrolysis Oil (B)mentioning

confidence: 99%

“…41 Both costs were corrected to the suitable capacity and adjusted to 2017 figures. The cost of the catalyst was estimated by using the costs of the materials required for their preparation as indicated in the Supporting Information provided by He et al 39 It is assumed that the catalyst is regenerated. Table 7 summarizes the material flow rates and costs associated with the wet oxidation unit.…”

Section: Started With the Liquid−liquid Extraction Of Pyrolysis Oil (B)mentioning

confidence: 99%

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Synthesis and Techno-Economic Analysis of Pyrolysis-Oil-Based Biorefineries Using P-Graph

et al. 2021

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The production of renewable fuels and chemicals is a critical component of global strategies to reduce greenhouse gas emissions. In this regard, pyrolysis oil obtained from biomass comprises hundreds of chemical compounds, thus rendering it a good precursor for manufacturing a variety of fuel products of commercial interest. Despite the large number of contributions describing the products’ extraction, upgrading, and potential refining schemes, no bio-oil refinery is currently in operation. The main challenge in building a bio-oil refinery lies in the lack of an economically viable process configuration. Systematic studies comparing alternative refinery concepts, or configurations, are needed to identify the most promising configuration. To the best of our knowledge, this study is the first to use process graph (P-graph) methodology for the synthesis of pyrolysis oil refineries. In particular, this work shows the effectiveness of P-graph methodology in simultaneously calculating the profitability of various biorefinery designs by using data reported in the literature and providing information on how the introduction of new technologies to the database will impact the formation of profitable biorefinery concepts. Our work demonstrates a methodology for the addition of new unit operations to the database generated from the literature. The addition of a centrifuge for water extraction and a wet oxidation system for acetic acid production resulted in the generation of 330 biorefinery configurations, seven of which have a profitability ranging from $1,650 to $23,666/h (USD) with acetic acid and levoglucosan as the main products, respectively. This demonstrates that P-graph methodology is useful for discovering optimum techno-economic scenarios that may otherwise be overlooked.

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Section: Started With the Liquid−liquid Extraction Of Pyrolysis Oil (B)mentioning

confidence: 99%

Section: Started With the Liquid−liquid Extraction Of Pyrolysis Oil (B)mentioning

confidence: 99%

Synthesis and Techno-Economic Analysis of Pyrolysis-Oil-Based Biorefineries Using P-Graph

et al. 2021

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“…Removal of phenols is by no means a new effort, and oxidation reaction studies specifically targeting phenol-contaminated water have been researched and published for several decades [10,12,18,25,34,43]. However, the bioenergy industry has stimulated a renewed effort in the treatment of aqueous effluents with highly dilute phenol concentrations [20,54]. Catalytic wet oxidation (CWO), a type of advanced oxidative process (AOP), has shown promise in the treatment of industrial aqueous wastes rich in organic compounds [6,21,53].…”

Section: Introductionmentioning

confidence: 99%

Nitrogen-doped char as a catalyst for wet oxidation of phenol-contaminated water

Tews

Garcia²,

Ayiania

et al. 2021

Biomass Conv. Bioref.

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Catalytic wet oxidation (CWO) of aqueous effluents rich in organic compounds is a very promising technology for the treatment of liquid wastes from biomass conversion processes. CWO reactions occur through the formation of free radical species, produced in the presence of an oxidant, which act on organic contaminates in the effluent. Although the reaction is well known, there exists a lack of affordable catalysts to conduct this process at the lower temperatures and pressures in novel bioenergy processes. This study assessed the catalytic effect of nitrogen-doped chars as such an option. Phenol in aqueous solution was used as a model waste effluent. Treatment was conducted at moderate temperatures (190 to 260°C), oxygen partial pressure of 1 MPa, and reaction times of 15, 30, and 45 min in stainless steel and glass-lined tube reactors. High pressure liquid chromatography (HPLC) analyses of the products quantified phenol and by-product concentrations used in the calculation of reaction activation energy. The char catalyst was studied by X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), and scanning electron microscopy (SEM) in order to gain insight into its structure and surface composition. The results indicate that nitrogen-doped char catalysts accelerate the oxidation of phenol by decreasing its reaction activation energy from 82.2 kJ/mol (non-catalyzed) to 40.4 kJ/mol (catalyzed). An analysis from first principles using density functional theory (DFT) was conducted to ascertain which N functional group has the most significant impact on free radical formation in the presence of oxygen. Among all the N functional groups studied, the dipyridinic functional groups showed the most promising characteristics to facilitate the formation of hydroxyl free radicals.

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“…The environmental impact of aqueous effluents of biomass thermochemical processing with large quantities of organics and the need to treat these effluents have been documented in the literature . Current research and development of novel biorefinery concepts focuses primarily on the production of fuels, value added coproducts, heat, and power from lignocellulosic materials with limited attention on the fate and treatment of aqueous waste effluents rich in organics. − Contaminated aqueous effluents can be obtained by both biochemical and thermochemical conversion technologies; ,,,− however, in this review, we will focus only on the effluents from thermochemical conversion. Specifically, hydrothermal liquefaction (HTL) of woody biomass to form biocrude and hydro-deoxygenation (HDO) of HTL biocrude and pyrolysis bio-oils will be addressed.…”

Section: Introductionmentioning

confidence: 99%

“…These molecules are collected in the form of bio-oils, chars, or as part of an aqueous phase. In the case of pyrolysis and hydrothermal liquefaction, the end products of the thermochemical step (liquid or solid) need further processing to reduce the oxygen content and make them infrastructure compatible . Removal of oxygen is achieved through hydro-deoxygenation and subsequent production of a separate aqueous phase.…”

Section: Introductionmentioning

confidence: 99%

Advanced Oxidative Techniques for the Treatment of Aqueous Liquid Effluents from Biomass Thermochemical Conversion Processes: A Review

Tews

Garcı̀a-Pèrez

2021

Energy Fuels

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This review explores advanced oxidative techniques of wet oxidation (WO) and catalytic wet oxidation (CWO) for treatment of primary aqueous effluents from hydrothermal liquefaction and pyrolysis (with subsequent upgrading) of biomass. Hydrothermal liquefaction and pyrolysis bio-oil upgrading processes produce an aqueous phase rich in organic carbon. However, the characterization of the compounds in such streams is limited and studies on their treatment are even more rare. Few studies have identified major compound families as phenols and smaller carboxylic acids. Often these compounds are overly toxic to existing wastewater treatment operations. Here, advanced oxidative techniques are reviewed with specific focus on how WO and CWO could affect some of these constituents such as phenols and carboxylic acids. Fundamental aspects of such reaction systems are reviewed including the most plausible oxidants (O 2 , O 3 , H 2 O 2 ), the physical and chemical stages of oxidant interactions with the contaminants themselves, and their formation under non-catalytic and catalytic process conditions. Differing types of catalysts (homogeneous, heterogeneous, active carbons) and their novel formation such as carbon nanotubes are considered. Central to the oxidation mechanism, regardless of oxidant or presence of catalyst, is the formation of oxygen-reactive species such as hydroxyl free radicals. While WO processes do generate such oxidative free radicals, it is often under stringent operating conditions. Through the addition of metal catalysts, the oxidative process is successful at removing contaminants at significantly reduced temperatures and pressure. Continuous reactors have shown the best success of removal at both the bench and pilot plant scale. However, many are plagued by oxidant transport deficiencies. To improve transport, novel reactor schemes are emerging for the next generation of oxidative continuous systems. Advanced wet oxidation processes are well suited for the treatment of thermochemical aqueous phase products such that the effluent stream is suitable for processing in wastewater treatment plants or subsequent bioenergy plant water recycle.

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Recycling Strategy for Bioaqueous Phase via Catalytic Wet Air Oxidation to Biobased Acetic Acid Solution

Cited by 8 publications

References 44 publications

Synthesis and Techno-Economic Analysis of Pyrolysis-Oil-Based Biorefineries Using P-Graph

Synthesis and Techno-Economic Analysis of Pyrolysis-Oil-Based Biorefineries Using P-Graph

Nitrogen-doped char as a catalyst for wet oxidation of phenol-contaminated water

Advanced Oxidative Techniques for the Treatment of Aqueous Liquid Effluents from Biomass Thermochemical Conversion Processes: A Review

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