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From Small Molecules to High-Value Chemicals: Theory and Practice

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A special issue of Processes (ISSN 2227-9717). This special issue belongs to the section "Chemical Processes and Systems".

Deadline for manuscript submissions: closed (15 October 2022) | Viewed by 10004

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Special Issue Editors

Dr. Yanbo Pan

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Guest Editor

Brewer Science Inc., Rolla, MO 65401, USA
Interests: heterogeneous catalysis; CO₂ utilization; C₁ chemistry; process integration; water desalination; process modeling; density functional theory; electrochemical CO₂ reduction
Special Issues, Collections and Topics in MDPI journals

Prof. Dr. Zhenmeng Peng

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Guest Editor

Department of Chemical, Biomolecular, and Corrosion Engineering, University of Akron, Akron, OH 44320, USA
Interests: electrocatalysis and catalysis; chemical and electrochemical reaction engineering; sustainable and renewable energy; C1 chemical conversion; advanced materials synthesis and applications
Special Issues, Collections and Topics in MDPI journals

Prof. Dr. Chunhai Yi

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Guest Editor

Department of Chemical Engineering, Xi'an Jiaotong University, Xi'an 710049, China
Interests: membrane separation technology; water treatment technology; chemical reaction engineering; polymer chemistry; polymeric membrane

Dr. Xiaochen Shen

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Guest Editor

Department of Chemical Engineering, Case Western Reserve University, Cleveland, OH 44106, USA
Interests: heterogenous catalysis; electrocatalysis; material discovery; fuel/flow cells

Special Issue Information

Dear Colleagues,

Converting small molecules, including CO, CO₂, CH₄, N₂, NO_x, etc., into high-value chemicals and energy carriers has been one long-lasting research topic for its significant practical meanings to human society. In recent years, owing to emerging global concerns such as global warming, the environmental pollution, and the energy crisis, the demand to realize a “green economy” is increasing rapidly. Thus, migrating such a conventional industry toward a more efficient and environmentally benign industry is urgent. Promising progress has been made over the past few years in reaching this target, such as developing electrochemical-based reaction systems, discovering novel structured high-performance catalysts, and establishing smart process integration and scaleup systems.

However, many challenges still exist in finding the efficient green-energy-driven reaction system and converting lab progress to a practical integrated industrial system. Herein, this Special Issue aims to cover recent progress and research efforts in the related field of converting small molecules into high-value chemicals, including innovative process development and integration, novel materials discovery and evaluation, as well as reaction mass/heat transfer studies. Topics include but are not limited to:

CO₂ hydrogenation to hydrocarbons;
Electrochemical CO₂ reduction to liquid fuels;
Selective catalytic reduction (SCR) of NO_x;
(Electro)chemical ammonia synthesis from N₂;
CH₄ partial oxidation to value-added chemicals;
CO preferential oxidation in H₂-rich atmosphere (CO PROX);
Modeling and simulation of the abovementioned processes.

All experimental and theoretical works falling into the scope of this Special Issue, including original research papers, short communications, review articles, and perspective articles, are invited for submission.

Dr. Yanbo Pan
Prof. Dr. Zhenmeng Peng
Prof. Dr. Chunhai Yi
Dr. Xiaochen Shen
Guest Editors

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Processes is an international peer-reviewed open access monthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2400 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

CO₂ hydrogenation
electrochemical CO₂ reduction
ammonia synthesis
NO_x transformation
electrochemical N₂ reduction
CH₄ conversion
C₁ chemistry
nitrogen economy

Published Papers (5 papers)

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Research

12 pages, 2373 KiB

Open AccessFeature PaperArticle

Optimization of Phycobiliprotein Solubilization from a Thermotolerant Oscillatoria sp.

by Andrés F. Barajas-Solano

Processes 2022, 10(5), 836; https://doi.org/10.3390/pr10050836 - 24 Apr 2022

Cited by 3 | Viewed by 1440

Abstract

The present study evaluated the effect of multiple variables (drying time, drying temperature, biomass/solvent ratio, glass beads/biomass ratio, extraction time, and extraction speed) in the solubilization of three different phycobiliproteins (C-PC, APC, and PE) from a thermotolerant Oscillatoria sp. The strain was grown in BG11 media (28 °C, light: dark cycle of 12:12 h at 100 µmol·m⁻²·s⁻¹, 20 days) and the experiments were conducted according to a two-level randomized factorial design with six center points (38 runs). Results show that biomass/solvent ratio, glass beads/biomass ratio, and extraction time, are the most significant variables in the extraction of all three proteins, whereas the glass beads/biomass ratio and extraction time significantly affect their purity. The optimized conditions allow a statistical increase in the concentration of C-PC, APC, and PE extracted from the biomass; however, the purity was lower in comparison with the expected value. The latter occurs due to a larger biomass/solvent ratio and longer extraction times, which enhanced the solubility of other hydrophilic metabolites (proteins and carbohydrates, etc.). Full article

(This article belongs to the Special Issue From Small Molecules to High-Value Chemicals: Theory and Practice)

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21 pages, 5237 KiB

Open AccessFeature PaperEditor’s ChoiceArticle

Catalytic Properties of Free-Base Porphyrin Modified Graphite Electrodes for Electrochemical Water Splitting in Alkaline Medium

by Bogdan-Ovidiu Taranu and Eugenia Fagadar-Cosma

Processes 2022, 10(3), 611; https://doi.org/10.3390/pr10030611 - 21 Mar 2022

Cited by 8 | Viewed by 2279

Abstract

Hydrogen generation via electrochemical water splitting is considered an eco-friendly pathway for obtaining this desired alternative energy source, and it has triggered an intensive search for low cost and efficient catalysts. Within this context, four free-base porphyrins were studied as heterogeneous catalysts for the oxygen and hydrogen evolution reactions (OER and HER) in alkaline aqueous solutions. TEM and STEM analyses of samples obtained by drop-casting the porphyrins from different organic solvents on TEM grids revealed a rich variety of aggregates due to the self-assembling property of the porphyrin molecules. Modified electrodes were manufactured by applying the four tetrapyrrolic macrocycles from various solvents on the surface of graphite supports, in one or more layers. Experiments performed in 0.1 M and 1 M KOH electrolyte solutions allowed the identification of the most electrocatalytically active electrodes for the OER and HER, respectively. In the first case, the electrode was manufactured by applying three layers of 5-(4-pyridyl)-10,15,20-tris(4-phenoxyphenyl)porphyrin on the graphite substrate from N,N-dimethylformamide solution was identified as overall catalytically superior. In the second case, the electrode obtained by applying one layer of 5,10,15,20-tetrakis(4-allyloxyphenyl)-porphyrin from benzonitrile solution displayed an HER overpotential value of 500 mV at i = −10 mA/cm² and a Tafel slope of 190 mV/dec. Full article

(This article belongs to the Special Issue From Small Molecules to High-Value Chemicals: Theory and Practice)

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Graphical abstract

20 pages, 9355 KiB

Open AccessFeature PaperArticle

A Comparison of Uric Acid Optical Detection Using as Sensitive Materials an Amino-Substituted Porphyrin and Its Nanomaterials with CuNPs, PtNPs and Pt@CuNPs

by Camelia Epuran, Ion Fratilescu, Diana Anghel, Mihaela Birdeanu, Corina Orha and Eugenia Fagadar-Cosma

Processes 2021, 9(11), 2072; https://doi.org/10.3390/pr9112072 - 19 Nov 2021

Cited by 5 | Viewed by 2016

Abstract

Hybrid nanomaterials consisting in 5,10,15,20-tetrakis(4-amino-phenyl)-porphyrin (TAmPP) and copper nanoparticles (CuNPs), platinum nanoparticles (PtNPs), or both types (Pt@CuNPs) were obtained and tested for their capacity to optically detect uric acid from solutions. The introduction of diverse metal nanoparticles into the hybrid material proved their capacity to improve the detection range. The detection was monitored by using UV-Vis spectrophotometry, and differences between morphology of the materials were performed using atomic force microscopy (AFM). The hybrid material formed between porphyrin and PtNPs hasthe best and most stable response for uric acid detection in the range of 6.1958 × 10⁻⁶–1.5763 × 10⁻⁵ M, even in the presence of very high concentrations of the interference species present in human environment. Full article

(This article belongs to the Special Issue From Small Molecules to High-Value Chemicals: Theory and Practice)

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13 pages, 40509 KiB

Open AccessArticle

Structured Thin Films Based on Synergistic Effects of MnTa₂O₆ Oxide and bis-Carboxy-phenyl-substituted Porphyrins, Capable to Inhibit Steel Corrosion

by Mihaela Birdeanu, Camelia Epuran, Ion Fratilescu and Eugenia Fagadar-Cosma

Processes 2021, 9(11), 1890; https://doi.org/10.3390/pr9111890 - 22 Oct 2021

Cited by 7 | Viewed by 1504

Abstract

Covering steel surfaces with suitable materials with the capacity to protect against corrosion represents a challenge for both research and industry, as steel, due to its paramount utility, is the most recycled material. This study presents the realization of new sandwich type materials based on 5,10-(4-carboxy-phenyl)-15,20-(4-phenoxy-phenyl)-porphyrin or 5,15-(4-carboxy-phenyl)-10,20-diphenylporphyrin and MnTa₂O₆ designed to improve corrosion inhibition of steel in aggressive media. The thin films, designed as single- or sandwich-type structures were obtained on carbon steel through the drop-casting technique. Morphological investigations of thin films were carried out by field emission-scanning electron microscopy (SEM) and atomic force microscopy (AFM). The inhibition of a steel corrosion process was evaluated in an aggressive environment of 0.1 M HCl by performing electrochemical investigations such as open circuit potential (OCP) and the potentiodynamic polarization technique. The influence of variations in the cathodic Tafel slopes β_c and anodic Tafel slopes β_a over the corrosion rates was discussed. The best corrosion inhibition efficiency of 91.76% was realized by the steel electrode covered with sandwich-type layers of 5,15-(4-carboxy-phenyl)-10,20-diphenylporphyrin on the bottom layer and MnTa₂O₆ on the top. The effect of location of the COOH groups in the cis or trans position on the tetrapyrrolic ring was also discussed to understand the corrosion inhibition mechanism. Full article

(This article belongs to the Special Issue From Small Molecules to High-Value Chemicals: Theory and Practice)

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8 pages, 2493 KiB

Open AccessFeature PaperCommunication

Synthesis of a Benzothiadiazole-Based D−A Molecule with Aggregation-Induced Emission and Controlled Assembly Properties

by Songhua Chen, Yongqi Liu, Meiyun He and Jianhua Huang

Processes 2021, 9(7), 1094; https://doi.org/10.3390/pr9071094 - 23 Jun 2021

Viewed by 1717

Abstract

An electron-donating−accepting (D−A) molecule, namely, 4-(1-(4-(9H-carbazol-9-yl)phenyl)-1H-1,2,3-triazol-4-yl)benzo[c][1,2,5]thiadiazole (BT-SCC) containing carbazole as the donor moiety and benzothiadiazole as the acceptor moiety is prepared. Single-crystal X-ray structure analysis elucidated the multiple intermolecular interactions, such as hydrogen bonds, CH…π, and π…π interplays. Interestingly, the aggregation-induced emission phenomenon is observed for BT-SCC featured with enhanced fluorescent quantum yield from diluted solution of CH₂Cl₂ (Φ = ca. 0.1) to CH₂Cl₂/hexane mixed solutions or solid states (Φ = ca. 0.8). Finally, aggregates of BT-SCC are obtained through precipitating from hot and saturated solutions or solvent-vapor methods and the aggregating morphologies could be easily controlled through different preparation methods. Fabulous cube-like micro-crystals and nanospherical structures are obtained, which is established by the synergistic effects of the multiple non-covalent interactions, endowing potential utility in the field of optoelectronic devices. Full article

(This article belongs to the Special Issue From Small Molecules to High-Value Chemicals: Theory and Practice)

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