Article
Chemistry, Physical
Jiachun Chai, Robert Pestman, Wei Chen, Noortje Donkervoet, A. Iulian Dugulan, Zhuowu Men, Peng Wang, Emiel J. M. Hensen
Summary: The kinetics of the transformation of metallic Fe to the active Fe carbide phase at the start of the Fischer-Tropsch (FT) reaction were studied. The diffusion rates of C atoms going in or out of the lattice were determined using C-13-labeled synthesis gas. It was found that in the initial stages, C diffused rapidly into the lattice, and the FT reaction started during this period. When reaching steady state, the diffusion rates of C in and out of the lattice converged, and the FT reaction continued via two parallel reaction mechanisms. The outer layers of the Fe carbide were involved in hydrocarbon formation via a slow reaction, contributing to around 10% of the total activity.
Article
Chemistry, Multidisciplinary
Maria Batuecas, Richard Y. Kong, Andrew J. P. White, Mark R. Crimmin
Summary: Selective reactions that combine H-2, CO, and organic electrophiles to form hydrogenated C-3 and C-4 carbon chains have been reported. These reactions involve CO homologation mediated by [W(CO)(6)] and an aluminum(I) reductant, followed by functionalization and hydrogenation of the chain ends. Kinetics and DFT calculations provide insight into the hydrogenation of a metal-locarbene intermediate, revealing the controlled production of well-defined products with desired chain length and functionality.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Applied
Amaury Indekeu, Esther Bailon-Garcia, Auguste Fernandes, Ruben Baltazar, Ana Maria Ferraria, Ana Maria B. do Rego, M. Filipa Ribeiro
Summary: New alternative routes to traditional Fischer-Tropsch Synthesis (FTS) must be established to achieve a more efficient process in terms of energy and sustainability. Solar photocatalytic-assisted FTS is a promising new approach for obtaining fuels from renewable resources. Metal-doped TiO2 catalysts show enhanced photocatalytic activity under solar radiation, lowering the band gap and increasing the methanation activity, as well as promoting the production of ethanol.
Article
Engineering, Environmental
Xin Li, Yao Chen, Shize Liu, Ning Zhao, Xiangning Jiang, Meng Su, Zhenhua Li
Summary: This study investigated the impact of the combination of Co-based catalysts and HZSM-5 on product distribution in Fischer-Tropsch synthesis. Results showed that proximity and reaction temperature significantly affected the selectivity, providing guidance for the rational design of bifunctional catalysts.
CHEMICAL ENGINEERING JOURNAL
(2021)
Review
Chemistry, Multidisciplinary
Yanping Chen, Jiatong Wei, Melis S. Duyar, Vitaly V. Ordomsky, Andrei Y. Khodakov, Jian Liu
Summary: This review summarizes the recent advances in the preparation of carbon-based catalysts for Fischer-Tropsch synthesis, highlighting the importance of support and metal properties, activity, product selectivity, and their interactions. Current challenges and future trends in the commercial utilization of carbon-based catalysts for FTS are also discussed.
CHEMICAL SOCIETY REVIEWS
(2021)
Article
Chemistry, Physical
Madita Einemann, Simon Haida, Nico Fischer, Nattawut Osakoo, Jatuporn Wittayakun, Frank Roessner
Summary: The role of cobalt chloride hexahydrate as a precursor of cobalt bulk catalysts was investigated for the Fischer-Tropsch reaction. Different oxygen-containing cobalt compounds were detected through in situ DRIFTS, in situ XANES, in situ XRD, and inverse TPR techniques. The reaction network of cobalt chloride transformation was discussed, taking into account the back mixing in different geometries of measuring cells. The choice of catalyst activation procedure is important for the formation of cobalt oxide and subsequent activity in the Fischer-Tropsch reaction.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Physical
Deizi Peron, Alan J. Barrios, Alan Taschin, Iulian Dugulan, Carlo Marini, Giulio Gorni, Simona Moldovan, Siddardha Koneti, Robert Wojcieszak, Joris W. Thybaut, Mirella Virginie, Andrei Y. Khodakov
Summary: The study found that antimony and tin have strong promoting effects on silica supported iron Fischer-Tropsch catalysts, significantly increasing the reaction rate and improving catalyst stability. The addition of these elements through impregnation can increase the intrinsic activity of iron surface sites by 7-10 times without affecting iron dispersion.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2021)
Article
Chemistry, Physical
Fangxu Lu, Xin Chen, Zhigang Lei, Lixiong Wen, Yi Zhang
Summary: Research on iron-based catalysts doped with SiO2 or Al2O3 has shown that adjusting the formation of iron carbides can enhance the activity of Fischer-Tropsch synthesis reactions. Characterization results using techniques such as XPS and CO-DRIFTS revealed that SiO2 or Al2O3 affects the electronic state of iron atoms and promotes the formation of Fe-Si or Fe-Al interactions on the surface of iron powder, which in turn plays a key role in the formation of the active phase ε-Fe2C. The content of ε-Fe2C is found to be more beneficial to activity compared to the traditionally recognized active phase χ-Fe5C2 in Fischer-Tropsch synthesis reactions.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2021)
Article
Engineering, Chemical
Imaad Davies, Klaus P. Moller
Summary: The kinetics of n-paraffin and 1-olefin formation in the Fischer-Tropsch reaction system are equilibrium-limited, allowing for an effective description of product distribution and observed reaction behavior trends. The model preserves the polymerization character of the reaction and successfully describes the dominant trends in product distribution as a function of CO conversion, temperature, and pressure.
CHEMICAL ENGINEERING SCIENCE
(2021)
Article
Chemistry, Physical
Yanping Chen, Lixuan Ma, Riguang Zhang, Runping Ye, Wei Liu, Jiatong Wei, Vitaly V. Ordomsky, Jian Liu
Summary: This study reports the design of a low-cost and scalable carbon-supported iron catalyst (K-Fe/NC) with tunable alcohol selectivity in Fischer-Tropsch synthesis. The catalyst exhibits a core-shell structure and facilitates the investigation of iron structural evolution. The dissociation and association of CO are thoroughly verified through theoretical calculations and experimental reactions. The synergistic effect between chi-Fe5C2/epsilon-Fe2C and Fe3O4 dual active sites is proposed as the mechanism for alcohol formation.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Chemistry, Physical
Faen Song, Xiaojing Yong, Xuemei Wu, Wei Zhang, Qingxiang Ma, Tiejian Zhao, Minghui Tan, Zhongshan Guo, Heng Zhao, Guohui Yang, Noritatsu Tsubaki, Yisheng Tan
Summary: The capsule catalyst FeMn@HZSM-5 was shown to effectively reduce CO2 formation and increase olefins selectivity in Fischer-Tropsch to olefins (FTO) reaction, outperforming other physically mixing catalysts. The HZSM-5 shell played a key role in affecting H2O diffusion and suppressing the water-gas shift reaction.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Engineering, Chemical
Umesh Pandey, Anders Runningen, Ljubisa Gavrilovic, Erik A. Jorgensen, Koteswara R. Putta, Kumar R. Rout, Erling Rytter, Edd A. Blekkan, Magne Hillestad
Summary: The detailed kinetic model developed in this study accurately describes the consumption of key components and product distribution in the Fischer-Tropsch synthesis over a commercial catalyst, incorporating a water-assisted CO dissociation mechanism and a novel approach to product distribution modeling. The model parameters are optimized against experimental data under various process conditions, showing a good fit with literature reported values. The model can accurately capture the effects of water and other process variables on the kinetics and product distribution, crucial for the design and optimization of Fischer-Tropsch reactors.
Article
Energy & Fuels
Dalia Liuzzi, Francisco J. Perez-Alonso, Sergio Rojas
Summary: Ru-Co/Al2O3 and Ru-Fe/Al2O3 catalysts prepared by reduction-deposition method exhibit high activity in Fischer-Tropsch Synthesis, showing different conversion rates and product selectivity. The interaction between Ru and Co in Ru-Co/Al2O3 enhances the activity, while Ru-Fe/Al2O3 displays superior initial performance but declines over time, with less enriched products compared to Ru/Al2O3.
Article
Chemistry, Physical
Mikhail Shipilin, David Degerman, Patrick Lomker, Christopher M. Goodwin, Gabriel L. S. Rodrigues, Michael Wagsta, Joergen Gladh, Hsin-Yi Wang, Andreas Stierle, Christoph Schlueter, Lars G. M. Pettersson, Anders Nilsson, Peter Amann
Summary: In this study, the effect of pressure, temperature, time, and gas feed composition on the growth dynamics of iron-carbon phases was investigated. The details of iron surface carburization and product formation under realistic conditions were revealed using a combination of experimental and theoretical approaches. This research provides important insights into the relationship between the catalyst's surface and the reaction.
Article
Chemistry, Physical
Mikhail Shipilin, David Degerman, Patrick Loemker, Christopher M. Goodwin, Gabriel L. S. Rodrigues, Michael Wagstaffe, Jorgen Gladh, Hsin-Yi Wang, Andreas Stierle, Christoph Schlueter, Lars G. M. Pettersson, Anders Nilsson, Peter Amann
Summary: This study investigates the detailed mechanism of carbide formation on iron-based catalysts and the effect of reaction conditions on the catalyst surface state through experiments and theoretical calculations.
Article
Engineering, Chemical
Chike George Okoye-Chine, Roy Forbes, Joshua Gorimbo, Mahluli Moyo, Xinying Liu, Diane Hildebrandt
Summary: The reduction pathway of Co catalysts supported on untreated SiO2 and two pretreated SiO2 support materials was investigated. The study revealed that ethylene glycol pretreated SiO2 supported Co catalyst showed smaller metal crystallites and highly dispersed Co, but had a low degree of reduction of CoO due to the strong Co-SiO2 interaction. In contrast, the annealing pretreated SiO2 supported Co catalyst exhibited better catalytic activity during FTS.
CHEMICAL ENGINEERING COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Boying Zhang, Haining Liu, Pengda Zhai, Ruijuan Zhang, Wenbo Wang, Phathutshedzo Khangale, Diane Hildebrandt, Xinying Liu, Shanlin Qiao
Summary: This study presents the design of conjugated reticular oligomers (CROs) using an aqueous micellar strategy for water electrolysis. These CROs show improved electrochemical performance compared to COFs due to the presence of a Schottky heterojunction that suppresses electron backflow and enhances adsorption of hydrogen protons and hydroxides.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Engineering, Chemical
Leonard U. Okonye, Yali Yao, Jianwei Ren, Xinying Liu, Diane Hildebrandt
Summary: This study investigates the Fischer-Tropsch Synthesis mechanism using the Arrhenius equation and finds that different mechanisms complement each other in the reaction, resulting in different products.
CHEMICAL ENGINEERING SCIENCE
(2023)
Article
Engineering, Chemical
Maria J. Fernandez-Torres, Diane Hildebrandt, David Glasser, Baraka Celestin Sempuga
Summary: High nitrate levels in groundwater need to be reduced to meet legal guidelines for human consumption. Although techniques like ion exchange and reverse osmosis have been successful on an industrial scale, the catalytic reduction of nitrate to nitrogen with hydrogen has not been commercialized due to the production of byproducts above allowed levels. This study suggests that thermodynamics, rather than kinetics, is the limiting factor in achieving desired selectivity, and it uses the attainable region approach to compare theoretical analysis with experimental data, revealing the challenges in avoiding byproduct formation.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2023)
Article
Food Science & Technology
Shuo Wang, Na Hu, Erjun Tang, Shenglan Yang, Xinying Liu, Linda Jewell
Summary: Porous phosphorylated chestnut starch (P-PCS) was prepared by enzymic hydrolysis and phosphorylation of chestnut starch (CS), and the phosphorylation conditions were optimized using response surface design. The optimal reaction conditions were a CP/P-CS mass ratio of 2:1, a reaction temperature of 146 degrees C, and a reaction time of 159 min. P-PCS exhibited improved light transmittance and Pb(II) adsorption performance compared to CS, indicating its potential as a natural polymer adsorbent in wastewater treatment.
Article
Chemistry, Multidisciplinary
Y. Ji, R. Y. Xie, C. Wu, X. Y. Liu, X. J. Zhang, L. Jiang
Summary: The rise in atmospheric CO2 levels has led to an urgent need for carbon removal technology. The use of biochar-based activated carbon (AC) in the adsorption process has shown promise as a post-combustion capture method. Two types of coconut shell derived ACs activated with KOH and NaOH were studied, and it was found that KOH had a greater activation effect on capture performance. The results also showed that PEI&CHCS-KOH composites had enhanced adsorption performance under humid flue gas conditions, indicating potential application in carbon capture.
JOURNAL OF CO2 UTILIZATION
(2023)
Review
Nanoscience & Nanotechnology
X. Cheng, C. Tang, C. Yan, J. Du, A. Chen, X. Liu, L. Jewell, Q. Zhang
Summary: In order to meet the energy storage needs of portable electronic devices, electric vehicles, renewable-coupled smart grids, and more, it is important to develop lithium-ion batteries (LIBs) with increased energy densities. Porous carbon spheres, with their high chemical stability, electrical conductivity, specific surface area, and porous structure, show promise as anode materials for LIBs. In this review, various preparation methods for porous carbon spheres are introduced, and strategies for improving the performance of LIBs anode materials are described.
MATERIALS TODAY NANO
(2023)
Review
Engineering, Chemical
Shan Wang, Ping Xiao, Jie Yang, Sonia A. C. Carabineiro, Marek Wisniewski, Junjiang Zhu, Xinying Liu
Summary: With the rapid development of industry, the removal of volatile organic compounds (VOCs) has become crucial due to their detrimental effects on the environment and human health. Catalytic combustion is a widely used technology for VOC removal, and this review focuses on the use of perovskite oxides as catalysts. The review discusses the challenges, prospects, and treatment mechanisms of these catalysts, providing a valuable reference for improving their performance.
FRONTIERS OF CHEMICAL SCIENCE AND ENGINEERING
(2023)
Article
Thermodynamics
W. Liu, Y. Huang, X. J. Zhang, M. X. Fang, X. Liu, T. Wang, L. Jiang
Summary: The paper proposes a steam-assisted temperature swing adsorption (S-TSA) process for carbon capture, in which a heat pump provides the driving force for desorption. Evaluation of the integrated system shows that increasing the feed gas flowrate raises CO2 purity but decreases the recovery rate. The heat and power consumption of the system increase significantly with higher purge flowrates.
CASE STUDIES IN THERMAL ENGINEERING
(2023)
Review
Green & Sustainable Science & Technology
Shuang Zong, Aibing Chen, Marek Wisniewski, Lebohang Macheli, Linda L. Jewell, Diane Hildebrandt, Xinying Liu
Summary: The electrochemical conversion of CO2 into high-value fuels and chemicals is considered a promising method to address greenhouse gas emissions. However, the slow kinetics and side reactions involved in the process lead to low selectivity and limited durability. The interference by the hydrogen evolution reaction and multiple electron transfer processes further decrease the selectivity for hydrocarbons. The reaction conditions, such as temperature and pressure, also play a significant role in the CO2RR process, but have been understudied.
CARBON CAPTURE SCIENCE & TECHNOLOGY
(2023)
Review
Engineering, Environmental
Samukeliso Dube, Joshua Gorimbo, Mahluli Moyo, Chike George Okoye-Chine, Xinying Liu
Summary: Membrane technology is highly valued in hydrogen purification systems, with particular focus on developing stable and selective Ni-based membranes. These membranes have attracted attention due to their high-temperature tolerance and low cost. Extensive studies have investigated the solubility, diffusivity, and permeability of nickel to hydrogen. This review provides a comprehensive overview of the synthesis, applications, and catalytic effects of Ni-based membranes in hydrogen purification systems. Further research is needed to explore the potential opportunities offered by catalytic nickel-based membranes, especially in multi-component systems.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2023)
Article
Chemistry, Physical
Yi-lei Li, Qing Zhao, Xu-jia Liu, Ying Liu, Ying-juan Hao, Xiao-jing Wang, Xin-ying Liu, Diane Hildebrandt, Feng-yu Li, Fa-tang Li
Summary: Precise regulation of photogenic electron transfer pathway is crucial for enhancing photocatalytic carbon dioxide reduction efficiency and product selectivity. In this study, a g-C3N4/CoCo-layered double hydroxide (LDH) heterostructure was fabricated by designing the interface chemical bond Co-N-2 bond at the atomic level. This heterostructure realizes high-speed electron transport through the precise connection of valence band and conduction band using the interfacial Co-N-2 bond. Experimental results show that the addition of CoCo-LDH reduces the overpotential of water oxidation, regulates the charge delocalization of g-C3N4, and lowers the energy barrier of the CO2 intermediate in the reduction half-reaction. The selectivity of carbon-based substances in the products reaches 100%, with an optimal CO yield of 71.39 μmol g(-1) h(-1), which is among the highest values for g-C3N4-based photocatalysts.
Article
Chemistry, Physical
Marek Wisniewski, Xinying Liu
Summary: This study investigates CO2 splitting by using a glow discharge reactor packed with carbonaceous materials, and the results indicate that the materials play a dual role as a solid adsorbent and an oxygen scavenger, shifting the overall reaction equilibrium towards CO - the product side.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Review
Chemistry, Multidisciplinary
Yibo Tang, Yiwen Liu, Jiabing Chen, Chengyang He, Xiaojun Lu, Rui Zhang, Xinying Liu
Summary: With the shift from fossil fuels to clean energy, studies on Fischer-Tropsch synthesis have expanded to include the synthesis of value-added chemicals. The FTS route offers an efficient way to synthesize chemicals directly from small molecules derived from carbon-containing resources, but there is still a challenge in controlling the CO2 selectivity.
REACTION CHEMISTRY & ENGINEERING
(2023)
