Article
Energy & Fuels
Xinyi Chen, Guangsheng Zou, Yanliang Yuan, Zuwei Xu, Haibo Zhao
Summary: The research investigates the use of Ni-doped nano-Fe/Ce oxygen carriers for the chemical looping dry reforming of methane. Thermodynamic analysis and reaction simulation are conducted on the CL-DRM process with iron-based oxygen carriers. The experimental results show that the Ni-doped Fe/Ce oxygen carriers achieve high performance and stable cyclic stability due to the high dispersion of Ni and the transformation of Fe oxides and CeO2.
Article
Energy & Fuels
Fang Liu, Weiliao Kang, Chen Song, Zhixuan Jia, Wenbin Chen, Li Yang
Summary: This study conducted experiments to investigate the attrition behavior of an iron-based oxygen carrier under different conditions in chemical looping combustion, revealing the importance of chemical stress on attrition and proposing the attrition mechanism of the oxygen carrier. The results show a dynamic increase process of contribution of chemical stress to attrition and a dominance of chemical stress after a certain number of cycles, indicating the significance of understanding and managing chemical stress in optimizing the performance of chemical looping combustion systems.
Article
Energy & Fuels
Siqi Liu, Fang He, Kun Zhao, Haibo Zhao, Zhen Huang, Guoqiang Wei, Wen Yang
Summary: Coal chemical looping gasification (CCLG) is a promising technology with high resource utilization rate and environmental protection properties, requiring suitable oxygen carriers and optimized operating conditions for coal conversion and H2&CO production. This study tested a Cu-Fe bi-ore oxygen carrier and found that the optimal gasification conditions were at 950 degrees C with a oxygen carrier-to-coal mass ratio of 3:1 and steam rate of 0.08 ml/min, achieving a syngas yield of 58 mmol/g, 75.2% syngas selectivity, and 85.3% carbon conversion.
Article
Energy & Fuels
Zichen Di, Duygu Yilmaz, Arijit Biswas, Fangqin Cheng, Henrik Leion
Summary: Industrial materials containing spinel ferrite structure can be potential substitutes for synthetic oxygen carriers in chemical looping combustion, showing similar reactivity and stability but lower oxygen transport capacity.
Article
Chemistry, Applied
Xintong Guo, Yankun Li, Qingjiao Zhu, Xiude Hu, Jingjing Ma, Qingjie Guo
Summary: Coal ash significantly affects the operating efficiency of pressurized coal chemical looping gasification (CLG), mainly by inhibiting the reduction performance of the oxygen carrier (OC). The deposition inhibition is due to the internal diffusion resistance generated by coal ash coating the surface of OC particles and blocking pores. The inhibitory mechanism of coal ash deposition varies under different pressure conditions.
FUEL PROCESSING TECHNOLOGY
(2021)
Review
Energy & Fuels
Guicai Liu, Grzegorz Lisak
Summary: This review summarizes the basic properties and opportunities of Cu-based OCs in various chemical looping processes. It covers the applications of Cu-based OCs in chemical looping combustion (CLC), chemical looping oxygen uncoupling (CLOU), chemical looping air separation (CLAS), chemical looping for syngas/H2 production, integrated CaO/CuO looping process, and thermochemical energy storage (TCES). The review also discusses the technical challenges and current strategies related to agglomeration, attrition, and ash accumulation. It provides insights and guidance for the design and development of Cu-based OCs and their applications in chemical looping processes.
Article
Engineering, Environmental
Zhenwu Miao, Laihong Shen, Haibo Zhao
Summary: A study found that a single natural ore oxygen carrier (OC) is limited in its industrial application due to its weak reactivity and cyclic stability. Chemical looping combustion (CLC) cycle tests were conducted on a composite hematite and copper ore OC prepared by spray drying granulation using a fluidized bed thermogravimetric analyzer (FB-TGA). The results revealed a high attrition rate of OC in the early stage of fluidization, which stabilized after 6 minutes at 0.28%/h. The redox cycle reaction subjected the OC to chemical and thermal stresses, leading to decreased mechanical strength, increased particle attrition and sintering. This hindered the oxidation stage and resulted in deep reduction of OC, causing particle agglomeration and loss of fluidization. Therefore, reducing the oxygen transfer capacity and residence time in the fuel reactor is beneficial for the safe operation of OC in industry.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Thermodynamics
Ali Ahmad, Md. Abdullah Al Mamun, Md. Al-Mamun, Saiful Huque, Mohammad Ismail
Summary: This study prepared various oxygen carrier materials using the citrate gel technique and conducted research on the chemical-looping process, finding that the oxygen release rate varied under different experimental conditions after increasing the surface area.
JOURNAL OF THERMAL ANALYSIS AND CALORIMETRY
(2022)
Article
Chemistry, Applied
Yunchang Dong, Yanan Wang, Jinchen Ma, Hengfeng Bu, Chuanbao Zheng, Haibo Zhao
Summary: In this study, composite oxygen carriers were prepared using extrusion-spheronization method with fine iron and copper ores as raw materials and inert aluminosilicates as binders. After optimization, the oxygen carriers showed good performance in terms of reactivity and stability, indicating the suitability of the method for large-scale preparation of oxygen carrier particles.
FUEL PROCESSING TECHNOLOGY
(2021)
Article
Chemistry, Applied
Jun Hu, Shiyi Chen, Wenguo Xiang
Summary: This study investigated the influence of different promoters (Ni, Co, and Cu) on Fe-based oxygen carriers, finding that promoters can enhance oxygen activity and CH4 conversion rate. Ni-promoted oxygen carriers showed the highest CH4 conversion rate and H2 yield.
FUEL PROCESSING TECHNOLOGY
(2021)
Article
Engineering, Environmental
Wei-Hsin Chen, Kuan-Hsiang Chen, Aristotle T. Ubando, Wen-Jhy Lee, Man -Hin Chio
Summary: Chemical looping combustion (CLC) using iron-based oxygen carriers can efficiently capture carbon dioxide and produce high yields of CO2 and H2O under specific operating conditions. Fe3O4 and Fe2O3 are the major components of iron in OCs during most reduction and oxidation reactions. Decreasing oxygen input leads to increased carbon formation in the system.
CHEMICAL ENGINEERING JOURNAL
(2021)
Article
Materials Science, Ceramics
Aref Basiri, Amir Hossein Nassajpour-Esfahani, Mohammad Reza Haftbaradaran-Esfahani, Amir Alhaji, Ali Shafyei
Summary: This study investigated the granulation process of magnesium aluminate spinel powders using spray freeze drying method. The optimal amount of binder was found to be 3%, and the ideal solid load was determined to be 35 wt%, resulting in granules of 10-50 μm in size. Powder granulation increased density by approximately 20% and improved the in-line transmission for the IR range by over 15%.
CERAMICS INTERNATIONAL
(2022)
Article
Chemistry, Physical
Fabio Blaschke, Marjan Bele, Brigitte Bitschnau, Viktor Hacker
Summary: The study focused on investigating the microscopic effects on the performance of the active catalytic system in the chemical looping process. Different materials were analyzed for their inhibiting and accelerating effects. ZrO2 doped with MgO and Y2O3 showed chemical inertness and formation of a porous morphology, which improved cyclic stability. The HT-XRD and DSC analyzes confirmed the role of microscopic phenomena in the process and their correlation to phase transition. Stabilization of the cubic/tetragonal crystal structure suppressed phase transition and exhibited the highest activity, revealing new principles for oxygen carrier design and understanding the influence of microscopic effects on stability.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Energy & Fuels
Amr Abdalla, Mohanned Mohamedali, Nader Mahinpey
Summary: Modifying CuO/ZrO2 oxygen carriers by adding WO3 can significantly increase the oxygen capacity, promote the formation of Cu-W intermediate phases, and enhance the redox characteristics of the oxygen carriers. Samples synthesized via coimpregnation method show higher oxygen release capacity, with higher Cu/W ratio and larger crystallite structure.
Article
Energy & Fuels
Lei Liu, Zhenshan Li, Ningsheng Cai
Summary: This study reports tonnage-scale preparation of manganese oxygen carrier particles using industrial spray drying granulation with original manganese ore and kaolin fines. It found that reaction temperature and gas concentrations of O-2, H-2, and CH4 have an impact on redox kinetics, with H-2 reduction being approximately 6 times faster than CH4 reduction.
Article
Chemistry, Physical
Eva Loccufier, Geert Watson, Yingrui Zhao, Maria Meledina, Robbe Denis, Parviz Gohari Derakhshandeh, Pascal Van Der Voort, Karen Leus, Damien P. Debecker, Klaartje De Buysser, Karen De Clerck
Summary: The challenge of converting CO2 and H2 into fuels can be addressed by developing a stable, reusable, and easy to handle heterogeneous catalyst. In this study, Ru nanoparticles were encapsulated inside the metal organic framework Cr-MIL-101 and loaded onto a silica nanofibrous membrane. The resulting catalytic membrane showed promising performance for the Sabatier methanation reaction, paving the way for efficient CO2 hydrogenation processes.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Multidisciplinary
Sander Borgmans, Sven M. J. Rogge, Juul S. De Vos, Pascal van der Voort, Veronique Van Speybroeck
Summary: Soft porous crystals with stimuli responsiveness are widely studied for various applications. However, the structural flexibility in 3D covalent organic frameworks (COFs) is not well understood. This study investigates the factors affecting the phase transformations of diamondoid COFs, including structural decoration, interpenetration, temperature, and guest adsorption. It provides a comprehensive understanding of the design principles for flexible diamondoid COFs.
COMMUNICATIONS CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Jiamin Sun, Himanshu Sekhar Jena, Chidharth Krishnaraj, Kuber Singh Rawat, Sara Abednatanzi, Jeet Chakraborty, Andreas Laemont, Wanlu Liu, Hui Chen, Ying-Ya Liu, Karen Leus, Henk Vrielinck, Veronique Van Speybroeck, Pascal Van Der Voort
Summary: Four highly porous covalent organic frameworks (COFs) containing pyrene units were prepared and explored for photocatalytic H2O2 production. Experimental studies and density functional theory calculations showed that the pyrene unit has higher activity for H2O2 production compared to bipyridine and (diarylamino)benzene units. The distribution of pyrene units over a large surface area of COFs was found to be crucial for catalytic performance.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Nanoscience & Nanotechnology
Maarten Debruyne, Sander Borgmans, Sambhu Radhakrishnan, Eric Breynaert, Henk Vrielinck, Karen Leus, Andreas Laemont, Juul De Vos, Kuber Singh Rawat, Siebe Vanlommel, Hannes Rijckaert, Hadi Salemi, Jonas Everaert, Flore Vanden Bussche, Dirk Poelman, Rino Morent, Nathalie De Geyter, Pascal Van Der Voort, Veronique Van Speybroeck, Christian V. Stevens
Summary: Covalent organic frameworks (COFs) are a new type of photoactive organic semiconductors with ordered structures and high surface areas. The band gaps of COFs can be tuned by the choice of building blocks and linkages, making them tailor-made for specific (photocatalytic) applications. However, there are still many unexplored building blocks for COFs as photocatalytic moieties, and the scope of photocatalyzed reactions by COFs is limited.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Ruqia Khan, Jeet Chakraborty, Kuber Singh Rawat, Rino Morent, Nathalie De Geyter, Veronique Van Speybroeck, Pascal Van Der Voort
Summary: A custom-crafted covalent triazine network has been developed as a metal-free functional organic network electrocatalyst for electrochemical two-electron water oxidation (2e WOR) reaction. The material exhibits high Faradaic Efficiency and H2O2 production rate, and the 2e WOR mechanism has been confirmed by experiments and supported by theoretical studies.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Amrita Chatterjee, Jiamin Sun, Kuber Singh Rawat, Veronique Van Speybroeck, Pascal van der Voort
Summary: Two donor-acceptor type tetrathiafulvalene (TTF)-based covalent organic frameworks (COFs) were studied as electrodes for symmetric supercapacitors in different electrolytes. The charge storage mechanism of IL electrolyte based supercapacitors depends on the micro pore size and surface charge density of COFs, which can be altered by different electron acceptor building blocks. The combination of these factors enhances the charge storage in highly microporous COFs. DFT calculations support this finding.
Article
Multidisciplinary Sciences
Emile Jules Beckwee, Geert Watson, Maarten Houlleberghs, Daniel Arenas Esteban, Sara Bals, Pascal Van Der Voort, Eric Breynaert, Johan Martens, Gino Baron, Joeri F. M. Denayer
Summary: This study reports a new type of periodic mesoporous organosilica (PMO) nanotubes, referred to as hollow ring PMO (HR-PMO), capable of promoting methane clathrate hydrate formation under mild working conditions and at high water loading. The HR-PMO nanotubes exhibit a steep single-stepped isotherm and a noticeably high methane storage capacity. Supported by ex situ cryo-electron tomography and x-ray diffraction, the findings suggest that HR-PMO nanotubes promote clathrate hydrate nucleation and growth by distributing and confining water in the mesopores of their outer wall, central channels, and external surface. These results highlight the potential application of organosilica materials for pressure-based storage of biomethane in confined clathrate hydrates.
Article
Chemistry, Inorganic & Nuclear
Wanlu Liu, Chunhui Liu, Luca Pilia, Hongliang Zhang, Pascal van der Voort, Anna M. Kaczmarek, Rik Van Deun
Summary: We synthesized a co-condensed hollow ethane-bipyridine periodic mesoporous organosilica (HEt-bpy-PMO) as a host material to anchor lanthanides for developing a multifunctional chemical sensor. The luminescence properties of the developed hybrid materials were studied in detail in the solid-state and after dispersing in water. The Eu3+ or Tb3+ incorporated materials showed ions selectivity towards Cu2+, Co2+, and Fe3+ as ion sensors, and exhibited excellent acetone sensing selectivity.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Multidisciplinary
Jonas Everaert, Karen Leus, Hannes Rijckaert, Maarten Debruyne, Kristof Van Hecke, Rino Morent, Nathalie De Geyter, Veronique Van Speybroeck, Pascal Van Der Voort, Christian V. Stevens
Summary: Covalent triazine frameworks (CTFs) based on polydentate ligands are promising catalyst supports that combine the reactivity of homogeneous catalysts with the robustness and recyclability of heterogeneous ones. In this study, a rhodium (III) complex was immobilized on a bipyridine-based CTF for the transfer hydrogenation of N-heteroarenes in water using sodium formate as the hydrogen source. The immobilized catalyst showed excellent activity for various quinoxalines and other N-heteroarenes, and maintained high activity during recycling, making it suitable for continuous flow synthesis.
Article
Materials Science, Multidisciplinary
Chunhui Liu, Anna M. Kaczmarek, Himanshu Sekhar Jena, Zetian Yang, Dirk Poelman, Pascal van der Voort
Summary: Recent research in lanthanide materials has contributed to the development of chemical sensors, but the current sensors still have limited detection range. We developed lanthanide-based hollow spheres for luminescence turn-off sensing of Hg2+ with low detection limit and wide detection range. This hybrid material exhibited both downshifting and upconversion luminescence.
JOURNAL OF MATERIALS CHEMISTRY C
(2023)
Article
Chemistry, Multidisciplinary
Maojun Deng, Jiamin Sun, Andreas Laemont, Chunhui Liu, Linyang Wang, Laurens Bourda, Jeet Chakraborty, Kristof Van Hecke, Rino Morent, Nathalie De Geyter, Karen Leus, Hui Chen, Pascal van der Voort
Summary: The photocatalytic activity of crystalline porous covalent organic frameworks (COFs) was significantly enhanced by extending their π-conjugation system through a post-sulfurization process. Thiazole-linked COFs exhibited the best photocatalytic performance, with a rate 5.8 and 3.7 times higher than imine-linked COFs 4PE-N and 4PE-TT, respectively.
Article
Chemistry, Physical
Juul S. De Vos, Sander Borgmans, Pascal Van Der Voort, Sven M. J. Rogge, Veronique Van Speybroeck
Summary: This article introduces a database called ReDD-COFFEE, which contains 268,687 covalent organic frameworks (COFs) with accompanying ab initio derived force fields that outperform generic ones. The database provides a large number of computer-ready structures with high diversity in terms of geometric properties, linker cores, and linkage types. Additionally, the textural properties of the database are analyzed and the most promising COFs for vehicular methane storage are identified. By making the database freely accessible, it is hoped that it can inspire others to further explore the potential of these intriguing functional materials.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Multidisciplinary
Amrita Chatterjee, Linyang Wang, Pascal Van Der Voort
Summary: There is an urgent need for cleaner production processes in the chemical field. Heterogeneous photocatalysis, which converts (visible) light into chemical energy, shows promise as an efficient alternative. Metal-organic frameworks (MOFs) have emerged as a favorable material for photocatalysis due to their large surface area, tunable properties, versatile functionality, and ability to form composites. Research is focusing on constructing Z-scheme heterojunctions in MOFs to enhance light harvesting capacity and improve the redox ability of photocatalysts.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Geert Watson, Nithin B. Kummamuru, Sammy W. Verbruggen, Patrice Perreault, Maarten Houlleberghs, Johan Martens, Eric Breynaert, Pascal van der Voort
Summary: This study explores the use of hydrophobic periodic organosilica nanoparticles for hydrogen storage as clathrate hydrates. The surface decoration with promoter agents enhances the formation and growth kinetics of clathrate hydrates, resulting in an increase in hydrogen storage capacity. These findings are of significant importance for the development of hydrogen clathrates in industrial applications.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Physical
Linyang Wang, Jiamin Sun, Maojun Deng, Chunhui Liu, Servet Ataberk Cayan, Korneel Molkens, Pieter Geiregat, Rino Morent, Nathalie De Geyter, Jeet Chakraborty, Pascal Van Der Voort
Summary: This study introduces two benzothiadiazole-based COFs with tunable electronic structures and electron affinities for photocatalytic H2O2 production. The triazine-containing TAPT-BT-COF exhibits outstanding charge separation and achieves high H2O2 production rate in pure water.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
