Article
Chemistry, Applied
Burcu Kekevi, E. Hilal Mert
Summary: Polymeric sorbent materials with excellent swelling capacity were developed using high internal phase emulsion (HIPE) templating approach. The influence of beta-myrcene concentration on emulsion stability and crosslinking was investigated. It was found that the maximum swelling capacities were reached in benzene, toluene, and hexane.
REACTIVE & FUNCTIONAL POLYMERS
(2021)
Review
Chemistry, Multidisciplinary
Shishir Tiwary, Soubhik Kumar Bhaumik
Summary: This review discusses theoretical approaches in high-temperature CO2 capture using CaO-based sorbent, including thermodynamics, sorbent-level kinetic models, and column-level hydrodynamic models. The theoretical prediction of plant-level performance is crucial for design upscale.
JOURNAL OF CO2 UTILIZATION
(2022)
Article
Engineering, Chemical
Xiaobin Chen, Yuting Tang, Chuncheng Ke, Chaoyue Zhang, Sichun Ding, Xiaoqian Ma
Summary: This study proposed a novel method to improve the CO2 capture performance in high-temperature pyrolysis technology. By co-precipitation modification with Ca, Mg, and Zr metals, the modified calcium-based sorbents were successfully prepared. The results showed that under certain conditions, the modified sorbents could effectively reduce the CO2 concentration in the pyrolysis gas.
CHINESE JOURNAL OF CHEMICAL ENGINEERING
(2022)
Article
Engineering, Chemical
Long Ren, Mingchun Li, Sijin Wang, Laishi Li, Yusheng Wu
Summary: In this study, limestone-derived sorbents with enhanced carbonation reactivity and diffusivity were prepared by incorporating Na+ ions into the CaO lattice. The modified sorbents showed improved CO2 capture capacity and durability due to the formation of solid-state ion transport channels within the product layer.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2022)
Article
Chemistry, Multidisciplinary
Maximilian Kroedel, Alexander Oing, Jan Negele, Annelies Landuyt, Agnieszka Kierzkowska, Alexander H. Bork, Felix Donat, Christoph R. Mueller
Summary: Developing nanostructured yolk-shell sorbents can enhance cyclic CO2 uptake stability of CaO-based solid sorbents, leading to lower CO2 capture costs. By comparing yolk-shell and core-shell architectures, the mechanisms behind delaying CaZrO3 formation and increasing possible CO2 uptake are identified.
Article
Engineering, Environmental
Wenfei Yue, Chuigang Fan, Wenli Song, Songgeng Li
Summary: This study investigates the effects of different precipitated CaCO3 precursors on the physical properties and CO2 capture performance of CaO sorbents. The results show that the presence of additives affects the crystal composition and porosity of the CaCO3 precursor, and CaO sorbents derived from CaCO3 modified with 8 mmol/L CTAB exhibit higher CO2 capture capacity than other sorbents.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2022)
Article
Energy & Fuels
Hewen Li, Jian Sun, Qiran Jiang, Hongqiang Xia, Shan Cheng, Zijian Zhou, Xinming Nie, Chuanwen Zhao
Summary: Highly efficient and stable Zr-incorporated CaO-based sorbents were synthesized using a cigarette butt-assisted combustion synthesis (CAC) method. The CAC method showed superior cyclic CO2 capture capability and shorter synthesis time compared to wet-mixing and sol-gel methods. The optimal combustion temperature for synthesizing Zr-incorporated CaO-based sorbents using CAC method was found to be 750 degrees C. Synthetic sorbents with 25 wt% ZrO2 exhibited outstanding CO2 capture performance due to the generation of extensive CaZrO3 grains. The combination of cigarette butt-assisted combustion and graphite-moulding enabled the preparation of practical Zr-incorporated CaO-based pellets.
Article
Engineering, Environmental
Yongqing Xu, Felix Donat, Cong Luo, Jian Chen, Agnieszka Kierzkowska, Muhammad Awais Naeem, Liqi Zhang, Christoph R. Mueller
Summary: This study investigates the effect of alkali metal salt promoter K2CO3 on the cyclic performance of CaO-based sorbents. It is found that low concentrations of K2CO3 significantly improve the cyclic performance of CaO, while high concentrations reduce the CO2 uptake performance. The stability of K2CO3 is influenced by the gas environment, with partial volatilization at high temperatures leading to a decrease in K content in the samples.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Engineering, Environmental
Tao Li, Bing Ding, Victor Malgras, Jongbeom Na, Zongyi Qin, Xiangjun Lu, Yoshio Bando, Hiroki Nara, Zeid A. Alothman, Jie Wang, Yusuke Yamauchi
Summary: In this study, hollow-structured mesoporous carbon (HOMC) nanoplates were successfully synthesized using a self-template method, with Fe-doped HOMC (Fe/HOMC) exhibiting higher electrocatalytic activity, efficiency, durability, and tolerance to methanol poisoning compared to traditional Pt/C benchmark. The Fe/HOMC also showed promising application in Zn-air batteries with high power densities and excellent cycling stability, demonstrating a new avenue for the design of ordered mesoporous materials with hollow structure.
CHEMICAL ENGINEERING JOURNAL
(2021)
Article
Chemistry, Multidisciplinary
Maximilian Krodel, Lorenz Abduly, Manouchehr Nadjafi, Agnieszka Kierzkowska, Alexander Yakimov, Alexander H. Bork, Felix Donat, Christophe Coperet, Paula M. Abdala, Christoph R. Mueller
Summary: Understanding the effects of different structural parameters of CaO-based CO2 sorbents on cyclic CO2 uptake is crucial for their advancement. Through mechanochemical activation, CaO-based sorbents with varying ratios of Na2CO3:CaCO3 were synthesized to investigate the impact of sodium species on the sorbents' structure, morphology, carbonation rate, and cyclic CO2 uptake. The addition of Na2CO3 in the range of 0.1-0.2 mol% significantly improved CO2 uptake by up to 80% after 10 cycles compared to untreated CaCO3, while higher Na2CO3 loadings (>0.3 mol%) led to a decrease of more than 40% in cyclic CO2 uptake due to accelerated deactivation caused by sintering and the presence of crystalline Na2Ca(CO3)(2) species with high mobility of Na.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Engineering, Environmental
Mingchun Li, Cunliang Shen, Jie Ji, Laishi Li, Yusheng Wu
Summary: Highly reactive CaO sorbents based on natural limestone with enhanced stability and re-usability were obtained through a pre-sintering-hydration method. These sorbents exhibited high CO2 capture capacity, improved cycle stability, and the ability to maintain a high capture capacity after multiple cycles. The improved properties can be attributed to the active mechanisms introduced by the pre-sintering-hydration treatment.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2022)
Article
Engineering, Environmental
Yingchao Hu, Hongyuan Lu, Hailong Li
Summary: In this study, CaO sorbents were successfully pelletized using agar-assisted moulding technique, with novel organometallic precursors showing impressive CO2 sorption performance. The excellent performance was attributed to the rich porosity and porous structures of the sorbents.
CHEMICAL ENGINEERING JOURNAL
(2021)
Article
Chemistry, Multidisciplinary
Debabrata Moitra, Narges Mokhtari-Nori, Kevin M. Siniard, Liqi Qiu, Juntian Fan, Zhun Dong, Wenda Hu, Hongjun Liu, De-en Jiang, Hongfei Lin, Jianzhi Hu, Meijia Li, Zhenzhen Yang, Sheng Dai
Summary: By harnessing the power of CaO- and SIL-engineered sorbents, high-performance and tunable sorbents in DAC of CO2 were developed. These sorbents exhibited high CO2 uptake capacity, rapid interaction kinetics, facile CO2 releasing, and stable sorption/desorption cycles. Operando DRIFTS analysis and solid-state NMR analysis demonstrated the critical roles of SIL species in low-concentration CO2 capture.
Article
Energy & Fuels
Xiaodi Niu, Yanyan Feng, Yonghui Xu, Wen Yang
Summary: This study investigated the effects of Mg(NO3)2·6H2O concentration and Al doping on the structure and CO2 adsorption performance of MgO spheres. The results showed that Al incorporation led to the formation of hollow MgO spheres with improved CO2 adsorption capacity. Overall, this work provided insights into enhancing CO2 adsorption using MgO-based adsorbents.
JOURNAL OF NATURAL GAS SCIENCE AND ENGINEERING
(2021)
Article
Nanoscience & Nanotechnology
Manohara Gudiyor Veerabhadrappa, M. Mercedes Maroto-Valer, Yuhang Chen, Susana Garcia
Summary: The study focuses on improving the CO2 capture capacities of LDHs-based MMOs through a modified amide hydrolysis method and aqueous exfoliation technique, leading to the development of pelletized structured sorbents. These structured sorbents exhibit good mechanical stability, high surface area, pore volume, and significantly improved CO2 capture capacities at different temperatures. The pellets outperformed commercially available LDH-based pellets by several fold.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Review
Chemistry, Multidisciplinary
David Lam, Dmitry Lebedev, Mark C. Hersam
Summary: Morphotaxy is a synthesis paradigm that utilizes the shape of an initial nanoscale precursor to template growth or chemical conversion for realizing low-dimensional materials. This approach allows for synthesizing diverse non-vdW materials in ultrathin form while preserving the shape of the original 2D layered material, enabling atomically precise heterojunctions and exotic structures. By expanding the family of low-dimensional materials using morphotaxy, vast possibilities for future fundamental studies and applied technologies are created.
Article
Chemistry, Physical
Pedro Castro-Fernandez, Deni Mance, Chong Liu, Paula M. Abdala, Elena Willinger, Aurelio A. Rossinelli, Alexander I. Serykh, Evgeny A. Pidko, Christophe Coperet, Alexey Fedorov, Christoph R. Mueller
Summary: This study investigates the effect of H2 treatment on the structure, acidity, and catalytic activity of γ/β-Ga2O3 nanoparticle catalysts. The results show that the presence of the β-Ga2O3 phase increases the PDH activity of the catalysts, and H2 treatment enhances the catalytic activity for all three catalysts through different mechanisms.
JOURNAL OF CATALYSIS
(2022)
Review
Chemistry, Multidisciplinary
Constantine Tsounis, Priyank Kumar, Hassan Masood, Rutvij Pankaj Kulkarni, Gopalakrishnan Sai Gautam, Christoph R. Mueller, Rose Amal, Denis A. Kuznetsov
Summary: MXenes, with their tailorable chemistry and favorable physical properties, have great potential in electrocatalytic energy conversion reactions. Further advances specific to electrocatalysis are required to fully exploit their potential. This review discusses the recent advances in performance, stability, compositional discovery and synthesis of MXenes, as well as their prospects in large scale synthesis and solution processing techniques.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Dmitry Lebedev, Jonathan Tyler Gish, Ethan Skyler Garvey, Teodor Kosev Stanev, Junhwan Choi, Leonidas Georgopoulos, Thomas Wei Song, Hong Youl Park, Kenji Watanabe, Takashi Taniguchi, Nathaniel Patrick Stern, Vinod Kumar Sangwan, Mark Christopher Hersam
Summary: 2D magnetic materials have promising applications in quantum and spintronic devices. 2D antiferromagnetic materials are of interest due to their insensitivity to external magnetic fields and faster switching speeds compared to 2D ferromagnets. However, their lack of macroscopic magnetization hampers the detection and control of antiferromagnetic order, emphasizing the need for magneto-electrical measurements.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
David D. Xu, Albert F. Vong, Dmitry Lebedev, Riddhi Ananth, Alexa M. Wong, Paul T. Brown, Mark C. Hersam, Chad A. Mirkin, Emily A. Weiss
Summary: Solid-state single photon emitters (SPEs) in atomically thin transition metal dichalcogenides (TMDs) have gained attention as scalable quantum light sources. In this study, strain fields were created in WSe2 monolayers (MLs) using nanoparticle (NP) arrays, leading to the formation of isolatable SPEs. The emission spectra of WSe2 MLs were quantified to provide insight into the mechanism for SPE production. Excitons selectively funneled through strongly coupled sub-bandgap states, resulting in anti-bunched behavior.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Yi-Hsuan Wu, Harshit Mehta, Elena Willinger, Jodie A. Yuwono, Priyank V. Kumar, Paula M. Abdala, Anna Wach, Agnieszka Kierzkowska, Felix Donat, Denis A. Kuznetsov, Christoph R. Mueller
Summary: Establishing generic catalyst design principles by identifying structural features of materials that influence their performance will advance the rational engineering of new catalytic materials. This study investigates the activity of metal-substituted manganese oxide (spinel) nanoparticles for the electrocatalytic oxygen reduction reaction (ORR) and rationalizes it based on the enthalpy of formation of the binary MO oxide, ΔH-f degrees(MO), and the Lewis acidity of the M2+ substituent. The incorporation of elements M with low ΔH-f degrees(MO) enhances the oxygen binding strength in Mn3O4:M, which affects its activity in ORR. Our work provides insights into the design of new compositions for oxygen electrocatalysis using rational substitution/doping by redox-inactive elements.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Nanoscience & Nanotechnology
Shizhou Jiang, Dmitry Lebedev, Loren Andrews, J. Tyler Gish, Thomas W. Song, Mark C. Hersam, Oluwaseyi Balogun
Summary: Two-dimensional (2D) semiconductors with ambient encapsulation exhibit unique physical properties desirable for various applications. However, limited studies have been conducted on the in-plane thermal conductivity measurements in encapsulated 2D semiconductors. To address this challenge, the authors integrated the FDTR and OTRS techniques in the same experimental platform.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
Manouchehr Nadjafi, Yifan Cui, Marlon Bachl, Alexander Oing, Felix Donat, Giancarlo Luongo, Paula M. Abdala, Alexey Fedorov, Christoph R. Mueller
Summary: The oxidative dehydrogenation of propane can occur through a gas-solid interface or in the gas phase via a radical chain process. This study found that an empty quartz reactor can achieve high propene and ethene selectivities and propane conversions comparable to those of state-of-the-art ODP catalysts. Optimizing the post-catalytic volume of a h-BN catalyst bed can increase propane conversion and propene selectivity, indicating it as an important variable for improving catalytic ODP performances.
Article
Chemistry, Multidisciplinary
Yea-Shine Lee, Dmitry Lebedev, Eric K. Qian, Paloma Lee, Mercouri G. Kanatzidis, Mark C. Hersam, Vinayak P. Dravid
Summary: Copper telluride undergoes phase transitions with slight stoichiometry modifications at high temperatures. We detect a low-temperature phase transition of copper telluride for the first time using Raman spectroscopy and X-ray diffraction. Our experimental study reveals how the liquid precursor contributes to the morphological orientations of Cu0.664Te0.336 crystals and presents liquid-assisted growth as a platform for materials engineering.
CRYSTAL GROWTH & DESIGN
(2023)
Article
Multidisciplinary Sciences
M. Iqbal Bakti Utama, Hongfei Zeng, Tumpa Sadhukhan, Anushka Dasgupta, S. Carin Gavin, Riddhi Ananth, Dmitry Lebedev, Wei Wang, Jia-Shiang Chen, Kenji Watanabe, Takashi Taniguchi, Tobin J. Marks, Xuedan Ma, Emily A. Weiss, George C. Schatz, Nathaniel P. Stern, Mark C. Hersam
Summary: The authors use a chemomechanical approach to modify single-photon emitters (SPEs) in monolayer WSe2 by combining localized mechanical strain with noncovalent surface functionalization, resulting in the simplification of complex defect-related emission into isolated SPEs with high single-photon purity.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Natasa Diklic, Adam H. H. Clark, Juan Herranz, Dino Aegerter, Justus S. S. Diercks, Alexandra Beard, Viktoriia A. A. Saveleva, Piyush Chauhan, Maarten Nachtegaal, Thomas Huthwelker, Dmitry Lebedev, Paula Kayser, Jose Antonio Alonso, Christophe Coperet, Thomas J. J. Schmidt
Summary: The large-scale deployment of polymer electrolyte water electrolysis (PEWE) is limited by the use of scarce and expensive iridium-based O-2 evolution reaction (OER) catalysts in PEWE anodes. To gain a better understanding of the relationship between the catalysts' activity and their physicochemical properties, the oxidation state of surface iridium in different iridium oxides with varying compositions, crystal structures, and OER activities was determined. The results showed that regardless of the catalysts' properties, the surface iridium underwent a linear, potential-driven oxidation that stabilized at a +5 state, which correlated with the onset of O-2 evolution, indicating the involvement of iridium in oxidation states ≥+5 in the OER.
Article
Chemistry, Multidisciplinary
Yea-Shine Lee, Dmitry Lebedev, Eric K. Qian, Paloma Lee, Mercouri G. Kanatzidis, Mark C. Hersam, Vinayak P. Dravid
Summary: We have observed the low-temperature phase transition of copper telluride for the first time using Raman spectroscopy and X-ray diffraction. We experimentally demonstrate how the liquid precursor contributes to the morphological orientations of Cu0.664Te0.336 crystals and propose a growth process based on tellurium supersaturation. Our study enhances understanding of temperature-dependent copper telluride phases and presents liquid-assisted growth as a platform for materials engineering opportunities.
CRYSTAL GROWTH & DESIGN
(2023)
Article
Materials Science, Multidisciplinary
Jovan Nelson, Teodor K. Stanev, Dmitry Lebedev, Trevor LaMountain, J. Tyler Gish, Hongfei Zeng, Hyeondeok Shin, Olle Heinonen, Kenji Watanabe, Takashi Taniguchi, Mark C. Hersam, Nathaniel P. Stern
Summary: Layer-dependent optical spin dynamics have been observed in few-layer and bulk InSe, indicating the potential for all-optical excitation and control of spin in this material.
Article
Chemistry, Physical
Giancarlo Luongo, Alexander H. Bork, Paula M. Abdala, Yi-Hsuan Wu, Evgenia Kountoupi, Felix Donat, Christoph R. Mueller
Summary: In this study, the underlying cause of the increase in oxygen release rate of an oxygen carrier during redox cycling was elucidated. The removal of surface carbonates was found to be the main factor behind this activation phenomenon. Furthermore, the re-formation of surface carbonates after exposure to CO2 resulted in the deactivation of the perovskite oxygen carrier. These findings are important for the performance of such materials in chemical looping at relatively low temperatures (<= 500 degrees C).
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Multidisciplinary
Maximilian Kroedel, Alexander Oing, Jan Negele, Annelies Landuyt, Agnieszka Kierzkowska, Alexander H. Bork, Felix Donat, Christoph R. Mueller
Summary: Developing nanostructured yolk-shell sorbents can enhance cyclic CO2 uptake stability of CaO-based solid sorbents, leading to lower CO2 capture costs. By comparing yolk-shell and core-shell architectures, the mechanisms behind delaying CaZrO3 formation and increasing possible CO2 uptake are identified.
