Article
Chemistry, Multidisciplinary
Zhiyu Zou, Alessandro Sala, Mirco Panighel, Ezequiel Tosi, Paolo Lacovig, Silvano Lizzit, Mattia Scardamaglia, Esko Kokkonen, Cinzia Cepek, Cristina Africh, Giovanni Comelli, Sebastian Guenther, Laerte L. L. Patera
Summary: The mechanism behind the growth of hydrocarbon chains during the synthesis of high-value fuels and plastics from small hydrocarbon molecules remains largely unknown. In this study, the formation of hydrocarbon chains resulting from acetylene polymerization on a Ni(111) model catalyst surface was investigated using X-ray photoelectron spectroscopy at near-ambient pressures. The intermediate species and reaction products were identified, and in situ scanning tunneling microscopy observations provided insights into the C-C coupling mechanism. The study revealed that polymerization occurs on the flat terraces of the metallic surface instead of the step edges commonly assumed as the active sites for C-C coupling.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Review
Chemistry, Applied
Renyang Zheng, Zaiku Xie
Summary: The sustainable development of the chemical industry requires novel and efficient catalysts and catalytic processes, especially eco-friendly and intrinsically safe processes. In-situ characterization of catalytic performance is of great significance for a comprehensive study on the structure-performance relationship of catalysts. Realizing full life cycle characterization of heterogeneous catalysts under industrial conditions remains a great challenge.
CHINESE JOURNAL OF CATALYSIS
(2021)
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
Chemistry, Multidisciplinary
Meng Cui, Qingli Qian, Jingjing Zhang, Ying Wang, Bernard Baffour Asare Bediako, Huizhen Liu, Buxing Han
Summary: The study presents the production of liquid fuel from CO2 hydrogenation by coupling homogeneous RuCl3 and heterogeneous Ru-0 catalysts at the lowest reported temperature (180 degrees C) and achieving the highest C5+ selectivity to date (71.1%). The synergy of homogeneous and heterogeneous catalysis is identified as the key factor for the outstanding performance.
Article
Chemistry, Applied
Lilia Sineva, Ekaterina O. Gorokhova, Kirill O. Gryaznov, Ilya S. Ermolaev, Vladimir Z. Mordkovich
Summary: The use of zeolite-containing Co catalysts in liquid hydrocarbon transformations during Fischer-Tropsch synthesis demonstrated a decrease in the average molecular weight of the products without increasing methane selectivity. The introduction of zeolites cleared the catalyst pore system of heavier hydrocarbons, suggesting a potential role in controlling product composition over hybrid catalysts.
Article
Multidisciplinary Sciences
lgor Levchenko, Shuyan Xu, Oleg Baranov, Kateryna Bazaka
Summary: Inhospitable and remote locations such as deserts, islands, and outer space offer unique opportunities for science, economy, and geopolitics, but the stable supply of energy is a critical challenge due to transportation difficulties and costs. This essay explores the advantages and challenges of integrating Fischer-Tropsch, artificial photosynthesis, and plasma catalysis into a self-contained system for energy harvesting, storage, and utilization.
Article
Chemistry, Multidisciplinary
Kun Liu, Adrian Ramirez, Xin Zhang, Mustafa Caglayan, Xuan Gong, Jorge Gascon, Abhishek Dutta Chowdhury
Summary: The CO2-to-aromatics process converts carbon dioxide (CO2) into valuable petrochemicals, specifically aromatics like benzene, toluene, and xylene, using metal/zeolite bifunctional catalytic systems. These aromatics are currently derived exclusively from fossil fuels and are used in various industrial applications. This process can help mitigate climate change by reducing greenhouse gas emissions and promoting a more sustainable and circular economy by reducing reliance on fossil fuels.
Article
Chemistry, Physical
Bang Gu, Deizi V. Peron, Alan J. Barrios, Mirella Virginie, Camille La Fontaine, Valerie Briois, Mykhailo Vorokhta, Bretislav Smid, Simona Moldovan, Siddardha Koneti, Thobani G. Gambu, Mark Saeys, Vitaly V. Ordomsky, Andrei Y. Khodakov
Summary: Metal nanoparticles on porous supports have wide applications in various scientific areas. This study demonstrates that bismuth promoter can enhance the stability of cobalt catalysts, leading to migration and redisersion of bismuth over the surface of cobalt nanoparticles during the reduction step. The preferential localization of mobile bismuth promoter at the steps and edges of cobalt nanoparticles hinders cobalt sintering and carbon deposition, resulting in improved catalyst stability.
JOURNAL OF CATALYSIS
(2021)
Article
Nanoscience & Nanotechnology
Joakim Tafjord, Erling Rytter, Anders Holmen, Rune Myrstad, Ingeborg-Helene Svenum, Bjorn E. Christensen, Jia Yang
Summary: This study describes a method to synthesize transition-metal nanoparticles anchored on carbon supports using low-molar-mass sodium alginate, followed by a pyrolysis step. The resulting catalysts exhibit high metal loadings and activity, with pyrolyzed Fe-alginate showing particularly high Fischer-Tropsch synthesis activity.
ACS APPLIED NANO MATERIALS
(2021)
Review
Chemistry, Multidisciplinary
Nuria Martin, Francisco G. Cirujano
Summary: This article reviews several iron-containing multifunctional catalysts for the direct transformation of CO2 into gasoline, discussing their preparation, characterization, and catalytic performance in this environmentally and industrially relevant application, and proposing future research directions.
JOURNAL OF CO2 UTILIZATION
(2022)
Article
Geology
Jingbo Nan, Helen E. King, Guusje Delen, Florian Meirer, Bert M. Weckhuysen, Zixiao Guo, Xiaotong Peng, Oliver Plumper
Summary: The study found a direct association between carbonaceous matter and the dominant Fe oxide in serpentinites, including nanosized Fe oxides playing a key role in the abiotic synthesis of complex carbonaceous matter.
Article
Chemistry, Physical
Bhupendra Kumar Singh, Yongseok Kim, Seungdon Kwon, Kyungsu Na
Summary: Mesoporous zeolites have become essential in the chemical industry due to their unique structural characteristics, offering versatile opportunities in both traditional and emerging catalysis fields. They have demonstrated longer lifetimes and better performance in catalytic reactions compared to their microporous counterparts.
Article
Chemistry, Physical
Erling Rytter, Christian Aaserud, Anne-Mette Hilmen, Edvard Bergene, Anders Holmen
Summary: The pretreatment and reduction time significantly influence the catalytic activity of cobalt foil catalysts, increasing the available surface area and cobalt site density, and enhancing the olefin hydrogenation reaction and selectivity to heavier components. However, prolonged reduction time leads to sintering of cobalt crystallites, while too short of a reduction time results in incomplete reduction.
Article
Energy & Fuels
Ruizhe Li, Yuan Li, Zhenhua Li, Weiqin Wei, Shuxin Ouyang, Hong Yuan, Tierui Zhang
Summary: This study successfully synthesized a novel catalyst of CoMn alloy-loaded MnO using a one-step wet-chemical method, which exhibited good selectivity for light olefins in photothermocatalytic FTS, along with low CO2 selectivity for effective use of carbon resources.
Review
Chemistry, Multidisciplinary
Justin C. Bui, Chanyeon Kim, Alex J. King, Oyinkansola Romiluyi, Ahmet Kusoglu, Adam Z. Weber, Alexis T. Bell
Summary: The electrochemical reduction of carbon dioxide (CO2R) driven by renewable electricity offers a promising route for reusing CO2 and producing carbon-containing chemicals and fuels sustainably. Optimizing the catalyst microenvironment and selectivity, as well as controlling the electrolyte and operating conditions, are crucial for achieving economic viability and high product yields.
ACCOUNTS OF CHEMICAL RESEARCH
(2022)
Correction
Energy & Fuels
Chanyeon Kim, Justin C. Bui, Xiaoyan Luo, Jason K. Cooper, Ahmet Kusoglu, Adam Z. Weber, Alexis T. Bell
Review
Chemistry, Multidisciplinary
Justin C. Bui, Eric W. Lees, Lalit M. Pant, Iryna V. Zenyuk, Alexis T. Bell, Adam Z. Weber
Summary: Electrochemical synthesis using renewable energy to convert feedstocks into chemicals and fuels is promising, but understanding phenomena in porous electrode systems is challenging. Continuum modeling aids in understanding observed behaviors and guiding next-generation device design. Simulating multiscale phenomena in porous electrodes helps understand and improve the performance of electrochemical synthesis devices.
Article
Multidisciplinary Sciences
Hassan A. Aljama, Martin Head-Gordon, Alexis T. Bell
Summary: In this study, a high-throughput screening process using density functional theory was implemented to identify the energetically most favorable active sites in cation exchanged-zeolites, which is important for understanding catalysis and adsorption behaviors in zeolites.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Physical
Joseph A. Gauthier, Zhou Lin, Martin Head-Gordon, Alexis T. Bell
Summary: This study investigates the mechanism of CO2RR under experimental conditions and reveals the differences in activation barriers between alkaline and acidic pathways, as well as the kinetic favorability of COH formation under high overpotential.
ACS ENERGY LETTERS
(2022)
Article
Chemistry, Physical
Tianyu Zhang, Justin C. Bui, Zhengyuan Li, Alexis T. Bell, Adam Z. Weber, Jingjie Wu
Summary: In this study, we developed segmented gas-diffusion electrodes (s-GDEs) to improve the management of CO intermediates in tandem catalysts, thereby enhancing C2+ Faradaic efficiency and current density.
Article
Chemistry, Physical
Paul Kim, Jeroen Van der Mynsbrugge, Martin Head-Gordon, Alexis T. Bell
Summary: Passive NOx adsorbers (PNAs) are proposed for trapping NOx in automotive exhaust during cold start. In this study, it is found that Pd+ cations can be formed through water adsorbed on zeolite acid sites and can be fully desorbed by adsorbing NO. These reactions are thermodynamically feasible and Pd+ is not formed in the absence of adsorbed water and can be readily reoxidized to Pd2+ by trace amounts of O2.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Multidisciplinary
Liang Qi, Sonali Das, Yanfei Zhang, Danna Nozik, Bruce C. Gates, Alexis T. Bell
Summary: Catalysts for ethene hydroformylation were prepared by grafting Rh into nests of -SiOZn-OH or -SiOCo-OH species in BEA zeolite. The Rh dispersion increased with increasing M/Rh ratio and had a positive effect on the turnover frequency for ethene hydroformylation. The Co-containing catalyst exhibited higher activity and selectivity than the Zn-containing catalyst.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Danna Nozik, Alexis T. Bell
Summary: Ethane and propane derived from shale gas are preferred feedstocks for the production of aromatics. Ga/H-MFI zeolite exhibits high activity and selectivity for light alkane dehydroaromatization, with Ga3+ sites playing a crucial role. The enhanced activity of Ga/H-MFI is attributed to cooperative effects between Ga3+ sites and Bronsted acid protons.
Article
Chemistry, Multidisciplinary
Brooke Soobrian, Alex J. King, Justin C. Bui, Adam Z. Weber, Alexis T. Bell, Frances A. Houle
Summary: Artificial photosynthesis is a promising method to produce commodity chemicals using abundant chemical feedstocks and renewable energy sources. However, affordable and effective hands-on activities for primary school students to demonstrate and teach artificial photosynthesis are lacking. Educating young students on this topic is crucial for developing a diverse next-generation energy workforce. This study confirms that an active learning-based lesson plan using cheap and accessible materials can effectively educate a broad range of young students on artificial photosynthesis, as demonstrated by the improved understanding of fifth grade students before and after the lesson plan.
JOURNAL OF CHEMICAL EDUCATION
(2023)
Article
Nanoscience & Nanotechnology
Alex J. King, Adam Z. Weber, Alexis T. Bell
Summary: A metal-insulator-semiconductor (MIS) structure is an attractive photoelectrode-catalyst architecture for promoting photoelectrochemical reactions, such as the formation of H2 by proton reduction. Understanding how the insulator layer determines the photovoltage and what properties lead to high photovoltages is critical to the development of MIS structures for solar-to-chemical energy conversion.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
John Safipour, Adam Z. Weber, Alexis T. Bell
Summary: Reactive carbon capture (RCC) is a promising solution for carbon capture and utilization. A systematic study found that RCC in aqueous environments is less effective and does not directly reduce into carbamate. Instead, the presence of amine solution suppresses the rate of CO formation while increasing that of H2.
ACS ENERGY LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Chanyeon Kim, Alex J. King, Shaul Aloni, Francesca M. Toma, Adam Z. Weber, Alexis T. Bell
Summary: Photoelectrochemical carbon-dioxide reduction (PEC CO2R) is a promising method for producing chemicals and fuels using sunlight, water, and carbon dioxide. However, the focus has been mostly on producing C-1 products, while the production of C2+ products has been rarely demonstrated. In this study, a Cu/TiO2/p-Si photocathode/catalyst structure was investigated to understand the effects of semiconductor-insulator interactions and illumination direction on the performance and product distribution. Coating the Cu surface with a thin bilayer of Sustainion/Nafion significantly enhanced the current density and faradaic efficiency to ethylene.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Annette Bohme, Justin C. Bui, Aidan Q. Fenwick, Rohit Bhide, Cassidy N. Feltenberger, Alexandra J. Welch, Alex J. King, Alexis T. Bell, Adam Z. Weber, Shane Ardo, Harry A. Atwater
Summary: We investigated how the micrometer-scale morphology of a CO2R gas diffusion electrode (GDE) affects the mass transport properties and local CO2R performance. Using fluorescence confocal laser scanning microscopy (CLSM), we created local pOH maps around a copper GDE and observed that pOH decreases in microtrenches compared to the electrode surface. Multiphysics simulations correlated well with experimental measurements and suggested that the decreased pOH inside microcavities leads to enhanced selectivity towards multicarbon products. This study highlights the importance of a GDE's micromorphology on CO2R performance.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Wan-Lu Li, Christianna N. Lininger, Kaixuan Chen, Valerie Vaissier Welborn, Elliot Rossomme, Alexis T. Bell, Martin Head-Gordon, Teresa Head-Gordon
Summary: This study evaluates the performance of DFT in predicting CO binding trends on different metal surfaces by considering thermal fluctuations, with the B97M-rV functional showing better performance on all surfaces. Thermally induced surface distortions are shown to influence the accurate prediction of binding preferences on metal surfaces, highlighting the importance of accounting for finite temperature fluctuations in comparisons with experimental and application data.
Article
Chemistry, Physical
Yifan Sun, Ye Lv, Wei Li, Jinli Zhang, Yan Fu
Summary: In this study, PtRu electrocatalysts were fabricated on carbon paper via cyclic electrodeposition for the electrocatalytic hydrogenation (ECH) of phenol. The Pt3Ru3 catalyst exhibited excellent activity and stability for the conversion of phenol to cyclohexanol at ambient temperature and various current densities. The in situ Raman spectroscopy and kinetic study revealed the hydrogenation mechanism of phenol over Pt3Ru3 in acidic electrolyte, providing an effective electrochemical strategy for the facile construction of durable electrode materials and efficient phenol hydrogenation.
JOURNAL OF CATALYSIS
(2024)
Article
Chemistry, Physical
Amir Shahzad, Khezina Rafiq, Muhammad Zeeshan Abid, Naseem Ahmad Khan, Syed Shoaib Ahmad Shah, Raed H. Althomali, Abdul Rauf, Ejaz Hussain
Summary: Photocatalytic hydrogen production through water splitting is an effective method for meeting future energy demands. In this study, researchers synthesized a 1 % Ag2S/Cu2S co-doped CdZnS catalyst and found that it can produce hydrogen at a higher rate. The co-doping of Ag2S and Cu2S in the CdZnS catalyst showed a synergistic effect, with Ag2S promoting oxidation reactions and Cu2S promoting reduction reactions.
JOURNAL OF CATALYSIS
(2024)