Article
Chemistry, Applied
Houqian Li, Jifeng Pang, Nicholas R. Jaegers, Libor Kovarik, Mark Engelhard, Anthony W. Savoy, Jianzhi Hu, Junming Sun, Yong Wang
Summary: The Ag-O-Si interfaces significantly enhanced the dehydrogenation of ethanol, while the Zr-O-Si interfaces promoted the condensation of acetaldehyde, leading to a high yield of 1,3-butadiene through the synergistic effects of these interfaces.
JOURNAL OF ENERGY CHEMISTRY
(2021)
Article
Chemistry, Physical
Denis D. Dochain, Ales Styskalik, Vit Vykoukal, Alexandre Vimont, Arnaud Travert, Damien P. Debecker
Summary: Cu-Ta-SiO2 catalysts prepared via non-hydrolytic sol-gel (NHSG) chemistry exhibit high performance in the conversion of ethanol to butadiene, with low selectivity towards dehydration byproducts, moderate Lewis acidity, smaller Cu nanoparticles, and higher active site proximity.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Naomi Miyake, Gordon Brezicki, Robert J. Davis
Summary: This study explores a multifunctional catalyst system composed of silica-supported Ag and ZrO2 for the cascade reaction of ethanol to butadiene. The catalyst showed high selectivity to butadiene and ethanol conversion with an appropriate ratio of Ag and ZrO2. Each component was synthesized on separate support particles for detailed characterization.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2022)
Article
Engineering, Environmental
Cheng Liu, Iran Li, Linlin Wu, Zhongfeng Geng
Summary: The kinetics of 1,3-butadiene synthesis from ethanol and acetaldehyde over ZrO2-MgO-SiO2 catalyst were studied, showing that the aldol condensation step followed the Langmuir-Hinshelwood mechanism. The obtained kinetics models were verified under different conditions, suggesting their validity for practical applications.
CHEMICAL ENGINEERING JOURNAL
(2021)
Article
Chemistry, Physical
Fan Lin, Vanessa Lebarbier Dagle, Austin D. Winkelman, Mark Engelhard, Libor Kovarik, Yilin Wang, Yong Wang, Robert Dagle, Huamin Wang
Summary: Ag-ZrO2/SBA-16 has been found to efficiently catalyze the conversion of ethanol to butene, but it deactivates over time due to coke deposition, Ag particle sintering, and Ag oxidation state change.
Article
Chemistry, Physical
Austin D. Winkelman, Vanessa Lebarbier Dagle, Teresa L. Lemmon, Libor Kovarik, Yong Wang, Robert A. Dagle
Summary: This paper discusses the enhanced catalytic performance of a 4Ag/4ZrO(2)/SBA-16 catalyst for ethanol conversion to butadiene through the addition of Na and K. While there is a slight decrease in conversion, the productivity is significantly increased with up to 50% improvement when 0.5% Na is added. The addition of Na or K reduces activity involving ethanol dehydration and results in higher butadiene selectivity.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Environmental Sciences
Parisa Ghofrani-Isfahani, Panagiotis Tsapekos, Maria Peprah, Panagiotis Kougias, Athanasios Zervas, Xinyu Zhu, Ziyi Yang, Carsten S. Jacobsen, Irini Angelidaki
Summary: In this study, two thermophilic trickle bed reactors (TBRs) packed with different packing densities were evaluated for their performance in ex-situ biogas upgrading process. The results showed that densely packed polyurethane foam (PUF) enhanced H-2 utilization efficiency and methane content in the output gas. High-rate nutrient trickling, however, had negative effects on biomethanation efficiency.
Article
Engineering, Environmental
Busuyi O. Adebayo, Han Yu, Ali A. Rownaghi, Xinhua Liang, Fateme Rezaei
Summary: In this study, Pt nanoparticles were loaded on SiO2, TiO2-SiO2, or ZrO2-SiO2 particles to investigate their performance in sequential adsorption and desorption/catalytic oxidation of benzene. The results showed that Pt nanoparticles and ZrO2 exhibited synergistic effects in catalytic oxidation.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Nanoscience & Nanotechnology
Sabrine M. Cypher, Magnus Pauly, Leslie G. Castro, Carrie L. Donley, Paul A. Maggard, Karen I. Goldberg
Summary: This study used a molecular catalyst integrated into a carbon nitride support to upgrade ethanol to n-butanol, which is one of the first examples of a supported molecular catalyst performing the Guerbet process. Initial studies using PTI with lithium or transition-metal cations imbedded in the support did not produce significant amounts of n-butanol. However, 59% selectivity for butanol (13% yield) was obtained at 145°C when using PTI-LiCl treated with [(Cp*)IrCl2] along with sodium hydroxide.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
J. A. Andersen, J. M. Christensen, M. ostberg, A. Bogaerts, A. D. Jensen
Summary: This study investigated the plasma-catalytic ammonia decomposition for producing hydrogen using a packed-bed dielectric barrier discharge reactor. The introduction of dielectric materials with certain dielectric constants improved the ammonia decomposition, with MgAl2O4 showing the highest conversion rate. Further studies are needed to optimize the efficiency of this technology.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2022)
Article
Chemistry, Organic
Wei-Hsin Hsu, Susanne Reischauer, Peter H. Seeberger, Bartholomaus Pieber, Dario Cambie
Summary: Metallaphotoredox catalysis is a versatile synthetic platform that enables mild cross-couplings without the need for noble metals. In this study, a continuous-flow approach using a heterogeneous catalyst that combines both photo- and nickel-catalysts in one material is reported. The catalyst is embedded in a packed-bed reactor, simplifying the translation from batch to continuous flow reactions. The catalyst exhibited stability and effectiveness in the metallaphotoredox cross-coupling reactions.
BEILSTEIN JOURNAL OF ORGANIC CHEMISTRY
(2022)
Article
Chemistry, Physical
Jose Lucas Vieira, Priscila Destro, Leticia O. Laier, Clelia M. P. Marques, Jean Marcel R. Gallo, Jose Maria C. Bueno
Summary: MgO/SiO2 catalysts prepared with different compositions were found to have significant effects on the properties and ethanol conversion activity. Lower loading of MgO resulted in higher activity for ethanol dehydration to ethylene, while increasing MgO loading produced strong basic sites capable of increasing ethanol conversion to 1,3-butadiene.
MOLECULAR CATALYSIS
(2022)
Article
Chemistry, Multidisciplinary
Juan Gancedo, Laura Faba, Salvador Ordonez
Summary: This study demonstrates the feasibility of producing aromatics through gas-phase Diels-Alder condensation using biomass platform molecules, with comparable results to using chemicals or more complex preparation procedures. It emphasizes the advantage of using waste biomass as a raw material to produce industrial high-value products through a renewable route, resulting in a double benefit for the environment.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2022)
Article
Chemistry, Physical
Tingting Yan, Mengting Zhang, Runze Liu, Weili Dai, Naijia Guan, Landong Li
Summary: The selective conversion of the acetone-butanol-ethanol (ABE) mixture to high-valuable chemicals is still challenging. In this study, a bifunctional Ga/HZSM-5 zeolite catalyst containing both Bri nsted acid sites and Lewis acid sites was designed and used for the conversion of the ABE mixture to aromatics, achieving a state-of-the-art aromatics yield of 77%. The mechanisms of aromatics formation and catalyst deactivation were investigated, and a synergistic catalysis between Lewis acidic Ga species and Bri nsted acid sites was proposed.
Article
Chemistry, Applied
Zhinuo Wang, Ming Yin, Jifeng Pang, Xianquan Li, Yanan Xing, Yang Su, Shimin Liu, Xiaoyan Liu, Pengfei Wu, Mingyuan Zheng, Tao Zhang
Summary: In this study, Cu was selected to modify NiMgAlO catalysts for improving ethanol conversion and n-butanol selectivity. The optimized 2%Cu-NiMgAlO catalyst showed enhanced ethanol conversion and n-butanol selectivity in a 200-hour reaction time. The key role of multiple active sites in this reaction was extensively investigated.
JOURNAL OF ENERGY CHEMISTRY
(2022)
Article
Chemistry, Applied
Simuck F. Yuk, Mal-Soon Lee, Sneha A. Akhade, Manh-Thuong Nguyen, Vassiliki-Alexandra Glezakou, Roger Rousseau
Summary: Understanding the hydrogenation of organic compounds in the aqueous phase is crucial for carbon neutral pathways. This study investigated the thermodynamic and kinetic profiles of benzaldehyde hydrogenation over Pd(111) and Pt(111) metal surfaces. The presence of surface charge and solvent greatly influenced the reaction.
Article
Chemistry, Multidisciplinary
Loukas Kollias, Difan Zhang, Sarah I. Allec, Manh-Thuong Nguyen, Mal-Soon Lee, David C. Cantu, Roger Rousseau, Vassiliki-Alexandra Glezakou
Summary: Increasing atmospheric concentrations of greenhouse gases due to industrial activity have led to concerning levels of global warming. Reducing carbon dioxide (CO2) emissions is crucial in mitigating further warming, and CO2 capture solvent systems are currently the only technology capable of achieving this on an industrial scale. Designing these solvents for specific applications is a complex task that requires optimizing both thermodynamic and transport properties. Atomic scale modeling can be an effective tool in studying the energetics and transport properties of these chemically complex solvents.
Article
Chemistry, Physical
Carlos E. Garcia-Vargas, Gregory Collinge, Dongmin Yun, Mal-Soon Lee, Valery Muravev, Ya-Qiong Su, Xavier Isidro Pereira-Hernandez, Dong Jiang, Vassiliki-Alexandra Glezakou, Emiel J. M. Hensen, Roger Rousseau, Abhaya K. Datye, Yong Wang
Summary: The study demonstrates that single atom copper catalysts prepared by high-temperature synthesis on ceria can maintain both activity and stability under variable reaction conditions by allowing charge transfer between active site and support, with the ability to dynamically respond to changes in catalyst environment.
Article
Chemistry, Multidisciplinary
Sichi Li, Maira R. Ceron, Hannah Eshelman, Anthony J. Varni, Amitesh Maiti, Sneha Akhade, Simon H. Pang
Summary: We investigated the oxidative degradation mechanism of polyamines through quantum chemistry, simulations, adsorbent synthesis, and degradation experiments, highlighting the critical role of aminoalkyl hydroperoxide decomposition in the process. We explained the observed variation in oxidative stability of polyamines with different backbone structures by the relationship between local chemical structure and the free energy barrier of aminoalkyl hydroperoxide decomposition, providing a theoretical basis for screening and designing more stable polyamines.
Article
Chemistry, Multidisciplinary
Thomas Moore, Anthony J. Varni, Simon H. Pang, Sneha A. Akhade, Sichi Li, Du T. Nguyen, Joshuah K. Stolaroff
Summary: CO2-Binding organic liquids (CO(2)BOLs) are non-aqueous solvents that can reduce the energy consumption of carbon capture processes. These solvents exhibit surprising mass transfer behavior, with the flux of CO2 into CO(2)BOLs decreasing exponentially with increasing temperature. This phenomenon is primarily driven by a shift in reaction equilibrium, reducing the enhancement of CO2 flux by chemical reactions. First-principles surface renewal models accurately replicate the mass transfer data for CO2 absorption into different CO(2)BOLs, and density functional theory calculations identify structural modifications that could improve CO2 flux.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Chemistry, Physical
Henry Yu, Stephen E. Weitzner, Joel B. Varley, Brandon C. Wood, Sneha A. Akhade
Summary: The electrochemical reduction of CO2 with Cu based catalysts is closely related to the instantaneous local chemical environment of the catalyst-electrolyte interface. This microenvironment fluctuates depending on the concentration of surface-adsorbed competing reaction intermediates and the applied electrode potential. Quantifying the complex interdependence between electrode potential, CO* coverage, and the interfacial field strength, our study reveals the strong influence of CO* coverage on the field strength, suggesting its significance in determining the selectivity towards multicarbon products. Additionally, our results demonstrate the potential of surface additives to modulate interfacial fields for tailored electrochemical pathways.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Physics, Condensed Matter
Michael Gottschalk, Mal-Soon Lee, Eric Goodwin, Camille Mikolas, Thomas Chasapis, Duck Young Chung, Mercouri G. Kanatzidis, Subhendra D. Mahanti, Stuart Tessmer
Summary: Using scanning tunneling spectroscopy, the effects of nitrogen gas exposure on the electronic density of states of Bi2Se3 were investigated. Nitrogen gas molecules were observed to physisorb near Se vacancies, resulting in a saturation of the exposure effect after approximately 50 min. Density functional theory calculations and molecular dynamics simulations support the dissociative adsorption of N2 molecules and their strong binding to Se vacancies, which modifies the position of the Fermi energy relative to the Dirac point.
SOLID STATE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Austin D. Winkelman, Vanessa Lebarbier Dagle, Teresa L. Lemmon, Libor Kovarik, Yong Wang, Robert A. Dagle
Summary: This paper discusses the enhanced catalytic performance of a 4Ag/4ZrO(2)/SBA-16 catalyst for ethanol conversion to butadiene through the addition of Na and K. While there is a slight decrease in conversion, the productivity is significantly increased with up to 50% improvement when 0.5% Na is added. The addition of Na or K reduces activity involving ethanol dehydration and results in higher butadiene selectivity.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Physical
Runze Ma, Christopher R. O'Connor, Gregory Collinge, Sarah I. Allec, Mal-Soon Lee, Zdenek Dohnalek
Summary: The dynamics of acetic acid on anatase TiO2(101) were investigated using scanning tunneling microscopy experiments and density functional theory calculations. The study showed the simultaneous diffusion of bidentate acetate and a bridging hydroxyl, as well as the transient formation of molecular monodentate acetic acid. The diffusion rate was found to be strongly dependent on the position of hydroxyl and adjacent acetate(s). A three-step diffusion process involving acetate and hydroxyl recombination, acetic acid rotation, and acetic acid dissociation was proposed. This study provides insights into the importance of bidentate acetate dynamics in the formation of monodentate species, which drive selective ketonization.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Applied
Christopher R. O'Connor, Runze Ma, Gregory Collinge, Mal-Soon Lee, Greg A. Kimmel, Zdenek Dohnalek
Summary: In this study, the adsorption and reaction of acetic acid on anatase TiO2(101) were investigated using various techniques. It was found that acetic acid can form two intermediates: dissociated, bidentate acetate and molecular, monodentate acetic acid. The presence of both intermediates was observed at low temperatures, while only the bidentate acetate was observed at high temperatures. This research provides important insights into the stability and reactivity of carboxylic acid surface-bound intermediates, which play a role in biomass upgrading via ketonization reactions.
TOPICS IN CATALYSIS
(2023)
Article
Chemistry, Physical
Jinshu Tian, Gregory Collinge, Simuck F. F. Yuk, Jindong Lin, Vassiliki-Alexandra Glezakou, Mal-Soon Lee, Yong Wang, Roger Rousseau
Summary: Through density functional theory calculations, in situ Raman characterization, and microkinetic modeling, it is found that dimerized di-coordinated boron sites are the active species for O-2 activation and peroxy-like structures are responsible for propane activation. The formation of adsorbed C3H7* radicals was found to be the main rate-controlling step. These findings provide significant insights into the mechanisms of oxidative dehydrogenation of propane on boron-based catalysts.
Article
Chemistry, Physical
Vanessa Lebarbier Dagle, Gregory Collinge, Mohammed Rahmana, Austin Winkelman, Wenda Hu, Jian Zhi Hu, Libor Kovarik, Mark Engelhard, Jennifer Jocz, Yong Wang, Mal-Soon Lee, Vassiliki-Alexandra Glezakou, Debmalya Ray, Roger Rousseau, Robert Dagle
Summary: This study reports on a Cu/ZrO2/SBA-16 catalyst with remarkable olefins selectivity and enhanced stability compared to the Ag/ZrO2/SBA-16 catalyst. Replacing Ag with Cu shifts the reaction pathway of crotonaldehyde hydrogenation, leading to the formation of butyraldehyde. Experimental and computational tools were used to verify the performance and stability advantage of the Cu/ZrO2/SBA-16 catalyst.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Physical
Viswanath Pasumarthi, Henry Yu, Sneha A. Akhade, Frank Abild-Pedersen, Joel B. Varley, Michal Bajdich
Summary: Solvation models are important for understanding electrochemical reactions. This study developed a framework to evaluate the effects of potential and electrical double layer on CO reduction. Different solvation models were compared and good agreement was found for intermediate products. This framework can be used to predict optimal electrochemical conditions for specific applications.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Review
Energy & Fuels
Tolga Han Ulucan, Sneha A. Akhade, Ajith Ambalakatte, Tom Autrey, Alasdair Cairns, Ping Chen, Young Whan Cho, Fausto Gallucci, Wenbo Gao, Jakob B. Grinderslev, Katarzyna Grubel, Torben R. Jensen, Petra E. de Jongh, Jotheeswari Kothandaraman, Krystina E. Lamb, Young-Su Lee, Camel Makhloufi, Peter Ngene, Pierre Olivier, Colin J. Webb, Berenger Wegman, Brandon C. Wood, Claudia Weidenthaler
Summary: Efficient storage of hydrogen is a significant challenge for the potential hydrogen economy. Liquid carriers provide an attractive alternative to low-temperature compression or liquefaction, offering cost-effective storage and easy integration with existing infrastructure.
PROGRESS IN ENERGY
(2023)
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)
