Article
Chemistry, Physical
Florian Goltl, Saurabh Bhandari, Manos Mavrikakis
Summary: Transition-metal exchanged zeolites show high selectivity in converting methane to methanol through a stepwise process. A comprehensive theoretical study is conducted to identify thermodynamically preferred active sites in Cu-exchanged zeolite SSZ-13 during the conversion and develop a thermodynamic model for different active sites anchored in various structures supported by different local Al distributions. The results are compared with experimental measurements, showing agreement and providing insights for optimizing the conversion process.
Article
Nanoscience & Nanotechnology
Reza Pamungkas Putra Sukanli, Muhammad Haris Mahyuddin, Adhitya Gandaryus Saputro, Mohammad Kemal Agusta, Hadi Teguh Yudistira, Kazunari Yoshizawa, Hermawan Kresno Dipojono
Summary: In this paper, density functional theory calculations were performed to evaluate the oxidation of CH4 to CH3OH using O2 on graphitic MN4G-BN and CuN4G-PN systems. It was found that B doping adjacent to Fe and Co centers as well as P doping adjacent to Cu center facilitated the dissociation of O=O bond, resulting in active M-O and inactive B/P-O sites. Among them, CuN4G-PN was predicted to be a potential catalyst for the stepwise conversion of CH4 to CH3OH using O2 at low temperatures.
ACS APPLIED NANO MATERIALS
(2023)
Article
Chemistry, Physical
Mikalai A. Artsiusheuski, Rene Verel, Jeroen A. van Bokhoven, Vitaly L. Sushkevich
Summary: Using in situ MAS NMR spectroscopy, the pathways of methane and methanol transformation over copper-containing mordenite were elucidated. Direct coupling of methane is not possible below 773 K, while the transformation of methanol and its partial oxidation products occur via the methanol-to-hydrocarbons (MTH) process. The presence of carbon monoxide leads to the formation of surface acetate species from methanol through the Koch carbonylation reaction, affecting the nature of the hydrocarbon pool species and the formed hydrocarbons.
Article
Chemistry, Physical
Aditya Prajapati, Rohan Sartape, Nishithan C. Kani, Joseph A. Gauthier, Meenesh R. Singh
Summary: By synthesizing an interface consisting of Cu-Ti bimetallic oxides, we have achieved highly selective electrochemical methane oxidation at ambient conditions. This reaction converts methane into value-added products such as CH3OH and HCOOH.
Article
Chemistry, Multidisciplinary
Haihong Meng, Bing Han, Fengyu Li, Jingxiang Zhao, Zhongfang Chen
Summary: This study explores the potential of metal dimers embedded in phthalocyanine monolayers as catalysts for methane conversion and systematically investigates the mechanisms involved. The results show different catalytic effects of various metal dimers on methane conversion, providing insights for catalyst development and the application of metal dimers in other catalytic reactions.
Article
Chemistry, Physical
Erwei Huang, Ning Rui, Rina Rosales, Jindong Kang, Slavomir Nemsak, Sanjaya D. Senanayake, Jose A. Rodriguez, Ping Liu
Summary: This study reports an inverse catalyst for the direct conversion of methane to methanol, achieving high selectivity by adding water to further enhance methanol production. The catalyst suppresses the full combustion of methane to carbon dioxide while still allowing dissociative adsorption of water, enabling a truly selective methane to methanol conversion.
Review
Chemistry, Multidisciplinary
Nicholas F. Dummer, David J. Willock, Qian He, Mark J. Howard, Richard J. Lewis, Guodong Qi, Stuart H. Taylor, Jun Xu, Don Bethell, Christopher J. Kiely, Graham J. Hutchings
Summary: The direct transformation of methane to methanol at a larger scale remains challenging due to the low reactivity of methane. This review examines several promising routes to methanol and evaluates the performance targets necessary for process development. It provides critical perspectives on future operation and discusses the emergence of active heterogeneous catalysts and their reaction mechanisms.
Article
Chemistry, Physical
Yikun Kang, Zhi Li, Xintong Lv, Weiyu Song, Yuechang Wei, Xiao Zhang, Jian Liu, Zhen Zhao
Summary: This study systematically investigated the effects of active oxygen (O*) on electrochemical methane conversion on 66 two-dimensional carbides (MXenes) through large-scale computations. The results showed that materials satisfying the stability condition of O* in the OER activity volcano map have potential application in methane conversion. Additionally, it was found that the p-band center of O* serves as an effective descriptor for catalyst design in terms of stability and reactivity.
JOURNAL OF CATALYSIS
(2021)
Article
Chemistry, Multidisciplinary
Yuehan Cao, Wang Yu, Chunqiu Han, Yuantao Yang, Zhiqiang Rao, Rui Guo, Fan Dong, Ruiyang Zhang, Ying Zhou
Summary: Based on the concept of a hydrogen bonding trap, a novel concept is proposed to modulate the methane conversion pathway and hinder the overoxidation of target products. Boron nitride is used as a model, and it is found that the designed N-H bonds can work as a hydrogen bonding trap to attract electrons, suppressing the continuous dehydrogenation process and improving the selectivity to oxygenates.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Jeewan Pokhrel, Daniel F. Shantz
Summary: This study describes the use of copper-exchanged SSZ-39 catalyst for the direct conversion of methane to methanol, and demonstrates its promising catalytic performance. Testing in a continuous flow reactor at 225 degrees C shows that Cu-SSZ-39 exhibits higher activity for methane partial oxidation compared to Cu-SSZ-13. A clear maximum in methanol productivity is observed for Cu-SSZ-39 at a Cu/Al ratio of approximately 0.2. Unlike SSZ-13, the reactivity of catalysts with a Cu/Al > 0.1 is significantly lower in the absence of oxygen.
JOURNAL OF CATALYSIS
(2023)
Review
Chemistry, Physical
Haomin Jiang, Luting Zhang, Zhiwei Han, Yang Tang, Yanzhi Sun, Pingyu Wan, Yongmei Chen, Morris D. Argyle, Maohong Fan
Summary: The article discusses the significance of converting methane to methanol and the challenges involved, as well as advanced electrochemical methods for this conversion under mild conditions, focusing on using active oxygen species to improve the efficiency of CH4 to CH3OH conversion.
GREEN ENERGY & ENVIRONMENT
(2022)
Review
Chemistry, Physical
Haomin Jiang, Luting Zhang, Zhiwei Han, Yang Tang, Yanzhi Sun, Pingyu Wan, Yongmei Chen, Morris D. Argyle, Maohong Fan
Summary: Developing a convenient method for direct conversion of methane to methanol is crucial for utilizing methane-rich resources. In the field of electrochemistry, researchers are exploring mild conversion pathways by activating methane with suitable catalysts and generating active oxygen species to efficiently convert methane to methanol without over-oxidation.
GREEN ENERGY & ENVIRONMENT
(2022)
Article
Chemistry, Physical
Tao Yu, Zhi Li, Lu Lin, Shengqi Chu, Yang Su, Weiyu Song, Aiqin Wang, Bert M. Weckhuysen, Wenhao Luo
Summary: The study demonstrates that the Cu-modified Fe/ZSM-5 catalyst is highly efficient for the direct conversion of methane into methanol in the liquid phase using H2O2 as an oxidant. Cu species in the catalyst play a crucial role in facilitating the formation of .OH radicals, which react quickly with .CH3 radicals to form methanol. This provides valuable insights into the rational design of metal-zeolite combinations for the selective oxidation of methane into methanol.
Article
Materials Science, Multidisciplinary
Lei Zhou, Ya-Qiong Su, Tong-Liang Hu
Summary: Twelve single-atom alloys (SAAs) were designed for the activation of methane, and the ones with superior catalytic activity were investigated for the selective oxidation of methane to methanol. The doping of Ir metal-atom into inert coinage hosts (Ag, Au, and Cu) enhanced the methane dissociation activity due to the interaction between the C-H bond and the unique projected d-band density of states of the Ir atom. The study provides important guidelines for designing active and efficient catalysts for direct methane conversion.
SCIENCE CHINA-MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Baiyang Yu, Lu Cheng, Sheng Dai, Yongjun Jiang, Bing Yang, Hong Li, Yi Zhao, Jing Xu, Ying Zhang, Chengsi Pan, Xiao-Ming Cao, Yongfa Zhu, Yang Lou
Summary: This study designs and constructs ZSM-5 supported Cu and Ag dual single atoms as a proof-of-concept catalyst to enhance the direct oxidation of methane. The synthesized Ag-1-Cu-1/ZSM-5 hetero-SAC exhibits high methanol productivity and selectivity, surpassing most noble metal catalysts. The synergistic interaction between silver and copper facilitates the formation of reactive surface hydroxyl species, activating the C-H bond and enhancing the catalytic performance of DOM compared to SACs.
Article
Chemistry, Physical
Naveen Dandu, Logan Ward, Rajeev S. Assary, Paul C. Redfern, Badri Narayanan, Ian T. Foster, Larry A. Curtiss
JOURNAL OF PHYSICAL CHEMISTRY A
(2020)
Article
Chemistry, Physical
Chengji Zhang, Naveen Dandu, Sina Rastegar, Saurabh N. Misal, Zahra Hemmat, Anh T. Ngo, Larry A. Curtiss, Amin Salehi-Khojin
ADVANCED ENERGY MATERIALS
(2020)
Article
Nanoscience & Nanotechnology
Sina Rastegar, Zahra Hemmat, Chengji Zhang, Samuel Plunkett, Jianguo Wen, Naveen Dandu, Tomas Rojas, Leily Majidi, Saurabh N. Misal, Anh T. Ngo, Larry A. Curtiss, Amin Salehi-Khojin
Summary: This study explores a novel synergy among InX3 bifunctional RMs, MoS2 nanoflakes, hybrid electrolyte, and LiTFSI salt to achieve long cycle-life operations of Li-O-2 batteries in a dry air environment at high charge-discharge rates. Experimental results demonstrate that batteries with InI3 or InBr3 as RMs exhibit significantly improved cycle life and current rates in a dry air atmosphere.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Physical
Levi Lystrom, Alyssa Roberts, Naveen Dandu, Svetlana Kilina
Summary: Thiol-based ligand-passivated cadmium chalcogenide quantum dots have various advantages in applications but their emission is sensitive to thiol concentrations, pH conditions, and temperatures. Thiolates can reduce the optical intensity of low-energy transitions in CdS QDs, but networking with the surface stabilizes trap states and brightens the lowest optical transitions.
CHEMISTRY OF MATERIALS
(2021)
Article
Chemistry, Physical
Jianzhong Yang, Qian Liu, Krzysztof Z. Pupek, Trevor L. Dzwiniel, Nancy L. Dietz Rago, Jiayu Cao, Naveen Dandu, Larry Curtiss, Kewei Liu, Chen Liao, Zhengcheng Zhang
Summary: The molecular engineering of electrolyte structures has led to the successful application of trifluoropropylene carbonate (TFPC) in high-voltage high-energy lithium-ion cells, demonstrating improved compatibility with graphite anodes and exceptional oxidation stability. The all-fluorinated electrolyte formulation showed excellent cycling stability in a high-voltage LiNi0.5Mn0.3Co0.2O2/graphite cell, indicating potential for next-generation battery technology.
ACS ENERGY LETTERS
(2021)
Article
Chemistry, Physical
Logan Ward, Naveen Dandu, Ben Blaiszik, Badri Narayanan, Rajeev S. Assary, Paul C. Redfern, Ian Foster, Larry A. Curtiss
Summary: This article introduces a method of using machine learning models to evaluate the solvation properties of molecules as a substitute for expensive quantum chemical calculations. Their trained models have high accuracy and provide convenient interfaces for others to easily run the model.
JOURNAL OF PHYSICAL CHEMISTRY A
(2021)
Article
Chemistry, Multidisciplinary
Aditya Prajapati, Rohan Sartape, Tomas Rojas, Naveen K. Dandu, Pratik Dhakal, Amey S. Thorat, Jiahan Xie, Ivan Bessa, Miguel T. Galante, Marcio H. S. Andrade, Robert T. Somich, Marcio Reboucas, Gus T. Hutras, Nathalia Diniz, Anh T. Ngo, Jindal Shah, Meenesh R. Singh
Summary: Current industrially relevant CO2 capture technologies are costly and energy-intensive, making them inefficient and unsustainable for long-term use. Researchers have developed a water-dependent CO2 capture system, utilizing the equilibrium between CO2 and carbonate and bicarbonate ions. By establishing a water gradient across a membrane, they achieved a high-efficiency CO2 capture process.
ENERGY & ENVIRONMENTAL SCIENCE
(2022)
Article
Chemistry, Physical
Nathan T. Hahn, Julian Self, Darren M. Driscoll, Naveen Dandu, Kee Sung Han, Vijayakumar Murugesan, Karl T. Mueller, Larry A. Curtiss, Mahalingam Balasubramanian, Kristin A. Persson, Kevin R. Zavadil
Summary: The study investigates the impact of ion interactions on solvation environments, revealing that salt dissociation is lower at lower concentrations. The transition in ion correlation in magnesium and calcium ion salts across different concentrations highlights the importance of controlling ion interactions in ether-based multivalent battery electrolytes.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Multidisciplinary
Zahra Hemmat, Alireza Ahmadiparidari, Shuxi Wang, Khagesh Kumar, Michael Zepeda, Chengji Zhang, Naveen Dandu, Sina Rastegar, Leily Majidi, Ahmad Jaradat, Anh Ngo, Katsuyo Thornton, Larry A. Curtiss, Jordi Cabana, Zhehao Huang, Amin Salehi-Khojin
Summary: This article introduces a solid solution transition metal trichalcogenide nanofiber material with outstanding electrical, thermal, and electrochemical characteristics. It demonstrates excellent performance in various applications, including CO2 conversion and high-rate Li-air batteries, showing its potential in these fields.
ADVANCED FUNCTIONAL MATERIALS
(2022)
Article
Chemistry, Physical
Naveen K. Dandu, Rajeev S. Assary, Paul C. Redfern, Logan Ward, Ian Foster, Larry A. Curtiss
Summary: G4MP2 theory has higher errors when applied to larger organic molecules, which is due to the higher-level correction not taking into account the element and bond type dependence. By introducing an atom-specific correction, G4MP2A method shows comparable accuracy to G4 theory with lower computational cost. The G4MP2A method also improves ionization potentials and electron affinities, and can be used in machine learning methods for predicting molecular energies.
JOURNAL OF PHYSICAL CHEMISTRY A
(2022)
Article
Multidisciplinary Sciences
Tolulope Michael Ajayi, Vijay Singh, Kyaw Zin Latt, Sanjoy Sarkar, Xinyue Cheng, Sineth Premarathna, Naveen K. Dandu, Shaoze Wang, Fahimeh Movahedifar, Sarah Wieghold, Nozomi Shirato, Volker Rose, Larry A. Curtiss, Anh T. Ngo, Eric Masson, Saw Wai Hla
Summary: Rare-earth complexes were formed and atomically controlled on a gold surface, allowing for precise manipulation of their rotational dynamics. This work opens up new possibilities for quantum and nanomechanical applications.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Sina Rastegar, Alireza Ahmadiparidari, Sachin Kumar Singh, Chengji Zhang, Zahra Hemmat, Naveen Dandu, Michael J. Counihan, Maryam Bagheri, Tomas Rojas, Leily Majidi, Shuxi Wang, Ahmad Jaradat, Rajeev S. Assary, Paul C. Redfern, Parisa Mirbood, Sanja Tepavcevic, Arunkumar Subramanian, Anh T. Ngo, Larry A. Curtiss, Amin Salehi-Khojin
Summary: In this study, a colloidal electrolyte made of MnO2 nanoparticles generated by KMnO4 was used to improve the performance of Li-O2 batteries. By using this electrolyte in combination with a stable binary transition metal dichalcogenide alloy as the cathode, the cycle life of the battery was increased, and it was able to operate at high current density and specific capacity in a dry air environment.
Article
Chemistry, Physical
Jijian Xu, Travis P. Pollard, Chongyin Yang, Naveen K. Dandu, Sha Tan, Jigang Zhou, Jian Wang, Xinzi He, Xiyue Zhang, Ai-Min Li, Enyuan Hu, Xiao-Qing Yang, Anh Ngo, Oleg Borodin, Chunsheng Wang
Summary: Liquefying halogen or inter-halogen compounds is crucial for achieving high reversibility in lithium halide cathodes. This can be done using interhalogen compounds with different electronegativity or by lowering the temperature. By demonstrating reversible LiCl conversion-intercalation chemistry in organic electrolytes, high reversible specific capacity is achieved in LiCl-LiBr-graphite cathodes at a lower cost than transition metal oxide cathodes.
Article
Chemistry, Physical
Naveen K. Dandu, Logan Ward, Rajeev S. Assary, Paul C. Redfern, Larry A. Curtiss
Summary: In previous research, accurate atomization energies of organic molecules were successfully predicted using machine learning models with an accuracy as low as 0.1 kcal/mol compared to the G4MP2 method. In this study, these machine learning models were extended for the prediction of adiabatic ionization potentials using data sets generated from quantum chemical calculations. Atomic specific corrections used to improve atomization energies were also implemented to enhance ionization potentials. The results demonstrate the successful use of machine learning assisted by quantum chemical calculations for predicting ionization potentials of organic molecules, which can be utilized in high throughput screening.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Proceedings Paper
Computer Science, Artificial Intelligence
Logan Ward, Ganesh Sivaraman, J. Gregory Pauloski, Yadu Babuji, Ryan Chard, Naveen Dandu, Paul C. Redfern, Rajeev S. Assary, Kyle Chard, Larry A. Curtiss, Rajeev Thakur, Ian Foster
Summary: Colmena is an open-source Python framework that accelerates scientific applications involving simulation ensembles. By providing individual task implementations and logic to guide activities, it can greatly improve the discovery rate of high-performance molecules.
PROCEEDINGS OF THE WORKSHOP ON MACHINE LEARNING IN HIGH PERFORMANCE COMPUTING ENVIRONMENTS (MLHPC 2021)
(2021)