Article
Chemistry, Multidisciplinary
Dong Gun Oh, Jaekyoung Lee, Eunseok Kim, Eun Jeong Jang, Ji Man Kim, Ja Hun Kwak
Summary: The study shows that Pd/SiO2 can be an active and durable catalyst for CH4 oxidation with higher activity than Pd/Al2O3 through simple reductive regeneration. It suggests that the deactivation of Pd/SiO2 mainly comes from the blockage of the Pd/PdO surface by the SiO2 overlayer formed during hydrothermal aging.
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
(2021)
Article
Chemistry, Physical
Gianni Caravaggio, Lioudmila Nossova, Matthew Turnbull
Summary: A series of methane oxidation catalysts were prepared by doping SBA-15 with different amounts of zirconia and loading with Pd and Pt. The catalysts were characterized and evaluated for methane oxidation, with the catalyst containing 15 wt% zirconia showing the best performance. The improved performance was attributed to the higher amount of reducible PtOx species near ZrO2 and the sulfur scavenging effect of zirconia.
Article
Engineering, Marine
Kati Lehtoranta, Paivi Koponen, Hannu Vesala, Kauko Kallinen, Teuvo Maunula
Summary: The study shows that using methane oxidation catalyst (MOC) can effectively reduce methane slip emissions in LNG ships. The use of a special sulfur trap can protect MOC against sulfur poisoning to some extent, and regeneration done once a day can recover the efficiency of MOC.
JOURNAL OF MARINE SCIENCE AND ENGINEERING
(2021)
Article
Environmental Sciences
Xiaochi Zhou, Seungju Yoon, Steve Mara, Matthias Falk, Toshihiro Kuwayama, Travis Tran, Lucy Cheadle, Jim Nyarady, Bart Croes, Elizabeth Scheehle, Jorn D. Herner, Abhilash Vijayan
Summary: This study focused on measuring methane emissions from non-associated natural gas well pads in California, finding that a small number of active well pads were responsible for the majority of emissions. The study also detected methane emissions from idle well pads with smaller magnitudes, suggesting the importance of identifying and fixing leaks to reduce emissions. Mobile measurement techniques proved to be effective in detecting emissions from more well pads compared to optical gas imaging cameras, indicating their potential in supporting leak detection and repair programs.
ATMOSPHERIC ENVIRONMENT
(2021)
Article
Chemistry, Multidisciplinary
Yongde Ma, Shusheng Li, Tianhua Zhang, Yangyu Zhang, Xiuyun Wang, Yihong Xiao, Yingying Zhan, Lilong Jiang
Summary: The study introduces a Pd(PdO)/Co3O4@SiO2 bimetallic oxide core-shell catalyst with improved catalytic activity in methane combustion, attributed to the enhanced metal interaction between Pd and Co in the core-shell structure. The weakening of the Co-O bond in the catalyst promotes the release of lattice oxygen species to enhance the catalytic performance at low temperatures.
Article
Chemistry, Physical
Sungyoon Jung, Nathan Reed, Gregory Yablonsky, Pratim Biswas
Summary: The study found that Pd loading impacts the size and chemical form of Pd particles, with Pd on the catalyst surface increasing in size due to sintering and PdO being reduced to metallic Pd and PdOx. The proportion of metallic Pd and/or reduced Pd oxide on the total surface area correlates linearly with the apparent reaction rate constants.
CATALYSIS SCIENCE & TECHNOLOGY
(2021)
Article
Nanoscience & Nanotechnology
Shi Tu, Liang Yu, Danxia Lin, Yongwei Chen, Ying Wu, Xin Zhou, Zhong Li, Qibin Xia
Summary: Developing energy-efficient alternatives for methane purification and capture is significant and challenging. A nickel-based metal-organic framework with abundant adsorption sites shows excellent separation performance.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Physical
Maila Danielis, Luis E. Betancourt, Ivan Orozco, Nuria J. Divins, Jordi Llorca, Jose A. Rodriguez, Sanjaya D. Senanayake, Sara Colussi, Alessandro Trovarelli
Summary: The milling of Palladium acetate and CeO2 under dry conditions results in robust and environmentally friendly catalysts with excellent methane oxidation activity. The characterization techniques used in this study identified the presence of Pd-0/Pd2+ species with different degrees of interaction with ceria (Ce3+/Ce4+), which are believed to be responsible for the enhanced catalytic activity. This study provides insight into the mechanistic understanding of the catalytic performance of Pd/CeO2 catalysts prepared by dry milling.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2021)
Article
Environmental Sciences
Sebastian Iwaszenko, Piotr Kalisz, Marcin Slota, Andrzej Rudzki
Summary: This study tested the use of a UAV equipped with a remote sensing methane detector for detecting natural gas leaks in pipeline networks. Machine learning methods were used to analyze the collected data to identify spatially correlated regions with increased methane concentrations.
Article
Engineering, Environmental
Junchen Du, Miaoxin Guo, Aimin Zhang, Han Zhao, Depeng Zhao, Chengxiong Wang, Tingting Zheng, Yunkun Zhao, Yongming Luo
Summary: The study demonstrates that Pd/Ba-Al2O3 catalysts with Ba addition exhibit superior performance in wet methane oxidation, attributed to their favorable location and enhanced O-2 activation capability.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Chemistry, Analytical
Fu Wan, Weiping Kong, Qiang Liu, Pinyi Wang, Mingyong Wang, Qiuchi Li, Xinrong Yao, Weigen Chen
Summary: C2H2 and H-2, as important chemical and energy raw materials, can be produced effectively and environmentally friendly by the partial oxidation (POX) of CH4. We propose a fluorescence noise eliminating fiber-enhanced Raman spectroscopy (FNEFERS) technique to simultaneously analyze the intermediate gas compositions in the multiprocess of POX. This study demonstrates the ability of FNEFERS to replace gas chromatography for simultaneous and multiprocess analysis of intermediate compositions and monitor other chemical and energy production processes.
ANALYTICAL CHEMISTRY
(2023)
Article
Chemistry, Physical
Hao Wang, Jingxian Wu, Zhihuang Xiao, Zhejie Ma, Ping Li, Xinwei Zhang, Hongying Li, Xiangchen Fang
Summary: The study investigated the effects of sulfidation factors on the structure and performance of Mo-based catalysts, finding that the optimal sulfidation conditions were around 500 degrees C for 1 hour, with two simultaneous MoS2 formation routes identified during the process. A relationship between catalyst structure and catalytic performance was established, suggesting that edge Mo atoms cooperate with neighboring surface Mo sites to catalyze the reaction.
CATALYSIS SCIENCE & TECHNOLOGY
(2021)
Article
Chemistry, Physical
Andoni Choya, Sylwia Gudyka, Beatriz de Rivas, Jose Ignacio Gutierrez-Ortiz, Andrzej Kotarba, Ruben Lopez-Fonseca
Summary: This study focused on the optimisation of Ce-promoted Co3O4 catalysts for the oxidation of traces amounts of methane. Lattice distortion caused by controlled amounts of Ce insertion increased the abundance of Co3+ and improved the redox properties and mobility of lattice oxygen species in the Co-Ce catalysts. The optimal catalyst formulation was found to be 10%Co3O4wt. with a Ce/Co molar ratio of 0.05, showing reasonable stability under cycled dry/humid conditions.
APPLIED CATALYSIS A-GENERAL
(2021)
Article
Energy & Fuels
Yinbo Zhou, Ruilin Zhang, Kunyun Tian, Shuang Zhao, Hanfeng Shi, Weidong Gong, Qing Lei
Summary: During coal mining, a significant amount of methane is released into the atmosphere annually, intensifying the greenhouse effect. Microbial methane oxidation technology offers a novel approach for reducing methane emissions and controlling methane in coal mines. Mixed methanotrophic consortia were selected from the natural environment to enhance the adaptability of microorganisms. These consortia exhibited robust growth during the 4th-10th days, peaking on the 7th day. The microbial metabolism increased the solution's pH and decreased the oxidation-reduction potential (ORP), showing a negative correlation between the two. The selected consortia displayed exceptional methane-oxidizing ability, leading to a 71.19% decrease in methane gas volume. Notably, the microorganisms maintained methane oxidation capacity even after the device's oxygen was depleted. The results demonstrated that the mixed methanotrophic consortia adjusted their population structure to adapt to environmental changes and continued exhibiting methane oxidation ability. The contact angle between the bacterial solution and coal sample surface was significantly lower than that of pure water and culture medium. Microorganisms adsorbed onto the coal sample's surface through self-movement, substantially improving the contact ability. Retention of microorganisms in the coal sample was influenced by flow velocity and particle size. Low flow velocity and a large contact area enhanced the contact efficiency of microorganisms on the coal surface. Mixed methanotrophic consortia offer high application value and feasibility for reducing methane emissions in coal mining and treating underground methane.
Article
Chemistry, Physical
Nathan Coutard, Charles B. Musgrave, Jisue Moon, Nichole S. Liebov, Robert M. Nielsen, Jonathan M. Goldberg, Meijun Li, Xiaofan Jia, Sungsik Lee, Diane A. Dickie, William L. Schinski, Zili Wu, John T. Groves, William A. Goddard, T. Brent Gunnoe
Summary: The catalytic partial oxidation of methane at low temperatures using manganese oxides and salts in organic mixtures has been studied. The mechanism involving soluble and molecular Mn species in the catalytic cycle has been proposed based on experimental studies and DFT calculations. This process has potential for the oxidation of other hydrocarbons such as ethane.
Article
Chemistry, Multidisciplinary
Yiqing Wu, Yue Ma, Yilin Wang, Kenneth G. Rappe, Nancy M. Washton, Yong Wang, Eric D. Walter, Feng Gao
Summary: This study investigates the key factors controlling the low-temperature NH3-SCR reaction using Cu/SSZ-13 catalysts. The kinetics of Cu loading and the dynamics of Cu ions are found to strongly affect the SCR reaction. Operando EPR spectroscopy reveals a strong correlation between Cu-ion dynamics and SCR kinetics.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Multidisciplinary Sciences
Mingwu Tan, Yanling Yang, Ying Yang, Jiali Chen, Zhaoxia Zhang, Gang Fu, Jingdong Lin, Shaolong Wan, Shuai Wang, Yong Wang
Summary: The migration of hydrogen atoms from metal particles to a nonreducible oxide support is limited by thermodynamics, but this process can be promoted by small oxygenate molecules, leading to improved hydrodeoxygenation rates. This finding offers a molecule-assisted approach to the design and optimization of multifunctional heterogeneous catalysts on non-reducible oxides.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Jianghao Zhang, Junrui Li, Berlin Sudduth, Junming Sun, Changbin Zhang, Hong He, Yong Wang
Summary: A Cs-G@CoFe catalyst with a bimetallic alloy core and graphene overlayers doped with Cs was developed for highly selective hydrodeoxygenation (HDO) of phenolics under liquid-phase conditions. The bimetallic catalyst showed significantly enhanced activity (>threefold) compared with the monometallic Fe-based catalyst. The structure of the CoFe alloy core wrapped by several graphene overlayers in the Cs-G@CoFe catalyst contributes to the selective C-O bond cleavage.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2022)
Article
Chemistry, Physical
Carlos E. Garcia-Vargas, Xavier Isidro Pereira-Hernandez, Dong Jiang, Ryan Alcala, Andrew T. DeLaRiva, Abhaya Datye, Yong Wang
Summary: We have successfully prepared a single atom Rh-1/CeO2 catalyst through the high temperature (800 degrees C) atom trapping (AT) method, which shows excellent stability under oxidative and reductive conditions. The presence of exclusively ionic Rh species was confirmed by infrared spectroscopy and electron microscopy characterization. The strong interaction between Rh and CeO2 achieved by the AT method ensures the stability of the ionic Rh species even under reducing conditions, resulting in high and reproducible CO oxidation activity. This is in contrast to catalysts synthesized by conventional impregnation approaches, where the ionic Rh species can be easily reduced to form Rh nanoclusters/nanoparticles and subsequently oxidized, leading to performance degradation.
Article
Chemistry, Multidisciplinary
Fan Lin, Wenda Hu, Nicholas R. Jaegers, Feng Gao, Jian Zhi Hu, Huamin Wang, Yong Wang
Summary: The effects of water on the carboxylic acid ketonization reaction over solid Lewis-acid catalysts were investigated using various analytical techniques. The presence of water vapor in the feed gas was found to decrease the reaction rate by increasing the activation barrier of acetic acid adsorption on anatase TiO2 catalyst. Water was found to associate with the adsorbed intermediates on the catalyst surface and alter their reactivity for the ketonization reaction. The presence of water vapor also affected the species present on the catalyst surface and led to lower ketonization activity.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Applied
Konstantin Khivantsev, Miroslaw A. Derewinski, Janos Szanyi
Summary: This review surveys the efforts to form and characterize cationic species in different zeolites, including both metal and non-metal cations, with an emphasis on their novel properties and reactivity. The authors describe how synthesis of such species was achieved by considering both cation identity and zeolite architecture, and synthesis methods. Well-defined cationic species were successfully obtained through careful choice of metal incorporation methods, Al distribution tuning, and synthesis parameters. Discoveries of previously unknown phenomena in zeolite and cation-zeolite chemistry using these well-defined systems are discussed in this review article. The methodology to enhance the stability of cations in zeolite for adsorption and catalytic applications, as well as the usefulness of these materials in elucidating unknown catalytic intermediates and mechanisms, is also examined.
MICROPOROUS AND MESOPOROUS MATERIALS
(2023)
Article
Chemistry, Physical
Nicholas C. Nelson, Tahrizi Andana, Kenneth G. Rappe, Yong Wang
Summary: The combination of metal oxide and zeolite phase in hybrid materials can promote low-temperature activity. The mixed oxide phase provides access to surface fast selective catalytic reduction (SCR) reaction channels via SCR generation of adsorbed nitrogen dioxide and its derivatives. The reaction of adsorbed nitrogen dioxide (derivatives) with ammonia to form ammonium nitrate is unfavorable at low temperatures, indicating that the fast SCR pathways on the oxide phase remain accessible and not blocked by ammonium nitrate deposits as they are on the pure zeolite component, which may contribute to the observed low-temperature SCR promotion. These results advance the understanding of hybrid SCR catalysts and have potential for further technological development in this area.
CATALYSIS SCIENCE & TECHNOLOGY
(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, Multidisciplinary
Konstantin Khivantsev, Nicholas R. Jaegers, Hristiyan A. Aleksandrov, Inhak Song, Xavier Isidro Pereira-Hernandez, Mark H. Engelhard, Jinshu Tian, Linxiao Chen, Debora Motta Meira, Libor Kovarik, Georgi N. Vayssilov, Yong Wang, Janos Szanyi
Summary: Atom trapping leads to catalysts with atomically dispersed Ru1O5 sites on (100) facets of ceria, showing excellent activity in catalytic NO oxidation and high NOx storage properties. The Ru1O5 sites exhibit higher stability during calcination and the Ru1/CeO2 catalyst is stable during continuous cycling and in the presence of moisture. In addition, the catalyst shows excellent reactivity for NO reduction by CO at low temperatures. This study highlights the applicability of novel ceria-based single-atom catalysts in NO and CO abatement.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(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
Engineering, Environmental
Jinshu Tian, Jian Guan, Mingliang Xu, Shuya Qian, Kai Ma, Shaolong Wan, Zhaoxia Zhang, Haifeng Xiong, Shuai Wang, Yong Wang, Jingdong Lin
Summary: In this study, an efficient method for stabilizing hexagonal boron nitride (h-BN) with high specific surface area (SSA) under harsh conditions was proposed. The vacancy defects in h-BN were repaired with metal ions to significantly improve the antioxidant stability of the material. The repaired h-BN maintained a few-layer structure and exhibited high SSA and strong oxidation resistance, making it an excellent platform for fundamental studies and applications.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Engineering, Chemical
Gengrui Zhang, Yan Li, Yong Chen, Xinning Hao, Xianhua Zhang, Shuai Wang, Jingdong Lin, Yong Wang, Shaolong Wan
Summary: The study designs and prepares a nickel-based syngas methanation catalyst with superior thermal stability, using a special ZnAl2O4 spinel support. The catalyst shows excellent reactivity and stability. The work elucidates the critical role and intrinsic mechanism of the spinel support for the construction of the desired methanation catalysts.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2023)
Article
Multidisciplinary Sciences
Rui Zhang, Yong Wang, Pierre Gaspard, Norbert Kruse
Summary: In this study, the mechanistic steps underlying the formation of higher hydrocarbons in CO hydrogenation using cobalt-based catalysts at atmospheric pressure were investigated. The research revealed nonisothermal rate and selectivity oscillations that were sustained for extended periods of time. Experimental and theoretical analyses showed that temperature oscillations played a crucial role in the rate and selectivity oscillations, and the thermokinetic origin of these oscillations was supported by phase portraits.
Article
Chemistry, Physical
Dong Jiang, Gang Wan, Joakim Halldin Stenlid, Carlos E. Garcia-Vargas, Jianghao Zhang, Chengjun Sun, Junrui Li, Frank Abild-Pedersen, Christopher J. Tassone, Yong Wang
Summary: The active structures of Pd on CeO2 can be reversibly adjusted in response to different reaction environments, leading to efficient methane removal. During the cold start of vehicles, Pd-1 single atoms are transformed into PdOx subnanometre clusters, enhancing low-temperature CH4 oxidation. At elevated temperatures, the dispersion of PdOx cluster into Pd-1 prevents metal sintering and provides excellent hydrothermal stability to the catalyst. This reversible modulation of supported metals overcomes the trade-off between low-temperature activity and high-temperature stability.
Article
Chemistry, Multidisciplinary
Ryan P. Loughran, Tara Hurley, Andrzej Gladysiak, Arunraj Chidambaram, Konstantin Khivantsev, Eric D. Walter, Trent R. Graham, Patrick Reardon, Janos Szanyi, Dylan B. Fast, Quin R. S. Miller, Ah-Hyung Alissa Park, Kyriakos C. Stylianou
Summary: We investigate the use of MIL-120, a water-stable and cost-effective metal-organic framework (MOF), for selectively capturing CO2 from wet flue gas. MIL-120, synthesized using inexpensive and environmentally benign reagents in water, has one-dimensional pores with hydroxyl-bridged Al(III) ions and benzene rings, and demonstrates high potential for CO2 capture. Breakthrough experiments show that MIL-120 can effectively capture CO2 from both dry and wet flue gas.
CELL REPORTS PHYSICAL SCIENCE
(2023)