Article
Chemistry, Multidisciplinary
Thomas Len, Mounib Bahri, Ovidiu Ersen, Yaya Lefkir, Luis Cardenas, Ignacio J. Villar-Garcia, Virginia Perez Dieste, Jordi Llorca, Noemie Perret, Ruben Checa, Eric Puzenat, Pavel Afanasiev, Franck Morfin, Laurent Piccolo
Summary: In Mo/TiO2 catalysts, the interaction between ultradispersed molybdate species and the support structure of rutile titanium nanorods plays a crucial role in achieving high activity and selectivity for methanol production.
Article
Engineering, Environmental
Jiahui Chen, Munir Ahmad, Yan Zhang, Huangqing Ye, Lei Wang, Jiujun Zhang, Xian-Zhu Fu, Jing-Li Luo
Summary: Developing high-performance electrocatalysts is crucial for efficient methanol electro-reforming. In this study, a NiCoMo alloy pre-catalyst with nanosheets covered nanowires arrays is proposed, which undergoes surface reconstruction and forms a Mo substituted NiCoOOH layer as the real catalyst. The surface engineered catalysts exhibit high activity and stability, achieving efficient co-production of hydrogen and formate. The incorporation of Mo plays multiple roles in stabilizing the structure, promoting surface reconstruction, modulating electronic structure, and boosting catalytic activity.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Electrochemistry
O. Ugalde-Reyes, H. B. Liu, P. Roquero, J. Alvarez-Ramirez, E. Sosa-Hernandez
Summary: In this study, Pt/C and PtMo/C catalysts were synthesized and their behavior in the methanol oxidation reaction was analyzed using Electrochemical Impedance Spectroscopy (EIS) and Distribution of Relaxation Times analysis (DRT). The results revealed a CO poisoning effect on the catalyst surfaces, leading to further optimization of the circuit model to better explain the various mechanisms involved in the reaction.
ELECTROCHIMICA ACTA
(2022)
Article
Chemistry, Applied
Chunyu Hao, Jie Gan, Yueqiang Cao, Wei Luo, Wenyao Chen, Gang Qian, Xinggui Zhou, Xuezhi Duan
Summary: By tailoring the surface properties of carbon nanotubes, this study achieved size-dependent methanol oxidation reaction activity in the preparation of Pt catalysts, with the 1.9 nm Pt catalyst on CNT-600-O support showing the highest peak current density. Insights into Pt size effects and active sites could guide the fabrication of highly efficient Pt-based MOR catalysts.
Article
Chemistry, Physical
Jaehyun Lee, Jiwoo Yang, Jun Hyuk Moon
Summary: The study demonstrated the efficient conversion of CH4 to CH3OH at room temperature using CuO/CeO2 catalyst in the presence of CO32-, with the optimal Cu:Ce ratio being 6:4. Isotope experiments confirmed that active oxygen provided by CO32- on the catalyst surface can activate CH4 to form CH3OH.
ACS ENERGY LETTERS
(2021)
Article
Electrochemistry
Zhijie Pan, Pengwei Huang, Yuanming Zhang, Xionghui Fu, Yi Zhu
Summary: Photoelectrocatalytic methanol oxidation to formaldehyde using electric/solar energy is a promising technology. In this study, Ag nanoparticles were decorated on Mo-doped BiVO4 to synthesize Ag/Mo: BiVO4 catalyst. As expected, the formaldehyde production of Ag/Mo: BiVO4 photoanode was 2.2 times higher than pristine BiVO4 photoanode, benefiting from the Mo-dopant and plasmonic effect of Ag nanoparticles. The Faradaic efficiency increased from 19% to 49% compared to the pure BiVO4 photoanode.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2022)
Article
Chemistry, Physical
Meng Yuan, Ruiyuan Tang, Xiangyu Sun, Zhimei Zhang, Yuanyu Tian, Yingyun Qiao
Summary: The newly designed Fe-Mo-based catalyst Mo:Fe(2)/HZSM-5(80 + 80) showed excellent catalytic performance in the one-step production of methylal from methanol, with a methylal yield reaching 81.33% and high selectivity for the target product.
SUSTAINABLE ENERGY & FUELS
(2021)
Article
Chemistry, Physical
Weiqiao Huang, Changgeng Wei, Yi Li, Yongfan Zhang, Wei Lin
Summary: This study investigates the mechanism and coke-resistance ability of the Ni-Mo catalyst in dry reforming of methane (DRM) by using Mo-doped Ni and MoOx adsorbed Ni surfaces. The electron donor effect of Mo inhibits the carbonization of Ni, while the strong interaction between Mo and O promotes the formation of MoOx species. The presence of Mo-O species enhances the carbon oxidation reaction.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Multidisciplinary
Hui Cheng, Boheng Dong, Qiong Liu, Fuxian Wang
Summary: This study demonstrates a direct methanol oxidation reaction (MOR) pathway on MoO3/Ni-(OH)2 without the formation of NiOOH. The research provides a facile strategy of regulating the intermediate process barrier for MOR.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Vladislav S. Menshikov, Ivan N. Novomlinsky, Sergey V. Belenov, Anastasya A. Alekseenko, Olga I. Safronenko, Vladimir E. Guterman
Summary: Pt/(SnO2/C) catalyst is the most active among the studied catalysts in methanol and formic acid electrooxidation reactions; the nature of the reagent affects the rates of corresponding reactions; Cu atoms and SnO2 nanoparticles positively influence the catalytic activity of platinum.
Article
Chemistry, Multidisciplinary
Svetlana S. Laletina, Mikhail Mamatkulov, Aleksey M. Shor, Elena A. Shor, Vasily V. Kaichev, Ilya Yudanov
Summary: Methanol dehydrogenation on Pt nanoparticles was studied to investigate the size and structure effects. The results showed that the morphology of nanoparticles affects the adsorption energy of COHx intermediates, and the size of nanoparticles influences the activity of adsorption sites.
Article
Electrochemistry
Xiaobo Yang, Xili Tong, Xingchen Liu, Kaixi Li, Nianjun Yang
Summary: A series of Ag-core/Pd-shell catalysts were synthesized and it was found that the Ag@Pd-3 catalyst exhibited the best performance for the methanol oxidation reaction. This catalyst showed significantly higher mass activity and specific activity compared to a Pd/C catalyst, making it a promising candidate for high-performance DMFCs. Computational calculations indicated that the enhanced performance of the Ag@Pd-3 catalyst was due to a stronger adsorption of CH3OH and OH on the Pd active sites.
ELECTROCHEMISTRY COMMUNICATIONS
(2021)
Article
Chemistry, Multidisciplinary
Marco A. Rossi, Luiz H. Vieira, Leticia F. Rasteiro, Marco A. Fraga, Jose M. Assaf, Elisabete M. Assaf
Summary: In-promoted Cu/CeO2 catalysts were applied in the CO2 hydrogenation to methanol. The catalysts had an inverse configuration with small single-domains of CeO2 particles deposited over large Cu particles. Highly dispersed indium decreased the CeO2 particle size, increasing the interface areas for CO2 adsorption. The indium-promoted catalysts showed a remarkable increase in methanol selectivity, with the formate route identified as the preferred route for methanol formation.
REACTION CHEMISTRY & ENGINEERING
(2022)
Article
Chemistry, Multidisciplinary
Bing Zhu, Haibo Li, Xue Wang, Subing Fan, Junmin Lv, Tian-sheng Zhao
Summary: The [Zn,Mo]/HZ-5 catalysts were prepared using the impregnation method, and the effect of Mo content on catalytic performance was investigated. The catalysts were characterized by various techniques, and it was found that coaromatization process had higher aromatics yield and better stability. The modification with Mo species regulated the acidity of Zn/HZ-5 and increased the amount of Zn(OH)(+) species, resulting in improved dehydroaromatization ability and higher aromatics yield. The carbon deposit and deactivation behaviors were also studied, and under the optimized conditions of 470°C and WHSV = 1.0 h(-1), the BTEX yield reached a maximum of 64.0%.
REACTION CHEMISTRY & ENGINEERING
(2023)
Review
Chemistry, Multidisciplinary
Jianmei Wang, Bingxing Zhang, Wei Guo, Lei Wang, Jian Chen, Hongge Pan, Wenping Sun
Summary: The study of direct methanol fuel cells (DMFCs) has been ongoing for around 70 years, but commercialization is still a distant goal. The methanol oxidation reaction (MOR) is the bottleneck reaction that limits the overall performance of DMFCs. This review summarizes the controversies and progress in electrocatalytic mechanisms, performance evaluations, and design science for MOR electrocatalysts. It also provides an overview of the recent development of emerging MOR electrocatalysts, focusing on the innovation of alloy, core-shell structure, heterostructure, and single-atom catalysts. Perspectives on future research directions are also discussed.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Liqun Kang, Bolun Wang, Adam Thetford, Ke Wu, Mohsen Danaie, Qian He, Emma K. Gibson, Ling-Dong Sun, Hiroyuki Asakura, C. Richard A. Catlow, Feng Ryan Wang
Summary: The study reports an air-stable surface [bipy-Ru-II(CO)(2)Cl-2] site capable of oxidizing CO, demonstrating practical control over geometric and electronic structures of single-site catalysts at the molecular level.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Applied
Carlos Hernandez-Tamargo, Ian P. Silverwood, Alexander J. O'Malley, Nora H. de Leeuw
Summary: The study investigated the dynamics of catechol in zeolite Beta, revealing that the presence of the second OH group in catechol significantly hinders its mobility due to stronger hydrogen bonding interactions with the Bronsted sites. Molecular dynamics simulations confirmed this increased immobility, showing lower translational diffusion coefficients for catechol compared to phenol in acidic zeolites. The study also found that catechol exhibits restricted and rapid rattling motion in the pore system of zeolite, indicating strong interaction of the molecules with the acid sites.
TOPICS IN CATALYSIS
(2021)
Article
Chemistry, Physical
Donato Decarolis, Adam H. Clark, Tommaso Pellegrinelli, Maarten Nachtegaal, Evan W. Lynch, C. Richard A. Catlow, Emma K. Gibson, Alexandre Goguet, Peter P. Wells
Summary: This study utilized operando spectroscopy to spatially profile a Pd/Al2O3 catalyst during NH3 oxidation, revealing insights into structure-activity relationships in catalysis. The results showed a direct correlation between the presence of PdNx and selectivity toward N-2, and proposed two simultaneous reaction pathways at high temperatures. These findings highlight the structural and catalytic diversity during catalysis, emphasizing the importance of understanding for improving emission control technologies like selective catalytic oxidation of NH3.
Article
Chemistry, Applied
Tommaso Pellegrinelli, Geoffrey McCullough, Roberto Caporali, Iain Murray, Veronica Celorrio, Emma K. Gibson, Christopher Hardacre, Alexandre Goguet
Summary: Hydrothermal degreening and ageing procedures were applied to a tri-metal (Pt-Pd-Rh) fully formulated lean NOx Trap catalyst to evaluate the effects of thermal stress on performance and structural properties. The size of platinum particles and ceria particles increased after ageing treatment, while a decrease in active NOx storage sites was observed. The aged sample showed a lower reductant consumption and more efficient reduction process, with a wider spread presence of NH3 and NOx slip observed during reduction due to different distributions of adsorbed species.
Article
Chemistry, Applied
Vainius Skukauskas, Elliot L. B. Johnson Humphrey, Iain Hitchcock, Andrew York, Joseph Kelleher, Emma K. Gibson, David J. Nelson, Ian P. Silverwood
Summary: The article introduces the method of using neutron probes to observe the progress of catalytic reactions and the recent progress and possibilities in realistic applications.
TOPICS IN CATALYSIS
(2021)
Article
Chemistry, Applied
Santhosh K. Matam, C. Richard A. Catlow, Ian P. Silverwood, Alexander J. O'Malley
Summary: The dynamics of methanol in H-ZSM-5 zeolite were studied at different temperatures, revealing a transition from rotational to translational diffusion as temperature increased. The translational diffusion of methanol was found to be confined to a sphere near the ZSM-5 channel.
TOPICS IN CATALYSIS
(2021)
Article
Chemistry, Physical
Thulani M. Nyathi, Mohamed Fadlalla, Nico Fischer, Andrew P. E. York, Ezra J. Olivier, Emma K. Gibson, Peter P. Wells, Michael Claeys
Summary: The study investigated the impact of different supports on the catalytic performance and phase stability of Co3O4 nanoparticles during CO-PrOx. Results showed that weak nanoparticle-support interactions (as in Co3O4/ZrO2) favored high CO oxidation activity, while stronger interactions (as in Co3O4/Al2O3) helped minimize Co-0 and CH4 formation. The study highlights the bi-functional role supports play in CO-PrOx, enhancing catalytic performance and improving the phase stability of Co3O4.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2021)
Article
Chemistry, Physical
Mattia Gaboardi, Ian Silverwood, Balthasar Braunewell, Jay Siegel, Felix Fernandez-Alonso
Summary: The condensed phases of carbon-based nanobowl corannulene were investigated in the temperature range of 200-573 K, revealing a well-defined thermal event at 382 K. Analysis of the neutron-scattering data identified the emergence of correlated stochastic dynamics with the formation of high-symmetry rotor-like states. Additionally, a robust hysteresis associated with previously unknown metastable liquid and disordered-solid phases was discovered, indicating novel opportunities for applications exploiting dynamical disorder at the nanoscale.
Article
Chemistry, Physical
Vainius Skukauskas, Ian P. Silverwood, Emma K. Gibson
Summary: Quasielastic neutron scattering was used to study the dynamics of water confined in copper-loaded MOR, MFI, and CHA zeolites at temperatures ranging from 100-300 K. The results show that the Cu content and cavity size affect the mobility of water, indicating diffusion within localized clusters.
CATALYSIS COMMUNICATIONS
(2022)
Article
Chemistry, Physical
A. J. Porter, C. H. Botchway, B. Kwakye-Awuah, C. Hernandez-Tamargo, S. K. Matam, S. L. McHugh, I. P. Silverwood, N. H. de Leeuw, A. J. O'Malley
Summary: The dynamical behavior of methanol confined in zeolite H-FER with different Si/Al ratios has been studied using quasielastic neutron scattering (QENS) and classical molecular dynamics (MD) simulations. The presence of Bronsted acid sites significantly reduces the diffusivity of methanol and limits its mobility in the catalyst.
CATALYSIS SCIENCE & TECHNOLOGY
(2022)
Article
Chemistry, Physical
Alexander P. Hawkins, Andrea Zachariou, Ian P. Silverwood, Chin Yong, Paul Collier, Ilian Todorov, Russell F. Howe, Stewart F. Parker, David Lennon
Summary: Quasi-elastic neutron scattering (QENS) and molecular dynamics (MD) simulations were used to investigate the dynamics of methane in H-ZSM-5 zeolite catalysts for methanol-to-hydrocarbons reactions. The study found that methane mobility was extremely high in fresh ZSM-5, and moderate levels of coke buildup had minimal effect on methane diffusion. However, highly coked samples resulted in confinement of methane to single zeolite pores with minimal long-range diffusion.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Applied
A. J. Porter, S. L. McHugh, T. Omojola, I. P. Silverwood, A. J. O'Malley
Summary: The dynamics of water confined in H-ZSM-5 with different Si/Al ratios have been studied using QENS and MD. The results showed that water diffusion was more confined in the low silica samples, while in the high silica zeolite, diffusion was less confined and more long range. MD simulations revealed that the Si/Al ratio had a significant effect on water diffusivity, reducing the self-diffusion coefficient. The results from MD simulations were in good agreement with the QENS experiments.
MICROPOROUS AND MESOPOROUS MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Shaojun Xu, Xue Han, Yujie Ma, Thien D. Duong, Longfei Lin, Emma K. Gibson, Alena Sheveleva, Sarayute Chansai, Alex Walton, Duc-The Ngo, Mark D. Frogley, Chiu C. Tang, Floriana Tuna, Eric J. L. McInnes, C. Richard A. Catlow, Christopher Hardacre, Sihai Yang, Martin Schroder
Summary: Efficient catalytic conversion of NO2 to non-harmful species using Cu-embedded metal-organic framework at room temperature is described in this study. The process achieves a high NO2 conversion rate and N-2 selectivity without the use of NH3 or other reducing agents.
CELL REPORTS PHYSICAL SCIENCE
(2021)
Article
Chemistry, Multidisciplinary
Biying Liu, Shaojun Xu, Man Zhang, Xin Li, Donato Decarolis, Yuqian Liu, Yuchen Wang, Emma K. Gibson, C. Richard A. Catlow, Kai Yan
Summary: A highly efficient ternary NiCoMn-layered double hydroxides (NiCoMn-LDHs) nanosheet catalyst with oxygen vacancy-rich properties has been developed for the electrooxidation of HMF and furfural to FDCA and FurAc, showing high yields and good faradaic efficiency. The mechanism for its superior performance lies in the exposure of more active sites with oxygen vacancies, promoting synergistic effects between HMF and furfural oxidation reactions.
