Article
Materials Science, Multidisciplinary
Swati Pandey, Ashish Kumar Mishra, M. P. Saravanan, P. K. Biswas, A. K. Yadav, S. N. Jha, D. Bhattacharyya, R. J. Choudhary, R. Rawat, V. Siruguri
Summary: We have found a quantum critical point in CeRu2-xCoxGe2 (0 x 2) through detailed heat capacity and muon spin relaxation (μSR) measurements. The results for the critical composition xC - 1.5 support the spin fluctuation model of the quantum critical point, and the x-ray absorption near edge structure at different temperatures confirms the presence of intermediate valence fluctuations. This study demonstrates the importance of the survival of valence and spin fluctuations in the quantum criticality of CeRu2-xCoxGe2.
Article
Chemistry, Multidisciplinary
Lucas C. Torres, Roman Dobrovetsky, Christopher B. Caputo
Summary: This study describes the synthesis of alkynyl phosphanes and their transformation to geminally substituted phosphonium borato-allene zwitterions upon reaction with B(C6F5)(3). Experimental and DFT calculations suggest the involvement of an unsaturated 3-coordinate phosphonium electrophile as an intermediate in this transformation.
CHEMICAL COMMUNICATIONS
(2021)
Article
Materials Science, Multidisciplinary
M. Barbier, M. Sundermann, A. Poux, A. Rogalev, D. Braithwaite, J. -P. Sanchez, F. Wilhelm
Summary: The archetypical heavy-fermion superconductor CeCu2Si2 exhibits two distinct superconducting phases under pressure. Changes in pressure and applied magnetic field cause a continuous increase in the valence of Ce, with only a continuous valence change observed so far.
Review
Chemistry, Multidisciplinary
Maxime Tricoire, Nolwenn Mahieu, Thomas Simler, Gregory Nocton
Summary: Over the past 50 years, intermediate valence states in lanthanide compounds have often led to unexpected or puzzling spectroscopic and magnetic properties. New theoretical models involving multiconfigurational electronic ground states have helped to rationalize these experimental singularities. Understanding and adjusting the ground-state multiconfigurational behavior in lanthanide complexes may lead to new avenues for modular and unusual reactivities.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Multidisciplinary
Teng Hu, Yanling Wang, Liyan Zhao, Shikuan Yang
Summary: The assembly of biomolecules and ions in nature has produced many complex structures, but human control over ion assembly processes is relatively weak. This study found that intermediate valency metal ions in the electrolyte can influence the growth speed of crystal facets and adjust the shape of electrodeposits. This control capability over the electrochemical assembly process of metal ions is significantly enhanced by introducing intermediate valence ions.
Article
Chemistry, Physical
Lei Li, Sutian Xue, Meijie Wei, Hui Yao, Yong Dai, Zhaoyang Fei
Summary: In this study, Pd/CeO2 catalysts with nanobundles structure were synthesized and showed superior performance in CO oxidation and CH4 combustion at low temperature. Characterization techniques revealed the surface concentration of Pd species and the mechanism of oxygen vacancy formation. Possible reaction mechanism was clarified by in-situ DRIFTS spectra.
APPLIED SURFACE SCIENCE
(2022)
Article
Chemistry, Inorganic & Nuclear
Wei-Dong Liu, Liu-Qing Chen, Qi-Hao Qiu, Ming-Qiang Qi, Han Xu, Chao-Long Chen, La-Sheng Long, Lan-Sun Zheng, Xiang-Jian Kong
Summary: In this study, a mixed valence cerium-oxo cluster was successfully synthesized through low-temperature crystallization, and the coexistence and distribution of Ce ions in different valence states were determined. The mechanism for the generation of +4 valence state was revealed, and the synthesized cluster exhibited strong ultraviolet absorption and long visible light absorption, as well as clear photocurrent response and high photocurrent intensity.
INORGANIC CHEMISTRY COMMUNICATIONS
(2024)
Article
Green & Sustainable Science & Technology
Jiaojie He, Conghong Pei, Yue Yang, Bo Lai, Yan Sun, Liwei Yang
Summary: Three cerium-based metal-organic frameworks, Ce-BDC-1, Ce-BDC-2, and Ce-BTC-1, were synthesized for effective phosphate uptake. Despite similar phosphate removal capacities, they exhibited distinct adsorption characteristics, such as adsorption speed and capacity.
JOURNAL OF CLEANER PRODUCTION
(2021)
Article
Nanoscience & Nanotechnology
Robert A. Yokel, Wendel Wohlleben, Johannes Georg Keller, Matthew L. Hancock, Jason M. Unrine, D. Allan Butterfield, Eric A. Grulke
Summary: Cerium oxide nanoparticles, or nanoceria, are engineered nanomaterials with varying physicochemical properties and applications. Industrial nanoceria like NM-212 are calcined, while those with pharmaceutical properties are often prepared by solvothermal synthesis. The dissolution of nanoceria is influenced by high-temperature exposure, leading to changes in solubility and surface cerium valence, which in turn affect their biological and catalytic properties.
BEILSTEIN JOURNAL OF NANOTECHNOLOGY
(2021)
Article
Materials Science, Multidisciplinary
Martin Sundermann, Andrea Marino, Andrei Gloskovskii, Chongli Yang, Yasuyuki Shimura, Toshiro Takabatake, Andrea Severing
Summary: CeRhSn with Ce atoms forming a quasikagome lattice has been studied in relation to quantum criticality driven by magnetic frustration. Substituting Rh with Pd leads to magnetic order, while the 4 f occupation decreases smoothly with the increase of x in CeRh1-xPdxSn series. Pd 4d states are further away from Ce 4 f states compared to Rh 4d states, resulting in a decrease in the effective binding energy of the 4 f states.
Article
Nanoscience & Nanotechnology
Hong-Guang Jin, Mingyu Wang, Jian-Xin Wen, Sheng-Hua Han, Xu-Jia Hong, Yue-Peng Cai, Guangli Li, Jincheng Fan, Zi-Sheng Chao
Summary: This study introduces a mixed-valence cerium MOF named CSUST-1 with isolated Ce(IV, III) arrays and abundant oxygen vacancies. The CSUST-1/CNT composite, as a separator coating material in Li-S batteries, accelerates redox kinetics and Li+ transportation, resulting in high specific capacity and long-term stability.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Engineering, Environmental
Bing Hou, Jingwen Pan, Tao Shi, Zhenhua Dang, Shu Yang, Lei Wang, Baoyu Gao
Summary: This study prepared nano-cerium based adsorbents with different surface defects and Ce(III) content to investigate their effects on the Cr(VI) adsorption capacity. The results showed that the optimized adsorbent performed well over a wide pH range and the performance was closely related to the contents of Ce(III) and surface defects.
JOURNAL OF HAZARDOUS MATERIALS
(2024)
Article
Chemistry, Physical
B. I. Rabiu, B. Huang, X. Luo, Y. Q. Yang
Summary: Doped and undoped ternary and binary Mg2Sn solid solutions were fabricated, and the effects of Cu2S addition on the thermoelectric properties were investigated. It was found that Cu2S addition increased the electrical conductivity and Seebeck coefficient, while decreasing the thermal conductivity. The ternary compositions with Si and Ge showed high power factors due to optimized Seebeck coefficient and electrical conductivity.
JOURNAL OF ALLOYS AND COMPOUNDS
(2024)
Article
Electrochemistry
Shengsheng Cui, Yuna Zhang, Cuili Xue, Haisong Tan, Shanshan Fan, Yi Lu, Xinni Pan, Yanlei Liu, Daxiang Cui
Summary: The oxygen evolution reaction is hindered in water electrolysis, necessitating catalysts to improve reaction kinetics. While precious metal catalysts are highly active, catalysts based on earth-abundant elements are gaining attention for their high performance, low cost, and practicality. The study focuses on electrodeposited cobalt stannide (CoSn2) as an efficient and stable oxygen evolution electrocatalyst, demonstrating competitive activity to precious-metal-containing benchmark catalysts.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2021)
Article
Chemistry, Inorganic & Nuclear
Pablo de la Mora, Gustavo Tavizon
Summary: Rare earth ARE2X4 (A = Cd, Mg; RE = Ho, Er, Tm, Yb, Lu; X = S, Se) spinels were studied to investigate their electronic structure, especially related to Intermediate-Valence and Heavy-Fermion behavior. The compounds with RE = Ho, Er, Tm, Lu were found to be insulators, while RE = Yb showed metallicity and Intermediate-Valent and Heavy-Fermion characters. Electron-doped ATm2X4 and AEr2X4 spinels exhibited Heavy-Fermion behavior.
JOURNAL OF SOLID STATE CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Pengxin Liu, Paula Macarena Abdala, Guillaume Goubert, Marc-Georg Willinger, Christophe Coperet
Summary: The study successfully synthesized single-crystalline MgO(111) nanosheets with a defect-rich surface, which exhibit high reactivity and can activate CO molecules at low temperatures and pressures.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Pedro Castro-Fernandez, Deni Mance, Chong Liu, Ilia B. Moroz, Paula M. Abdala, Evgeny A. Pidko, Christophe Coperet, Alexey Fedorov, Christoph R. Mueller
Summary: The study investigated the coordination environment and acidity of surface sites in different Ga2O3 catalysts for propane dehydrogenation, with spectroscopic data suggesting that weak Lewis acid surface sites in beta-Ga2O3 contribute to its superior catalytic activity compared to alpha-Ga2O3 and gamma-Ga2O3.
Article
Chemistry, Applied
Athanasia Tsoukalou, Alexander Serykh, Elena Willinger, Agnieszka Kierzkowska, Paula M. Abdala, Alexey Fedorov, Christoph R. Mueller
Summary: The formation and nature of surface indium species in zirconia-supported catalysts for CO2 hydrogenation to methanol were investigated. It was found that In2O3/m-ZrO2(redox) catalyst had the highest activity and concentration of surface indium sites capable of H-2 activation, making it the most promising catalyst for CO2 hydrogenation to methanol.
Article
Multidisciplinary Sciences
Hui Zhou, Zixuan Chen, Evgenia Kountoupi, Athanasia Tsoukalou, Paula M. Abdala, Pierre Florian, Alexey Fedorov, Christoph R. Mueller
Summary: Early transitional metal carbides, such as 2D-Mo2C, show promising catalytic activity for CO2 hydrogenation through surface group manipulation, resulting in tunable selectivity and activity for the reaction. This study highlights the importance of surface termination groups in controlling the performance of carbide catalysts for CO2 conversion to value-added chemicals.
NATURE COMMUNICATIONS
(2021)
Article
Chemistry, Physical
Athanasia Tsoukalou, Nikolai S. Bushkov, Scott R. Docherty, Deni Mance, Alexander Serykh, Paula M. Abdala, Christophe Coperet, Alexey Fedorov, Christoph R. Mueller
Summary: The phase of the ZrO2 support has a significant influence on the nature and formation rates of surface species during methanol synthesis from CO2 hydrogenation. The m-ZrO2:In catalyst exhibits higher activity, with faster formation of formate and methoxy species. Only formate species are detected on t-ZrO2 and am-ZrO2 catalysts, while methoxy and formate species are found on m-ZrO2:In and In2O3/am-ZrO2, respectively. In contrast, only a weak formate peak is observed on In2O3/t-ZrO2 catalyst. The presence of an india-zirconia interface is crucial for the effective stabilization of formate species in unsupported In2O3.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Hui Zhou, Zixuan Chen, Anna Vidal Lopez, Estefania Diaz Lopez, Erwin Lam, Athanasia Tsoukalou, Elena Willinger, Denis A. Kuznetsov, Deni Mance, Agnieszka Kierzkowska, Felix Donat, Paula M. Abdala, Aleix Comas-Vives, Christophe Coperet, Alexey Fedorov, Christoph R. Mueller
Summary: In this study, an optimized Cu/Mo2CTx interface was achieved through engineering methods, leading to higher efficiency in the catalytic conversion of CO2 to methanol. Density functional theory calculations confirmed the critical role of the interface between Cu and Mo2CTx in stabilizing reaction intermediates.
Article
Chemistry, Physical
Pedro Castro-Fernandez, Deni Mance, Chong Liu, Paula M. Abdala, Elena Willinger, Aurelio A. Rossinelli, Alexander I. Serykh, Evgeny A. Pidko, Christophe Coperet, Alexey Fedorov, Christoph R. Mueller
Summary: This study investigates the effect of H2 treatment on the structure, acidity, and catalytic activity of γ/β-Ga2O3 nanoparticle catalysts. The results show that the presence of the β-Ga2O3 phase increases the PDH activity of the catalysts, and H2 treatment enhances the catalytic activity for all three catalysts through different mechanisms.
JOURNAL OF CATALYSIS
(2022)
Article
Chemistry, Physical
Manouchehr Nadjafi, Yifan Cui, Marlon Bachl, Alexander Oing, Felix Donat, Giancarlo Luongo, Paula M. Abdala, Alexey Fedorov, Christoph R. Mueller
Summary: The oxidative dehydrogenation of propane can occur through a gas-solid interface or in the gas phase via a radical chain process. This study found that an empty quartz reactor can achieve high propene and ethene selectivities and propane conversions comparable to those of state-of-the-art ODP catalysts. Optimizing the post-catalytic volume of a h-BN catalyst bed can increase propane conversion and propene selectivity, indicating it as an important variable for improving catalytic ODP performances.
Article
Multidisciplinary Sciences
Margarita Rekhtina, Maximilian Krodel, Yi-Hsuan Wu, Agnieszka Kierzkowska, Felix Donat, Paula M. Abdala, Christoph R. Muller
Summary: The structural dynamics of a NaNO3-promoted, MgO-based CO2 sorbent were investigated using in situ time-resolved powder x-ray diffraction. The sorbent initially deactivates due to an increase in MgO crystallite size, reducing the availability of nucleation points for MgCO3 growth. However, after the third cycle, the sorbent shows continuous reactivation, attributed to the in situ formation of Na2Mg(CO3)2 crystallites that act as seeds for MgCO3 nucleation and growth.
Article
Chemistry, Multidisciplinary
Annelies Landuyt, Priyank V. Kumar, Jodie A. Yuwono, Alexander H. Bork, Felix Donat, Paula M. Abdala, Christoph R. Mueller
Summary: MgO-based CO2 sorbents promoted with molten alkali metal nitrates have shown great potential for CO2 capture and storage technologies. The carbonation mechanism of these sorbents, especially when the promoter is in the molten state, has been investigated using O-18 isotope labeling experiments. Results suggest a fast oxygen exchange between CO2 and MgO through reversible formation of surface carbonates, and subsequent dissolution of these carbonates in the molten NaNO3 promoter.
Review
Chemistry, Multidisciplinary
Nora K. Zimmerli, Christoph R. Mueller, Paula M. Abdala
Summary: Heterogeneous catalysts are complex materials that require advanced structural characterization tools to determine structure-performance relationships. Pair distribution function (PDF) analysis is a powerful method for extracting structural information from the atomic to the nanoscale.
TRENDS IN CHEMISTRY
(2022)
Article
Chemistry, Physical
Zixuan Chen, Scott R. Docherty, Pierre Florian, Agnieszka Kierzkowska, Ilia B. Moroz, Paula M. Abdala, Christophe Coperet, Christoph R. Mueller, Alexey Fedorov
Summary: Catalysts with well-defined isolated Ni(ii) surface sites have been prepared on three different silica-based supports. The Ni catalysts with a higher density of strong Bronsted acid sites (BAS) show higher initial activity and productivity in the ethene-to-propene conversion. Propene productivity is closely related to the concentration of C-8 aromatics, suggesting the formation of propene via a carbon-pool mechanism. Furthermore, the deactivation of catalysts with Ni(ii) sites on AlOx can be reversed by calcination, while catalysts with Ni silicate or aluminosilicate sites irreversibly deactivate by forming Ni nanoparticles.
CATALYSIS SCIENCE & TECHNOLOGY
(2022)
Article
Chemistry, Physical
Alexey Kurlov, Dragos Stoian, Ali Baghizadeh, Evgenia Kountoupi, Evgeniya B. Deeva, Marc Willinger, Paula M. Abdala, Alexey Fedorov, Christoph R. Mueller
Summary: In this study, Mo2C nanobelts and Mo2C/SiO2 were synthesized through thermal carburization, and they exhibited excellent catalytic activity and stability in dry reforming of methane. The influence of Mo2C morphology and silica dispersion on the structural evolution and oxidation behavior of the catalysts under reaction conditions were investigated by in situ X-ray absorption spectroscopy.
CATALYSIS SCIENCE & TECHNOLOGY
(2022)
Article
Chemistry, Physical
Pedro Castro-Fernandez, Alexander I. Serykh, Alexander V. Yakimov, Igor P. Prosvirin, Andrey V. Bukhtiyarov, Paula M. Abdala, Christophe Coperet, Alexey Fedorov, Christoph R. Mueller
Summary: This work investigates how H-2 pretreatment at 550 degrees C affects the structural transformation and catalytic performance of two gallia-based propane dehydrogenation catalysts. The results show that the nanocrystalline gamma/beta-Ga2O3 phase in gamma-Ga2O3/SiO2-H-2 exhibits increased disorder and stronger Lewis acid sites compared to the calcined gamma-Ga2O3/SiO2 phase. Ga/SiO2-H-2, on the other hand, shows poor performance.
CATALYSIS SCIENCE & TECHNOLOGY
(2022)
Article
Chemistry, Physical
Nur Sena Yuezbasi, Andac Armutlulu, Thomas Huthwelker, Paula M. Abdala, Christoph R. Mueller
Summary: Chemical looping is a promising technology for producing high purity hydrogen while capturing CO2. This study investigates the addition of sodium in the synthesis of Fe2O3-Al2O3 oxygen carriers to counteract cyclic deactivation. The addition of sodium prevents the formation of FeAl2O4 and stabilizes the oxygen carrier, resulting in a stable hydrogen yield.
JOURNAL OF MATERIALS CHEMISTRY A
(2022)