Article
Biochemistry & Molecular Biology
Pavel Smirnov, Evgeny Filatov, Natalia Kuratieva, Pavel Plyusnin, Sergey Korenev
Summary: In this study, seven new double-complex salts (DCS) were synthesized and their crystal structure and composition were analyzed using SCXRD, XRD, CHN, and IR methods. The complex salts of [M-1(NH3)(6)][M-2(C2O4)(3)] (M-1, M-2 = Co, Rh) can crystallize as either a crystalline hydrate [M-1(NH3)(6)][M-2(C2O4)(3)]•3H(2)O or an anhydrous complex, depending on the synthesis conditions. The formation of [Rh(NH3)(6)][Rh(C2O4)(3)] is temperature-dependent, with a mixture of [Rh(NH3)(6)][Rh(C2O4)(3)] and K-3[Rh(NH3)(6)][Rh(C2O4)(3)](2)•6H(2)O observed at room temperature, and the target product [Rh(NH3)(6)][Rh(C2O4)(3)] crystallizing at elevated temperatures. The thermal decomposition of the double-complex salts leads to the formation of metals or CoxRh1-x solid solutions at temperatures of 320-450°C, as determined by STA, EGA-MS, IR, and XRD methods.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2023)
Article
Materials Science, Coatings & Films
Elizabeth A. Jamka, Maxwell Z. Gillum, Christina N. Grytsyshyn-Giger, Faith J. Lewis, Daniel R. Killelea
Summary: Heterogeneously catalyzed reactions over transition metal surfaces play a crucial role in the chemical industry and global energy demand. CO oxidation is used to study the reactivity of various oxygenaceous surface phases, and surface IR spectroscopy provides valuable information about the reaction mechanism.
JOURNAL OF VACUUM SCIENCE & TECHNOLOGY A
(2022)
Article
Thermodynamics
Peter Glarborg
Summary: Amine/NO2 interactions play a crucial role in ignition and N2O emissions. This study reinterpreted the reported results from batch and flow reactors, and provided additional results on the impact of O2 on the NH3/NO2 reaction. The analysis constrained the rate constants for NH3 and NH2 reactions with NO2, as well as the subsequent steps involving H2NO and HNO intermediates. The experimental and modeling findings support the present understanding of the reaction kinetics.
COMBUSTION AND FLAME
(2023)
Article
Chemistry, Physical
Jun Cai, Yunjian Ling, Hui Zhang, Bo Yang, Fan Yang, Zhi Liu
Summary: In this work, an in situ study of Rh-O species and their activity for CO oxidation over the Rh(110) surface was reported using advanced surface science techniques. It was found that Rh-O species, including (2 x 1)-O, (10 x 2)-O, trilayer O-Rh-O, and Rh2O3, were formed in sequence as the O-2 chemical potential increases. The reactivity of the Rh-O species followed the sequence (2 x 1)-O > (10 x 2)-O > trilayer O-Rh-O >> Rh2O3, with the titration reaction on the trilayer oxide being a two-step process.
Article
Chemistry, Multidisciplinary
Samantha Carter, Wenjie Tao, Rajat Majumder, Alexander Yu. Sokolov, Shiyu Zhang
Summary: We investigate the spin switching behavior of dicopperoxo nitrosyl [Cu-2(O)(NO)](2+) complexes at different temperatures and its influence on hydrogen atom transfer (HAT) reactivity. Our findings indicate that the HAT reaction is predominantly mediated by the S = 1/2 isomer of [Cu-2(O)(NO)](2+) complexes at low temperatures (198 K). Moreover, the introduction of functional groups that create an unsymmetric secondary coordination environment enhances the HAT rates by perturbing the spin equilibria. These findings suggest that metalloenzymes in natural proteins may employ similar strategies to control HAT reactions due to their often unsymmetric coordination environments.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Jiao-Jiao Chen, Si-Dun Wang, Zi-Yu Li, Xiao-Na Li, Sheng-Gui He
Summary: This study demonstrates the catalytic conversion of toxic nitrogen oxide (NO) and carbon monoxide (CO) into nitrogen (N-2) and carbon dioxide (CO2) using rhodium-cerium oxide clusters as the active site. The unique chemical environment in the cluster greatly improves the selectivity of N-2 production.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Wei-Chieh Chang, Helena Randel, Thomas Weyhermueller, Alexander A. A. Auer, Christophe Fares, Christophe Werle
Summary: In this study, a cooperative [Rh/P(O)nBu(2)] template was used for the catalytic hydrodefluorination (HDF) of perfluoroarenes under mild reaction conditions. The system showed high chemoselectivity and practicality, even in the presence of electron-donating functionalities and heterocycles. Mechanistic and theoretical studies identified a rhodium(I) dihydride complex as the catalytically relevant species and the crucial role of phosphine oxide as a cooperative fragment. Overall, this work demonstrates the potential of molecular templates for enhancing the reactivity in challenging bond activations.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Shiguang Zhang, Xinyan Li, Yun Su, Yang Yang, Hao Yu, Haibo Wang, Qing Zhang, Yaxiang Lu, Dawei Song, Shanfeng Wang, Qinghua Zhang, Xiaohui Rong, Lianqi Zhang, Liquan Chen, Yong-Sheng Hu
Summary: A rational four-in-one strategy to enhance the performance of Na-x[Ni,Mn]O-2 materials is proposed, involving innovative composition design and elegant synthesis management. After modification, the capacity retention rate of half-cells increases from 45% to 77% after 250 cycles at 1 C rate, and the capacity of full cells is maintained at 83% after 300 cycles at 0.5 C rate. This strategy provides new insights into the overall optimization of cathode materials for Na-ion batteries.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Rui Gao, Zhen Liu, Zeyu Liu, Jie Su, Liangbing Gan
Summary: An open-cage fullerene derivative was prepared by Malaprade oxidation of a vicinal triol moiety. The orifice above the 17-membered ring contains a carboxyl group, and there are three ketone carbonyl groups and one lactone carbonyl group on the rim of the orifice. The carboxylic and carbonyl oxygen atoms around the orifice act as strong polydentate ligands for a sodium ion and also form various isomeric rhodium complexes with comparable stability when reacted with [Rh(CO)(2)Cl](2). The fullerene C=C bond on the rim of the orifice forms a stable platinum complex when treated with Pt(PPh3)(4), and one of the carboxylic oxygen atoms above the orifice forms a H-bond with the water molecule trapped in the cage as revealed by the single crystal X-ray diffraction data.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Shunsaku Yasumura, Taisetsu Kato, Yucheng Qian, Takashi Toyao, Zen Maeno, Ken-ichi Shimizu
Summary: The dynamic structural evolution of Rh species in MOR zeolite was studied, revealing oxidation and cluster formation of Rh species under NO and H2 flow. Al sites increased the thermodynamic stability of Rh+ species and prevented over-oxidation reactions. NO capture and selective reduction to NH3 were observed using in situ IR measurements.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Hiroki Nakayama, Makoto Nagata, Toshihisa Tomie, Tomoaki Ishitsuka, Nobuyuki Matsubayashi, Yukihiro Shimizu
Summary: In this study, the valence band spectra of Rh catalysts on various supports were measured and correlated with the catalytic activities in the CO-NO reaction. The effects of SMSI on the activities of Rh catalysts were analyzed using density functional theory calculations. The study reveals the critical mechanisms whereby SMSIs contribute to oxygen-mediated reactions on catalyst surfaces.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Inorganic & Nuclear
Yipeng Zang, Yueyue Wang, Ruili Sang, Li Xu
Summary: The redox reaction of monovalent Rh-2(CO)(4)Cl(2) and Bi-n(n-) (n = 2, 3) in ethylenediamine solution led to the formation of a decabismuthide-hexarhodium dianion [Rh@Bi-10(RhCO)(5)](2-) (1a), where a novel Bi10-bowl was constructed from oxidized 2Bi(3)/2Bi(2) open triangles/dimers. The structure of 1a was stabilized by strong bonding to a reduced Rh@(RhCO)(5) square pyramid. Weak interactions between two 1a dianions formed a dimer [Rh@Bi-10(RhCO)(5)](2)(4-) (1). The structure and bonding of the novel polybismuthide heteroanion 1 are discussed.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Physical
Anna Zawada, Malgorzata Lubas, Iwona Przerada
Summary: This study focuses on the production of amorphous glasses by melting materials containing iron and aluminum oxides, and evaluates the effect of iron and aluminum ions on the glass structure. The results show that the incorporation of iron and aluminum ions can strengthen the glass network and increase its viscosity.
JOURNAL OF MOLECULAR STRUCTURE
(2023)
Article
Engineering, Environmental
Wo Bin Bae, Do Yeong Kim, Sang Woo Byun, Seong Jun Lee, Su Keun Kuk, Hyuk Jae Kwon, Hyun Chul Lee, Melanie J. Hazlett, Chong Liu, Young Jin Kim, Minkyu Kim, Sung Bong Kang
Summary: This study investigates the application of Rh-supported metal oxides for direct nitrogen oxide decomposition (DND) and finds that the catalytic activity is deactivated over time due to oxygen poisoning, but can be regenerated through reductive treatments.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Physical
Shipeng Jia, Jonathan Counsell, Michel Adamic, Antranik Jonderian, Eric McCalla
Summary: Na-ion batteries are considered environmentally favorable alternatives to Li-ion batteries, and research has found that in Na-Fe-Mn-O materials, the under-studied P3 and Mn-rich P2 regions show the best stability in air. High-throughput methods were used to systematically screen the pseudo-ternary system and identify over 50 single-phase materials of potential interest for battery applications.
JOURNAL OF MATERIALS CHEMISTRY A
(2021)
Article
Chemistry, Physical
Ming-Yi Chen, Ngoc Thanh Thuy Tran, Ahmed Abubakar Alao, Wen-Dung Hsu
Summary: This study demonstrates the significance of surface Pt atom arrangement for the efficiency of ORR in PEMFCs and reveals the correlation between Pt-Pt average distance and O2 dissociation barrier. Furthermore, the study discovers a robust correlation between the level of the catalyst's d-band center and O2 adsorption energy. High-entropy alloy substrates provide potential for controlling Pt arrangement and O2 dissociation barrier.
APPLIED CATALYSIS A-GENERAL
(2024)
Article
Chemistry, Physical
Eduardo C. Atayde Jr, Babasaheb M. Matsagar, Yu-Cheng Wang, Kevin C. -W. Wu
Summary: This study presents the first application of an acidic MOF, Sulfated MOF-808, in catalyzing the HAA reactions of furan oligomers for the production of biofuel precursors. The catalyst showed high yield, selectivity, and recyclability, making it versatile for different starting materials.
APPLIED CATALYSIS A-GENERAL
(2024)
Article
Chemistry, Physical
Maria do Carmo Rangel, Francieli Martins Mayer, Soraia Jesus de Oliveira, Sergio Gustavo Marchetti, Fabricio Luiz Faita, Doris Ruiz, Giovanni Saboia, Mariana Kieling Dagostini, Jonder Morais, Maria do Carmo Martins Alves
Summary: This study developed a new catalyst by investigating the effect of magnesium on the catalytic properties of hematite in ethylbenzene dehydrogenation. The catalyst showed important differences in activity, selectivity, and stability, making it a promising candidate for commercial applications.
APPLIED CATALYSIS A-GENERAL
(2024)
Article
Chemistry, Physical
Yanjun Li, Qian Wang, Hui Tian, Mingyuan Zhu, Yuanyuan Liu
Summary: A novel strategy using microwave-assisted precipitation was proposed to prepare defective CsH3PMo11VO40 catalyst for the oxidation of methacrolein to methacrylic acid. Microwave treatment accelerates crystallization, increases vanadyl species content, and forms defective Keggin structures, thereby enhancing the oxidation capacity of the catalyst.
APPLIED CATALYSIS A-GENERAL
(2024)
Article
Chemistry, Physical
Rajeshwari Athavale, Sailee Gardi, Fatima Choudhary, Dayanand Patil, Nandkishor Chandan, Paresh More
Summary: In this study, a novel acidic ionic liquid catalyst was prepared and used for the synthesis of bis-indolyl methane derivatives. The catalyst exhibited short reaction times, easy purification, and reusability.
APPLIED CATALYSIS A-GENERAL
(2024)
Article
Chemistry, Physical
Masatomo Hattori, Takato Hattori, Masakuni Ozawa
Summary: Cu-added gamma-Al2O3 catalysts were prepared with varying Cu loadings and the effects of copper oxidation states on catalytic activity were investigated. The results showed that the addition of copper increased the catalyst activity, but excessive copper loading decreased catalytic activity. XRD and TEM analysis indicated the formation of a solid solution of copper oxide species on the surface of gamma-Al2O3. XAS and TPR data demonstrated variations in copper oxidation states among the catalysts.
APPLIED CATALYSIS A-GENERAL
(2024)
Article
Chemistry, Physical
Liwei Fang, Shiyang Niu, Shengsen Wang, Yiqing Lu, Yuanhui Cheng
Summary: In this study, PtNi alloy on nitrogen-doped carbon and SnO2 dual-support was designed to modulate the metal-support interaction, resulting in improved catalytic activity and stability for oxygen reduction reaction. The SnO2/PtNi/NC catalyst exhibited a strongly coupled interface, enhanced electron transfer, and higher half-wave potential compared to PtNi/NC and commercial Pt/C.
APPLIED CATALYSIS A-GENERAL
(2024)
Article
Chemistry, Physical
Shohei Harada, Duanxing Li, Kenta Iyoki, Masaru Ogura
Summary: This study investigates the catalytic performance of a composite catalyst composed of ZnZrOX and H-zeolite for the hydrogenation of CO2. The deactivation of the composite catalyst is influenced by ion exchange of Zn2+ and/or coke, with their effects differing based on the zeolite structure. Separating the grains of the composite catalyst can prevent deactivation.
APPLIED CATALYSIS A-GENERAL
(2024)
Article
Chemistry, Physical
Laura Proano, Christopher W. Jones
Summary: In this study, NiGa alloy particles supported on CeO2, ZrO2, and ZrO2-CeO2 solid solutions were prepared and characterized. The nature of the support was found to have a significant influence on the catalyst's activity and selectivity, with the crystalline structure of ZrO2 having the greatest impact. Pure ZrO2 showed the highest methanol selectivity and CO2 conversion at high Zr:Ce ratios. In equimolar and Ce-rich conditions, basic sites and oxygen vacancies were found to be the key parameters affecting methanol production.
APPLIED CATALYSIS A-GENERAL
(2024)
Article
Chemistry, Physical
Liyan Zhang, Yinze Yang, Leilei Zhou, Fengyu Zhao, Haiyang Cheng
Summary: 1,6-Hexamethylenediamine was successfully synthesized via the reductive amination of 1,6-hexanediol using a Ru/PRL(x)-Al2O3 catalyst. The highly dispersed and anchored Ru species, formed by 1,10-phenanthroline (PRL), played a crucial role in the catalytic reaction. The formation of new acid-base pairs, electron deficient Ru species, and smaller nanoparticles contributed to the improved catalytic performances of the Ru/PRL-Al2O3 catalyst.
APPLIED CATALYSIS A-GENERAL
(2024)
Article
Chemistry, Physical
Anita Horvath, Miklos Nemeth, Andrea Beck, Gyorgy Safran, Valeria La Parola, Leonarda Francesca Liotta, Gregor Zerjav, Matevz Roskaric, Albin Pintar
Summary: This study investigates the catalytic and structural changes caused by the addition of 0.25 wt% indium in a 3% Ni/CeO2-Al2O3 catalyst prepared by impregnation method. The results show that the addition of indium can decrease the activity of the catalyst, but it improves its stability and reduces coking.
APPLIED CATALYSIS A-GENERAL
(2024)
Article
Chemistry, Physical
Ankush Kularkar, Vaibhav Vilas Khedekar, Sachin D. Chaudhari, Mudavath Ravi, Sadhana S. Rayalu, Penumaka Nagababu
Summary: Efficiently addressing the challenges of photocatalytic CO2 reduction to CH3OH is crucial. This study developed Zn-BTC MOF and its composites with CaIn2S4, achieving highly efficient and robust photocatalytic CO2 reduction to CH3OH under ambient conditions, using H2O2 as the hydrogen source. Among the composites, ZMCIS4 demonstrated excellent performance with a CH3OH evolution of 49100 μmol/g.cat and a quantum efficiency of approximately 78.41%. The enhanced performance was attributed to the production of nascent hydrogen atoms (H center dot) through the photo-splitting of H2O2 on the ZMCIS surface.
APPLIED CATALYSIS A-GENERAL
(2024)
Article
Chemistry, Physical
Dan Liu, Yudong Li, Chengyu Wang, Haiyue Yang, Rong Wang, Shujun Li, Xiaohui Yang
Summary: In this study, a self-supporting three-dimensional porous Co3O4 nanobelt array decorated on nickel foam (P-Co3O4 -NBA@NF) electrode with numerous active sites was successfully constructed for the oxidation of 5-Hydroxymethylfurfural (HMF) to 2,5-furan dicarboxylic acid (FDCA). The P-Co3O4 -NBA@NF electrode demonstrated high conversion efficiency, selectivity, and Faraday efficiency, as well as remarkable long-term stability. This research provides a promising electrocatalyst for biomass conversion.
APPLIED CATALYSIS A-GENERAL
(2024)
Article
Chemistry, Physical
Yimin Li, Enggah Kurniawan, Fumiya Sato, Takayoshi Hara, Yasuhiro Yamada, Satoshi Sato
Summary: In this study, several silica-alumina catalysts modified with Ag were examined for the dehydration of 1,3-butanediol to 1,3-butadiene. Among them, an amorphous silica-alumina catalyst (SAL-3) modified with Ag showed the highest improvement in catalytic activity and stability when operated in H2 flow. The generation of reversible acid sites was found to be the reason behind the enhanced activity and stability of this Ag/SAL-3 catalyst. The effects of various parameters on the catalytic activity of Ag/SAL-3, such as reaction temperature, contact time, Ag content, and carrier gas, were investigated.
APPLIED CATALYSIS A-GENERAL
(2024)