Article
Chemistry, Multidisciplinary
Rui Shi, Wenjie Liao, Pedro J. Ramirez, Ivan Orozco, Mausumi Mahapatra, Jindong Kang, Adrian Hunt, Iradwikanari Waluyo, Sanjaya D. Senanayake, Ping Liu, Jose A. Rodriguez
Summary: This study investigates the structure and reactivity of potassium oxides in contact with the gold surface, using various techniques. It reveals a significant correlation between the structure, oxidation state, and chemical activity of the alkali oxide.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Applied
Ryohei Sato, Yutaka Amao
Summary: The study investigates the participation of protein motions in the biocatalytic reaction of formate oxidation catalyzed by CbFDH by means of isotope substitution of the substrate. It is found that isotope-labelled NAD+ and deuterium or 13C-labelled formate exhibit an isotope effect in the formate oxidation reaction, while 13C-labelled formate does not significantly affect the reaction rate. The results suggest that C-H bond cleavage of formate and nucleophilic attack of hydrogen on NAD+ dominate the reaction rate in CbFDH-catalyzed formate oxidation, and the hydrogen bonds formed between formate, NAD+, and water molecules also play an important role in the oxidation of formate to CO2.
Article
Engineering, Environmental
Zhen Li, Xiyang Wang, Xinbo Li, Minli Zeng, Carl Redshaw, Rui Cao, Ritimukta Sarangi, Changmin Hou, Zuolong Chen, Wenhua Zhang, Nannan Wang, Xiaofeng Wu, Yanqiu Zhu, Yimin A. Wu
Summary: Cation segregation near the surface or interfaces of solid catalysts is crucial for catalytic reactions. Perovskite oxides are often hindered by passivated A-site segregation, affecting their catalytic activity and durability. This study presents a wet exsolution method to reconstruct surface segregation in perovskite cobalt oxide, successfully transforming inert surface Sr segregation into active Co3O4 segregation. By controlling the reaction time, different coverage of active Co3O4 segregation on the perovskite oxide surface was achieved. The results reveal a volcano-shaped relationship between CO oxidation activity and the coverage of Co3O4 segregation, with optimal coverage significantly enhancing catalytic activity through improved interface interactions.
JOURNAL OF HAZARDOUS MATERIALS
(2022)
Article
Chemistry, Physical
Chetan Joshi, Juliet M. Macharia, Joseph A. Izzo, Victor Wambua, Sungjin Kim, Jennifer S. Hirschi, Mathew J. Vetticatt
Summary: Experimental and theoretical C-13 kinetic isotope effects (KIEs) were used to gain atomistic insight into the catalytic mechanism of the Pd(PPh3)(4)-catalyzed Suzuki-Miyaura reaction. The results suggest that oxidative addition of aryl bromides occurs to a 12-electron monoligated palladium complex (Pd(PPh3)). It was also found that the binding of iodoarene to Pd(PPh3) likely precedes oxidative addition. The transmetalation step was shown to proceed via a tetracoordinate boronate (8B4) intermediate with a Pd-O-B linkage.
Article
Chemistry, Inorganic & Nuclear
Xi Liang, Shuaishuai Zhang, Meng Zhao, Jing Xu, Yang Yu, Shuyan Song, Hongjie Zhang
Summary: Co3O4/CeO2 multi-shelled nanospheres with various Ce/Co ratios were prepared using a bimetallic coordination polymer as a sacrificial template for low-temperature CO oxidation. The addition of cerium significantly increased the surface area, enriching oxygen vacancies and enhancing accessible active sites, leading to superior catalytic performance. This work presents an alternative approach for constructing multi-shelled nanosphere composites.
DALTON TRANSACTIONS
(2021)
Article
Chemistry, Inorganic & Nuclear
Le Zhang, Feng Huo, Anqi Wang, Shaohua Chai, Jian Guan, Guijun Fan, Wuxinchen Yang, Guojun Ma, Ning Han, Yunfa Chen
Summary: Currently, the active sites of cobalt (Co) cations in different coordination structures remain elusive and challenging, despite the potential of Co-based oxides in catalytic ozone elimination. In this study, controllable synthesis of different Co-based oxides were achieved and their valences and coordinations were verified. The ozone decomposition performances revealed that Co-Oh(3+) and Co-Oh(2+) in octahedral coordination were superior to Co-Td(2+) in tetrahedral coordination. Notably, MgCo with octahedral coordination exhibited the highest decomposition efficiency and remained stable after long-term running. The high activity of MgCo can be attributed to the d-orbital splitting, facilitating electron transfer in ozone decomposition reactions.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Physical
Ning Sun, Yongfeng Zhang, Liying Wang, Zhenzhu Cao, Junmin Sun
Summary: In this study, the CoyCu3-y-MOF-74 precursor material was synthesized using a cost-effective and environmentally friendly mechanochemical method. The resulting bimetallic Co-Cu oxide catalyst, M-CoyCu3-yOx, showed a high efficiency for the catalytic oxidation of toluene. The effects of calcination temperature and Co/Cu molar ratio on the catalyst's redox properties, catalytic activity, and structural properties were systematically studied. The MCo2Cu1Ox catalyst exhibited complete toluene conversion at 225℃ and with a space velocity of 30,000 ml/(g h). XPS, Raman spectroscopy, EPR, and DRIFTS experiments provided further insights into the catalyst's properties and reaction intermediates. The catalyst also demonstrated excellent durability and water resistance. The green and facile mechanical synthesis of the MOF-74 precursor proved to be beneficial for the design and synthesis of highly efficient mixed metal oxide catalysts for toluene oxidation.
JOURNAL OF ALLOYS AND COMPOUNDS
(2022)
Article
Chemistry, Applied
Ping Li, Xiaoyin Chen, Yongdan Li, Johannes W. Schwank
Summary: La0.9Sr0.1CoO3 perovskite oxides were prepared by hard template and sol-gel methods, with the former showing improved catalytic activity for CO and C3H6 oxidation due to higher surface area and easier oxygen release. Both catalysts demonstrated stable activity for simultaneous oxidation of CO and C3H6 under simulated diesel exhaust conditions.
Article
Engineering, Environmental
Liantao Sun, Xiaoliang Liang, Hongmei Liu, Haijie Cao, Xuehua Liu, Ye Jin, Xingyun Li, Sheng Chen, Xiaodong Wu
Summary: Defects engineering in metal oxide is crucial for enhancing the catalytic oxidation of VOCs. In this study, the influence of crystal facet of Co3O4 on propane oxidation was investigated, and intelligent Cu doping was performed on the most active (110) facet exposed Co3O4 catalyst. The optimized catalyst demonstrated significantly enhanced activity by activating Co-O bond and generating active oxygen species. This study provides valuable insights for the design of non-precious metal catalysts in VOCs abatement.
JOURNAL OF HAZARDOUS MATERIALS
(2023)
Article
Engineering, Environmental
Xiaomin Cheng, Xiao Wang, Cheng Ma, Jitong Wang, Wenming Qiao, Licheng Ling
Summary: The schistose-like Mn-Co oxides synthesized by thermal decomposition of inorganic salts show high conversion rates and stability as catalysts for low-temperature NO oxidation.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2022)
Article
Engineering, Environmental
Huafang Li, Qi Pan, Jianxun Liu, Wei Liu, Qian Li, Liguo Wang, Zhongpeng Wang
Summary: In this study, a series of Pr6O11 catalysts were developed by CTAB-assisted coprecipitation method and their catalytic performances for soot oxidation and NOx adsorption were investigated. The Pr6O11 catalysts exhibited excellent catalytic activities for both soot oxidation and NOx adsorption at low temperature, which was attributed to their relatively large surface area, strong NO oxidation ability, and high intrinsic activity. The presence of NO was found to promote the soot oxidation, and the possible mechanism of the soot oxidation reaction process was explored using in situ DRIFTS.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2023)
Article
Chemistry, Physical
Liman Fan, Mingyang Li, Cheng Zhang, Ahmed Ismail, Boren Hu, Yujun Zhu
Summary: By adjusting the Cu/Co ratio and optimizing the surface properties of the catalyst, the activity of the oxidant can be improved, leading to a more efficient toluene oxidation reaction.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2021)
Article
Multidisciplinary Sciences
Si Woo Lee, Jong Min Kim, Woonghyeon Park, Hyosun Lee, Gyu Rac Lee, Yousung Jung, Yeon Sik Jung, Jeong Young Park
Summary: The interaction between metal and oxides is a crucial factor influencing the selectivity of a desirable reaction. Designing a well-formed metal-oxide interface in a heterogeneous catalyst is important for understanding selectivity and surface electronic excitation at the interface. The study demonstrates the real-time detection of hot electron flow and impact of metal-oxide interface on catalytic selectivity in a nanoscale catalytic Schottky diode.
NATURE COMMUNICATIONS
(2021)
Article
Chemistry, Multidisciplinary
Mei Wang, Lei Qi, Xinheng Li
Summary: Oxygen defects in Co3O4 crystals were found to be crucial in improving catalytic activity for the removal of propane.
Article
Chemistry, Multidisciplinary
Kyung Rok Lee, Danim Yun, Dae Sung Park, Yang Sik Yun, Chyan Kyung Song, Younhwa Kim, Jungwon Park, Jongheop Yi
Summary: The d-band centers of Au and Pt metals are upshifted when an electric field is applied, leading to enhanced CO adsorption strength and consequent changes in CO conversions in CO oxidation reactions.
CHEMICAL COMMUNICATIONS
(2021)
Article
Energy & Fuels
Jixi Zhang, Yutong Liu, Rodney D. L. Smith
Summary: This study analyzed structural defects in hematite photoanodes and identified three types of defects that exert unique influences on photoelectrochemical behavior, each dominant under specific fabrication conditions. The research provides a straightforward approach to detecting defects in photoelectrodes and determining their impact on photoelectrode properties and behavior.
Article
Nanoscience & Nanotechnology
Yutong Liu, Rodney D. L. Smith
Summary: The highly variable behavior and performance of hematite as photoanodes for the oxygen evolution reaction highlight the importance of understanding the interplay between defects and photoelectrochemical performance. By analyzing the structure-property relationship of hematite samples synthesized under different environments, it was found that different defects, namely oxygen vacancies and iron vacancies, affect the photoelectrochemical performance. These defects cause structural distortions that can be observed using Raman spectroscopy.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Multidisciplinary
Giovanna M. A. Rogati, Chiara Capecci, Enza Fazio, Scolastica Serroni, Fausto Puntoriero, Sebastiano Campagna, Leonardo Guidoni
Summary: The structure of a decanuclear dendrimer based on Ru(II) polypyridine subunits, suitable for artificial photosynthesis as a light-harvesting species, has been investigated through computer modeling. Molecular dynamics and quantum mechanics simulations were used to study the stability of possible isomers of each monomer, revealing a prevalence of MER isomerism in the central core. Additionally, the self-aggregation of the dendrimer and the distribution of counterions around the complexes were investigated using Molecular Dynamics in both implicit and explicit acetonitrile solution, suggesting a self-aggregation mechanism for the dendrimers.
CHEMISTRY-A EUROPEAN JOURNAL
(2022)
Correction
Chemistry, Inorganic & Nuclear
Nataraju Bodappa, Sarah Stepan, Rodney D. L. Smith
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Physical
Leonardo Ratini, Chiara Capecci, Francesco Benfenati, Leonardo Guidoni
Summary: The study introduces a modified VQE method named WAHTOR, which adapts the form of the molecular Hamiltonian to the circuit ansatz through an optimization procedure, making it more flexible. The method has been successfully applied to simulations of small molecules, demonstrating advantages over traditional VQE methods, being less dependent on circuit topology and less likely to be trapped in high-energy local minima.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2022)
Review
Plant Sciences
Mehdi Khosravi, Mohammad Reza Mohammadi
Summary: There has been an increasing interest in water oxidation in recent years, particularly due to the discovery of a mysterious catalytic layer formed upon applying an anodic potential to an indium tin oxide electrode immersed in a phosphate buffer containing Co-(II) ions. This has led to research focusing on better understanding the catalyst layer, improving performance, and designing cobalt coordination complexes for water splitting. Although debates remain regarding the true catalysts responsible for water oxidation, this review mainly highlights recent progress and developments in the design and application of cobalt oxide-based materials in catalytic, electrocatalytic, photocatalytic, and photoelectrocatalytic water oxidation reactions.
PHOTOSYNTHESIS RESEARCH
(2022)
Article
Chemistry, Physical
A. Reyhani, S. Z. Mortazavi, A. Taherkhani, M. R. Mohammadi, M. Mehrabi, P. Parvin
Summary: Pd nanoparticles were decorated on MWCNTs using various techniques, and the hydrogen adsorption mechanism was studied using X-ray absorption spectroscopy. Results showed the presence of Pd-Pd and Pd-C(O) bonds in the samples, with bond restructuring occurring during cycles of exposure to He/H2. The heating process under He/H2 exposure had a destructive effect on the Pd-C(O) bonds, and hydrogen adsorption resulted in an enlargement of the Pd-Pd bond distance, with PLAL samples experiencing more significant changes in bond distances.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Plant Sciences
Mario Frezzini, Anna Scortica, Matteo Capone, Daniele Narzi, Manuel Benedetti, Francesco Angelucci, Benedetta Mattei, Leonardo Guidoni
Summary: OGOX1 is an enzyme that oxidizes pectin fragments (OGs) and releases H2O2, thereby reducing the activity of OGs. Molecular dynamics simulations and enzyme kinetics studies have revealed the molecular determinants of OGOX1 that are responsible for binding OGs of different lengths. The results suggest that the binding between OGOX1 and OG5 is the most stable, with salt-bridge interactions stabilizing the optimal conformation of OG5 for efficient oxidation by the enzyme.
PLANT PHYSIOLOGY AND BIOCHEMISTRY
(2023)
Article
Energy & Fuels
Jhon Paniagua Rojas, Joaquin E. Gonzalez-Hernandez, Jorge M. Cubero-Sesin, Zenji Horita, Diego Gonzalez-Flores
Summary: Aluminum-air batteries are a promising alternative for high-energy density storage, but the self-corrosion of aluminum alloys in alkaline electrolytes hinders their performance. In this study, severe plastic deformation (SPD) technique was used to improve the corrosion resistance of various aluminum alloys. The ultrafine-grained microstructure achieved through SPD improved the corrosion resistance, and Al-3%Mg alloy demonstrated the best performance in an aluminum-air cell.
Article
Chemistry, Multidisciplinary
Mohamad Zandieh, Una E. Hogan, Rodney D. L. Smith, Juewen Liu
Summary: The wettability of microplastics can change due to surface transformations. This study investigated the adsorption of spherical nucleic acids (SNAs) and linear DNA on microplastics to understand their wettability. Soaking microplastics in water for 3 months increased SNA adsorption, while the adsorption of linear DNA remained the same. Reversibility was observed when the soaked microplastics were dried and rehydrated. Heating the microplastics had a similar effect to long-term soaking.
Article
Multidisciplinary Sciences
Paul Greife, Matthias Schoenborn, Matteo Capone, Ricardo Assuncao, Daniele Narzi, Leonardo Guidoni, Holger Dau
Summary: Photosynthesis stores solar energy in chemical form, which supports life on Earth. The splitting of water at the manganese cluster of photosystem II during photosynthesis has resulted in an oxygen-rich atmosphere. This study reveals the crucial stage of oxygen formation in photosynthesis and its mechanistic role.
Article
Chemistry, Physical
Gianluca Parisse, Daniele Narzi, Benny Danilo Belviso, Vito Capriati, Rocco Caliandro, Massimo Trotta, Leonardo Guidoni
Summary: Deep eutectic solvents (DESs) are versatile solvents that can be manipulated to improve the performance of biomolecules. A recent study has investigated the effects of hydrated DESs on protein dynamics using molecular dynamics simulations. The results show that DESs can restrict protein motion and increase the overall structural rigidity. Furthermore, specific interactions between DES components and protein residues have been identified, suggesting the potential for protein crystallization in the presence of hydrated DESs.
JOURNAL OF PHYSICAL CHEMISTRY B
(2023)
Proceedings Paper
Health Care Sciences & Services
Julio Castro, Carolina Flores, Diego Gonzalez, Vanessa Quintero, Aramis Perez
Summary: The way towards managing end-of-life lithium-ion batteries is crucial for a sustainable energy future. Developing simple tests to understand the potential of degraded batteries for less demanding applications is of utmost importance.
2022 PROGNOSTICS AND HEALTH MANAGEMENT CONFERENCE, PHM-LONDON 2022
(2022)
Article
Chemistry, Multidisciplinary
Guangye Han, Petko Chernev, Stenbjorn Styring, Johannes Messinger, Fikret Mamedov
Summary: Photosynthesis is a vital process for storing solar energy as chemical energy, and the efficiency of this process is crucial. In this study, the turnover efficiency of different S states in the Photosystem II reaction was quantified using electron paramagnetic resonance spectroscopy. The results showed that the turnover efficiencies were limited by reactions occurring in the water oxidizing complex. Structural changes and chemical events during the reaction cycle were found to be correlated to the low efficiencies. These findings were confirmed by measurements of flash-induced oxygen release patterns and explained based on S state dependent structural changes at the CaMn4O5-cluster.
Article
Chemistry, Multidisciplinary
Elif Pinar Alsac, Keyu Zhou, Wen Rong, Soma Salamon, Joachim Landers, Heiko Wende, Rodney D. L. Smith
Summary: The uniform electrochemical behavior of FexNi1-x(OH)(2) is remarkable despite variations in fabrication protocols and composition-dependent structural changes. Multiple unique Fe(iii) coordination environments exist in these materials, and the presence of formamide affects their structure and performance. Iron ions within the Ni(OH)(2) lattice are deemed to be the catalytically relevant feature.
ENERGY & ENVIRONMENTAL SCIENCE
(2022)