Review
Chemistry, Applied
Jing Du, Yuan-Yuan Ma, Huaqiao Tan, Zhen-Hui Kang, Yangguang Li
Summary: Electrochemical CO2 reduction to value-added fuels and chemicals is an effective strategy due to its high efficiency and economic feasibility. Polyoxometalates (POMs) are promising candidates for efficient CO2RR electrocatalysts and play significant roles in the process and performance of catalytic CO2RR.
CHINESE JOURNAL OF CATALYSIS
(2021)
Article
Chemistry, Inorganic & Nuclear
Tao Song, Hai Liu, Errui Liu, Fei Wang, Li Cui, Xiaoli Zhang, Tianxia Liu
Summary: This study reported a strategy to promote the electrochemical reduction of carbon dioxide to carbon monoxide in CuO nanosheets by metal doping. The CuO/Bi, CuO/In, and CuO/Sn catalysts showed high efficiency and selectivity for the electrocatalytic reduction of carbon dioxide to carbon monoxide at low overpotential, while inhibiting the occurrence of hydrogen evolution reaction. Moreover, the CuO/Sn catalyst demonstrated excellent stability in 0.1 mol/L KHCO3 electrolyte, with a constant current density for 6 hours.
INORGANIC CHEMISTRY COMMUNICATIONS
(2023)
Article
Nanoscience & Nanotechnology
Qian Xiang, Fan Li, Jiale Wang, Wenlong Chen, Qiushi Miao, Qingfeng Zhang, Peng Tao, Chengyi Song, Wen Shang, Hong Zhu, Tao Deng, Jianbo Wu
Summary: The study demonstrates that in situ synthesis of ZnO on Zn foil can significantly enhance the CO2 reduction performance, leading to higher Faraday efficiency for CO and improved stability. This enhancement is attributed to the exposed edge facets of ZnO that accelerate electron transfer and increase the number of active sites.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Physical
Yongjie Xi, Tingting Wang, Jia Wang, Jinlei Li, Fuwei Li
Summary: This study comprehensively investigates the mechanism of CO2 hydrogenation to ethanol, revealing the crucial role of CO surface coverage in affecting the reaction energy profiles. CO adsorption facilitates the CH-CO coupling and CH hydrogenation, increasing the selectivity towards ethanol.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Marcel J. J. Rost, Leon Jacobse, Marc T. M. Koper
Summary: By analyzing the distribution of nuclei-distance, it is found that a rare and non-random nucleation process occurs in chemical surface systems. This process involves the formation of special, preferential nucleation sites via a precursor, eventually leading to a semi-ordered Pt-oxide structure. This precursor mechanism may also explain the formation of nano-islands on other surfaces/reactions.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Review
Chemistry, Physical
Jinxian Feng, Jun Ni, Hui Pan
Summary: This article discusses the prospects, challenges, and solutions of the electrochemical reduction reaction for converting CO2 to liquid fuels in aqueous conditions, emphasizing the critical importance of rational design of the composition and structure of electrocatalysts to improve reaction efficiency.
JOURNAL OF MATERIALS CHEMISTRY A
(2021)
Article
Electrochemistry
Shuyan Shao, Tao Wen, Ziqun Wang, Xiaoshuang Yin, Ying Liu, Wenzhong Yang, Yun Chen
Summary: By developing a SnSe2-graphene composite catalyst, efficient electrocatalytic reduction of CO2 to formate has been achieved, with a maximum Faraday efficiency of 95.1% under optimal conditions.
ELECTROCHIMICA ACTA
(2022)
Article
Chemistry, Physical
Timo Fuchs, Valentin Briega-Martos, Jan O. Fehrs, Canrong Qiu, Marta Mirolo, Chentian Yuan, Serhiy Cherevko, Jakub Drnec, Olaf M. Magnussen, David A. Harrington
Summary: The initial step of electrochemical surface oxidation involves extracting a metal atom from its lattice site to a location in a growing oxide. Through simultaneous electrochemical and in situ high-energy surface X-ray diffraction measurements, it has been observed that the extraction of Pt atoms from Pt(111) is a fast, potential-driven process, while the formation of adsorbed oxygen-containing species occurs at a slower rate and is not directly coupled with the extraction process. It can be concluded that potential independently plays a key role in electrochemical surface oxidation.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Timo Fuchs, Valentin Briega-Martos, Jan O. Fehrs, Canrong Qiu, Marta Mirolo, Chentian Yuan, Serhiy Cherevko, Jakub Drnec, Olaf M. Magnussen, David A. Harrington
Summary: The initial step of electrochemical surface oxidation involves the extraction of metal atoms from their lattice sites to form a growing oxide. By conducting fast simultaneous electrochemical and in situ high-energy surface X-ray diffraction measurements, it has been demonstrated that the extraction of Pt atoms from Pt(111) is a fast process driven by potential, while the charge transfer for the formation of oxygen-containing species occurs at a much slower rate and appears to be decoupled from the extraction process. It is thus concluded that potential plays an independent and crucial role in electrochemical surface oxidation.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Review
Chemistry, Multidisciplinary
Yueshen Wu, Yongye Liang, Hailiang Wang
Summary: Heterogenization of molecular catalysts on substrates allows for optimization of CO2 electroreduction reactions, with factors like active material dispersion and support conductivity playing crucial roles in controlling activity. Modifying ligand substituents can enhance the redox properties of the molecule, improving catalytic activity and stability.
ACCOUNTS OF CHEMICAL RESEARCH
(2021)
Article
Chemistry, Physical
Shuai Li, Shujuan Sun, Wei Suo, Guihua Liu, Guirong Wang, Yanji Wang, Jingde Li, Zisheng Zhang
Summary: Density functional theory was used to study the reduction mechanism of CO2 on Cu, Sn@Cu, and Sn surfaces in this research. The results suggest that doping Sn onto the Cu surface may be a potential strategy for improving the efficiency of CO2 electrocatalyst.
APPLIED SURFACE SCIENCE
(2021)
Article
Chemistry, Analytical
Silvia Mena, Esteve Ribas, Clara Richart, Iluminada Gallardo, Jordi Faraudo, Scott K. Shaw, Gonzalo Guirado
Summary: The paper focuses on the role of carbon dioxide in controlling the Earth's temperature and the environmental problems caused by its increased concentration in the atmosphere. It discusses the use of ionic liquids for efficient CO2 capture and conversion, utilizing electrochemical, spectroscopic, and molecular dynamics techniques to understand the reduction mechanism under various conditions. The research opens up possibilities for theoretical-experimental approaches to determine the CO2 reduction mechanism and the dependency of product formation on the electrode material and solvent used.
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
(2021)
Article
Materials Science, Multidisciplinary
Xiaoyu Han, Nikolas Kaltsoyannis
Summary: The effect of the Hubbard U parameter on the properties of bulk PuO2 and its {111} surface was investigated using periodic boundary condition PBE+U calculations. Comparison with experimental data was conducted for various properties, including band gap, lattice parameter, hybridization of Pu 5 f and O 2 p states, peak separation in the valence band, and surface work function. A U value of 3 eV was recommended and used to study the reactions of H2O and NO on PuO2 {111}, both individually and sequentially. The role of Pu 5 f band centre and its relation to the Fermi level were found to be significant in determining the reactions.
JOURNAL OF NUCLEAR MATERIALS
(2023)
Article
Chemistry, Physical
Najrul Hussain, Mohammad Ali Abdelkareem, Hussain Alawadhi, Shamima Begum, Khaled Elsaid, A. G. Olabi
Summary: The synthesis and characterizations of the tricomponent CuO-ZnO-MoS2 composite material is reported for the first time in this work. The composite possessed outstanding catalytic performance in CO2 reduction to alcohol with maximum faradaic efficiency of 24.6% for methanol and 11.1% for ethanol.
JOURNAL OF POWER SOURCES
(2022)
Review
Chemistry, Multidisciplinary
Yingji Zhao, Lingling Zheng, Dong Jiang, Wei Xia, Xingtao Xu, Yusuke Yamauchi, Jianping Ge, Jing Tang
Summary: Using metal-organic frameworks (MOFs) for electrochemical CO2 reduction reaction (CO2RR) processes has attracted considerable research attention due to their atomically dispersed active sites, large surface area, high porosity, controllable morphology, and remarkable tunability. The improvement of conductivity, introduction of active centers, and formation of carbon-based single-atom catalysts (SACs) from well-defined MOFs have been explored for the development of CO2 conversion. The review summarizes the progress on pristine MOFs, MOF hybrids, and MOF-derived carbon-based SACs for the electrocatalytic reduction of CO2, and discusses the limitations and potential improvement directions in this field of research.
Article
Chemistry, Physical
Bjoern Kirchhoff, Christoph Jung, Hannes Jonsson, Donato Fantauzzi, Timo Jacob
Summary: The activity and stability of platinum nanoparticles are influenced by their shape. In this study, a simulation method was used to investigate the oxidation process and behavior of platinum nanoparticles with different shapes, and a relationship between oxidation behavior and surface structure was established.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Yorick L. A. Schmerwitz, Aleksei Ivanov, Elvar O. Jonsson, Hannes Jonsson, Gianluca Levi
Summary: A variational, time-independent density functional approach is used to accurately describe the energy surfaces of twisting and pyramidal distortion in ethylene, even with the use of a semilocal functional approximation. The findings suggest the possibility of using a single determinant time-independent density functional approach for simulating nonadiabatic dynamics in large systems.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Physical
Abid Ali, Hannes Jonsson
Summary: This study uses density functional theory calculations to investigate the atomic scale transitions corresponding to diffusion and interlayer transport of a Au adatom on the low energy, close packed Au(111) surface. The results suggest that kinks on island edges provide paths for adatom descent and a descent mechanism near kink sites can promote the formation of new rows of step atoms, opening up new low activation energy paths for 2D growth.
SURFACES AND INTERFACES
(2022)
Article
Electrochemistry
G. S. Sun, H. Jonsson
Summary: Kinetic Monte Carlo simulations were used to study the factors that affect the shape of islands during growth, including the difference in adatom binding energy at different types of edges, the height of diffusion barriers, incident flux, and temperature. The results showed that the shape of the islands and the growth mode of the crystal are strongly influenced by these factors. An unexpected edge nucleation effect was observed, which significantly affects the shape of small islands, especially at low flux.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2022)
Article
Chemistry, Physical
Elvar Orn Jonsson, Soroush Rasti, Marta Galynska, Jorg Meyer, Hannes Jonsson
Summary: This study presents a potential function for describing a system of flexible H2O molecules, which accurately reproduces the results of high-level electronic structure calculations. The function includes various multipole expansion coefficients and adjustable parameters to achieve good agreement with experimental measurements, representing a significant improvement over previous rigid models.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2022)
Article
Chemistry, Physical
Hemanadhan Myneni, Elvar Orn Jonsson, Hannes Jonsson, Asmus Ougaard Dohn
Summary: A polarizable potential function for acetonitrile molecules is introduced and compared with electronic structure calculations, showing good agreement.
JOURNAL OF PHYSICAL CHEMISTRY B
(2022)
Article
Chemistry, Physical
Jan Kloppenburg, Livia B. Partay, Hannes Jonsson, Miguel A. Caro
Summary: A Gaussian approximation machine learning interatomic potential for platinum is developed based on density-functional theory (DFT) data. The potential exhibits excellent transferability and agreement with DFT in various properties such as bulk elasticity, surface energetics, and nanoparticle stability. It provides state-of-the-art accuracy at a low computational cost. Two examples are presented to demonstrate the potential's capability in modeling Pt systems: the pressure-temperature phase diagram of Pt calculated using nested sampling and a study of the spontaneous crystallization of a large Pt nanoparticle based on classical dynamics simulations over several nanoseconds.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Yorick L. A. Schmerwitz, Gianluca Levi, Hannes Jonsson
Summary: Excited electronic states are calculated by finding saddle points on the energy surface. This method has advantages in density functional calculations as it avoids collapse to the ground state and allows for variationally optimized orbitals. A mode following method is presented to find higher-order saddle points, allowing for calculations even at avoided crossings. Results are presented for charge transfer excitations and a diplatinum-silver complex, demonstrating the applicability of the method to larger molecules.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Materials Science, Multidisciplinary
M. N. Potkina, I. S. Lobanov, H. Jonsson, V. M. Uzdin
Summary: The lifetime of a magnetic skyrmion in a two-dimensional lattice is investigated and found to increase with the size of the skyrmion. This is due to the decrease in entropy of the transition state compared to the skyrmion state, resulting in a significant increase in the pre-exponential factor, and the activation energy reaching an upper bound. The largest skyrmions studied include over 20,000,000 spins.
Article
Chemistry, Physical
Sander o. Hanslin, Hannes Jonsson, Jaakko Akola
Summary: Transition metal dichalcogenides (TMDs) are inexpensive and abundant alternatives to precious metals as catalyst materials. Experimental measurements show that MoS2 has significant electrocatalytic activity for the hydrogen evolution reaction (HER). However, the activity varies depending on the preparation method. To understand the mechanism and active sites for HER, calculations were performed on transition metal doped basal plane of MoS2 under electrochemical conditions, taking into account electrode potential and solvent effects.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Materials Science, Multidisciplinary
Moritz Sallermann, Hannes Jonsson, Stefan Bluegel
Summary: Magnetic hopfions are three-dimensional, string-like topological solitons with a Hopf number. They serve as a fundamental prototype for magnetic quasiparticles and have potential applications in spintronics. While their existence has been predicted in certain magnets, the physical realization of freely moving hopfions in bulk magnets has been challenging.
Article
Chemistry, Physical
Alec E. Sigurdarson, Yorick L. A. Schmerwitz, Dagrun K. V. Tveiten, Gianluca Levi, Hannes Jonsson
Summary: In this study, density functional calculations were performed on several molecules to investigate their Rydberg excited states up to high energy. The results show that the generalized gradient approximation (GGA) functional of Perdew, Burke, and Ernzerhof (PBE) can accurately predict the excitation energy when combined with self-interaction correction and complex-valued orbitals. The results from the Tao, Perdew, Staroverov, and Scuseria (TPSS) and r2SCAN meta-GGA functionals did not provide a systematic improvement over the uncorrected PBE functional.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Sander O. Hanslin, Hannes Jonsson, Jaakko Akola
Summary: This study employs a grand-canonical approach to calculate the kinetics of the hydrogen evolution reaction on intrinsic sites of MoS2. The results reveal that certain edge configurations, particularly S-deficient edges on the Mo-termination, exhibit significantly higher activity. The findings suggest that catalyst design for transition metal dichalcogenides should focus on modifying the metal sites rather than activating the chalcogen sites.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Materials Science, Multidisciplinary
Alejandro Pena-Torres, Abid Ali, Michail Stamatakis, Hannes Jonsson
Summary: Calculations reveal that the diffusion of a Au adatom on the reconstructed Si(100)-2 x 1 surface involves an indirect mechanism where the adatom is promoted to higher-energy sites on top of a dimer row before migrating along the row. This top-of-row mechanism becomes more significant at lower temperatures.
Article
Chemistry, Multidisciplinary
Jan Kloppenburg, Andreas Pedersen, Kari Laasonen, Miguel A. Caro, Hannes Jonsson
Summary: This study reveals that icosahedral Au clusters with three and four shells of atoms deviate significantly from commonly assumed Mackay structures. The introduction of additional atoms in the surface shell and a vacancy in the cluster's center can significantly lower the energy per atom. Similar icosahedral structures with five and six shells of atoms are also found to be more stable than Mackay icosahedra. The optimized clusters exhibit hexagonal rings at some vertices and inner shell atoms moving outward into the surface shell, which can strongly influence the properties of these clusters.