Article
Chemistry, Physical
Ruijie Hou, Ziling Zeng, Shaoshan Wang, Dengfang Tang, Yuan Tan, Xingkun Chen, Wenshao Yang, Chuanqi Huang, Qing Guo, Yunjie Ding, Xueming Yang
Summary: Oxygen dissociation and surface activation are crucial in heterogeneous catalysis and oxidation processes. In this study, we conducted scanning tunneling microscopy experiments and density functional theory calculations to investigate the oxidation process on a Co(0001) surface. Our results provide atomic-level insights into the oxidation of Co(0001) at different temperatures.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Physical
Minhua Zhang, Suocheng Chi, Heyuan Huang, Yingzhe Yu
Summary: Research shows that the addition of manganese can promote the dissociation of CO and the removal of oxygen, significantly improving dissociation efficiency.
APPLIED SURFACE SCIENCE
(2021)
Article
Chemistry, Physical
Sabine Wenzel, Dajo Boden, Richard van Lent, Elahe Motaee, Mahesh K. Prabhu, Hamed Achour, Irene M. N. Groot
Summary: We have conducted near-ambient-pressure X-ray photoelectron spectroscopy on Co(0001) model catalysts during exposure to CO and H-2 gases, relevant to Fischer-Tropsch synthesis. Our results show that at this pressure, CO is more efficient in maintaining the metallic surface of Co(0001) compared to H-2. This finding has important implications for the study and optimization of the Fischer-Tropsch synthesis process.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Zihao Fang, Anran Bao, Yuemiao Lai, Lanlan Yao, Ziling Zeng, Ruijie Hou, Junhao Li, Dengfang Tang, Xiao Chen, Chuanqi Huang, Yuan Tan, Xingkun Chen, Qing Guo, Xueming Yang, Wenshao Yang
Summary: The interaction of CO with oxygen-poisoned Co(0001) surface was investigated using scanning tunneling microscopy, temperature-programmed desorption, and density functional theory calculation. The study provided direct visualization of the CO adsorption process and revealed the poisoning effect of oxygen on the catalyst.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Alexander Bagger, Oliver Christensen, Vladislav Ivanistsev, Jan Rossmeisl
Summary: This work investigates the theoretical differences and similarities of CO2/CO catalytic reduction reactions in gas, aqueous solution, and aprotic solution. The binding energy serves as a good descriptor for the gaseous and aqueous phases and allows catalysts to be categorized by reduction products. However, descriptors alone are insufficient for mapping in the aprotic phase, requiring the use of a microkinetic model.
Article
Chemistry, Physical
Danjo De Chavez, Jun-ya Hasegawa
Summary: To understand the influence of incongruent strain on heterogeneous catalysis, the effect of isotropic and anisotropic strains in the catalytic activity of terrace Ru(0001) and stepped Ru(1015) surfaces have been studied. Adsorption-strain relations were investigated using the d-band model and the novel eigenstress model, and it was found that strain can alter the adsorption energies and activation energies, offering a potential route to break the Bronsted-Evans-Polyani relation in catalysis.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
C. J. Weststrate, J. W. Niemantsverdriet
Summary: The adsorbate overlayer structures formed by CO on highly covered Co(0001) were investigated, and a new structure model was proposed. Different structures were found at different CO coverages, and the formation of structures was influenced by temperature and CO chemical potential. These findings are important for the characterization of catalyst surfaces.
JOURNAL OF CATALYSIS
(2022)
Article
Chemistry, Physical
B. M. Pabon, O. Rodriguez de la Fuente
Summary: The identification of the active phase of a catalyst under operando conditions is crucial in catalysis research. In this study, the CO catalytic oxidation reaction on Ru(0001) surfaces was investigated, revealing that the highest activity is achieved when a disordered and thin Ru oxide is formed at the surface under oxidizing conditions. Furthermore, it was found that defective surfaces with a high density of surface steps enhance this reaction due to the easy incorporation of atomic oxygen and the formation of the oxide.
SURFACES AND INTERFACES
(2023)
Article
Chemistry, Physical
Peng Chai, Hong Xu, Longxia Wu, Haocheng Wang, Cong Fu, Weixin Huang
Summary: This study reported an in situ NAP-XPS investigation of CO activation and hydrogenation on a Co(0001) surface, revealing distinct changes in CO coverage and decomposition under different temperatures and atmospheres. These results contribute to a better understanding of the mechanisms involved in Co-catalyzed FTS reactions.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Chemistry, Physical
Chuan Qin, Bo Hou, Jungang Wang, Zhongyi Ma, Congbiao Chen, Litao Jia, Debao Li, Mingyue Ding
Summary: The preparation of cobalt-based Fischer-Tropsch synthesis (FTS) catalysts that can be used directly in a fixed-bed reactor without the need for further reduction is crucial but challenging. This study addresses the problem by tuning the carbon deposits on the cobalt catalyst surface. A screen-like surface carbon can prevent the oxidation of metallic cobalt, resulting in high activity and low CH4 selectivity without further reduction. The role of surface carbon and penetrating carbon in FTS performance is explored, with surface carbon improving adsorption ability and long-chain hydrocarbon formation, while penetrating carbon increases undesired CH4 selectivity.
Article
Materials Science, Ceramics
Ming Hao, Peizhang Gao, Wei Liu, Baizeng Fang, Jinsheng Liang, Tingting Zhang, Youpeng Ding, Hui Zhang, Fei Wang
Summary: A novel Co/CoAl2O4/sepiolite nanocomposite was synthesized in this study, with optimal conditions identified for fabrication. The nanocomposite showed fine cobalt nanoparticles anchored on the surface of CoAl2O4, leading to higher selectivity for high-carbon hydrocarbons in Fischer-Tropsch synthesis. This work provides an effective strategy for low-cost batch fabrication of efficient cobalt-based catalysts.
CERAMICS INTERNATIONAL
(2021)
Article
Energy & Fuels
Dalia Liuzzi, Francisco J. Perez-Alonso, Sergio Rojas
Summary: Ru-Co/Al2O3 and Ru-Fe/Al2O3 catalysts prepared by reduction-deposition method exhibit high activity in Fischer-Tropsch Synthesis, showing different conversion rates and product selectivity. The interaction between Ru and Co in Ru-Co/Al2O3 enhances the activity, while Ru-Fe/Al2O3 displays superior initial performance but declines over time, with less enriched products compared to Ru/Al2O3.
Article
Chemistry, Physical
Kangzhong Shi, Lisheng Guo, Wei Zhang, Yong Jiang, Da Li, Kai Liu, Mengmeng Li, Zhaoming Xue, Song Sun, Changjie Mao
Summary: The study found that H-2 can effectively assist in the dissociation of CO on the surface of different cobalt species, thereby regulating the reaction of Fischer-Tropsch synthesis process, improving the selectivity of products and catalytic activity.
Article
Chemistry, Applied
Nothando C. Shiba, Yali Yao, Roy P. Forbes, Chike G. Okoye-Chine, Xinying Liu, Diane Hildebrandt
Summary: The study showed that mixed CoO-Co nanoparticles dispersed on a SiO2 support exhibit high activity for Fischer-Tropsch synthesis reactions, with a synergistic effect between CoO and Co degrees. This research provides valuable information for the design of commercial Fischer-Tropsch cobalt-based catalysts.
FUEL PROCESSING TECHNOLOGY
(2021)
Article
Chemistry, Physical
Tshepo Molefe, Dean Barrett, Beatriz Diaz, Roy Forbes, Neil J. Coville
Summary: This study reports on the synthesis and application of osmium nanoparticles supported on and/or encapsulated in hollow carbon spheres for Fischer-Tropsch Synthesis (FTS). It is demonstrated that the interaction between osmium and cobalt has a significant effect on the catalyst activity when loaded together. Proximity of osmium and cobalt leads to higher FTS activity and C5+ production through the primary spillover effect. This study reveals the effect of osmium on FTS catalysts for the first time.
JOURNAL OF CATALYSIS
(2023)
Article
Chemistry, Applied
Denzil Moodley, Michael Claeys, Eric van Steen, Pieter van Helden, Deshen Kistamurthy, Kees-Jan Weststrate, Hans Niemantsverdriet, Abdool Saib, Willem Erasmus, Jan van de Loosdrecht
Article
Chemistry, Applied
C. J. Weststrate, Mehdi Mahmoodinia, Mari Helene Farstad, Ingeborg-Helene Svenum, Marie D. Stromsheim, J. W. Niemantsverdriet, Hilde J. Venvik
Article
Energy & Fuels
Foteini M. Sapountzi, Elena D. Orlova, Juliana P. S. Sousa, Laura M. Salonen, Oleg I. Lebedev, Georgios Zafeiropoulos, Mihalis N. Tsampas, Hans J. W. Niemantsverdriet, Yury V. Kolen'ko
Article
Chemistry, Applied
C. J. Weststrate, Devyani Sharma, Daniel Garcia Rodriguez, Michael A. Gleeson, Hans O. A. Fredriksson, J. W. Niemantsverdriet
TOPICS IN CATALYSIS
(2020)
Article
Chemistry, Physical
Dongdong Lv, Yechen Lei, Dongsheng Zhang, Xin Song, Yong-Wang Li, J. W. H. Niemantsverdriet, Weichang Hao, Yonghong Deng, Ren Su
JOURNAL OF PHYSICAL CHEMISTRY C
(2020)
Article
Chemistry, Inorganic & Nuclear
Kgauhelo Mentoor, Linette Twigge, J. W. Hans Niemantsverdriet, Jannie C. Swarts, Elizabeth Erasmus
Summary: The treatment of silica nanopowders resulted in the generation of supported Lewis acids and Lewis bases, forming a series of frustrated Lewis pairs (FLPs) that successfully captured CO2 and converted it to formic acid. Spectroscopic characterization of the synthesized products was performed to analyze the reaction outcomes.
INORGANIC CHEMISTRY
(2021)
Article
Chemistry, Physical
Mohamed Fadlalla, Sundaram Ganesh Babu, Thulani M. Nyathi, C. J. Kees-Jan Weststrate, Nico Fischer, J. W. Hans Niemantsverdriet, Michael Claeys
Article
Chemistry, Physical
Qiqi Wu, Jiani Ye, Wei Qiao, Yongwang Li, J. W. (Hans) Niemantsverdriet, Emma Richards, Feng Pan, Ren Su
Summary: Research shows that the addition of Pd cocatalyst in the photocatalytic oxidation of VOC mixtures can effectively inhibit the formation of toxic methylphenols, promoting the complete mineralization of VOC mixtures into CO2. This is achieved by removing surface -OH groups of TiO2, activating O2 into 'OH radicals, and directing the radicals to attack the methyl group for better overall photocatalytic performance.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2021)
Article
Chemistry, Physical
Rudaviro Garidzirai, Phillimon Modisha, Innocent Shuro, Jacobus Visagie, Pieter van Helden, Dmitri Bessarabov
Summary: In this study, the effects of Mg and Zn dopants on the catalytic performance of Pt/Al2O3 catalyst for dehydrogenation of H18-DBT were investigated. The results showed that Pt/Mg-Al2O3 exhibited the highest average hydrogen flowrate and hydrogen yield, demonstrating improved catalytic performance compared to Pt/Zn-Al2O3 and Pt/Al2O3.
Article
Chemistry, Physical
Guihang Li, Xin Yu, C. J. Weststrate, Pengju Ren, Jian Xu, Qian Xu, Yong Yang, Yongwang Li, J. W. Niemantsverdriet, Xiaodong Wen, Junfa Zhu
Summary: The study shows that FeO(111) islands have a significant impact on the thermal stability of Cu2O/Cu(100) and Cu2O/Cu(100) surfaces, promoting the reduction of oxygen-covered copper surface and potential reaction with carbon atoms upon annealing. The interface plays an important role in the properties of hybrid surface structures.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Chemistry, Multidisciplinary
Yuel W. Abraha, Chih-Wei Tsai, J. W. Hans Niemantsverdriet, Ernst H. G. Langner
Summary: Zeolitic imidazolate frameworks, such as ZIF-8, were modified using solvent-assisted ligand exchange (SALE) with various functionalized imidazole derivatives to enhance the CO2 adsorption capacity. Different imidazole functionalizations resulted in varying degrees of CO2 uptake improvement, with nitro (NO2)-functionalized SALE products showing the most significant enhancements.
Article
Chemistry, Physical
Yang He, C. J. Weststrate, Dan Luo, J. W. Niemantsverdriet, Kai Wu, Jian Xu, Yong Yang, Yongwang Li, Xiaodong Wen
Summary: The structure and reactivity of Co-Si polycrystalline surfaces formed at room temperature were investigated. It was found that coordination of Co to Si suppresses CO adsorption, but when the cobalt dose reaches a certain level, CO adsorption occurs.
APPLIED SURFACE SCIENCE
(2021)
Article
Engineering, Environmental
Zhenghang Zhu, Matthieu Weber, Marcel A. Verheijen, Ageeth A. Bol, Veaceslav Spinu, Leyla Ozkan, A. C. P. M. (Ton) Backx, J. W. (Hans) Niemantsverdriet, Hans O. A. Fredriksson
Summary: A novel setup for studying the impact of fast, high temperature pulses on catalytic reactions has been developed. By utilizing a microreactor and generic catalyst support, with an integrated heater, rapid temperature changes can be achieved and monitored in real time. The results show that the application of fast, well-controlled temperature pulses can significantly enhance reaction rates and reduce power input required for the reaction, offering new insights into reaction kinetics.
CHEMICAL ENGINEERING JOURNAL
(2021)
Article
Chemistry, Physical
C. J. (Kees-Jan) Weststrate, Daniel Garcia Rodriguez, Devyani Sharma, J. W. (Hans) Niemantsverdriet
Summary: This study investigates the interaction between hydrogen and cobalt surfaces, revealing the adsorption and desorption behavior of hydrogen on different surface structures. It also discovers the variation of hydrogen adsorption strength and equilibrium constant under different conditions.
JOURNAL OF CATALYSIS
(2022)
Article
Chemistry, Physical
Foteini M. Sapountzi, Marek Lavorenti, Wilbert Vrijburg, Sofia Dimitriadou, Beata Tyburska-Pueschel, Peter Thune, Hans Niemantsverdriet, Tobias Pfeiffer, Mihalis N. Tsampas
Summary: This study demonstrates the potential of a vapor-based process, involving spark ablation and impaction, to fabricate efficient and durable Ir- and Pt-coated membranes. Compared to commercial membranes, spark-ablation membranes can reduce the demand for Ir by up to five times without compromising activity. The durability of spark-ablation membranes has been investigated under constant and dynamic load profiles, revealing different degradation mechanisms for each case.
Article
Chemistry, Physical
Erhao Gao, Wenjing Feng, Qi Jin, Li Han, Yi He
Summary: The influence of K-doping on the reactive oxygen species and elementary reactions of HCHO catalytic oxidation was investigated using density functional theory (DFT). The introduction of K-doping changed the electronic structures of Ce and O, facilitating the adsorption and activation of HCHO and O2 molecules, enhancing lattice oxygen mobility, and reducing the energy barrier for HCHO oxidation. K-doping also promoted the formation of hydroxyl groups, facilitating HCHO adsorption and oxidation.
Article
Chemistry, Physical
Hao Fu, Zhangliang Xu
Summary: In this study, the adsorption mechanisms and detection performance of formaldehyde, ammonia, and sulfur dioxide on undoped and metal-doped ZnO surfaces were investigated using density functional theory. The results showed that formaldehyde and ammonia were physically adsorbed on the undoped ZnO surface, while sulfur dioxide was weakly chemisorbed. The adsorption energy was enhanced when ZnO was doped with metals. These findings provide theoretical guidance for the application of ZnO substrate materials in gas sensitivity research.
Article
Chemistry, Physical
Atsushi Nomura, Tohru Kurosawa, Migaku Oda, Satoshi Demura, Shogo Kuwahara, Sora Kobayashi, Hideaki Sakata
Summary: The study investigates the tunneling spectra of 1T-TiSe2 in the CDW state and the dip structure below the Fermi level, aiming to determine whether this dip is a CDW gap. The answer to this question is crucial for understanding the driving mechanism of CDW.
Article
Chemistry, Physical
A. S. Petrov, D. I. Rogilo, A. I. Vergules, V. G. Mansurov, D. V. Sheglov, A. V. Latyshev
Summary: This study investigates Si mass transport and morphological transformations on the Si(111) surface during (root 3 x root 3)-Sn reconstruction formation and Si homoepitaxy. The research shows that the formation of different Sn phases at different temperatures affects the Si island nucleation and monatomic step shift, which in turn impact the morphology of the Sn/Si(111) interface. Electromigration-induced drift of disordered Sn domains leads to enhanced noncompensated Si mass transport and surface roughening.
Article
Chemistry, Physical
D. V. Gruznev, L. V. Bondarenko, A. Y. Tupchaya, A. A. Yakovlev, A. N. Mihalyuk, A. V. Zotov, A. A. Saranin
Summary: Deposition of thallium (Tl) onto the Au/Si(111)5 x 2 reconstruction followed by annealing results in the formation of a surface structure with 4 x 2 periodicity. The immiscibility of Au and Tl leads to the migration of Tl atoms over the Si chains. Thallium donates electrons to the surface, converting the metallic surface into an insulating state and altering the inter-chain distance within the array of Au atomic wires.
Article
Chemistry, Physical
Simone Giusepponi, Francesco Buonocore, Barbara Ferrucci, Massimo Celino
Summary: Using ab-initio calculations, the interaction between lead adatom and both clean and doped iron (100) surfaces was investigated. It was found that the lead adatom prefers to adsorb in the hollow site, which is more stable compared to the top and bridge sites, and in this position, it is energetically favorable over the iron adatom. Moreover, lead adsorbed in the hollow site of the iron (100) surface doped with chromium was found to create a more stable system compared to nickel-doped surfaces with an iron adatom in the same position. The study also explored inter-layer distances, bonding mechanisms, magnetic behaviors, and charge density differences. The results provide insights into the role of doping in the interaction between lead adatom and iron surface, and have implications for the analysis of corrosion processes caused by liquid lead.
Article
Chemistry, Physical
Shuo Zhang, Jin-Ho Choi
Summary: The recent synthesis of two-dimensional layered WSi2N4 has attracted attention due to its potential applications. This study investigates the catalytic performance of WSi2N4 monolayers with nitrogen vacancies in the hydrogen evolution reaction using first-principles calculations. The results show that the defective WSi2N4 monolayers exhibit remarkably high catalytic activity comparable to platinum catalysts. Electronic structure calculations also reveal the emergence of spin-polarized states due to the introduction of nitrogen vacancies.
Article
Chemistry, Physical
Xiaoyan Yu, Xin Cao, Wei Kang, Shanhua Chen, Ao Jiang, Yuhao Luo, Wenwei Deng
Summary: First-principles calculations were used to investigate the electronic properties of a TiO2 heterostructure modified with Bi2Te3 co-catalyst. The study revealed that the Bi2Te3/TiO2 interface introduced optimal band offsets, effectively suppressing electron-hole recombination and enhancing the utilization efficiency of photo-generated carriers. Additionally, the Bi2Te3 co-catalyst introduced extra catalytic active sites, further boosting the photo-catalytic hydrogen evolution efficiency.
Article
Chemistry, Physical
Filippo Longo, Emanuel Billeter, Selim Kazaz, Alessia Cesarini, Marin Nikolic, Aarati Chacko, Patrik Schmutz, Zbynek Novotny, Andreas Borgschulte
Summary: Alkaline water electrolysis is a simple and efficient method for renewable hydrogen production, utilizing cheap and abundant transition metals. The catalytic properties of Ni materials are enhanced by the formation of oxidized compounds on the surface. The high electrocatalytic activity of Ni (oxy)-hydroxides is directly related to water intercalation in the passivation layer, supporting the hypothesis of a water mediated OH- diffusion mechanism. The self-organization of the surface structure during passivation layer formation enables high electrode performance.
Article
Chemistry, Physical
Mohan Kumar Kuntumalla, Miriam Fischer, Alon Hoffman
Summary: By investigating the bonding, retention, and thermal stability of nitrogen in H-Diamond (100), it was found that nitrogen can partially recover its bonding with carbon atoms after high-temperature annealing, indicating a high thermal stability of nitrogen in diamond.
Article
Chemistry, Physical
Dong Yue, Liangying Wen, Rong Chen, Jianxin Wang, Zhongqing Yang
Summary: The adsorption behavior of Cl2 molecules on the TiC surface and the formation and transfer of reaction products were studied using first-principles ab initio calculations. The results show that the Cl atoms bonded to the surface Ti atoms are more stable, and the TiCl3 intermediate is easier to form than the TiCl2 intermediate.
Article
Chemistry, Physical
Yatao Wang, Peng Zhang, Hongjuan Li, Qiuju Xu, Shujun Liu, Xiaopeng Liu, Xuehua Guo, Yitao Li, Jinzhang Liu, Sen Dong, Zhi Wei Seh, Qianfan Zhang
Summary: In this study, the adsorption performance of two types of metal-organic frameworks (MOFs) for thiophene and benzene was experimentally investigated. The results showed that IZE-1 exhibited high selectivity and superior adsorption capacity for thiophene, especially at low concentrations. First-principles calculations and molecular dynamics simulations provided insights into the mechanism of thiophene adsorption and the high selectivity observed. This research demonstrates the potential of MOFs for thiophene adsorption, particularly at high concentrations.
