Article
Green & Sustainable Science & Technology
Z. Zhang, X. Liu, Y. Hu, X. Zhou
Summary: Based on density functional theory, the adsorption processes of fluorine-containing gases on different surfaces were investigated. Co and Pd doping greatly improved the adsorption properties of adsorbents for F2 and SOF2 gas molecules. New chemical bond formation occurred during the adsorption process, leading to different adsorption behaviors.
MATERIALS TODAY SUSTAINABILITY
(2023)
Article
Chemistry, Physical
Junjie Shi, Cameron J. Owen, Hio Tong Ngan, Siyu Qin, Vikram Mehar, Philippe Sautet, Jason F. Weaver
Summary: A single atom Ti-Cu(111) surface alloy can be generated by depositing small amounts of Ti onto Cu(111) at slightly elevated surface temperatures. Different structures of Ti are formed on the Cu(111) surface at different temperatures, and CO adsorbs differently on the single atom Ti-Cu(111) surface alloy and Cu-covered Ti-containing domains.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Huan Xie, Yangyang Wan, Xiaoming Wang, Jiashun Liang, Gang Lu, Tanyuan Wang, Guoliang Chai, Nadia Mohd Adli, Cameron Priest, Yunhui Huang, Gang Wu, Qing Li
Summary: Bi-Pd single atom alloy (SAA) nanodendrites (NDs) exhibit high CO production rates and Faradic efficiencies, attributed to the decreased reaction barriers for H-2 formation and reduced free energy for *COOH generation resulted from Bi doping.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2021)
Article
Chemistry, Physical
Buddhika S. A. Gedara, Michael Trenary
Summary: Scanning tunneling microscopy was used to compare the evolution of Pd islands on Ag(111) and Au(111) surfaces. Different behaviors were observed, with large Pd islands and vacancy pits forming on Ag(111), while smaller Pd islands and no vacancy pits were observed on Au(111). The annealing process resulted in Pd diffusion into the subsurface for both surfaces, but the behavior on Au(111) was significantly different due to the herringbone reconstruction providing higher binding energy sites.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
H. Okuyama, D. Yamamoto, S. Hatta, T. Aruga
Summary: The interaction between Ag atoms and graphene moire on Rh(111) was investigated using scanning tunneling microscopy. At 15 K, Ag atoms mainly existed as monomers at specific sites in the moire unit cell due to suppressed thermal diffusion. The presence of Ag(5s)-C(2pz) anti-bonding state was identified by the dI/dV peak at around 0.5 V above the Fermi level. At higher temperatures, Ag adatoms were thermally activated to diffuse and form clusters, with the barrier for activation depending on the moire periodicity. Additionally, injection of tunneling electrons into the anti-bonding state induced migration. This study provides atomic-scale insight into the aggregation process of metal adatoms on metal-supported graphene.
Article
Chemistry, Physical
Buddhika S. A. Gedara, Mark Muir, Arephin Islam, Dairong Liu, Michael Trenary
Summary: The study found that Ag atoms can migrate to cover Pd islands at room temperature, leading to vacancies in the middle of the islands and second layer growth. Upon annealing, most Pd islands are encapsulated by Ag atoms to form an Ag/Pd/Ag(111) structure.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Chemistry, Physical
Wataru Osada, Shunsuke Tanaka, Kozo Mukai, Mitsuaki Kawamura, YoungHyun Choi, Fumihiko Ozaki, Taisuke Ozaki, Jun Yoshinobu
Summary: Hydrogen spillover processes on the single atom alloy catalyst Pd/Cu(111) were investigated using experimental and theoretical methods. Real-time observation of hydrogen spillover onto Cu(111) was achieved using infrared reflection absorption spectroscopy, providing insights into the reaction mechanism.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Fei Wang, Zhao Li, Honghong Wang, Min Chen, Changbin Zhang, Ping Ning, Hong He
Summary: This study demonstrates that Ag-0 nanoparticle has an advantage over single-atom Ag species in its intrinsic activity for CO oxidation. The larger Ag-0 particle benefits oxygen activation and improves valence stability during oxidation reactions, leading to superior performance in CO oxidation.
Article
Chemistry, Physical
Junqing Yin, Masahiro Ehara, Shigeyoshi Sakaki
Summary: Single-atom alloys (SAAs) are promising catalysts that can reduce costs without sacrificing activity. The relative stability of SAAs depends on the interaction energy and coverage between different metal atoms. The electronic structures play a significant role in determining the properties of SAAs, with copper and nickel atoms having weaker interaction energies compared to gold and platinum atoms. These findings are important for the design of efficient catalysts.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Vladimir A. Nasluzov, Elena A. Ivanova-Shor, Aleksey M. Shor, Svetlana S. Laletina, Konstantin M. Neyman
Summary: Density functional calculations were used to study the formation of various COx species upon the adsorption and oxidation of CO on palladium and silver single atoms supported on a model ceria nanoparticle. The characteristics of palladium and silver intermediates differ, with CO oxidation found to be more favorable at silver centers atomically dispersed on ceria nanostructures compared to palladium centers.
Article
Chemistry, Physical
Laura Fernandez, Sebastian Thussing, Anton X. Brion-Rios, Daniel Sanchez-Portal, Peter Jakob
Summary: The study reveals an attractive interaction between TiOPc molecules on Ag(111) surface, while repulsive interaction is found between CuPc molecules. Dense two-dimensional islands of TiOPc molecules with long-range order are observed at temperatures below 75 K, in contrast to the disordered arrangement of adsorbed CuPc molecules.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Chemistry, Physical
Alexander Rassolov, Igor S. Mashkovsky, Galina O. Bragina, Galina N. Baeva, Pavel Markov, Nadezhda S. Smirnova, Johan Warna, Alexander Yu Stakheev, Dmitry Yu Murzin
Summary: The study showed that Pd1Ag3/Al2O3 single-atom alloy catalyst exhibits excellent selectivity in the liquid-phase hydrogenation of DPA, which is not influenced by hydrogen pressure or DPA concentration.
MOLECULAR CATALYSIS
(2021)
Article
Materials Science, Multidisciplinary
Jinjuan Zhang, Xiaodong Zhu, Kaixing Zhu, Jinbo Shen, Yan Xu, Da Chen, Peng Wang
Summary: In this study, we investigated the structures, electronic properties, and gas adsorption performance of single-atom (Co, Pd, Pt)-decorated 2H-MoS2 monolayer for adsorption of typical toxic gases, NO2 and NH3, using spin-polarized density functional theory calculations. The results indicate that the decorated metal atoms substantially improved the activity and electronic properties of the MoS2 monolayer, and further enhanced the adsorption and sensing performance for NO2 and NH3. The Pd-MoS2 monolayer is found to be a promising highly efficient gas sensing material for both gases in the temperature range of 400-500 K. On the other hand, the CoMoS2 and Pt-MoS2 monolayers are not suitable for gas sensing applications, however, they can be considered as gas capture materials. These findings provide valuable references for the design and development of single-atom decorated MoS2 monolayer as high-performing gas sensing or scavenging materials for environmental monitoring and other related applications.
RESULTS IN PHYSICS
(2023)
Article
Chemistry, Physical
Tianhui Liu, Tianze Peng, Bina Fu, Dong H. Zhang
Summary: This study investigates the reactivity of HCl on a strained Ag monolayer on Au(111) surface. The research finds that despite a lower barrier for HCl+Ag/Au(111) than pure Ag(111), the Ag-Au interaction significantly suppresses the reactivity of HCl. This suppression is attributed to charge transfer between Ag and Au, where electronegative Au makes the top Ag layer on Ag/Au(111) electropositive, unlike that on pure Ag(111). The electropositive Ag attracts Cl, resulting in an unfavorable H-Cl configuration and reduced reactivity. These findings deepen our understanding of polar molecule interactions on bimetallic surfaces and have implications for catalyst design in heterogeneous catalysis.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Multidisciplinary Sciences
Yating Pan, Yunyang Qian, Xusheng Zheng, Sheng-Qi Chu, Yijun Yang, Chunmei Ding, Xi Wang, Shu-Hong Yu, Hai-Long Jiang
Summary: Metal-organic framework (MOF) stabilized bimetallic Pd@Pt nanoparticles with adjustable Pt coordination environment and controlled structure from core-shell to single-atom alloy (SAA) have been fabricated. It was found that Pt surface charge regulation can be achieved by changing its coordination environment and the structure of the Pd@Pt co-catalyst, redistributing the charge between Pd and Pt. The optimized Pd-10@Pt-1/MOF composite, featuring an unprecedented SAA co-catalyst, exhibits exceptionally high photocatalytic hydrogen production activity surpassing its corresponding counterparts.
NATIONAL SCIENCE REVIEW
(2021)
Article
Chemistry, Physical
Dominic A. Esan, Michael Trenary
Summary: The adsorption behavior of CO on Pt nanoclusters on a single layer of graphene grown on the Ru(0001) surface was studied using RAIRS and TPD, revealing that the complete coverage of Ru(0001) by graphene can reduce CO adsorption. The RAIRS intensity for CO on Pt/Gr/Ru(0001) was found to be nine times higher than that on Ru(0001) on a per molecule basis.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
David L. Molina, Mark Muir, Mohammed K. Abdel-Rahman, Michael Trenary
Summary: The study investigated the selective hydrogenation of acetylene on both a clean Ag(111) surface and on a Pd/Ag(111) single-atom-alloy surface using RAIRS and TPR techniques. By exposing the surfaces to atomic hydrogen generated by a hot filament, hydrogen atoms were found to react with acetylene to produce adsorbed ethylene at 85 K. The formation of ethylene and ethane was detected, but no acetylene coupling products, such as benzene, were found.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Buddhika S. A. Gedara, Mark Muir, Arephin Islam, Dairong Liu, Michael Trenary
Summary: The study found that Ag atoms can migrate to cover Pd islands at room temperature, leading to vacancies in the middle of the islands and second layer growth. Upon annealing, most Pd islands are encapsulated by Ag atoms to form an Ag/Pd/Ag(111) structure.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Correction
Chemistry, Physical
Minhui Lee, Emiko Kazuma, Chi Zhang, Michael Trenary, Jun Takeya, Jaehoon Jung, Yousoo Kim
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Physical
Minhui Lee, Emiko Kazuma, Chi Zhang, Michael Trenary, Jun Takeya, Jaehoon Jung, Yousoo Kim
Summary: The dissociation of O-2 molecules chemisorbed on silver surfaces has been studied at the single-molecule level on Ag(110) using a scanning tunneling microscope (STM). The dissociation reaction was predominantly triggered by inelastically tunneled holes from the STM tip, influenced by the significantly distributed density of states below the Fermi level of the substrate. Action spectroscopy with the STM and density functional theory calculations revealed that direct ladder-climbing excitation of high-order overtones of the O-O stretching mode, enhanced by molecule-surface interactions, is the cause of the O-2 dissociation reaction.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Chemistry, Physical
Michelle R. Brann, Stephen P. Hansknecht, Mark Muir, S. J. Sibener
Summary: The research systematically examines the interaction of acetone with various D2O ices using RAIRS, finding that more hydrogen bonding occurs between acetone and porous amorphous ice compared to other types. By quantifying hydrogen bonding through RAIR spectral changes, it was discovered that changing the water structure to be more porous leads to a further reduction in hydrogen bonding, indicating a lack of access to surface sites with dangling bonds in the pores.
JOURNAL OF PHYSICAL CHEMISTRY A
(2022)
Article
Chemistry, Physical
Ravi Ranjan, Mark Muir, David L. Molina, Michael Trenary
Summary: In this study, the reflection absorption infrared spectra (RAIRS) of 1-propanol on the Ag(111) surface were simulated using density functional theory calculations. The results were compared to the corresponding experimental spectra, indicating that 1-propanol adsorbs as one specific conformer on the surface.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Buddhika S. A. Gedara, Michael Trenary
Summary: Scanning tunneling microscopy was used to compare the evolution of Pd islands on Ag(111) and Au(111) surfaces. Different behaviors were observed, with large Pd islands and vacancy pits forming on Ag(111), while smaller Pd islands and no vacancy pits were observed on Au(111). The annealing process resulted in Pd diffusion into the subsurface for both surfaces, but the behavior on Au(111) was significantly different due to the herringbone reconstruction providing higher binding energy sites.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Multidisciplinary
Dairong Liu, Linfei Li, Buddhika S. A. Gedara, Michael Trenary, Nan Jiang
Summary: Extensive research on ultrathin ferrous oxide (FeO) islands and films has significantly contributed to understanding their structural and catalytic properties. In this study, scanning tunneling microscopy (STM) was used to investigate the interaction of Pd and Pt with FeO grown on Au(111). The results demonstrate different metal affinities of FeO edges, with Pd preferentially growing on the Fe-terminated edge and Pt preferentially growing on the O-terminated edge, resulting in selectively blocked FeO edges. This study provides new insights into the edge reactivity of FeO/Au(111) and suggests a potential approach for controlling the selectivity of FeO catalysts.
MATERIALS CHEMISTRY FRONTIERS
(2023)
Article
Chemistry, Physical
Emiko Kazuma, Minhui Lee, Jaehoon Jung, Michael Trenary, Yousoo Kim
Summary: This study used a scanning tunneling microscope to observe molecular motion and the dissociation of O-2 molecules adsorbed on the Ag(110) surface at a single-molecule level. It demonstrated that plasmonic hot carriers can enable multiple reaction pathways due to their broad energy distribution, allowing access to various adsorbate states.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
David L. Molina, Maki Inagaki, Emiko Kazuma, Yousoo Kim, Michael Trenary
Summary: Reflection absorption infrared spectroscopy and temperature-programmed desorption experiments were carried out to investigate the properties of Pt/Cu(111) surfaces. Pt coverage on Cu(111) was varied from multilayer to 0.23 monolayer. As the Pt coverage decreased, isolated Pt atoms and Pt islands were observed, indicating the presence of Pt atoms embedded in the Cu(111) surface. Low coverages of Pt at different temperatures formed single atom alloys (SAAs) with surface Pt only present as isolated atoms replacing Cu atoms in the topmost atomic layer. Adsorption of CO on the Pt atoms of the SAAs led to red-shifted C-O stretch peaks compared to CO on Pt(111), indicating how nearby Cu atoms alter the Pt-CO bonding.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Arephin Islam, David L. Molina, Michael Trenary
Summary: The adsorption behavior of acrolein and its hydrogenation products on Cu(111) was studied using RAIRS and TPD. The results showed that all four molecules adsorb weakly to the surface and desorb at temperatures below 225 K. The alcohols, 2-propenol and 1-propanot, exhibited strong hydrogen bonding in the multilayers but not in the monolayers. The orientation of the molecules changed between the monolayers and multilayers, as indicated by the shift in peak positions.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Arephin Islam, Mohammed K. Abdel-Rahman, Michael Trenary
Summary: RAIRS was used to study reversible adsorption of propyne on Cu(111) surface at pressures of 5-100 nTorr at room temperature. The pressure dependence of propyne coverage followed a Langmuir isotherm. Thermodynamic parameters such as adsorption heat and entropy change were determined and found to be consistent with literature values.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)