Article
Chemistry, Physical
Zdenek Rafaj, Jozef Krutel, Vaclav Nehasil
Summary: Rhodium (Rh) is predominantly used in the automotive industry for three-way catalysis (TWC), with improved efficiency achieved by adding CeO2-active support for oxygen storage capacity. In this study, the CO oxidation mechanism of Rh nanoparticles on CeO2(111) and CeO2(110) was investigated, revealing higher performance on Rh/CeO2(110) due to weaker CO-Rh bond and increased oxygen exchange activity.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Chemistry, Physical
Joachim D. Bjerregaard, Kurt V. S. Mikkelsen, Matthew Johnson
Summary: This study investigates the oxidation of CO on the (110) surface of CeO2 and identifies a high activation barrier for the formation of a carbonate species as an alternative pathway to the desorption of CO2. The findings suggest that modeling catalyst activity using a reduced cluster of atoms is accurate, flexible, and advantageous.
CHEMICAL PHYSICS LETTERS
(2022)
Article
Chemistry, Physical
Alexander Simanenko, Maximilian Kastenmeier, Lesia Piliai, Yuliia Kosto, Tomas Skala, Nataliya Tsud, Sascha Mehl, Mykhailo Vorokhta, Iva Matolinova, Yaroslava Lykhach, Joerg Libuda
Summary: The redox capacity of Pt-CeO2 catalysts for low-temperature CO oxidation was investigated using various spectroscopy methods. Different Pt species were prepared and their oxidation states were monitored upon CO exposure. Metallic Pt-0 nanoparticles, ultra-small Pt*/PtOx clusters, and Pt4+ species were found to serve as CO adsorption sites at low temperature. The redox pathway for low-temperature CO oxidation involved CO spillover and the formation of bidentate carbonate species, while above 400 K, the Mars-van Krevelen mechanism was observed.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Physical
Li-Yuan Wang, Ya-Hui Fang
Summary: This study presents the first theoretical attempt to elucidate the potential-dependent co-electrosorbed species on the Pd(110) surface using machine-learning-based global optimization and modified Poisson-Boltzmann continuum solvation. The potential-dependent adsorption/absorption hydrogen phases, phase transition, and co-electrosorbed surface structures are revealed. The intermediates Hri-NH2 and Hri-NH3 are found to be favorable for the N2 reduction reaction, with subsurface H playing a key role in NH2 hydrogenation on the Pd(110) electrode.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Yan-Yang Qin, Ya-Qiong Su
Summary: The study investigated the influence of highly dispersed Pt on CeO2(110) on CO oxidation activity, finding that a structure with two Pt atoms replacing a surface Ce atom exhibited higher activity due to coordinative unsaturation of one Pt atom and the presence of a neighboring two-fold O atom. This highly stable and active structure suggests a potential for effective catalysis on ceria surfaces.
Article
Chemistry, Physical
Binjing Zhang, Xiaoqiu Ye, Wenhua Luo, Ge Sang
Summary: In this study, the effects of Nb/Ta modified ZrCo(110) surfaces on the adsorption, dissociation, and diffusion of hydrogen were investigated using first-principles calculations. The results showed that hydrogen easily dissociates on the pure ZrCo(110) surface and is captured by surface vacancies. After entering the subsurface, hydrogen tends to fill the subsurface and continue to diffuse inward. Nb/Ta doping reduced the dissociation energy barrier and diffusion energy barrier of hydrogen on the surface and subsurface, leading to an improvement in the bonding strength of hydrogen. The findings confirmed that Nb/Ta doping can enhance the hydrogen storage performance of ZrCo.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Article
Nanoscience & Nanotechnology
Chengzhang Zhu, Qiming Xian, Qiuying He, Chuanxiang Chen, Weixin Zou, Cheng Sun, Shaobin Wang, Xiaoguang Duan
Summary: By developing an innovative hybrid photocatalyst, this study has achieved high charge separation efficiency and superior hydrogen evolution rate through optimal structure and phase engineering. The design provides a new approach for solar energy conversion.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Physical
Yongke Wang, Qiuyue Zhang, Yuwen Lin, Wujun Huang, Ding Ding, Yanping Zheng, Mingshu Chen, Huilin Wan
Summary: Stabilizing Cu+ on the surface of CeO2 was found to achieve high selectivity for CO oxidation, while Cu-0 was more favorable for H-2 oxidation at higher temperatures.
APPLIED SURFACE SCIENCE
(2021)
Article
Engineering, Chemical
Fan Li, Bing Zhao, Yifeng Tan, Wenlin Chen, Mengkui Tian
Summary: In this study, Al2O3-CeO2 carriers were synthesized by hydrothermal method, and CuO/Al2O3-CeO2 catalysts were prepared for the oxidation reactions of CO and C3H8. The results showed that the introduction of CeO2 improved the dispersion of CuO on the catalyst surface and enhanced the catalytic activity. In addition, the increase of CeO2 content led to a decrease in specific surface area and pore volume of the sample. XPS results indicated that the synergistic effect of Ce-3(+) + Cu2+ promoted the generation of oxygen vacancies, thus improving the activity of the catalyst. The surface Cu+ species obtained from the reduction of Cu2+ played a crucial role in the catalytic oxidation reactions, as observed from in situ DRIFTS results.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2022)
Article
Chemistry, Physical
Yaqian Deng, Xiaobing Shi, Longqing Wei, Hao Liu, Ju Li, Xuemei Ou, Lihui Dong, Bin Li
Summary: This study investigated the symbiosis effect of CuO-CeO2 catalyst and the influence of different ratios of CeO2 and CuO on its structure and catalytic performance. It was found that Cu1Ce2 catalyst exhibited excellent catalytic performance and resistance to SO2 and H2O. In the catalytic reaction, Cu+ played a crucial role in the catalyst and was related to the active site for NO molecule dissociation.
JOURNAL OF ALLOYS AND COMPOUNDS
(2021)
Article
Chemistry, Physical
Luca Schio, Gregor Bavdek, Cesare Grazioli, Carolina Gutierrez Bolanos, Andrea Goldoni, Andrea Vittadini, Massimo Tormen, Luca Floreano
Summary: The efficiency of interfacial charge transfer for metal-tetraphenylporphyrins (M-TPPs) on rutile TiO2(110) depends on the molecular adsorption site and configuration. M(II)-TPPs with M = Co, Ni, Cu, Zn adsorb on the O-br rows with the same molecular conformation and form a commensurate phase with the same symmetry. The tendency to axial coordination determines the molecular adsorption energy and the preference for adsorption atop one O-br atom or on a bridge between two O-br atoms.
APPLIED SURFACE SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Haocheng Xiong, Qiwen Sun, Kedang Chen, Yifei Xu, Xiaoxia Chang, Qi Lu, Bingjun Xu
Summary: Researchers have developed a method to determine the standard adsorption enthalpy of CO on Cu surfaces using quantitative surface enhanced infrared absorption spectroscopy. The results show that on dendritic Cu at -0.75 V vs. SHE, the standard adsorption enthalpy, entropy and Gibbs free energy are 1.5 kJ mol(-1), 37.9 J/(mol K), and -9.8 kJ mol(-1), respectively. Comparison between oxide-derived Cu and dendritic Cu suggests the presence of stronger binding sites on OD Cu, which could favor multicarbon products. This work will help establish the correlation between CO binding energy and CO(2)RR activity.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Materials Science, Multidisciplinary
Jingli Shi, Hailiang Wang, Tao Gao, Wenhua Luo
Summary: In this study, the interfacial interactions of H2O and H2 molecules with defective PuH2 (100), (110) and (111) surfaces were explored using DFT + U approach. The adsorption energy results suggest that H2O may have a competitive advantage over H2. The H atoms from H2O and H2 attempt to heal the vacancy by interacting with the OH group or O atom from H2O.
Article
Chemistry, Physical
Shenwei Chen, Zeying Cai, Zengfu Ou, Zhiqiang Wang, Donghui Guo, Dingyong Zhong
Summary: This study explores the covalent coupling of pentacene molecules on Au(110) surfaces, showing that pentacenes undergo direct aryl-aryl coupling via C-H bond activation on the reconstructed Au(110) surface, forming linear and T-shaped dimers as the predominant products. The aryl C-H bond activation barrier is significantly reduced on the Au(110)-(1 x 3) reconstructed surfaces, where the extra row of gold atoms in the (1 x 3) reconstructed grooves plays a key role.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Noemi Bosio, Mengqiao Di, Magnus Skoglundh, Per-Anders Carlsson, Henrik Gronbeck
Summary: This study uses first-principles-based kinetic Monte Carlo simulations and kinetic experiments to investigate CO oxidation over Pt/CeO2, showing that the reaction orders over Pt/CeO2 are close to zero for both CO and O-2, indicating the absence of CO/O-2 site competition and highlighting the relevance of interface reactions.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
