Article
Chemistry, Physical
Pablo G. Lustemberg, Zhongtian Mao, Agustin Salcedo, Beatriz Irigoyen, M. Veronica Ganduglia-Pirovano, Charles T. Campbell
Summary: Research has shown that cationic Ni atoms in clusters at step edges on the CeO2(111) surface are the most active sites for methane conversion reactions, with their small size and high Ni chemical potential contributing to their activity. Density functional theory calculations have clarified the reasons behind this observation, highlighting the importance of the size and morphology of supported Ni nanoparticles, strong Ni-support bonding, and charge transfer at step edges for high catalytic activity, particularly in the activation barrier for C-H bond cleavage during CH4 dissociative adsorption. This knowledge is expected to inspire the development of more efficient catalysts for these reactions.
Review
Chemistry, Applied
Chunpeng Wang, Zhe Wang, Shanjun Mao, Zhirong Chen, Yong Wang
Summary: This review comprehensively surveys and summarizes the structural complexity and catalytic role of supported metal catalysts, with a focus on analyzing the effects of multiple factors on the coordinated environment of active centers and the influence of structure-performance relationship on catalytic reactions. Additionally, it provides a summary of key structure characterization techniques for determining the coordination structure of active metal sites and offers personal perspectives on the further development in the field of heterogeneous metal catalysts.
CHINESE JOURNAL OF CATALYSIS
(2022)
Article
Chemistry, Physical
Jeremy W. Arvay, Wei Hong, Christina Li, W. Nicholas Delgass, Fabio H. Ribeiro, James W. Harris
Summary: In this study, the difference in catalytic roles of extracrystalline and intracrystalline gold nanoparticles in direct propylene epoxidation was investigated. The results showed that the activation energy and reaction orders for propylene epoxidation were similar for both types of nanoparticles. However, the activation energy for hydrogen oxidation differed, indicating a change in rate-limiting step or active site. An active site model was developed to estimate catalytic turnover frequencies and it was found that the simultaneous mechanism occurring over proximal Au-Ti sites alone is not sufficient to explain the observed rate of propylene epoxidation, suggesting the kinetically relevant short-range migration of hydrogen peroxide. The study also found that the rates of hydrogen oxidation varied proportionally to the amount of surface gold atoms, indicating the importance of gold dispersion in the catalysts.
Article
Chemistry, Physical
Jeremy W. Arvay, Wei Hong, Christina Li, Fabio H. Ribeiro, W. Nicholas Delgass, James W. Harris
Summary: The catalytic roles of extracrystalline and intracrystalline gold nanoparticles on the direct propylene epoxidation were investigated, and it was found that there was no intrinsic difference between the two. The kinetics of the reaction were measured and the results were consistent with previous studies on intracrystalline gold nanoparticles. An active site model was developed and the estimated turnover frequencies were 20 times higher than previous estimates. The dispersion of gold was found to affect the rate of hydrogen oxidation.
Article
Chemistry, Multidisciplinary
Shiyu Zhen, Gong Zhang, Dongfang Cheng, Hui Gao, Lulu Li, Xiaoyun Lin, Zheyuan Ding, Zhi-Jian Zhao, Jinlong Gong
Summary: This paper presents a large-scale simulation to obtain realistic CuZn nanoparticle models and the atomic structure of active sites for C2+ products on CuZn catalysts in CO2ER. Two kinds of active sites, both facilitating C-C coupling, are identified and verified through subsequent calculations and experiments. This work provides a paradigm for the design of high-performance Cu-based catalysts and a general strategy to accurately identify the atomic structures of active sites in complex catalytic systems.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Multidisciplinary Sciences
Dongfang Cheng, Zhi-Jian Zhao, Gong Zhang, Piaoping Yang, Lulu Li, Hui Gao, Sihang Liu, Xin Chang, Sai Chen, Tuo Wang, Geoffrey A. Ozin, Zhipan Liu, Jinlong Gong
Summary: This study reveals the active sites for CO2 electroreduction over oxide-derived copper (OD-Cu) catalysts, identifying square-like sites responsible for specific products. Planar and convex square sites are found to be responsible for ethylene production, while the step square site favors alcohols generation, providing fundamental insights into the origin of activity and selectivity over Cu-based catalysts.
NATURE COMMUNICATIONS
(2021)
Article
Nanoscience & Nanotechnology
Aiai Zhang, Jinfang Wu, Lei Xue, Caixia Li, Shanghong Zeng, Dominic Caracciolo, Shan Wang, Chuan-Jian Zhong
Summary: The catalyst morphology significantly influences the electrocatalytic activity, with petal-shaped catalysts showing enhanced performance due to the presence of abundant AuO- species. The coexistence of different gold species on the surface of Cu2O particles affects the catalytic properties, leading to a clearer understanding of the relationship between morphology and electrocatalytic performance.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Physical
Tiantong Zhang, Bao Wang, Yao Nian, Menghui Liu, Yiming Jia, Jinli Zhang, You Han
Summary: In this study, the active sites on Cu-based catalysts for acetylene hydrochlorination were investigated. It was found that the indirect ligand-coordinated sites induced by excess copper chloride exhibited superior performance. Molecular dynamics simulation and density functional theory calculations revealed that excess copper chloride molecules spontaneously formed chain structures, leading to the formation of indirect ligand-coordinated sites and electron transfer along the copper chloride chain, which were crucial for the high catalytic activity. These findings provide fundamental insights into the origin of activity and the identification of active sites in Cu-ligand catalysts for acetylene hydrochlorination.
Article
Chemistry, Physical
Shih-Yuan Chen, Chih-Li Chang, Masayasu Nishi, Wei-Chih Hsiao, Yves Ira A. Reyes, Hiroyuki Tateno, Ho-Hsiu Chou, Chia-Min Yang, Hsin-Yi Tiffany Chen, Takehisa Mochizuki, Hideyuki Takagi, Tetsuya Nanba
Summary: The development of efficient and stable Ru catalysts is crucial for the synthesis of decarbonized NH3. By tuning the interface between the Ru particles and the CsOH-Cs0 species, the surface acidity/basicity of the catalyst can be changed, and new active sites can be generated, promoting NH3 synthesis.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Chemistry, Applied
E. Kolobova, P. Maki-Arvela, A. Grigoreva, E. Pakrieva, S. A. C. Carabineiro, J. Peltonen, S. Kazantsev, N. Bogdanchikova, A. Pestryakov, D. Yu Murzin
Summary: The study highlighted the significance of support materials for gold catalysts in the oxidation of betulin, showing that the nature of support impacts the size and distribution of gold nanoparticles and thus influences catalytic performance. The oxidation of betulin catalyzed by gold was found to be structure-sensitive, requiring an optimal size of gold nanoparticles around 3.3 nm.
Article
Energy & Fuels
Ankit Agrawal, Omvir Singh, Ashok Kumar Yadav, Shailendra Tripathi, Anjan Ray, Vivek Pawar, Bipul Sarkar
Summary: On-purpose dehydrogenation technologies are gaining attention for the production of light olefins. Our study on a Mo-based bi-metallic catalyst, MoSn/Y, provides insights into the interatomic interactions between metals. This catalyst exhibits high selectivity, activity, and stability for the direct dehydrogenation of propane to propylene.
Article
Chemistry, Physical
Emmanuel Iro, Hiroko Ariga-Miwa, Takehiko Sasaki, Kiyotaka Asakura, Maria Olea
Summary: Gold catalysts with different particle sizes were synthesized on mesoporous silica and their catalytic activities were tested. The results showed that smaller particles had higher activity and better stability.
Article
Engineering, Environmental
Jingchen Zhao, Tao Zhang, Guoxin Ma, Jianning Zhang, Sixuan Li, Weiyu Song, Jian Liu
Summary: A series of CenTiOx catalysts were prepared by a solvothermal method and their performance in the selective catalytic reduction (SCR) of NOx with NH3 was investigated. Among them, Ce0.3TiOx showed the best SCR performance. By combining various characterizations with DFT calculations, it was found that dinuclear sites, acid and redox sites, were successfully constructed on the Ce0.3TiOx surface. The outstanding oxidation ability of this catalyst was crucial for active adsorbed NH3 and NHNO intermediates, which are critical for the NH3-SCR reaction. A plausible NH3-SCR reaction pathway on CenTiOx catalysts was proposed.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2023)
Article
Chemistry, Multidisciplinary
Asato Nakagiri, Kazuya Imamura, Kazumichi Yanagisawa, Ayumu Onda
Summary: The surface acid-base nature of hydroxyapatite catalysts can be continuously controlled by altering elemental compositions such as bulk Ca/P ratio and sodium content, leading to excellent catalytic properties for various reactions, including alkanediol conversion.
Article
Chemistry, Physical
Antai Li, Dawei Yao, Youwei Yang, Wenting Yang, Zhuoshi Li, Jing Lv, Shouying Huang, Yue Wang, Xinbin Ma
Summary: In this study, rod-shaped ceria-supported copper catalysts with different copper sizes were prepared and the Cu-0-Cu sigma+ interface was identified as the primary active site for MA hydrogenation. This insight may provide guidance for high-performance catalyst design.