Article
Chemistry, Multidisciplinary
Feng Yang, Haofei Zhao, Wu Wang, Lei Wang, Lei Zhang, Tianhui Liu, Jian Sheng, Sheng Zhu, Dongsheng He, Lili Lin, Jiaqing He, Rongming Wang, Yan Li
Summary: This study reveals the occurrence of interfacial reaction induced SMSI in silica supported Co and Pt catalysts under reductive conditions at high temperature, demonstrating its significant boosting effect on catalytic hydrogenation. The findings highlight the universality of SMSI in oxide supported catalysts and its importance for catalyst design and understanding catalytic mechanisms.
Article
Chemistry, Physical
Ya-Qiong Su, Yan-Yang Qin, Tiantian Wu, De-Yin Wu
Summary: Single-atom catalysis is a hot topic in heterogeneous catalysis, but determining the stability and activity of single atoms on oxide supports compared to clusters and nanoparticles remains challenging. It was found that single Au atoms at step-edges serve as active sites for low-temperature CO oxidation, and the interface between Au nanoparticles and CeO2 can directly catalyze CO oxidation through the Mars-van Krevelen mechanism.
JOURNAL OF CATALYSIS
(2022)
Article
Chemistry, Physical
Dmitrii German, Ekaterina Pakrieva, Ekaterina Kolobova, Sonia A. C. Carabineiro, Marta Stucchi, Alberto Villa, Laura Prati, Nina Bogdanchikova, Vicente Cortes Corberan, Alexey Pestryakov
Summary: This study investigated the effect of noble metal-based catalysts on the selective oxidation of HMF to FDCA, finding that higher FDCA selectivity was achieved when metals were supported on Sibunit carbon. Furthermore, functionalization of the Sibunit carbon surface with HNO3 and NH4OH led to a change in the active states of Pd and Au, resulting in increased FDCA production.
Article
Chemistry, Physical
Akbar Mahdavi-Shakib, Todd N. N. Whittaker, Tae Yong Yun, K. B. Sravan Kumar, Lauren C. C. Rich, Shengguang Wang, Robert M. M. Rioux, Lars C. C. Grabow, Bert D. D. Chandler
Summary: Hydrogen spillover is the migration of H atom equivalents from metal nanoparticles to a support. This study measures weak, reversible H-2 adsorption on Au/TiO2 catalysts and determines the surface concentration of spilled-over hydrogen. The adsorption behavior of H* on the titania surface is found to increase with temperature, which is attributed to high proton mobility, configurational surface entropy, and increasing hydroxyl acid-base equilibrium constants.
Article
Multidisciplinary Sciences
Yifan Wang, Jake Kalscheur, Ya-Qiong Su, Emiel J. M. Hensen, Dionisios G. Vlachos
Summary: Understanding the evolution of the catalyst's structure under working conditions is challenging. The study introduces a multiscale modeling framework and machine learning to investigate the structures and nucleation of CeO2-supported Pd clusters and single atoms at different catalyst loadings, temperatures, and exposures to CO. Experimental data lacks simultaneous temporal and spatial resolution, hindering accurate structure determination.
NATURE COMMUNICATIONS
(2021)
Article
Chemistry, Multidisciplinary
Ahmed M. A. ElSheikh, Gordana Backovic, Raisa C. P. Oliveira, Cesar A. C. Sequeira, James McGregor, Biljana Sljukic, Diogo M. F. Santos
Summary: The research demonstrates that palladium-based trimetallic catalysts synthesized via a facile procedure show great potential for borohydride-based fuel cells in compact environments. Three different routes were used to prepare carbon-supported trimetallic catalysts, each showing unique structural and activity characteristics.
Article
Chemistry, Physical
Muhua Chen, Weizhen Wang, Yuping Qiu, He Wen, Guangyao Li, Zhiqing Yang, Ping Wang
Summary: This study experimentally identified the active sites in HCHO oxidation over TiO2-supported Pt catalysts and revealed the cooperative mechanism involved.
Article
Chemistry, Physical
Yue Zhang, Cong Wu, Zhiqiang Wang, Jiawei Ji, Haiqin Wan, Weixin Zou, Qing Tong, Jingfang Sun, Lin Dong, Yu-Wen Chen
Summary: Bimetallic Pt-Ir alloy nanoparticles were successfully prepared by a microwave-assisted method and used as catalysts for toluene combustion. The Pt2.5Ir/CeO2 catalyst showed excellent low-temperature catalytic activity, attributed to the interaction between Pt and Ir, richer adsorbed oxygen species, and low-temperature reducibility.
APPLIED SURFACE SCIENCE
(2022)
Article
Chemistry, Physical
Ali Aldalbahi, Mohamed H. El-Newehy, Hany El-Hamshary, Edmund Samuel, Sam S. Yoon
Summary: In this study, a facile and efficient method was reported to fabricate methanol oxidation electrocatalysts. The catalyst, composed of porous carbon flakes (PCFs)-supported nickel nanoplates (Ni NPs), was synthesized in one step using molten salt synthesis. Characterization techniques revealed a finely dispersed Ni NPs with a highly crystalline structure on the PCFs. The Ni NPs@PCFs catalyst exhibited high electrocatalytic activity and stability in alkaline media.
Article
Chemistry, Physical
Jeremy Hu, Eun Mi Kim, Michael J. Janik, Konstantinos Alexopoulos
Summary: Density functional theory was used to investigate the mechanisms of hydrogen activation and spillover on anatase TiO2-supported Ag single-atom catalysts. The presence of Ag single atoms was found to facilitate the formation of surface oxygen vacancies and promote H2 dissociative adsorption.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Oleksii Bezkrovnyi, Albert Bruix, Dominik Blaumeiser, Lesia Piliai, Simon Schoetz, Tanja Bauer, Ivan Khalakhan, Tomas Skala, Peter Matvija, Piotr Kraszkiewicz, Miroslawa Pawlyta, Mykhailo Vorokhta, Iva Matolinova, Joerg Libuda, Konstantin M. Neyman, Leszek Ke Pinski
Summary: Understanding the metal-support interaction in catalytic materials is crucial for heterogeneous catalysis research. In this study, gold nanoparticles and ceria supports were investigated using in situ methods and theoretical calculations. The results revealed an inhomogeneous charge distribution between the gold nanoparticles and ceria supports, and electron transfer occurred from the reduced ceria substrate to the supported gold nanoparticles after exposure to CO.
CHEMISTRY OF MATERIALS
(2022)
Article
Chemistry, Physical
Yifan Wang, Ya-Qiong Su, Emiel J. M. Hensen, Dionisios G. Vlachos
Summary: Subnanometer catalysts provide high noble metal utilization and superior performance for various reactions. However, understanding their atomic-scale structures and properties under working conditions is challenging due to the large configurational space. In this study, an efficient multiscale framework integrating density functional theory (DFT) calculations, cluster expansion, machine learning, and structure optimization is introduced to predict the stability of catalysts exposed to adsorbates. The framework enables automatic discovery of stable catalyst structures and a systematic strategy to exploit properties at the subnanometer scale. Simulation results for CO-adsorbed Pd-n (n = 1-55) clusters on CeO2(111) reveal that CO can facilitate restructuring by stabilizing smaller planar structures and bilayer structures of specific intermediate sizes.
CHEMISTRY OF MATERIALS
(2022)
Article
Chemistry, Physical
Hansaem Jang, Jeong-Hyeon Lee, Jeon Ryang Lee, Tae-Won Kim
Summary: Only a few materials can remain stable under acidic conditions, which limits the choice of catalysts and supports. The strong metal-support interaction in Ir/ATO structures, synthesized using the polyol process, can paradoxically deactivate the structures by causing reduction of the Sb dopant. This reduces the electrical conductivity of Ir/ATO and hinders electron transfer, deteriorating electrocatalytic activity towards OER.
ACS APPLIED ENERGY MATERIALS
(2022)
Review
Chemistry, Multidisciplinary
Eric S. Wiedner, Aaron M. Appel, Simone Raugei, Wendy J. Shaw, R. Morris Bullock
Summary: Pendant amines play a crucial role in chemical reactivity, especially for molecular catalysts. Inspired by [FeFe]-hydrogenases, synthetic catalysts have been developed to incorporate a pendant amine for multifunctionality. Cyclic diphosphine ligands containing pendant amines have profound effects on catalyst reactivity and have been used for oxidation and hydrogen production electrocatalysts. The optimal benefit of the pendant amine requires suitable basicity and positioning relative to the metal center.
Article
Engineering, Environmental
Lukas Schick, Vicenta Gonzalez-Alfaro, Adrian Garcia, J. M. Lopez, David J. Morgan, Said Agouram, Stuart H. Taylor, Tomas Garcia, Benjamin Solsona
Summary: The nature of the support and calcination temperature significantly influence the catalytic performance of iridium oxide supported catalysts for the total oxidation of VOCs. Silica, ZSM-5 zeolites, and titania are suitable supports for IrOx, while gamma-alumina is not suitable. The Lewis acidity of the support has a strong influence on the turnover frequency of the iridium oxide.
CHEMICAL ENGINEERING JOURNAL
(2021)
Article
Chemistry, Physical
Robert Hure, Samuel Simoneau, Bert D. Chandler, Jennifer M. Steele
Article
Chemistry, Physical
Camilah D. Powell, Arthur W. Daigh, Meagan N. Pollock, Bert D. Chandler, Christopher J. Pursell
JOURNAL OF PHYSICAL CHEMISTRY C
(2017)
News Item
Chemistry, Multidisciplinary
Bert D. Chandler
Article
Chemistry, Physical
Gregory M. Mullen, Edward J. Evans, Iliya Sabzevari, Brittany E. Long, Khalid Alhazmi, Bert D. Chandler, C. Buddie Mullins
Article
Chemistry, Multidisciplinary
Johnny Saavedra, Christopher J. Pursell, Bert D. Chandler
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2018)
Article
Chemistry, Multidisciplinary
Gaurav Kumar, Luke Tibbitts, Jaclyn Newell, Basu Panthi, Ahana Mukhopadhyay, Robert M. Rioux, Christopher J. Pursell, Michael Janik, Bert D. Chandler
Article
Chemistry, Physical
James E. Bruno, K. B. Sravan Kumar, Nicolas S. Dwarica, Alexander Huther, Zhifeng Chen, Clemente S. Guzman, Emily R. Hand, William C. Moore, Robert M. Rioux, Lars C. Grabow, Bert D. Chandler
Article
Chemistry, Multidisciplinary
K. B. Sravan Kumar, Todd N. Whittaker, Christine Peterson, Lars C. Grabow, Bert D. Chandler
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2020)
Article
Chemistry, Physical
James E. Bruno, Nicolas S. Dwarica, Todd N. Whittaker, Emily R. Hand, Clemente S. Guzman, Anish Dasgupta, Zhifeng Chen, Robert M. Rioux, Bert D. Chandler
Article
Chemistry, Physical
Akbar Mahdavi-Shakib, Janine Sempel, Lauren Babb, Aisha Oza, Maya Hoffman, Todd N. Whittaker, Bert D. Chandler, Rachel Narehood Austin
Article
Chemistry, Multidisciplinary
Akbar Mahdavi-Shakib, K. B. Sravan Kumar, Todd N. Whittaker, Tianze Xie, Lars C. Grabow, Robert M. Rioux, Bert D. Chandler
Summary: H-2 adsorption on Au catalysts is weak and reversible, posing challenges for quantitative studies. By investigating H-2 adsorption on Au/TiO2 catalysts, electron transfer to the support was observed, leading to shifts in FTIR background signals, which were used to quantify H-2 adsorption. Additionally, a new H-O-H bending vibration associated with proton adsorption on distinct metal-support interface sites was identified, providing new insights into the nature and dynamics of H-2 adsorption at the Au/TiO2 interface.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Akbar Mahdavi-Shakib, Lauren C. Rich, Todd N. Whittaker, Bert D. Chandler
Summary: Infrared spectroscopy reveals that H-2 adsorption on Au/TiO2 catalysts occurs heterolytically at the metal-support interface, generating stable protonated MSI hydroxyls. Au modifies the local structural and electronic properties of the support, leading to an increase in the basicity of electron-rich MSI hydroxyls. This synergism between Au and TiO2 results in electron-deficient Au particles and more electron-rich MSI hydroxyls, contributing to stronger Lewis acids and Bronsted bases, respectively.
Article
Nanoscience & Nanotechnology
Tae Yong Yun, Bert D. Chandler
Summary: Surface hydroxyl groups on metal oxides have significant effects in catalyst synthesis and catalytic reactions, yet their broader material properties are not regularly reported. This study provides direct methods to quantify fundamental properties of surface hydroxyls on different titania- and alumina-based supports. The results show variations in surface hydroxyl density and intrinsic acidity/basicity among different titania sources, as well as the temperature effects on surface acid-base properties and isoelectric point changes.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
Akbar Mahdavi-Shakib, Todd N. N. Whittaker, Tae Yong Yun, K. B. Sravan Kumar, Lauren C. C. Rich, Shengguang Wang, Robert M. M. Rioux, Lars C. C. Grabow, Bert D. D. Chandler
Summary: Hydrogen spillover is the migration of H atom equivalents from metal nanoparticles to a support. This study measures weak, reversible H-2 adsorption on Au/TiO2 catalysts and determines the surface concentration of spilled-over hydrogen. The adsorption behavior of H* on the titania surface is found to increase with temperature, which is attributed to high proton mobility, configurational surface entropy, and increasing hydroxyl acid-base equilibrium constants.