Review
Chemistry, Physical
Xiaorui Du, Hailian Tang, Botao Qiao
Summary: The discoveries and development of the oxidative strong metal-support interaction (OMSI) phenomena have not only advanced the understanding of strong metal-support interaction (SMSI) but also provided an alternative approach to developing supported heterogeneous catalysts with enhanced performance. The identification and characterization methods of OMSI, along with its application in catalyst performance enhancement and influence on the discovery of new types of SMSI, are discussed in this review. Ultimately, the study presents a brief summary and proposes potential future directions.
Article
Chemistry, Multidisciplinary
Jie Xu, Heng Xu, Anqi Dong, Hao Zhang, Yitong Zhou, Hao Dong, Bo Tang, Yifei Liu, Lexi Zhang, Xijun Liu, Jun Luo, Lijian Bie, Sheng Dai, Yuhang Wang, Xuhui Sun, Yanguang Li
Summary: This study developed Ir single atoms anchored on a WO3 support with a strong electronic metal-support interaction (EMSI), achieving higher conversion efficiency and stability in CO2 cycloaddition reactions. Density functional theory calculations revealed the impact of EMSI effect on the catalytic mechanism.
ADVANCED MATERIALS
(2022)
Review
Chemistry, Multidisciplinary
Hai Wang, Liang Wang, Feng-Shou Xiao
Summary: Supported metal nanoparticles on solid carriers are highly efficient catalysts in industrial reactions, but their deactivation due to sintering and leaching under harsh conditions can be prevented by strong metal-support interactions (SMSIs). New routes for constructing SMSIs without high-temperature reduction treatments have emerged, offering advantages in stabilizing metal NPs and optimizing catalytic performances.
SCIENCE CHINA-CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Arik Beck, Hannes Frey, Xing Huang, Adam H. Clark, Emmett D. Goodman, Matteo Cargnello, Marc Willinger, Jeroen A. van Bokhoven
Summary: Platinum nanoparticles supported by titania can form overlayer due to strong metal-support interaction, which can enhance the catalyst's properties and prevent sintering. The overlayer can be reversed through oxidative treatments, but recent findings suggest its stability in oxygen. In our study, we used in situ transmission electron microscopy to investigate the changes in the overlayer under different conditions and found that high temperature and oxygen atmosphere preserved the overlayer, preventing platinum evaporation.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Felipe Polo-Garzon, Thomas F. Blum, Zhenghong Bao, Kristen Wang, Victor Fung, Zhennan Huang, Elizabeth E. Bickel, De-en Jiang, Miaofang Chi, Zili Wu
Summary: The study reveals that during the catalytic conversion of 2-propanol on Pd/TiO2 at low temperatures, coverage of Pd sites occurs due to the generation of SMSIs. The SMSIs that appear during the reaction fully reverse upon exposure to O-2 at room temperature, which may have contributed to the challenge of identifying them in the past.
Article
Chemistry, Physical
Xiaohan Yuan, Tiancheng Pu, Mengwei Gu, Minghui Zhu, Jing Xu
Summary: This study systematically investigates a series of nickel-iron-based bimetallic catalysts to unveil the nature of active sites for the CO2 hydrogenation reaction, revealing an environmental-sensitive strong metal-support interaction between Ni nanoparticles and iron oxides. Iron oxides migrate and entirely cover the metallic Ni nanoparticles during the reaction, yielding a more active core-shell-type structure with much-improved reducibility, a process indirectly monitored in a time-resolved manner by in situ DRIFTS and confirmed to complete within 30 min of the reaction.
Article
Chemistry, Physical
Tiancheng Pu, Jiacheng Chen, Weifeng Tu, Jing Xu, Yi-Fan Han, Israel E. Wachs, Minghui Zhu
Summary: In this study, the strong metal-support interaction (SMSI) phenomenon for supported Ni/CeO2 catalysts with different CeO2 nanomorphologies was systematically explored. The degree of encapsulation of Ni particles originating from the SMSI effect was found to be positively correlated with the CO2 hydrogenation activity. Quasi in situ XPS and in situ DRIFTS techniques were used to reveal the relevant species and reaction pathways. These findings provide a fundamental strategy for tailoring catalytic performance by adjusting the support surface structure.
JOURNAL OF CATALYSIS
(2022)
Article
Chemistry, Multidisciplinary
Hai Wang, Xue Dong, Yu Hui, Yiming Niu, Bingsen Zhang, Lujie Liu, Ji Cao, Mizuho Yabushita, Yoshinao Nakagawa, Keiichi Tomishige, Yucai Qin, Lijuan Song, Jianping Xiao, Liang Wang, Feng-Shou Xiao
Summary: A new form of strong metal-support interaction (SMSI) has been achieved by creating oxygen-saturated overlayers on Au/TiO2 catalyst through steaming treatment, which demonstrates improved stability compared to classical SMSI. The study shows that the strong interaction between the TiOxHy (x ≥ 2) species and Au surface causes the migration of TiO2 to encapsulate Au nanoparticles. The oxygen-saturated oxide overlayers exhibit stability in oxidative, reductive, and humid atmospheres, providing enhanced performance for metal nanoparticle catalysts under various reaction conditions, surpassing classical SMSI.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Review
Chemistry, Multidisciplinary
Tiancheng Pu, Wenhao Zhang, Minghui Zhu
Summary: Strong metal-support interactions (SMSI) is a classic yet fast-growing area in catalysis research. By regulating the interfacial interactions, SMSI phenomenon can encapsulate and stabilize metal nanoparticles, significantly impacting catalytic performance. Engineering SMSI provides a promising approach to steer catalytic performance and tackle energy and environmental challenges effectively.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Yang Zhou, Wei Xi, Zixin Xie, Zhixin You, Xunzhu Jiang, Bing Han, Rui Lang, Chuande Wu
Summary: The study demonstrates the fabrication of high loading Pt single-atom catalysts on diatomite by modifying it with CeO2 nanoparticles to increase defect sites on the support. The enhanced metal-support interaction results in above 1 wt.% loading of Pt species with atomic dispersion, showing good performance in the selective hydrogenation of phenylacetylene to styrene.
CHEMISTRY-AN ASIAN JOURNAL
(2021)
Review
Chemistry, Physical
Zhouxin Luo, Guoqiang Zhao, Hongge Pan, Wenping Sun
Summary: This review provides a comprehensive overview and analysis of the formation mechanisms and surface energy minimization mechanisms of SMSI, as well as its applications in catalysts. It offers important insights for further research and design of advanced heterogeneous catalysts.
ADVANCED ENERGY MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
F. M. Harth, B. Likozar, M. Grilc
Summary: This article discusses the application of rhenium as a catalyst in biomass conversion and the related deactivation mechanisms, detection methods, and coping strategies. It focuses on the correlation between rhenium leaching and catalyst deactivation, and systematically assesses the material properties, reaction conditions, and other factors influencing rhenium leaching. The article also presents insights into the detection of rhenium leaching and the correlation between leaching and catalyst deactivation, and proposes strategies for purposefully using rhenium leaching.
MATERIALS TODAY CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Weijie Yang, Xiaoshuo Liu, Xuelu Chen, Yue Cao, Shaoping Cui, Long Jiao, Chongchong Wu, Chuanmin Chen, Dong Fu, Ian D. Gates, Zhengyang Gao, Hai-Long Jiang
Summary: A new single-atom catalyst Fe-1-N-4-C with excellent catalytic activity and sulfur resistance has been developed for the oxidation of NO and Hg-0, showing promising potential for cleaner coal-fired power plant operations.
ADVANCED MATERIALS
(2022)
Review
Engineering, Chemical
Huan Li, Yao Zhong, Luxi Wang, Qiang Deng, Jun Wang, Zheling Zeng, Xinxiang Cao, Shuguang Deng
Summary: In this study, a class of benzenesulfonic acid-grafted metal-organic frameworks with strong acidity and hydrophobicity were successfully prepared and applied in the catalytic conversion of fructose to HMF. Due to its better hydrophobicity and oleophilicity, the hydrophobic MOF exhibited higher catalytic activity and selectivity in the HMF synthesis.
CHINESE JOURNAL OF CHEMICAL ENGINEERING
(2021)
Article
Chemistry, Multidisciplinary
Shenghua Wang, Kai Feng, Dake Zhang, Deren Yang, Mengqi Xiao, Chengcheng Zhang, Le He, Binhang Yan, Geoffrey A. Ozin, Wei Sun
Summary: Cu-based catalysts supported by SiO2 with strong metal-support interaction (SMSI) show excellent activity and long-term stability in high-temperature CO2 hydrogenation reactions. A simple and scalable method has been developed to prepare 2D silica (2DSiO(2)) supported Cu catalysts with SMSI, which may shed light on the realistic applications of stabilizing Cu catalysts.
Article
Chemistry, Multidisciplinary
Marcella Guenther, Soroush Lotfi, Sergio Sanchez Rivas, Dominic Blaette, Jan P. Hofmann, Thomas Bein, Tayebeh Ameri
Summary: Although zinc oxide is widely used in organic solar cells, its light-soaking issues can lead to reversible degradation and incorrect stability measurements. The re-adsorption of oxygen trapped at the interface of ZnO causes this reversible aging, which can be undone with a UV exposure. However, this UV pretreatment compromises device efficiency and production in an oxygen-free environment.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Liang Liang, Quanchen Feng, Xingli Wang, Jessica Huebner, Ulrich Gernert, Marc Heggen, Longfei Wu, Tim Hellmann, Jan P. Hofmann, Peter Strasser
Summary: This study investigates the chemical selectivity and faradaic efficiency of high-index Cu facets for the CO2 reduction reaction (CO2RR). Shape-controlled nanoparticles with Cu {hk0} facets are fabricated using Cu multilayer deposition on Au truncated ditetragonal nanoprisms (Au DTPs). The high-index {hk0} facets of 7 nm Au@Cu DTPs exhibit a CH4 : CO product ratio of almost 10 : 1 compared to a 1 : 1 ratio for reference Au@Cu nanoparticles.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Correction
Chemistry, Multidisciplinary
Matteo Monai, Marianna Gambino, Sippakorn Wannakao, Bert M. Weckhuysen
CHEMICAL SOCIETY REVIEWS
(2023)
Article
Chemistry, Multidisciplinary
Marcus Einert, Arslan Waheed, Stefan Lauterbach, Maximilian Mellin, Marcus Rohnke, Lysander Q. Q. Wagner, Julia Gallenberger, Chuanmu Tian, Bernd M. M. Smarsly, Wolfram Jaegermann, Franziska Hess, Helmut Schlaad, Jan P. P. Hofmann
Summary: The physico- and (photo-) electrochemical properties of ordered mesoporous (CoNiCuZnMg)Fe2O4 thin films synthesized by a soft-templating and dip-coating approach are reported for the first time. These high entropy oxides exhibit unique and unexpected physicochemical properties, making them promising candidates for energy applications.
Article
Multidisciplinary Sciences
Guusje Delen, Matteo Monai, Katarina Stanciakova, Bettina Baumgartner, Florian Meirer, Bert M. Weckhuysen
Summary: Researchers have discovered that the sorption and conversion of gaseous molecules on the surface of functional materials preferentially occur on specific undercoordinated high-index surface sites. By combining in situ PiFM with DFT calculations, they have studied the site-specific sorption and conversion of formaldehyde on faceted ZIF-8 microcrystals and observed preferential adsorption on high-index planes. They have also visualized unsaturated nanodomains and found structure sensitive conversion mediated by Lewis acidity on defective ZIF-8 crystals.
NATURE COMMUNICATIONS
(2023)
Editorial Material
Chemistry, Physical
Javier Perez-Ramirez, Bert M. Weckhuysen, Maria E. Southall
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Laurens D. B. Mandemaker, Christia Jabbour, Nikolaos Nikolopoulos, Joren M. Dorresteijn, Miguel Rivera-Torrente, Bert M. Weckhuysen
Summary: The growth mechanisms and molecular phenomena of UiO-67, UU-1, and ZIF-8 metal-organic framework (MOF) films on transparent substrates are studied using transmission-based characterization. UiO-67 follows a Volmer-Weber growth mechanism with assistance from solution-grown seeds. UU-1 exhibits fiber-like morphology and inter-fiber macroporosity, while ZIF-8 shows a similar Volmer-Weber growth mode. CO probe molecule adsorption FT-IR spectroscopy reveals the effects of methanol exposure, with UiO-67 becoming inaccessible to CO, UU-1 undergoing a topotactic transformation, and ZIF-8 remaining stable with impurity removal. This approach opens new possibilities for studying other film materials using transmission-based spectroscopy.
ADVANCED MATERIALS INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Clement Maheu, Mohammad Amin Zare Pour, Iban Damestoy, David Ostheimer, Maximilian Mellin, Dominik C. Moritz, Agnieszka Paszuk, Wolfram Jaegermann, Thomas Mayer, Thomas Hannappel, Jan P. Hofmann
Summary: Interfaces in III-V semiconductor devices are usually buried and difficult to characterize. However, the Tapered Cross Section Photoelectron Spectroscopy (TCS-PES) approach provides a promising method to address this challenge. In this study, the TCS-PES was used to investigate the heterojunction in epitaxial III-V architectures prepared by metalorganic chemical vapor deposition. The results showed that the preparation of TCSs under an uncontrolled atmosphere led to the modification of the pristine properties of buried heterointerfaces.
ADVANCED MATERIALS INTERFACES
(2023)
Article
Green & Sustainable Science & Technology
Agneev Mukherjee, Pieter Bruijnincx, Martin Junginger
Summary: The maritime sector accounts for a significant amount of global greenhouse gas emissions and is facing pressure to decarbonise. Renewable fuels show potential, but their high costs are a barrier. Carbon Capture and Storage (CCS) can enhance marine fuel decarbonisation, but adds to the cost. This study compares the costs of four renewable carbon fuels and considers the impact of carbon taxation. The results show that without carbon taxation, renewable fuels are not competitive, and methanol and DME produced using CO2 capture are the most cost-effective options.
RENEWABLE & SUSTAINABLE ENERGY REVIEWS
(2023)
Article
Chemistry, Multidisciplinary
Arjan T. Smit, Emanuela Bellinetto, Thomas Dezaire, Oussama Boumezgane, Luke A. Riddell, Stefano Turri, Michiel Hoek, Pieter C. A. Bruijnincx, Gianmarco Griffini
Summary: This study presents a novel strategy for tailoring lignin molar mass and hydroxyl group reactivity in polyurethane (PU) coatings. By fractionation and partial depolymerization, lignin fractions with specific molar mass ranges were obtained, allowing the production of coatings with different properties. The study also shows that lignin depolymerization can significantly improve lignin reactivity and enhance coating flexibility.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Article
Chemistry, Multidisciplinary
Arjan T. Smit, Thomas Dezaire, Luke A. Riddell, Pieter C. A. Bruijnincx
Summary: Lignin partial depolymerization by reduction (PDR) is a strategy to modify the molar mass and heterogeneity of technical lignin, and increase its reactivity in polymer applications. The process aims to break the remaining lignin beta-O-4 linkages, reducing the molar mass of large lignin fragments. The PDR process provides control over key lignin characteristics, allowing for tailored biobased polymer properties.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Article
Chemistry, Physical
Thuy T. Le, Wei Qin, Ankur Agarwal, Nikolaos Nikolopoulos, Donglong Fu, Matthew D. Patton, Conan Weiland, Simon R. Bare, Jeremy C. Palmer, Bert M. Weckhuysen, Jeffrey D. Rimer
Summary: This study reveals that the presence of a catalytically inactive siliceous exterior rim on ZSM-5 particles can significantly reduce diffusion limitations, leading to an improved catalyst lifetime. The synthesis of Si-zoned ZSM-5 catalysts improves the diffusion properties of the catalyst. Operando ultraviolet-visible light diffuse reflectance spectroscopy shows a substantial reduction in external coking among Si-zoned samples. Molecular dynamics simulations demonstrate that there are significantly reduced transport limitations in the zoned regions, which contributes to the improved catalyst activity of Si-zoned zeolites compared to ZSM-5 with a homogeneous acid-site distribution.
Article
Chemistry, Multidisciplinary
Florian Zand, Suzanne J. T. Hangx, Christopher J. Spiers, Peter J. van den Brink, James Burns, Matthew G. Boebinger, Jonathan D. Poplawsky, Matteo Monai, Bert M. Weckhuysen
Summary: Understanding and controlling the structure and composition of nanoparticles in supported metal catalysts are crucial for improving chemical processes. Atom probe tomography (APT) is a powerful tool for three-dimensional chemical imaging of materials with nanometer resolution. However, APT has not been used for mesoporous oxide-supported metal catalysts due to sample fracture. In this study, we developed a high-pressure resin impregnation strategy to overcome this issue and successfully applied APT to high-porous supported Pd-Ni catalyst materials active in CO2 hydrogenation. Our results demonstrate the capability of APT to quantitatively assess the size, composition, and metal distribution of nanoparticles in industrial catalysts.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Materials Science, Ceramics
Jiongjie Liu, Chuanmu Tian, Tianshu Jiang, Emmanuel Ricohermoso, Zhaoju Yu, Emanuel Ionescu, Leopoldo Molina-Luna, Jan P. Hofmann, Ralf Riedel
Summary: A series of silicon oxycarbide ceramics with different carbon content were prepared by thermal pyrolysis and spark plasma sintering. The high carbon content resulted in a porous microstructure, and the sample with 40 wt% carbon content exhibited a porosity of 34% and a specific surface area of 262 m(2)/g at 1600 degrees C. The electrochemical behavior of SiOC was evaluated and showed certain electrocatalytic activity, with the sample containing 10 wt% carbon showing an overpotential of 450 mV vs. RHE at 10 mA.cm(-2) in acid medium. The electrochemical behavior was found to be closely related to the phase composition and microstructure of the ceramics.
JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Razvan C. Cioc, Eva Harsevoort, Martin Lutz, Pieter C. A. Bruijnincx
Summary: Diels-Alder cycloaddition is an important transformation in chemistry, especially in the synthesis of versatile bio-based platform molecules. However, the reactivity of common furanic compounds presents a major challenge for industrial applications. In this study, we report a highly efficient intramolecular Diels-Alder reaction between allyl acetals of different furfurals, resulting in the formation of oxanorbornene derivatives with high chemo-, regio-, and stereoselectivity. These derivatives can be easily diversified into valuable products, offering potential for scalable production of renewable chemical building blocks from inexpensive bioderived platform molecules.
