Article
Chemistry, Multidisciplinary
Vivek Polshettiwar, Rajesh Belgamwar, Rishi Verma, Tisita Das, Sudip Chakraborty, Pradip Sarawade
Summary: A highly active and stable Cu-based catalyst was developed for the conversion of CO2 to CO by creating a strong metal-support interaction (SMSI) between Cu active sites and TiO2-coated dendritic fibrous nano-silica (DFNS/TiO2). The catalyst exhibited excellent catalytic performance and remained active even after 200 hours of reaction. The presence of SMSI between Cu and TiO2 was confirmed by various spectroscopic techniques. The continuous generation and regeneration of defects during the reaction led to long-term high catalytic activity and stability.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Applied
Danyu Wang, Zhe Li, Tian-Yi Luo, Michael B. Schmithorst, Sunghwan Park, Wenqian Xu, Yurun Miao, Kaivalya Gawande, Chaoyun Tang, Brandon C. Bukowski, Bradley F. Chmelka, Howard Fairbrother, Efrosini Kokkoli, Michael Tsapatsis
Summary: Adenosine triphosphate (ATP) and other nucleotides can be irreversibly bound to the metal-organic framework (MOF) MIL-101(Cr). Analysis suggests that ATP is bound to MIL-101(Cr) through the terminal phosphate group with Cr(III) of the framework. The MOF-supported nucleotides can function as stable and reusable enantioselective heterogeneous catalysts in the presence of Cu(II) ions.
MICROPOROUS AND MESOPOROUS MATERIALS
(2023)
Review
Chemistry, Physical
Jia Yu, Yida Yang, Yuliang Li, Changyan Cao, Weiguo Song
Summary: Supported metal catalysts using GDY as a promising catalyst support have shown rapid progress in thermocatalytic reactions, benefiting from the electronic interaction between the support and active components.
Review
Chemistry, Multidisciplinary
Qiming Sun, Ning Wang, Jihong Yu
Summary: Zeolite-supported metal catalysts have shown superior activity and thermal stability in catalytic reactions, being widely applied in hydrogenation, dehydrogenation, oxidation, and other reactions, with promising prospects for future advancements.
ADVANCED MATERIALS
(2021)
Article
Chemistry, Physical
He Wang, Yunzuo Cui, Jinghui Shi, Xin Tao, Guangshan Zhu
Summary: In this study, B, N, P co-doped porous carbon materials were prepared and Lewis acidic/basic defects were detected in their structures. The obtained material BNP@C-800 exhibited excellent catalytic performance for glycerol carbonylation with urea under metal-free conditions, achieving high glycerol conversion and glycerol carbonate selectivity. A heterogeneous Lewis acid-base synergistic catalysis mechanism was proposed based on spectroscopic characterization of key reaction intermediates.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Review
Chemistry, Multidisciplinary
Yizhen Chen, Hanlei Sun, Bruce C. Gates
Summary: Metal nanoparticles on supports exhibit new catalytic properties when made smaller to the point of atomic dispersion. Advanced characterization techniques enhance understanding of catalyst performance, opening up possibilities for new discoveries in catalysis.
Article
Chemistry, Physical
Ewa Chukwu, Lindsay Molina, Conner Rapp, Luis Morales, Zehua Jin, Stavros Karakalos, Hui Wang, Sungsik Lee, Michael J. Zachman, Ming Yang
Summary: Increasing the surface population of supported catalytic sites is generally a beneficial approach to improving performance; however, we found that in the case of Pt/a-MoC catalysts with atomically dispersed Pt, the intrinsic activity declines as Pt loading increases. The shrinking inter-Pt-atom space hinders CO2 activation at Pt-Mo interfaces, and even when Pt is atomically dispersed, it is underutilized in crowded conditions. This cautionary observation is applicable to other systems where the support plays a crucial catalytic role.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
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)
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, 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.
Review
Materials Science, Multidisciplinary
Guangfu Liao, Li Zhang, Chunxue Li, Shi-Yong Liu, Baizeng Fang, Huaming Yang
Summary: Carbon-supported single-atom catalysts (SACs) show great promise for biomedical applications due to their unique advantages such as uniform nanoscale size, ease of preparation and functionalization, low cost and toxicity, and good biodegradability and biocompatibility.
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, Multidisciplinary
Ben Ma, Qi Xia, Deyang Wang, Ji-Kang Jin, Zekun Li, Qiu-Jiang Liang, Meng-Ying Sun, Dongyi Liu, Li-Juan Liu, Hui-Xing Shu, Jun Yang, Dan Li, Jian He
Summary: Visible-light copper photocatalysis has become a viable technology for sustainable synthetic processes. In this study, a metal-organic framework (MOF)-supported copper(I) photocatalyst was developed for iminyl radical-mediated reactions. The heterogenized copper photosensitizer exhibited higher catalytic activity than its homogeneous counterpart due to site isolation. The immobilization of copper species on MOF supports using a hydroxamic acid linker allowed for high recyclability of the heterogeneous catalysts and the preparation of previously unavailable monomeric copper species through post-synthetic modification on MOF surfaces. This study highlights the potential of MOF-based heterogeneous catalytic systems in addressing challenges in synthetic methodologies and mechanistic investigations of transition-metal photoredox catalysis.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Jian Zheng, Laura Loebbert, Saumil Chheda, Navneet Khetrapal, Julian Schmid, Carlo Alberto Gaggioli, Benjamin Yeh, Ricardo Bermejo-Deval, Radha Kishan Motkuri, Mahalingam Balasubramanian, John L. Fulton, Oliver Y. Gutierrez, J. Ilja Siepmann, Matthew Neurock, Laura Gagliardi, Johannes A. Lercher
Summary: Homotopic sites are ideal for mechanistic studies and optimal control of catalytic transformations. Nickel cations in different environments show different selectivity in the reaction of 1-butene, and the reaction mechanism follows the Cossee-Arlman mechanism.
JOURNAL OF CATALYSIS
(2022)
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
Weiwei Yang, Felipe Polo-Garzon, Hua Zhou, Zhennan Huang, Miaofang Chi, Harry Meyer III, Xinbin Yu, Yuanyuan Li, Zili Wu
Summary: In this study, different Pd single atom catalysts on ceria support were obtained by thermal pretreatment, leading to enhanced activity for methane oxidation. The enhanced activity is related to the oxygen-deficient local structure and elongated interacting distance with ceria.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Engineering, Environmental
Weiwei Yang, Mi-Young Kim, Felipe Polo-Garzon, Jian Gong, Xiao Jiang, Zhennan Huang, Miaofang Chi, Xinbin Yu, Xiang Wang, Yanbing Guo, Zili Wu
Summary: This study investigates the effects of thermal aging and sulfur poisoning on the efficiency and lifetime of natural gas three-way catalysts (TWCs). The results show that both thermal aging and sulfur-induced deactivations lead to a degradation in CH4 combustion performance due to the reconstruction of Pd species and decreased reducibility of the support. Sulfation aging promotes the activation of CH4 and O2, but the sulfate also hinders the exchange of lattice oxygen.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Physical
Yang He, Junyan Zhang, Felipe Polo-Garzon, Zili Wu
Summary: Since the 1970s, researchers have been studying the strong metal-support interactions (SMSIs) in supported metal catalysts to enhance stability and create novel catalytic sites. They have discovered that SMSIs are more common than initially thought and that various adsorbed species can promote SMSI in catalytic systems. The understanding of SMSIs has implications for catalyst stability, catalytic rates, and product selectivity in heterogeneous catalysis.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Jacob Smith, Zhennan Huang, Wenpei Gao, Guannan Zhang, Miaofang Chi
Summary: Cryogenic four-dimensional scanning transmission electron microscopy (4D-STEM) imaging is a valuable technique for studying quantum materials and their interfaces at atomic scale, but its applications are restricted by the instability of cryo-stages and electronics. To address this issue, an algorithm is developed to correct complex distortions in the atomic resolution cryogenic 4D-STEM data sets. This method involves nonrigid registration and affine transformations to minimize information loss in both reciprocal and real spaces, enabling the reconstruction of sample information from 4D-STEM data sets. It is computationally inexpensive, fast, and suitable for on-the-fly data analysis in future in situ cryogenic 4D-STEM experiments.
Review
Chemistry, Multidisciplinary
Xinbin Yu, Yongqiang Cheng, Yuanyuan Li, Felipe Polo-Garzon, Jue Liu, Eugene Mamontov, Meijun Li, David Lennon, Stewart F. Parker, Anibal J. Ramirez-Cuesta, Zili Wu
Summary: Understanding the structure-catalysis relationship in heterogeneous catalysis relies on spectroscopic and scattering tools, with neutron scattering providing unique information due to its interaction with nuclei. Neutron techniques, including vibrational spectroscopy, diffraction, and quasielastic scattering, have been extensively used to study surface adsorbates, reaction mechanisms, and catalyst structures. This review comprehensively summarizes recent advances in neutron scattering investigations of heterogeneous catalysis and discusses the challenges and future opportunities in this field.
Article
Chemistry, Physical
Xinbin Yu, Jisue Moon, Yongqiang Cheng, Luke Daemen, Jue Liu, Sung Wng Kim, Abinash Kumar, Miaofang Chi, Victor Fung, Anibal J. Ramirez-Cuesta, Zili Wu
Summary: NH3 synthesis is a critical industrial process. Ru catalysts have high activity in this reaction but are susceptible to hydrogen poisoning. By using supports like electrides and hydrides, the problem of hydrogen poisoning can be alleviated. However, there is limited research on the structural dynamics of Ru/electride catalysts during the reaction.
CHEMISTRY OF MATERIALS
(2023)
Article
Microscopy
Alex W. W. Robinson, Jack Wells, Daniel Nicholls, Amirafshar Moshtaghpour, Miaofang Chi, Angus I. I. Kirkland, Nigel D. D. Browning
Summary: Interpreting scanning transmission electron microscopy (STEM) images at the atomic scale can be challenging due to various factors affecting contrast. Simulations are often used to validate or interpret experimental images, but they can be time-consuming or require specialized hardware. Recent research in compressive sensing for experimental STEM images has shown that it is possible to reduce the acquired signal and still recover the full image without significant loss of quality. This paper proposes applying similar methods to STEM simulations to increase efficiency.
JOURNAL OF MICROSCOPY
(2023)
Article
Chemistry, Physical
Meijia Li, Tianyu Zhang, Shi-Ze Yang, Yifan Sun, Junyan Zhang, Felipe Polo-Garzon, Kevin M. Siniard, Xinbin Yu, Zili Wu, Darren M. Driscoll, Alexander S. Ivanov, Hao Chen, Zhenzhen Yang, Sheng Dai
Summary: A mechanochemistry-driven approach was used to construct strong metal-support interactions (SMSIs) under neat and ambient conditions, resulting in enhanced catalysis. The encapsulation degree and overlayer structures could be customized, leading to improved hydrogenation activity.
Article
Nanoscience & Nanotechnology
Zhun Dong, Wenda Hu, Hongjun Liu, Zhenzhen Yang, Debabrata Moitra, De-en Jiang, Sheng Dai, Jian Zhi Hu, Di Wu, Hongfei Lin
Summary: It is found that treating UiO-66 with methanol solvent and thermal activation can significantly enhance its CO2 adsorption capacity. Methanol treatment effectively removes residual impurities in the micropores of UiO-66 and improves its surface area, pore volume, and void fraction, leading to a close-to-ideal CO2 adsorption capacity.
ACS APPLIED NANO MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Haoyang Ni, Zhenyao Wu, Xinyi Wu, Jacob G. Smith, Michael J. Zachman, Jian-min Zuo, Lili Ju, Guannan Zhang, Miaofang Chi
Summary: The atomic configurations of atomically dispersed catalysts (ADCs), such as atom-atom distances and clustering, greatly affect their catalytic performance. This study presents a CNN-based algorithm that can quantify the spatial arrangement of different adatom configurations. The algorithm was proven effective in accurately identifying atom positions and analyzing large data sets of ADCs. It offers a robust method to overcome the bottleneck in STEM analysis for ADC catalyst research and has the potential to be used as an on-the-fly analysis tool for catalysts in future in situ microscopy experiments.
Article
Chemistry, Physical
Kristen Wang Romero, Felipe Polo-Garzon, Zili Wu, Aditya Savara, De-en Jiang
Summary: Using first-principles density functional theory and microkinetic modeling, we investigated the catalytic mechanism of acetylene semi-hydrogenation on a perovskite oxyhydride (POH), cubic BaTiO(2.5)H(0.5) (BTOH). We found that at 523K, mechanism 1 is more active than mechanism 2, leading to selective formation of ethylene.
Article
Chemistry, Multidisciplinary
Sourav Biswas, Sakiat Hossian, Taiga Kosaka, Jin Sakai, Daichi Arima, Yoshiki Niihori, Masaaki Mitsui, De-en Jiang, Saikat Das, Song Wang, Yuichi Negishi
Summary: This article discusses the challenges of synthesizing highly symmetric Cu(I)-thiolate nanoclusters and presents a nested Keplerian architecture of [Cu58H20(SPr)(36)(PPh3)(8)](2+) (Pr = CH2CH2CH3). The structure consists of five concentric polyhedra of Cu(I) atoms, providing enough space to accommodate five ligand shells within a range of 2 nm. This intriguing structural architecture is also correlated with the unique photoluminescence properties of the nanoclusters.
CHEMICAL COMMUNICATIONS
(2023)
Article
Nanoscience & Nanotechnology
Ounjit Sodpiban, Tanika Kessaratikoon, Jacob Smith, Guodong Ren, Silvano Del Gobbo, Sonali Das, Miaofang Chi, Valerio D'Elia, Bruce C. Gates
Summary: This study prepares atomically dispersed cerium catalysts to enhance their activity in CO oxidation reaction. By using Ce-(III) and Ce-(IV) precursors, the cerium catalysts on MgO support were successfully prepared and characterized before and after catalysis using various techniques. The results show that the excellent catalyst maintains stable activity during the 2-day reaction time and exhibits improved reducibility with the transformation of cerium ions.
ACS APPLIED MATERIALS & INTERFACES
(2023)