Article
Chemistry, Physical
Umang Agarwal, Marcello S. Rigutto, Erik Zuidema, A. P. J. Jansen, Ali Poursaeidesfahani, Shrinjay Sharma, David Dubbeldam, Thijs J. H. Vlugt
Summary: A reactor model that deconvolutes the thermodynamics of hydrocarbon adsorption and intraporous reaction kinetics in zeolite Beta was studied using Configurational-bias Monte Carlo simulations. The model provides a quantitative description of significant reactions and determines the activation enthalpies of different reactions. The model can be used to investigate the effect of pore structure on adsorption and reaction kinetics.
JOURNAL OF CATALYSIS
(2022)
Article
Chemistry, Applied
Mengheng Wang, Jincan Kang, Xuewei Xiong, Fuyong Zhang, Kang Cheng, Qinghong Zhang, Ye Wang
Summary: Recent studies show that bifunctional catalysts of metal oxides and zeolites can control hydrocarbon distribution in syngas conversion. SAPO zeolites' micropore window size primarily determines the distribution, while cage size and reaction conditions only affect it within a narrow range of chain length. Zeolite topology has a similar impact on hydrocarbon distribution in syngas conversion compared to methanol conversion.
Review
Engineering, Chemical
Juan Mirena, Joris W. Thybaut, Guy B. Marin, Johan A. Martens, Vladimir V. Galvita
Summary: Bifunctional catalysts play a key role in hydrocracking processes, where the balance of activity between metal and acid sites determines performance. The spatial distribution and distance between active material sites also influence effectiveness, with diffusion playing a crucial role in discussions on intimacy criteria. Balancing site dispersion and mass transport properties within the catalyst can guide the tuning or design of ideal bifunctional catalysts.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2021)
Article
Chemistry, Applied
Qiang Wang, Ley Boon Sim, Jianrong Xie, Songshou Ye, Jile Fu, Jiexiang Wang, Nuowei Zhang, Jinbao Zheng, Binghui Chen
Summary: This study synthesized ZSM-22 zeolites with Ce/Al molar ratios ranging from 0 to 1 and loaded them with Pt for n-hexadecane hydroisomerization. Various characterization methods confirmed the incorporation of Ce into the zeolite framework and the volcanic nature of the framework Ce content. The study demonstrated that manipulating the Ce content could alter the textural and acidity properties of the samples, leading to improved i-hexadecane selectivity and catalyst stability for Pt/ZSM-22.
MICROPOROUS AND MESOPOROUS MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Yuhao Wang, Genyuan Wang, Lars I. van der Wal, Kang Cheng, Qinghong Zhang, Krijn P. de Jong, Ye Wang
Summary: The catalytic performance of composite catalysts is influenced by the interaction between components and the migration of metals. Different metals exhibit different migration behavior towards zeolite, affecting the selectivity of hydrocarbon products.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Applied
Chunmu Guo, Wei Wang, Yang Zhang, Hailong Lin, Guozhi Jia, Tong Li, Qing Xin, Xuefeng Bai, Wei Wu
Summary: Hydroisomerization of n-alkanes over bifunctional catalysts with different metal-acid proximities has been investigated, showing that catalysts with moderate proximity demonstrate enhanced catalytic performance at high temperatures. This work provides an effective route for the simple preparation of bifunctional catalysts with lower Pd loading and favorable metal-acid balance for highly selective hydroisomerization of long-chain n-alkanes.
FUEL PROCESSING TECHNOLOGY
(2021)
Article
Chemistry, Multidisciplinary
Jiang He, Zhijie Wu, Qingqing Gu, Yuanshuai Liu, Shengqi Chu, Shaohua Chen, Yafeng Zhang, Bing Yang, Tiehong Chen, Aiqin Wang, Bert M. Weckhuysen, Tao Zhang, Wenhao Luo
Summary: By confining ultra-small Ru metal nanoclusters within the micropores of zeolite Y, the chemical selectivity towards the production of pentanoic biofuels can be significantly enhanced, leading to potential applications in the biomass conversion process. The addition of La element can maintain the activity site intimacy and prevent zeolite lattice deconstruction, thus improving catalyst stability during the HDO process.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Pandong Ma, Yubing Li, Hexun Zhou, Mengheng Wang, Mengsi Zhu, Yaoyao Han, Xin Zhang, Kang Cheng, Abhishek Dutta Chowdhury
Summary: Redox-acid bifunctional zeolites have unique physicochemical properties that make them essential in the petrochemical industry, particularly in the hydro-conversion of linear alkanes to produce high-octane fuels. Current research focuses on evaluating the communication criteria between catalytically active sites and reducing the use of noble metals in catalysis. However, the chemistry behind the interaction mode between metallic and acid sites during the hydro-conversion of n-alkanes over Pt or Pd/zeolites remains largely unexplored.
MATERIALS TODAY CHEMISTRY
(2023)
Article
Chemistry, Applied
Xiaojun Zeng, Xudong Hu, Hanbin Song, Guohua Xia, Zong-Yang Shen, Ronghai Yu, Martin Moskovits
Summary: Zeolites are a class of crystalline nanoporous inorganic materials that have regular micropores and highly tunable functionalities, and microwave technology can efficiently prepare uniform and controllable zeolites with remarkable functions. Current research focuses on the synthesis of zeolites using microwave technologies and their applications, especially in catalysis, gas sensing, CO2 capture, and biomedicine. The future development of this field shows great potential for growth and innovation.
MICROPOROUS AND MESOPOROUS MATERIALS
(2021)
Article
Chemistry, Physical
Zijun Huang, Yanan Dong, Xiaolin Jiang, Fang Wang, Chen-Xia Du, Yuehui Li
Summary: In this study, carbazole derived phosphine ligands containing a pyridine moiety were designed and prepared to enable the Pd-catalyzed Markovnikov-selective alkoxycarbonylation of aliphatic alkenes, yielding branched ester products. Preliminary mechanistic studies suggest that the bridging bromide between Pd and Mn centers is crucial for enhancing regioselectivity.
JOURNAL OF CATALYSIS
(2022)
Article
Chemistry, Multidisciplinary
Maria Roslova, Viktor J. Cybulskis, Mark E. Davis, Stacey Zones, Xiaodong Zou, Dan Xie
Summary: The structure of zeolite SSZ-43 was determined using various techniques, revealing its unique channel and window structure. New organic structure-directing agents were designed to produce SSZ-43 in a wider range of compositions.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Materials Science, Multidisciplinary
Yuchao Lyu, Weilong Zhan, Zhumo Yu, Xinmei Liu, Ye Yang, Xiaoxing Wang, Chunshan Song, Zifeng Yan
Summary: A facile one-pot synthesis method was used to prepare Ni-SAPO-11 hydroisomerization catalyst with excellent metal-acid synergy, featuring highly dispersed nickel nanoparticles and more strong acid sites, leading to better activity and selectivity compared to traditional catalysts.
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
(2021)
Article
Chemistry, Multidisciplinary
Jahaziel Amaya, Cesar Calderon, Rafael Molina, Sonia Moreno
Summary: This study synthesized Ni bifunctional catalysts supported on vermiculite, halloysite, and bentonite using various synthesis methods and characterized their catalytic performance. The choice of synthesis method and mineral type affected the catalytic activity, and the catalysts exhibited high resistance to carbonaceous residues formation on their surface.
REACTION CHEMISTRY & ENGINEERING
(2022)
Article
Chemistry, Multidisciplinary
Claudia E. Berdugo-Diaz, Melissa T. Manetsch, Yang Sik Yun, Jieun Lee, Jing Luo, Xue Chen, David W. Flaherty
Summary: Esters can be reduced to ethers and alcohols through C-O bond cleavage by hydrogenation and hydrogenolysis pathways on Bronsted acidic faujasite (M-FAU) supported metal nanoparticles. The rates and selectivities of each pathway are influenced by the metal identity (M=Co, Ni, Cu, Ru, Rh, Pd, and Pt). Pt-FAU catalyst exhibits propyl acetate consumption rates up to 100 times higher than other M-FAU catalysts and achieves a 34% selectivity for ethyl propyl ether. The reduction of esters appears to involve a bifunctional mechanism, with stepwise addition of H* atoms to the carbonyl to form hemiacetals on the metal sites, followed by hemiacetal diffusion to Bronsted acid sites for dehydration to ethers or decomposition to alcohol and aldehyde. The reduction rates of propyl acetate seem to be determined by H* addition to the carbonyl and C-O cleavage of hemiacetal.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Inorganic & Nuclear
Risheng Wang, Zhihua Peng, Pingping Wu, Hongman Sun, Yu Zhang, Fazle Subhan, Hailiang Yin, Youhe Wang, Zifeng Yan
Summary: This study presents a novel approach to synthesize nanorod stacked hierarchical ZSM-48 (NSH-ZSM-48) using a newly designed organic structure-directing agent (OSDA). The synthesized NSH-ZSM-48 exhibits abundant mesopores and high surface area, leading to enhanced catalytic activity and selectivity in the selective oxidation of cyclohexane.
INORGANIC CHEMISTRY FRONTIERS
(2022)
Article
Chemistry, Physical
Jiadong Xiao, Kang Cheng, Xiaobin Xie, Mengheng Wang, Shiyou Xing, Yuanshuai Liu, Thomas Hartman, Donglong Fu, Koen Bossers, Marijn A. van Huis, Alfons van Blaaderen, Ye Wang, Bert M. Weckhuysen
Summary: A new synthesis method for metal oxide-zeolite double-shelled hollow spheres is proposed, demonstrating superior catalytic performance in producing a variety of products without the need for separating or purifying intermediates. This research is expected to advance the rational synthesis and study of hierarchically hollow, core-shell, multifunctional catalyst materials.
Article
Physics, Applied
Yutaka Ohno, Jianbo Liang, Hideto Yoshida, Yasuo Shimizu, Yasuyoshi Nagai, Naoteru Shigekawa
Summary: The chemical composition around diamond/silicon heterointerfaces fabricated through surface activated bonding (SAB) at room temperature was examined. Iron impurities were found to segregate at the bonding interfaces, while oxygen impurities were found to segregate off the bonding interfaces in the silicon side. When the bonding interfaces were annealed, the amorphous compound converted to cubic silicon carbide (c-SiC) and nano-voids were formed between silicon and c-SiC. These nano-voids acted as sites for metal impurities to agglomerate and helped to improve the electronic properties of the bonding interfaces through impurity gettering.
JAPANESE JOURNAL OF APPLIED PHYSICS
(2022)
Article
Multidisciplinary Sciences
Kang Cheng, Luc C. J. Smulders, Lars van der Wal, Jogchum Oenema, Johannes D. Meeldijk, Nienke L. Visser, Glenn Sunley, Tegan Roberts, Zhuoran Xu, Eric Doskocil, Hideto Yoshida, Yanping Zheng, Jovana Zecevic, Petra E. de Jongh, Krijn P. de Jong
Summary: By rational arrangement of functional sites, the minimum loading of platinum can be reduced, enhancing the performance of catalysts. Deposition of trace amounts of platinum nanoparticles on the alumina binder or the outer surface of zeolite crystals increases selectivity and preserves the metal and acid functions.
Article
Chemistry, Physical
Yubing Li, Mengheng Wang, Suhan Liu, Fangwei Wu, Qinghong Zhang, Shuhong Zhang, Kang Cheng, Ye Wang
Summary: In this study, the influence of distance between metal and acid sites on the effectiveness of reactions in a methanol-mediated syngas conversion system was evaluated. The distance requirements depend on the diffusivity of reaction intermediates and the formation mechanism of products. In the syngas to aromatics reaction, the intimate contact of metal and acid sites is necessary to eliminate surface hydrogen species.
Article
Chemistry, Physical
Lei Zeng, Wei Li, Xueer Wei, Jiawei Cheng, Wei Zhou, Yanping Zheng, Fan Cai, Yuefeng Liu, Kang Cheng, Qinghong Zhang, Ye Wang
Summary: The industrial catalysts for alkane dehydrogenation to olefins often deactivate quickly due to coking and sintering. In this study, iridium, a rarely used noble metal for C-H activation, was used to create an ultra-stable IrGa/Al2O3 catalyst for propane dehydrogenation (PDH). A synergetic effect between metallic Ir and GaOx was discovered, leading to high PDH activity and propylene selectivity. The Ir0.5Ga2/Al2O3 catalyst exhibited 98% propylene selectivity at a 19% propane conversion at 550 degrees C and 86% propylene selectivity at a 35% propane conversion at 600 degrees C. The IrGa/Al2O3 catalyst demonstrated stable PDH performance for 100 hours after deactivation. Its catalytic performance is comparable to Pt-based catalysts, making the Ir-based catalyst promising for dehydrogenation reactions.
Article
Chemistry, Physical
Savannah J. Turner, Dennie F. L. Wezendonk, Robert J. A. M. Terorde, Krijn P. de Jong
Summary: In situ transmission electron microscopy technique provides insights into nanoscale processes during particle growth of supported metal catalysts. Nickel nanoparticles from a nickel phyllosilicate catalyst precursor were observed to rapidly grow to a final size of 3.5-7 nm within 3-4 minutes under specific conditions. Most of the particles were immobile, but some exhibited sintering behavior without significant size increase. The results support the hypothesis that the size of the nickel species' origin determines the particle size.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Multidisciplinary
Wangyang Wang, Wei Zhou, Yuchen Tang, Weicheng Cao, Scott R. Docherty, Fangwei Wu, Kang Cheng, Qinghong Zhang, Christophe Coperet, Ye Wang
Summary: Gold nanoparticles dispersed on mordenite efficiently catalyze the selective oxidation of methane to methanol by molecular oxygen in aqueous medium in the presence of carbon monoxide. The methanol productivity reaches 1300 mu mol g(cat) (-1) h(-1) or 280 mmol g(Au) (-1) h(-1) with 75% selectivity at 150 degrees C, outperforming most catalysts reported under comparable conditions. Both hydroxyl radicals and hydroperoxide species participate in the activation and conversion of methane, while the lower affinity of methanol on gold mainly accounts for higher methanol selectivity.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Luc C. J. Smulders, Johan H. van de Minkelis, Johannes D. Meeldijk, Min Tang, Anna Liutkova, Kang Cheng, S. Tegan Roberts, Glenn J. Sunley, Emiel J. M. Hensen, Petra E. de Jongh, Krijn P. de Jong
Summary: In this study, the heat treatment of the catalyst precursor was found to influence the location of Pd precursor within SAPO-11 and ZSM-22 zeotype materials, which in turn affects the performance of the catalyst. The catalytic performance of the Pd-on-zeotype catalysts prepared using the direct reduction approach is intermediate between that of the Pd-in-zeotype catalysts prepared using the calcination-reduction approach and that of the Pd-on-alumina catalysts.
CHEMISTRY-SWITZERLAND
(2023)
Article
Chemistry, Multidisciplinary
Zhiqiang Yang, Benjamin J. Dennis-Smither, Zhuoran Xu, Zhenchao Zhao, Meiling Guo, Neil Sainty, Guangjin Hou, Xuebin Liu, Glenn J. Sunley
Summary: Methyl carboxylate esters have been found to promote the conversion of methanol to dimethyl ether during low-temperature methanol dehydration. This study used various techniques to investigate the promotional mechanism of methyl carboxylate esters, confirming that it involves a bimolecular reaction between methanol and esters adsorbed on the catalyst active sites.
CHEMISTRY-SWITZERLAND
(2023)
Article
Chemistry, Physical
Tom A. J. Welling, Suzan E. Schoemaker, Krijn P. de Jong, Petra E. de Jongh
Summary: Gas-cell transmission electron microscopy has enabled direct, nanoscale imaging of catalysts during reaction. We compared the growth rates of carbon nanofibers measured gravimetrically in a reactor and observed through electron microscopy, and found good agreement. This allowed for detailed insight into the contribution of individual catalyst nanoparticles in these heterogeneous catalysts to overall carbon growth. The methodology of nanoscale in situ observations paves the way for understanding macroscopic rates of catalyzed reactions.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Multidisciplinary Sciences
Jingting Hu, Zeyu Wei, Yunlong Zhang, Rui Huang, Mingchao Zhang, Kang Cheng, Qinghong Zhang, Yutai Qi, Yanan Li, Jun Mao, Junfa Zhu, Lihui Wu, Wu Wen, Shengsheng Yu, Yang Pan, Jiuzhong Yang, Xiangjun Wei, Luozhen Jiang, Rui Si, Liang Yu, Ye Wang, Dehui Deng
Summary: In this study, a potassium-modified edge-rich molybdenum disulfide catalyst is reported, which enables selective CO hydrogenation to higher alcohols by regulating the reaction kinetics of C-O cleavage, C-C coupling, and desorption of alcohols.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Hui Chen, Wei Li, Mingchao Zhang, Wangyang Wang, Xian-Hua Zhang, Fa Lu, Kang Cheng, Qinghong Zhang, Ye Wang
Summary: In this study, a multifunctional Pt-Zn@H-ZSM-5 catalyst with a unique structure was reported, which exhibited excellent performance in the propane dehydroaromatization reaction. The catalyst enhanced the dehydrogenation of propane and suppressed side reactions, leading to a significant increase in the yield of aromatics.
CATALYSIS SCIENCE & TECHNOLOGY
(2022)
