Article
Chemistry, Multidisciplinary
Qingtao Wang, Yiqi Xu, Jing Zhou, Longyu Xu, Lu Yu, Dahao Jiang, Chunshan Lu, Zhiyan Pan, Qunfeng Zhang, Xiaonian Li
Summary: A novel and highly effective Pd catalyst (Pd@S-1@IL) was fabricated for selective hydrogenation of acetylene, showing remarkable selectivity and stability attributed to the core-shell structure and ionic liquid layer.
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
(2021)
Article
Chemistry, Multidisciplinary
Chao Qin, Qing Guo, Jianping Guo, Ping Chen
Summary: A simple and efficient Pd/MgO catalyst with ppm level of Pd loaded (7.8 ppm) for semi-hydrogenation of acetylene to ethylene was reported. The catalyst exhibited excellent performance with high conversion of acetylene (97%), high selectivity of ethylene (89%) and good stability. Furthermore, it was found that atomically dispersed Pd atoms are not active for ethylene hydrogenation, and H-2 dissociates at isolated Pd atoms in a heterolytic manner forming O-H bond, which may contribute to the high selectivity.
CHEMISTRY-AN ASIAN JOURNAL
(2021)
Article
Chemistry, Physical
Qianqian Zhang, Yifan Sun, Wei Li, Jinli Zhang, Yan Fu
Summary: In this study, Pd/SnO2 nanocatalysts were synthesized and used for selective hydrogenation of a, b-unsaturated aldehydes. The results showed high selectivity and faradaic efficiency, outperforming commercial Pd/C catalysts.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2022)
Review
Biochemistry & Molecular Biology
Xinxiang Cao, Ben W. -L. Jang, Jiaxue Hu, Lei Wang, Siqi Zhang
Summary: Selective semi-hydrogenation of acetylene is important both in industry and theory. Palladium is the most active metal and is widely used for this reaction, but it has poor selectivity towards ethylene. A commonly used strategy to improve the catalytic performance is introducing a secondary metal to tune the geometric and electronic structures of Pd nanoparticles. Various supported Pd-based bimetallic catalysts have been studied in the past decade, and their preparation methods, advantages, and disadvantages are summarized in this review.
Article
Chemistry, Physical
Zhu Xu, Shuzhen Zhou, Mingyuan Zhu
Summary: The Ni/AC-N-x catalyst synthesized by a simple impregnation method showed high acetylene conversion rate at 200 degrees Celsius under high gas hourly space velocity, while the Ni/AC catalyst exhibited a lower acetylene conversion rate.
CATALYSIS COMMUNICATIONS
(2021)
Article
Chemistry, Physical
Kyunglim Hyun, Younghwan Park, Minkee Choi
Summary: In this study, the catalytic effect of chain length of organic modifiers on the selective partial hydrogenation of acetylene was systematically investigated. It was found that longer chain length of the modifiers improved the selectivity of acetylene partial hydrogenation by inhibiting ethylene adsorption and full hydrogenation. Additionally, longer chain length of the modifiers also contributed to better long-term catalyst stability.
JOURNAL OF CATALYSIS
(2022)
Article
Chemistry, Physical
Pratya Promchana, Kittisak Choojun, Wanwisa Limphirat, Yingyot Poo-arporn, Tawan Sooknoi
Summary: Acetylene in ethylene-rich feed can be removed via acetylene/ethylene cross-metathesis over WO3-supported catalysts at 450 degrees C, yielding 1,3-butadiene with cyclohexene as a minor product. The catalyst must be treated with ethylene at 600 degrees C to generate a genuinely active site of tungsten (IV) alkylidene species (W=CH2). The H2 treatment decreases surface W--O concentration, and hence the activity.
APPLIED CATALYSIS A-GENERAL
(2023)
Article
Chemistry, Multidisciplinary
Fatemeh Dodangeh, Alimorad Rashidi, Hossein Aghaie, Karim Zare
Summary: A novel nanocatalyst was developed for selective hydrogenation of acetylene to ethylene, utilizing mesoporous carbon nitride as the catalyst support and modifying the Pd active sites with different Ag/Pd ratios. The modified nanocatalysts showed excellent performance in terms of acetylene conversion and ethylene selectivity, with the sample prepared using the optimal Ag/Pd ratio (1:1) achieving 98.1% ethylene selectivity at 200 degrees C.
JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
(2021)
Article
Chemistry, Physical
Hong-Yan Ma, Gui-Chang Wang
Summary: The study reveals that metal clusters of different sizes have different catalytic mechanisms in CO2 methanation reaction. The Ru-4 catalyst shows the highest catalytic activity and stability among the tested catalysts.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Chemistry, Multidisciplinary
Kaili Zhang, Qinglei Meng, Haihong Wu, Jiang Yan, Xuelei Mei, Pengfei An, Lirong Zheng, Jing Zhang, Mingyuan He, Buxing Han
Summary: CeO2-supported Ru single-atom catalysts enable the hydrogenation of the benzene ring and catalyze etheric C-O(R) bond cleavage, leading to high yields of cyclohexanols.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Physical
Lena Puntscher, Panukorn Sombut, Chunlei Wang, Manuel Ulreich, Jiri Pavelec, Ali Rafsanjani-Abbasi, Matthias Meier, Adam Lagin, Martin Setvin, Ulrike Diebold, Cesare Franchini, Michael Schmid, Gareth S. Parkinson
Summary: The adsorption/desorption behavior of ethene on Fe3O4(001) surface was investigated. Ethene was found to adsorb intact at all coverages and interact most strongly with surface defects and Fe adatoms. It primarily adsorbs on surface Fe sites and desorbs at a coverage with a desorption energy of 0.36 eV. The total capacity of the surface for ethene adsorption is approximately 4 molecules per unit cell.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Engineering, Environmental
Aiqun Kong, Menghui Liu, Houjun Zhang, Zifan Cao, Jinli Zhang, Wei Li, You Han, Yan Fu
Summary: In this study, electrocatalytic hydrogenation was used to convert benzoic acid into cyclohexanecarboxylic acid. Carbon fibers with different degrees of graphitization were used as the support for commercial platinum carbon electrode without external hydrogen. The results showed that the conversion of benzoic acid and the selectivity of cyclohexanecarboxylic acid reached 100% using carbon fiber paper (CFP)-supported Pt/C electrode at room temperature and 1 atm pressure in 0.05 M H2SO4 solution.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Chemistry, Applied
Yuan Zhang, Xun Sun, Yali Zhao, Huijuan Su, Toru Murayama, Caixia Qi
Summary: The study found that the catalyst Au/CNA, prepared by carbonizing organic precursors containing C and N atoms on Al2O3, showed higher catalytic activity in the selective hydrogenation of acetylene to ethylene, with a TOF value five times higher than Au/Al(2)O(3) at 250 degrees Celsius. The interaction between N species on the CNA support and nano-gold particles is likely a key factor in the improved catalytic performance of Au/CNA.
TOPICS IN CATALYSIS
(2021)
Article
Chemistry, Physical
Daria V. V. Yurpalova, Tatyana N. N. Afonasenko, Igor P. P. Prosvirin, Andrey V. V. Bukhtiyarov, Maxim A. A. Panafidin, Zakhar S. S. Vinokurov, Mikhail V. V. Trenikhin, Evgeny Yu. Gerasimov, Tatyana I. I. Gulyaeva, Larisa M. M. Kovtunova, Dmitry A. A. Shlyapin
Summary: Novel bimetallic Pd-Co catalysts supported on Sibunit carbon material were synthesized and used for selective acetylene hydrogenation to produce ethylene. Increasing the Pd:Co molar ratio from 1:0 to 1:2 in 0.5%Pd-Co/C catalysts, treated at 500 degrees C under hydrogen, led to an increase in ethylene selectivity from 60 to 67% (T = 45 degrees C). The catalysts were characterized using various methods and it was found that the optimal catalytic properties were observed in catalysts with a Pd:Co molar ratio of 1:2-1:4.
Article
Chemistry, Multidisciplinary
Qiang Gao, Zihao Yan, Weijie Zhang, Hemanth Somarajan Pillai, Bingqing Yao, Wenjie Zang, Yuanqi Liu, Xue Han, Bokki Min, Hua Zhou, Lu Ma, Bukuru Anaclet, Sen Zhang, Hongliang Xin, Qian He, Huiyuan Zhu
Summary: This study reports the synthesis of Pd-Cu nanocubes as a highly active and selective catalyst for the hydrogenation of acetylene to ethylene. The core/shell structure with high surface density of active Pd sites isolated by Cu in the B2 intermetallic matrix enhances the catalytic performance compared to pristine Pd and Cu catalysts.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Loukas Kollias, Roger Rousseau, Vassiliki-Alexandra Glezakou, Matteo Salvalaglio
Summary: In this study, the collective assembly of building units during the early stages of metal-organic framework (MOF) nucleation was investigated using large-scale molecular dynamics simulations. The choice of solvent, introduction of ions, and relative populations of MOF building unit isomers were found to greatly influence the cluster formation process, leading to variations in shape, size, nucleation and growth rates, crystallinity, and order. Graph theory analysis revealed that only a few molecular descriptors were needed to understand MOF self-assembly and these descriptors can be experimentally observed. This approach provides valuable insights into the complex processes of MOF synthesis and scale-up.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Editorial Material
Chemistry, Multidisciplinary
Vassiliki-Alexandra Glezakou, Roger Rousseau, Tong Lin
Article
Physics, Condensed Matter
Michael Gottschalk, Mal-Soon Lee, Eric Goodwin, Camille Mikolas, Thomas Chasapis, Duck Young Chung, Mercouri G. Kanatzidis, Subhendra D. Mahanti, Stuart Tessmer
Summary: Using scanning tunneling spectroscopy, the effects of nitrogen gas exposure on the electronic density of states of Bi2Se3 were investigated. Nitrogen gas molecules were observed to physisorb near Se vacancies, resulting in a saturation of the exposure effect after approximately 50 min. Density functional theory calculations and molecular dynamics simulations support the dissociative adsorption of N2 molecules and their strong binding to Se vacancies, which modifies the position of the Fermi energy relative to the Dirac point.
SOLID STATE COMMUNICATIONS
(2023)
Review
Chemistry, Multidisciplinary
Manh-Thuong Nguyen, Carlos A. Fernandez, Mostofa Haider, Kung-Hui Chu, Guoqing Jian, Somayeh Nassiri, Difan Zhang, Roger Rousseau, Vassiliki-Alexandra Glezakou
Summary: Cement and concrete are essential materials for constructing durable habitats and infrastructure. However, concrete cracking leads to expensive repairs and contributes to climate change. Therefore, the development of more durable cementitious materials with self-healing capabilities is urgently needed. This review presents five different strategies to achieve self-healing in cement-based materials and discusses the self-healing agents and mechanisms involved.
Article
Chemistry, Physical
Runze Ma, Christopher R. O'Connor, Gregory Collinge, Sarah I. Allec, Mal-Soon Lee, Zdenek Dohnalek
Summary: The dynamics of acetic acid on anatase TiO2(101) were investigated using scanning tunneling microscopy experiments and density functional theory calculations. The study showed the simultaneous diffusion of bidentate acetate and a bridging hydroxyl, as well as the transient formation of molecular monodentate acetic acid. The diffusion rate was found to be strongly dependent on the position of hydroxyl and adjacent acetate(s). A three-step diffusion process involving acetate and hydroxyl recombination, acetic acid rotation, and acetic acid dissociation was proposed. This study provides insights into the importance of bidentate acetate dynamics in the formation of monodentate species, which drive selective ketonization.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Linxiao Chen, Sarah I. Allec, Manh-Thuong Nguyen, Libor Kovarik, Adam S. Hoffman, Jiyun Hong, Debora Meira, Honghong Shi, Simon R. Bare, Vassiliki-Alexandra Glezakou, Roger Rousseau, Janos Szanyi
Summary: Research interest in single-atom catalysts (SACs) has been increasing, however, the lack of understanding of their dynamic behaviors during applications hinders catalyst development and mechanistic understanding. This study reports on the evolution of active sites over a Pd/TiO2-anatase SAC in the reverse water-gas shift (rWGS) reaction. The insights gained about SAC dynamics and the structure-function relationship are valuable for mechanistic understanding and catalyst design.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Applied
Christopher R. O'Connor, Runze Ma, Gregory Collinge, Mal-Soon Lee, Greg A. Kimmel, Zdenek Dohnalek
Summary: In this study, the adsorption and reaction of acetic acid on anatase TiO2(101) were investigated using various techniques. It was found that acetic acid can form two intermediates: dissociated, bidentate acetate and molecular, monodentate acetic acid. The presence of both intermediates was observed at low temperatures, while only the bidentate acetate was observed at high temperatures. This research provides important insights into the stability and reactivity of carboxylic acid surface-bound intermediates, which play a role in biomass upgrading via ketonization reactions.
TOPICS IN CATALYSIS
(2023)
Article
Chemistry, Physical
Jinshu Tian, Gregory Collinge, Simuck F. F. Yuk, Jindong Lin, Vassiliki-Alexandra Glezakou, Mal-Soon Lee, Yong Wang, Roger Rousseau
Summary: Through density functional theory calculations, in situ Raman characterization, and microkinetic modeling, it is found that dimerized di-coordinated boron sites are the active species for O-2 activation and peroxy-like structures are responsible for propane activation. The formation of adsorbed C3H7* radicals was found to be the main rate-controlling step. These findings provide significant insights into the mechanisms of oxidative dehydrogenation of propane on boron-based catalysts.
Article
Chemistry, Physical
Vanessa Lebarbier Dagle, Gregory Collinge, Mohammed Rahmana, Austin Winkelman, Wenda Hu, Jian Zhi Hu, Libor Kovarik, Mark Engelhard, Jennifer Jocz, Yong Wang, Mal-Soon Lee, Vassiliki-Alexandra Glezakou, Debmalya Ray, Roger Rousseau, Robert Dagle
Summary: This study reports on a Cu/ZrO2/SBA-16 catalyst with remarkable olefins selectivity and enhanced stability compared to the Ag/ZrO2/SBA-16 catalyst. Replacing Ag with Cu shifts the reaction pathway of crotonaldehyde hydrogenation, leading to the formation of butyraldehyde. Experimental and computational tools were used to verify the performance and stability advantage of the Cu/ZrO2/SBA-16 catalyst.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Multidisciplinary
Oliva M. M. Primera-Pedrozo, Shuai Tan, Difan Zhang, Brian T. T. O'Callahan, Wenjin Cao, Eric T. T. Baxter, Xue-Bin Wang, Patrick Z. Z. El-Khoury, Venkateshkumar Prabhakaran, Vassiliki-Alexandra Glezakou, Grant E. E. Johnson
Summary: This study synthesized Keggin POMs with both tungsten and vanadium atoms and used ion soft landing to deliver these POMs to different self-assembled monolayer surfaces on gold. The interactions between POMs and supports, as well as POMs and neighboring POMs, were characterized using various spectroscopic techniques. The results showed that surface functional groups and nanoscale heterogeneity can modulate the observed spectroscopic signatures, and POM-POM interactions also affect the spectral shifts.
