Article
Chemistry, Physical
Ekaterina G. Ragoyja, Vitaly E. Matulis, Oleg A. Ivashkevich, Dmitry A. Lyakhov, Dominik Michels
Summary: In this study, a comprehensive investigation of the mechanism of NO reduction on Ag/gamma-Al2O3 catalyst is conducted. Two mechanisms are proposed based on the silver concentration and reaction centers. Density functional theory calculations confirm the feasibility of the proposed mechanisms and explain the observed product selectivity. Additionally, the effects of the aluminum oxide support and catalytic center nature on NO, N2, and N2O adsorption are studied.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Multidisciplinary
Weijie Deng, Yunfei Hu, Jinhui Hu, Xinling Li, Yibiao Li, Yubing Huang
Summary: A metal-free electrochemically induced strategy has been developed for the regioselective hydro/deuterophosphonylation of electron-rich alkenes with P(O)H compounds, providing various Markovnikov-type adducts in high yields. Monodeuterated organophosphorus compounds with high deuterium incorporation can be obtained by adding D2O as the D source. The protocol offers broad substrate scope, low energy consumption, high atom economy, and scalability.
CHEMICAL COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Kyungseok Lee, Byungchul Choi
Summary: A combined Ag/Al2O3 and Pd/Al2O3 catalyst was found to be effective for the selective catalytic reduction of NOx by H-2-assisted C3H6. The sequential arrangement of 1 wt% Ag/Al2O3 followed by 1Pd/Al2O3 enabled the reduction of NOx, C3H6, CO, and H-2 over wide reaction temperatures, with negligible formation of by-products.
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
(2021)
Article
Nanoscience & Nanotechnology
Xueyan Chen, Shuo Hu, Xiaoxiao Qin, Min Chen, Jianghao Zhang, Xiaolei Bao, Changbin Zhang
Summary: In this study, Ag/Al-600H(2) catalyst was prepared by loading Ag precursor onto Al2O3 and reducing with H-2. It was found that H-2 reduction had a significant effect on the activity and water resistance of Ag-based catalyst in HCHO oxidation.
ACS APPLIED NANO MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Xiaofeng Xu, Xin Hu, Zuwei Luo, Yueqiang Cao, Yi-An Zhu, Wei Li, Jinghong Zhou, Xinggui Zhou
Summary: Egg-shell-type Ag/SiO2 pellet catalysts with different thicknesses of Ag-shell were synthesized to study the diffusion effects on DMO hydrogenation to MG. The egg-shell-type catalyst with optimized Ag-shell thickness exhibited improved hydrogenation activity and MG selectivity.
NEW JOURNAL OF CHEMISTRY
(2023)
Article
Chemistry, Physical
Krishna R. Iyer, Aditya Bhan
Summary: We measured the active site density of a promoted Ag/alpha-Al2O3 ethylene epoxidation catalyst using trifluoroethanol as a chemical titrant. The introduction of trifluoroethanol into the reactant stream allowed us to assess catalytic site densities by depositing stable trifluoroethoxy or trifluoromethyl groups on the Ag surface. The measured active site densities varied between 52 and 69 mu mol(TFE) g(cat)(-1) and were distinct from those evaluated using ex-situ N2O decomposition.
Article
Chemistry, Physical
Zeycan Keskin, Tayfun Ozgur, Himmet Ozarslan, Ali Cem Yakaryilmaz
Summary: In this study, the low temperature activity of Ag-Ti-Cu/Cordierite catalyst was investigated using LPG and H-2-LPG mixture as reductant. The results showed that the presence of H-2-LPG as reductant significantly improved SCR performance, especially at low temperatures.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2021)
Article
Chemistry, Physical
Arun Arunima Balachandran Kirali, Sreejith Sreekantan, Banu Marimuthu
Summary: Ce-promoted Cu/γ-Al2O3 catalysts were prepared with varying amounts of Cu and Ce, showing high selectivity and yields in the conversion of glucose to 1,2-propanediol under mild reaction conditions.
CATALYSIS COMMUNICATIONS
(2022)
Article
Energy & Fuels
Yuewen Shao, Qingyin Li, Xinyi Dong, Junzhe Wang, Kai Sun, Lijun Zhang, Shu Zhang, Leilei Xu, Xiangzhou Yuan, Xun Hu
Summary: This study achieved a unprecedented yield of 90.5% in the direct conversion of biomass-derived furfural to GVL through consecutive hydrogenation and acid-catalyzed reactions over CuAl and a co-catalyst (i.e. H-ZSM-5) in ethanol. The abundance of hydrogenation sites and acidic sites plays a key role in determining the reaction network and product transfer, with different mechanisms of deactivation for the acid and hydrogenation catalysts needing consideration in future catalyst development.
Article
Chemistry, Applied
Claudia J. Keijzer, Luc C. J. Smulders, Dennie Wezendonk, Jan Willem de Rijk, Petra E. de Jongh
Summary: This study investigates the catalytic behavior of alpha-alumina supported silver catalysts in the presence of chloride. It is found that the particle size of silver can affect the selectivity of the catalyst, but different strategies lead to different results. In this size range, the selectivity of ethylene oxide is correlated to the Ag : Al2O3 surface ratio.
Article
Chemistry, Physical
L. F. Bobadilla, A. Munoz-Murillo, J. Gandara-Loe, A. Perez, O. H. Laguna, T. L. M. Martinez, A. Penkova, M. A. Centeno, J. A. Odriozola
Summary: This study focuses on the development of efficient catalysts for selective CO methanation in practical conditions. The results show that Rh significantly enhances the activity and selectivity, while Pt has a negative effect. These findings suggest that RuRh-based catalysts could be important for treating industrial-volume streams.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Article
Chemistry, Physical
Krishna R. Iyer, Aditya Bhan
Summary: Ethylene epoxidation on promoted Ag/α-Al2O3 catalysts shows high ethylene oxide selectivity, with complex interdependencies among ethylene oxidation, chlorine deposition and removal, and EO degradation catalytic cycles. The impact of organochloride promoters on EO synthesis kinetics is illustrated by systematic variations in ethylene and oxygen reaction orders. EO degradation rates, while not influenced by the chlorine promoter, can significantly reduce net EO selectivity.
Article
Multidisciplinary Sciences
Huan Yan, Kun He, Izabela A. Samek, Dian Jing, Macy G. Nanda, Peter C. Stair, Justin M. Notestein
Summary: The study demonstrated that growing In2O3 over Pt/Al2O3 using atomic layer deposition results in a nanostructure that kinetically couples domains through surface hydrogen atom transfer, improving the selective oxidative dehydrogenation of propane. In contrast, other nanostructures, such as Pt on In2O3 or Pt mixed with In2O3, were unable to organize the reactions effectively, resulting in more propane combustion.
Article
Chemistry, Multidisciplinary
He Zhang, Shengchun Wang, Xiaoyu Wang, Pengjie Wang, Hong Yi, Heng Zhang, Aiwen Lei
Summary: By utilizing inexpensive K2S2O8 as the oxidant at room temperature, the phenoxazination/phenothiazination of electron-rich anilines has been successfully achieved. This catalyst-free method demonstrates complete para-selective amination, showing high efficiency and simplicity in flow-chemistry synthesis.
Article
Chemistry, Multidisciplinary
Shaeel Ahmed Althabaiti, Zaheer Khan, Katabathini Narasimharao, Salem Mohamed Bawaked, Soad Zahir Al-Sheheri, Mohamed Mokhtar, Maqsood Ahmad Malik
Summary: An Ag-modified TiO2 nanomaterial was synthesized using a one-pot method. The structure and morphology of the synthesized material were determined using X-ray diffraction, scanning electron microscopy, and transmission electron microscopy. The results showed that the addition of metallic Ag nanoparticles decreased the optical band gap and photoluminescence intensity of TiO2, while increasing the Raman peak intensity and absorbance. The Ag-modified TiO2 nanomaterial exhibited higher photocatalytic efficiency than bare TiO2 and Ag metal NPs, attributed to the synergistic effect between Ag metal and TiO2 structures.
Article
Chemistry, Physical
Frederic C. Meunier, Taha Elgayyar, Kassioge Dembele, Helena Kaper
Summary: Operando diffuse reflectance FT-IR spectroscopy often detects overlapping signals between gas-phase CO and adsorbates when studying catalysts. Removing CO(g) physically may result in a rapid decay of adsorbate signals. Our study shows that carbonyls adsorbed on metallic Pt sites disappeared completely within 10 minutes at 30 degrees C upon removing CO(g) when using redox supports. However, a broad band assigned to CO adsorbed on oxidized Pt sites remained stable.
Article
Chemistry, Applied
Frederic C. Meunier
Summary: The hydrogenation of CO and especially that of CO2 has gained increasing attention for the production of base chemicals and fuels. This contribution discusses the insights that can be obtained through in situ and operando FT-IR studies on CO and CO2 hydrogenations. It emphasizes the importance of quantitative IR studies for drawing relevant conclusions and discusses the limitations and pitfalls of diffuse reflectance spectroscopy. The potential of IR spectroscopy in unraveling the properties of CO2 trapping-methanation materials is briefly discussed.
Article
Chemistry, Physical
Pauline Bredy, David Farrusseng, Yves Schuurman, Frederic C. Meunier
Summary: An operando IR study reveals that the decline in selectivity to higher hydrocarbons over cobalt-based Fischer-Tropsch catalysts when CO is replaced with CO2 is mainly attributed to surface coverage effects.
JOURNAL OF CATALYSIS
(2022)
Article
Chemistry, Physical
Frederic C. Meunier, Isaac Dansette, Kimleang Eng, Yves Schuurman
Summary: The surface species formed during the hydrogenation of CO2 with H-2 over a ZrO2-supported Cu catalyst were studied. The reactivity of two different formates located on zirconia was investigated, and it was found that the hydroxyl groups on ZrO2 were the sites where carbonates and formates were hydrogenated to methoxy species. The rate constant of the most reactive ZrO2-bound formates was about 65 times higher than that of the slower formate.
Article
Chemistry, Physical
Doldet Tantraviwat, Andrew Nattestad, Jun Chen, Burapat Inceesungvorn
Summary: The development of efficient and selective photocatalytic materials for renewable energy-based organic synthetic processes has become increasingly important. In this study, a visible-light-driven BiOI/Bi2WO6 (BI/BW) microflower heterostructure was reported as a photocatalyst for the selective oxidation of benzylamines and its derivatives. Decorating the hydrothermally prepared Bi2WO6 with BiOI significantly improved benzylamine conversion and selectivity to desired imine products. These outstanding performances are attributed to enhanced electron-hole separation and transfer efficiency, as well as a greater preference for adsorption of benzylamine and extended visible-light absorption range.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Frederic C. Meunier, Isaac Dansette, Anaelle Paredes-Nunez, Yves Schuurman
Summary: Cu/ZrO2 is a promising catalyst for CO2 hydrogenation to methanol. Three different types of formates were observed under reaction conditions, with one bound to metallic Cu and the other two bound to ZrO2. The Cu-bound formate, representing only about 7% of surface formates, was found to be highly reactive and the sole source of methanol production. This study highlights the importance of quantitative IR analysis and transient methods in understanding the role of surface species.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Partha Samanta, Albert Sole-Daura, Remy Rajapaksha, Florian M. Wisser, Frederic Meunier, Yves Schuurman, Capucine Sassoye, Caroline Mellot-Draznieks, Jerome Canivet
Summary: Molecularly defined organometallic rhodium phosphine complexes were immobilized within a MOF structure without losing their molecular nature and catalytic behavior. These MOF-based catalysts showed high activity for ethylene hydroformylation and successfully catalyzed the hydroformylation of longer and bulkier alkenes. The combination of experimental and computational methods allowed for a better understanding of the active species and molecular mechanisms involved in the catalytic reactions. The use of MOF-808 as a solid ligand offers advantages such as molecular-scale understanding, site isolation, and recycling ability.
Editorial Material
Chemistry, Physical
Frederic C. Meunier, Canio Scarfiello
Summary: The IR work in Jo et al.'s paper is critically re-analyzed and alternative interpretations are proposed, challenging some of the conclusions made by the authors.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Physical
Frederic C. Meunier, Xianwei Wang, Thomas Buergi
Summary: The presence of negatively charged gold species on Au surfaces or supported Au nanoparticles has been widely reported based on the appearance of IR bands of adsorbed CO below 2090 cm-1. However, some researchers have suggested that these bands may be solely attributed to the presence of Ni-CO species contaminating the sample surfaces. In this study, CO adsorption was monitored using a CO supply, DRIFTS reaction cell, and lines that excluded nickel contamination. The results show that a band at 2067 cm-1 appeared without the involvement of Ni carbonyls, supporting the idea of CO adsorption on negatively charged Au surfaces. © 2023 Elsevier Inc. All rights reserved.
JOURNAL OF CATALYSIS
(2023)
Article
Chemistry, Applied
Pauline Bredy, Ludovic Fine, David Farrusseng, Yves Schuurman, Frederic C. Meunier
Summary: In situ and operando diffuse reflectance FT-IR (DRIFTS) studies often require consideration of changes in optical properties. This study investigated the variation of IR optical pathlength of Fe and Co-based Fischer-Tropsch catalysts by using an internal standard CaCO3 mixed with the catalyst. The results showed the importance of considering changes in optical pathlength for quantitative DRIFTS analysis.
Article
Chemistry, Physical
Partha Samanta, Albert Sole-Daura, Remy Rajapaksha, Florian M. Wisser, Frederic Meunier, Yves Schuurman, Capucine Sassoye, Caroline Mellot-Draznieks, Jerome Canivet
Summary: Molecularly defined organometallic rhodium phosphine complexes were efficiently immobilized within a MOF structure, maintaining their molecular nature and catalytic behavior. The resulting MOF-heterogenized catalysts showed high activity in ethylene hydroformylation and successfully catalyzed the hydroformylation of longer and bulkier alkenes. The study also provided insights into the structure, evolution, and mechanisms of the active species within the MOF under catalytic conditions.
Article
Materials Science, Multidisciplinary
Collins Akor, Ahmed Osman, Christopher S. McCallum, Neha Mehta, Kevin Morgan, Pamela Walsh, Beatrice Smyth, David W. Rooney, Gary N. Sheldrake
Summary: The increasing use of anaerobic digestion (AD) for the production of renewable methane from agri-food waste has raised issues related to the handling of the digestate. This study focuses on the potential of converting the solid fraction of the digestate into biofuel and fine chemicals. The catalytic extraction of the lignin constituent of the digestate shows promising results, with the production of bio-oil and octane booster.
MATERIALS ADVANCES
(2023)
Article
Chemistry, Multidisciplinary
Loren Acher, Tristan Laredo, Thierry Caillot, Akim Kaddouri, Frederic C. Meunier
Summary: This study investigated CO2 capture and methanation using solid adsorbents, microwave absorbers, and a methane catalyst. The research demonstrated the potential of using inexpensive microwave technology to convert trapped CO2 into valuable products.
APPLIED SCIENCES-BASEL
(2023)
Article
Chemistry, Physical
Frederic C. Meunier
Summary: Formation of ppm levels of volatile Ni(CO)(4) occurred on a worn commercial cell used for reflectance FT-IR in the presence of 1 kPa CO, but not on a more recent cell. The presence of Ni(CO)(4) resulted in nickel deposition on Au and Cu-based catalysts with specific Ni-CO IR bands. In contrast, no Ni-CO IR bands were observed on plain silica, indicating the requirement of specific sites for Ni(CO)(4) decomposition. The unambiguous evolution of the carbonyl signal on Au/SiO2 can be used to test the presence of ppm levels of Ni(CO)(4) in in situ and operando IR cells.
CATALYSIS SCIENCE & TECHNOLOGY
(2022)
Article
Chemistry, Multidisciplinary
Prutthipong Tsuppayakorn-aek, Wiwittawin Sukmas, Prayoonsak Pluengphon, Burapat Inceesungvorn, Piya Phansuke, Pungtip Kaewtubtim, Rajeev Ahuja, Thiti Bovornratanaraks, Wei Luo
Summary: This study investigates novel compounds with a wide range of changes in structural properties affected by hydrogen using the first-principles cluster expansion technique. It is found that lanthanum hydride compounds LaH3 become stabilized by yttrium substitution under moderate pressure and exhibit semiconductor or semi-metallic characteristics. These findings provide a deeper understanding of this class of rare-earth ternary hydrides.
Article
Chemistry, Physical
Zi-Ye Liu, Qian-Yu Wang, Ji-Ming Hu
Summary: In this study, a layered carbon dot composite catalyst (NiFe LDH@CDs) was prepared using a one-step coprecipitation method, without the need for heating or hydrothermal treatment. The CD-functionalized catalyst facilitated rapid charge transfer and accelerated the oxygen evolution reaction. Additionally, the heterojunction structure formed between NiFe LDH and CDs efficiently suppressed photoelectron-hole recombination.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
Article
Chemistry, Physical
Rohit Kumar, Ankit Kumar Srivastava, Palaniyappan Nagarasu, Vedichi Madhu, Ekambaram Balaraman
Summary: We designed and synthesized a NN-CoII bidentate complex and used it for the amination of alcohols under mild and solventless conditions. The complex exhibited good reactivity towards both primary and sterically hindered secondary alcohols, providing high yields of amines. The pyrazole moiety in the ligand played a crucial role in the reaction. Furthermore, we demonstrated the reusability of the complex as a homogeneous cobalt catalyst.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
Article
Chemistry, Physical
Shivanand Chettri, Liang-Ting Wu, Sagarmani Rasaily, Debesh Sharma, Bikram Gurung, Rajani Dewan, Sudarsan Tamang, Jyh-Chiang Jiang, Anand Pariyar
Summary: Replicating the enzymatic surface microenvironment in vitro is challenging, but constructing an analogous model could facilitate our understanding of surface effects and aid in developing an efficient bioinspired catalytic system. In this study, five unique Cu2O morphologies were generated, and the surface morphology variations were found to be a consequence of differences in the exposure of low-index facets. The reactivity of Cu2O was found to be influenced by the proportion of {110} planes, with r-Cu2O exhibiting the highest reactivity.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
Article
Chemistry, Physical
Yong Tang, Jianhao Qiu, Dingliang Dai, Guanglu Xia, Lu Zhang, Jianfeng Yao
Summary: Defect engineering has been shown to improve the photocatalytic performance. This study investigated the use of defect-rich UiO-66-NH2 wrapped by ZnIn2S4 as a catalyst for photocatalytic H2O2 production. The defects in UiO-66-NH2 enhanced O-2 adsorption and charge separation, leading to higher H2O2 yield. The insights from this work can advance the research in defect engineering of MOFs and photocatalytic H2O2 synthesis.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
Article
Chemistry, Physical
Ruiyang Qu, Shuxin Mao, Jana Weiss, Vita A. Kondratenko, Evgenii V. Kondratenko, Stephan Bartling, Haifeng Qi, Annette-Enrica Surkus, Kathrin Junge, Matthias Beller
Summary: The hydrogenation of amides, a challenging reaction usually performed at high temperatures, has been achieved under milder conditions using a new Pt-MoOx/TiO2 catalyst. This catalyst system enables the selective hydrogenation of various amides and imides.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
Article
Chemistry, Physical
Xiaoran Niu, Ao Wang, Lei Tong, Lei Wang, Yuan Kong, Chenliang Su, Hai-Wei Liang
Summary: This study introduces a novel intermetallic PdCu3 catalyst supported on defective nanodiamond-graphene (ND@G), which exhibits high selectivity (95%) and remarkable activity (turnover frequency: 2940 h(-1)), six times higher than that of the commercial Lindlar catalyst.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
Review
Chemistry, Physical
Zhiyuan Zheng, Yiming Yue, Hongying Zhuo, Qinggang Liu, Yanqiang Huang
Summary: This review presents the recent research advances on single-atom catalysis for deep reduction of CO2. Detailed introductions and summaries were classified into three categories based on proton-coupled multi-electron transfer approaches: strengthening metal-support interaction, rational design and regulation of coordination environment, and development of SACs with multi-atom active sites. The challenges and future research directions in the field of SACs for CO2 reduction are also proposed.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
Article
Chemistry, Physical
Shiv Kumar, Paramita Datta, Anup Bhunia, Swadhin K. Mandal
Summary: This article reports a transition-metal-free process for in situ denitrogenation of tosylhydrazones, resulting in the production of various sulfones. The authors used a phenalenyl-based odd alternant hydrocarbon as a photoredox catalyst, which acted as a potent oxidant to facilitate the denitrogenation reaction. The method showed wide functional-group tolerance and high yields, making it suitable for late-stage modification of natural products.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
Article
Chemistry, Physical
L. A. Luque-Alvarez, J. Gonzalez-Arias, F. Romero-Sarria, T. R. Reina, L. F. Bobadilla, J. A. Odriozola
Summary: Currently, the production of acetic acid through the carbonylation reaction of methanol has limitations, leading to the exploration of alternative methods using heterogeneous catalysts. This study investigates the methanol carbonylation reaction over a Cu-H-MOR catalyst and proposes a reaction mechanism based on the catalytic behavior and performance of the catalyst. The results provide insights into the reaction mechanism and the involvement of acid and redox centers.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
