Review
Chemistry, Multidisciplinary
Yueqing Wang, Hongxing Wang, Xiao Kong, Yulei Zhu
Summary: This review highlights recent advances in the thermocatalytic conversion of 5-hydroxymethylfurfural (HMF) into value-added chemicals, including hydrogenation, oxidation, and other reactions. The roles of metal properties, supports, and additives are discussed, along with challenges in this research area.
Article
Energy & Fuels
Lin Ai, Haonan Shi, Jixiang Chen
Summary: In this study, Ni-Re alloy catalysts supported on TiO2 were prepared and tested for the in situ deoxygenation of methyl palmitate to hydrocarbons in aqueous phase using methanol as hydrogen donor. The results demonstrated that NiO and ReO4- species could interact to form Ni-O-Re(=O)(3) species in the calcined catalysts, which facilitated the formation of Ni-Re alloy and enhanced the dispersion of Ni during reduction with H-2. Compared to Ni/TiO2, NiRe(x:y)/TiO2 exhibited significantly higher deoxygenation activity and lower activity for C-C bond hydrogenolysis due to the synergistic effect between Ni and Re species and the geometrical effect of Re. The yield of C-6 to C-16 liquid hydrocarbons could reach up to 98.0% on NiRe(3:4)/TiO2 at 330 degrees C. No obvious sintering of Ni-Re alloy and TiO2 support particles was observed during the recycling of NiRe(3:4)/TiO2, while the catalyst activity was slightly reduced by carbon deposition and leaching of Re species.
JOURNAL OF THE ENERGY INSTITUTE
(2023)
Article
Chemistry, Multidisciplinary
Xin Yuan, Kwanpyung Lee, Michael T. Bender, J. R. Schmidt, Kyoung-Shin Choi
Summary: This study elucidates the key mechanistic differences between hydrogenation and hydrogenolysis reactions and demonstrates that lowering the pH can promote the hydrogenolysis of aldehydes and alcohols.
Article
Green & Sustainable Science & Technology
Fei Wang, Robert Pace, Yaying Ji, Jianchun Jiang, Xiaoxiang Jiang, Anna Krystianiak, Olivier Heintz, Gilles Caboche, Eduardo Santillan-Jimenez, Mark Crocker
Summary: In this study, the catalytic activity of Ni catalysts in the decarboxylation/decarbonylation of triglycerides to hydrocarbons was improved by employing Pd as a promoter and using multifunctional supports. Pd addition promoted Ni reduction, leading to an increase in the number of active sites. The use of SiO2-Al2O3 as a support further enhanced the catalyst performance by promoting Ni reduction, as well as providing a high surface area and strong acidity.
Article
Chemistry, Physical
Leilei Zhou, Weiwei Lin, Xinchao Wang, Zhuangqing Wang, Yinze Yang, Liyan Zhang, Haiyang Cheng, Masahiko Arai, Fengyu Zhao
Summary: The production of biofuels from renewable biomass resources has been studied, with a focus on the catalytic hydrodeoxygenation of methyl laurate. The study investigates the effects of different catalysts and their acid sites on the reaction rate and product distribution. It is found that the amount of acid sites and the presence of specific active species play an important role in the formation of desired hydrocarbons.
CATALYSIS SCIENCE & TECHNOLOGY
(2022)
Article
Chemistry, Applied
Xiaoxia Wu, Qingfeng Ge, Xinli Zhu
Summary: Catalytic hydrodeoxygenation of phenolics is a crucial step in converting lignin-biomass to chemicals and fuels, with catalysts based on group 10 metals widely used. Achieving a high yield toward the desirable product remains a challenge due to competing reactions, resulting in a complex product distribution. Recent advances in understanding the reaction mechanism on group 10 metal catalysts and strategies for selective deoxygenation of phenolics have focused on improving the selectivity of HDO to aromatics.
Article
Chemistry, Inorganic & Nuclear
Huanshi Lan, Zuzeng Qin, Shaolin Shi, Xingcong Zhang, Xiaohui He, Hongbing Ji
Summary: Atomically dispersed Pt species supported on Fe2O3 (Pt1/Fe2O3) are successfully constructed via a simple ball milling process. Pt1/Fe2O3 exhibits excellent selectivity and conversion rate in the selective hydrogenation of cinnamaldehyde (CAL) in pure water medium, attributed to its superior dissociation ability of H-2 and preferential adsorption of CAL via C=O.
DALTON TRANSACTIONS
(2022)
Article
Energy & Fuels
Chunli Li, Mingxia Zhang, Hao Li, Yahui Zhang
Summary: In this study, biomass tar was utilized for the preparation of biocarbon catalysts, which demonstrated high catalytic activity for the hydrodeoxygenation of vanillin. The use of K2FeO4 as an activator led to catalysts with improved graphitization and stronger acidity, resulting in better catalytic performance and recyclability.
Article
Chemistry, Inorganic & Nuclear
Neha Antil, Ajay Kumar, Naved Akhtar, Rajashree Newar, Wahida Begum, Kuntal Manna
Summary: A heterogeneous catalyst based on aluminum metal-organic framework and cobalt(II) hydride was reported for selective and efficient deoxygenation of a wide range of carbonyls and alcohols. The catalyst can be recycled and operates under ambient hydrogen pressure.
INORGANIC CHEMISTRY
(2021)
Article
Chemistry, Physical
Claudia E. Berdugo-Diaz, Yang Sik Yun, Melissa T. Manetsch, Jing Luo, David G. Barton, Xue Chen, David W. Flaherty
Summary: The direct reduction of esters to ethers offers an efficient pathway to obtain ethers from renewable intermediates. This study elucidates the reaction pathways of propyl acetate in the presence of hydrogen over Pd nanoparticles supported on high-surface area Nb2O5. The results show that esters react via three primary pathways, leading to the formation of different products. The formation of ethers is not affected by the pressure of C5H10O2 but is dependent on the pressure of H-2.
Article
Chemistry, Physical
Zhongwen Luo, Jiahan Xie, Nicholas Kaylor, Diane A. Dickie, Hannah E. Ketcham, Robert J. Davis, T. Brent Gunnoe
Summary: Silica-supported Pd, Rh, and Pt metal nanoparticles catalyze the hydrogenolysis of the Pt-OPh bond of ((t)bpy)Pt(OPh)Cl to release PhOH. Kinetic studies show that Pd exhibits higher reactivity compared to Rh and Pt. The results of kinetic studies with Pd/SiO2 are consistent with a first-order dependence on the catalyst and the molecular Pt(II) complex ((t)bpy)Pt(OPh)Cl. TEM-EDS mapping and ICP-OES measurements reveal approximately 10-16% Pt deposition on the surface of Pd/SiO2 after 1 hour of hydrogenolysis of ((t)bpy)Pt(OPh)Cl.
Article
Chemistry, Physical
Desen Fu, Xiaoxia Wu, Beilei Cui, Yonghua Guo, Hua Wang, Jinyu Han, Qingfeng Ge, Xinli Zhu
Summary: In this study, a solid solution Ru0.05Ce0.95O2 catalyst was used for the selective hydrodeoxygenation of m-cresol, demonstrating high oxygen vacancy concentration and the ability to catalyze toluene production with significant inhibition of competing hydrogenolysis and hydrogenation reactions. The active sites for deoxygenation were proposed to be Ru-O-V-Ce sites, and the inhibition of C-C hydrogenolysis and phenyl hydrogenation was attributed to the reduced size of the Ru ensembles due to strong interaction in the solid solution.
Article
Chemistry, Multidisciplinary
Thorben Lenk, Valentin Ruess, Janko Gresch, Uwe Schroeder
Summary: This research investigates the use of various Pd- and Pt-containing electrocatalyst materials for electrochemical ring hydrogenation of aromatic compounds. The focus is on selectivity of the reaction based on the composition of the electrocatalyst, as well as understanding the electrocatalytic activity during repetitive electrode use. Different furanic derivatives are used as starting materials for mechanistic considerations. The study finds that furfural, furfuryl alcohol, and furan show high reactivity in ring hydrogenation reactions, while furoic acid and 2-methyl furan do not exhibit this behavior. Selectivities of up to 15.3% (from furfural) and 33% (from furfuryl alcohol) for tetrahydrofurfuryl alcohol are observed.
Article
Chemistry, Multidisciplinary
Yazhou Zhang, Shaoqi Zhan, Kunlong Liu, Mengfei Qiao, Ning Liu, Ruixuan Qin, Liangping Xiao, Pengyao You, Wentong Jing, Nanfeng Zheng
Summary: In this study, a Pd nanoparticles catalyst supported on hexagonal boron nitride (h-BN) was developed for the hydrogenation of aldehydes/ketones to alcohols via hydrogen spillover. The feasibility of hydrogen spillover from Pd to h-BN is determined by the nitrogen vacancies in h-BN. The hydrogen spillover-based hydrogenation mechanism leads to a high tolerance to CO poisoning for the catalyst system.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Shedrack G. Akpe, Sun Hee Choi, Hyung Chul Ham
Summary: This study used DFT techniques to investigate the conversion of xylose to xylitol on five notable transition metal surfaces, revealing that the structural rearrangement of cyclic xylose into its acyclic form is the starting process of the reaction.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Gengnan Li, Shanka Dissanayake, Steven L. Suib, Daniel E. Resasco
APPLIED CATALYSIS B-ENVIRONMENTAL
(2020)
Article
Electrochemistry
Reda Bababrik, Daniel Santhanaraj, Daniel E. Resasco, Bin Wang
Summary: This study compares the selectivity in aqueous-phase thermal catalytic and electrocatalytic conversion of furfural and reveals fundamental differences in elementary steps in the two reaction systems. In electrocatalysis, 2-methylfuran dominates as the product, while in thermal catalysis, furfural alcohol and its derivatives are the major products.
JOURNAL OF APPLIED ELECTROCHEMISTRY
(2021)
Article
Chemistry, Physical
Gengnan Li, Bin Wang, Daniel E. Resasco
JOURNAL OF CATALYSIS
(2020)
Article
Engineering, Chemical
Nuttapong Makmeesub, Chonlada Ritvirulh, Kittisak Choojun, Teng-Hao Chen, Yingyot Poo-arporn, Daniel E. Resasco, Tawan Sooknoi
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2020)
Article
Chemistry, Physical
Gengnan Li, Duong T. Ngo, Yu Yan, Qiaohua Tan, Bin Wang, Daniel E. Resasco
Article
Chemistry, Physical
Feifei Yang, Mallikharjuna Rao Komarneni, Nicole J. Libretto, Liwen Li, Wei Zhou, Jeffrey T. Miller, Qingfeng Ge, Xinli Zhu, Daniel E. Resasco
Summary: This study reports a bimetallic NiW/SiO2 catalyst that exhibits high efficiency in HDO reaction and inhibition of CH4 formation, with a unique structure that shows excellent performance in aromatic synthesis. Detailed characterization of the catalyst structure was conducted using multiple techniques.
Article
Chemistry, Physical
Gengnan Li, Zheng Zhao, Tong Mou, Qiaohua Tan, Bin Wang, Daniel Resasco
Summary: The study evaluates the effects of different solvents on the hydrogenation reactions catalyzed by Pd/alumina, revealing that the solvent can shift the rate determining step of the reaction by competitive adsorption. The results show that non-polar solvents decrease surface coverage of reactants and intermediates, leading to different hydrogenation rates for different solvents.
JOURNAL OF CATALYSIS
(2021)
Article
Chemistry, Multidisciplinary
Camila Abreu Teles, Priscilla Magalhaes de Souza, Raimundo Crisostomo Rabelo-Neto, Alejandra Teran, Gary Jacobs, Daniel E. Resasco, Fabio B. Noronha
Summary: The study on the catalytic upgrading of biomass pyrolysis products emphasizes the importance of understanding competitive adsorption in the process. Different catalyst supports influence the rate of elimination of hydroxyl and methoxy groups, leading to the formation of various oxygenated products. Preferential reactions of hydroxyl groups were observed in binary mixtures, highlighting the impact of competitive adsorption on product selectivity.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2021)
Article
Chemistry, Physical
Kuizhi Chen, Anya Zornes, Reda Bababrik, Jacob Crouch, Walter Alvarez, Matt Wulfers, Daniel Resasco, Bin Wang, Steven Crossley, Jeffery L. White
Summary: Modification of Zeolite ZSM-5 catalysts with varying amounts of H3PO4 results in increased structural heterogeneity of phosphates with higher loadings, while similar experiments on silicalite show formation of only free phosphates.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Gengnan Li, Nebojsa Marinkovic, Bin Wang, Mallikharjuna Rao Komarneni, Daniel E. Resasco
Summary: Precise tuning of the local environment surrounding the active site is crucial for engineering catalytic materials. This study explores a nanoconfined catalytic system in which organic surfactants anchored on metal surfaces not only modify catalytic performance but also regulate solvent distribution at the liquid-solid interface. The combination of catalyst synthesis, spectroscopic characterization, reaction kinetics analysis, and computational techniques provides a quantitative description of a catalyst with a tunable local environment near the active site.
Article
Chemistry, Physical
Laura A. Gomez, Caleb Q. Bavlnka, Tianhao E. Zhang, Daniel E. Resasco, Steven P. Crossley
Summary: The study investigates the selective deoxygenation of carboxylic acid on promoted MoO3, revealing the potential for synthesizing valuable renewable products. The results suggest that the deoxygenation of pentanoic acid on an oxygen vacancy of MoO3 can be explained by a Langmuir-Hinshelwood mechanism. The incorporation of Pt shifts the reaction order with respect to hydrogen and alters the rate-determining step.
Article
Chemistry, Multidisciplinary
Gengnan Li, Mallikharjuna Rao Komarneni, Bin Wang, Nebojsa Marinkovic, Daniel E. Resasco
Summary: In this study, the role of water in the selective hydrogenation of cinnamaldehyde was investigated. It was found that boron species exsolve from the bulk phase and become enriched on the surface, forming acidic species that enhance the activity and selectivity of carbonyl bond hydrogenation. Metal-support interactions result in smaller particles and a drop in selectivity towards unsaturated alcohol. The presence of boron species and strong metal-support interactions protect the catalysts from water attack, resulting in enhanced stability.
CELL REPORTS PHYSICAL SCIENCE
(2023)
Article
Engineering, Chemical
Nilson F. L. de Paula, Tuong V. Bui, Daniel E. Resasco
Summary: This study presents a method using titration technique and reaction-diffusion model to quantify mass-transfer limitations in microporous acid zeolites. The method allows for the determination of the extent of mass-transport limitations in the system by observing the variation in reaction rate and manipulating site density. The results also indicate that the degree of mass transfer limitations can influence the selectivity of product formation in the reaction.
CHEMICAL ENGINEERING SCIENCE
(2023)
Article
Nanoscience & Nanotechnology
Patrick McKernan, Needa A. Virani, Gabriela N. F. Faria, Clement G. Karch, Ricardo Prada Silvy, Daniel E. Resasco, Linda F. Thompson, Roger G. Harrison
Summary: The study demonstrates that a novel treatment combining photothermal therapy with targeted single-walled carbon nanotubes and immunostimulation can significantly increase the survival rate of patients with metastatic breast cancer, showing a remarkable anti-cancer immune effect.
NANOSCALE RESEARCH LETTERS
(2021)
Article
Chemistry, Physical
Camila A. Teles, Raimundo C. Rabelo-Neto, Nhung Duong, Jhon Quiroz, Pedro H. C. Camargo, Gary Jacobs, Daniel E. Resasco, Fabio B. Noronha
APPLIED CATALYSIS B-ENVIRONMENTAL
(2020)
Article
Chemistry, Physical
Yifan Sun, Ye Lv, Wei Li, Jinli Zhang, Yan Fu
Summary: In this study, PtRu electrocatalysts were fabricated on carbon paper via cyclic electrodeposition for the electrocatalytic hydrogenation (ECH) of phenol. The Pt3Ru3 catalyst exhibited excellent activity and stability for the conversion of phenol to cyclohexanol at ambient temperature and various current densities. The in situ Raman spectroscopy and kinetic study revealed the hydrogenation mechanism of phenol over Pt3Ru3 in acidic electrolyte, providing an effective electrochemical strategy for the facile construction of durable electrode materials and efficient phenol hydrogenation.
JOURNAL OF CATALYSIS
(2024)
Article
Chemistry, Physical
Amir Shahzad, Khezina Rafiq, Muhammad Zeeshan Abid, Naseem Ahmad Khan, Syed Shoaib Ahmad Shah, Raed H. Althomali, Abdul Rauf, Ejaz Hussain
Summary: Photocatalytic hydrogen production through water splitting is an effective method for meeting future energy demands. In this study, researchers synthesized a 1 % Ag2S/Cu2S co-doped CdZnS catalyst and found that it can produce hydrogen at a higher rate. The co-doping of Ag2S and Cu2S in the CdZnS catalyst showed a synergistic effect, with Ag2S promoting oxidation reactions and Cu2S promoting reduction reactions.
JOURNAL OF CATALYSIS
(2024)
