Article
Engineering, Environmental
Phuoc Hoang Ho, Jieling Shao, Dawei Yao, Rojin Feizie Ilmasani, Muhammad Abdus Salam, Derek Creaser, Louise Olsson
Summary: This study investigates the effect of the Pt/Pd ratio on the oxidation activity and sulfur resistance of diesel oxidation catalysts (DOC). The formation of Pt-Pd alloy enhances the sintering resistance of Pt and retains a high fraction of Pd. The Pt-Pd alloy also improves the oxidation resistance and enhances the activity of the catalysts for CO and C3H6 oxidation. Bimetallic catalysts show lower temperatures for NO reduction but lower absolute conversion of NO due to the decrease in Pt active sites. Moreover, bimetallic catalysts exhibit significantly improved sulfur resistance compared to monometallic Pd catalysts.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2022)
Article
Engineering, Environmental
Yuxuan Xie, Yuan Li, Ziruo Zeng, Ping Ning, Xin Sun, Fei Wang, Kai Li, Lidong Wang
Summary: In this study, the activity and selectivity of Pt- and Pd-loaded alumina-based catalysts were investigated, revealing significant differences between them. Pd/Al2O3 catalysts showed better performance at low temperatures, while Pt/Al2O3 catalysts had a higher propensity for converting CS2 to methane but Pd/Al2O3 catalysts demonstrated a greater tendency for coke deposition. The capability of H-2 spillover along with the adsorption capacity of CS2 played critical roles in determining the observed differences, and the key intermediate species involved in methanation and coke pathways were identified.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Huan Wang, Weitao Wang, Xulu Jiang, Zhen-Hong He, Kuan Wang, Yang Yang, Zhao-Tie Liu, Buxing Han
Summary: In this study, a fast and self-propagated carbonization (SPC) method was proposed for the preparation of phosphorus-doped carbon (PDC) and hybrid materials. PdZr/PDC prepared by the SPC method exhibited excellent catalytic performance in the partial oxidation of benzyl alcohol to benzaldehyde and the partial hydrogenation of phenol to cyclohexanone. The method is simple, clean, and suitable for large-scale material preparation.
Article
Energy & Fuels
Artita Na Rungsi, Thuong Hai Truong, Chachchaya Thunyaratchatanon, Apanee Luengnaruemitchai, Nuwong Chollacoop, Shih-Yuan Chen, Takehisa Mochizuki, Hideyuki Takagi, Yuji Yoshimura
Summary: The study investigated the partial hydrogenation of soybean oil-derived fatty acid methyl esters using MCM-41 mesoporous silica-supported Pd-Pt bimetallic catalysts, resulting in the production of H-FAME enriched in mono-FAME as a potential source for high blends of biodiesel fuel. Various MCM-41 supports with different structural properties and morphologies were synthesized using different amounts of ammonia solution, leading to a series of Pd-Pt/MCM-41 bimetallic catalysts with tunable porosity.
Article
Chemistry, Physical
Mengjie Ma, Yi Zhang, Yujin Ji, Qi Shao, Kui Yin, Wenxiang Zhu, Junjun Yang, Fan Liao, Zhenglong Fan, Yang Liu, Youyong Li, Mingwang Shao, Zhenhui Kang
Summary: This study reports a versatile strategy for enhancing the catalytic activity and anti-poisoning ability of noble metal catalysts towards ORR by decorating them with size-controlled silicon nanoclusters (DS). DS-Pd exhibits superior ORR performance and enhanced anti-poisoning performance compared to commercial catalysts.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Chemistry, Physical
Wenyan Dong, Cong Xu, Wenhui Zhao, Mudi Xin, Yanjuan Xiang, Aiguo Zheng, Meiling Dou, Shaojie Ke, Juncai Dong, Limei Qiu, Guangtong Xu
Summary: This study investigates the poisonous influence of trace impurities (H2S, CS2, and COS) on the performance of Pt/C catalysts in hydrogen oxidation reaction (HOR) in proton exchange membrane fuel cells (PEMFCs). The results show that CS2 poses a more severe threat to the HOR activity than H2S, while COS poses a weaker threat. Both CS2 and COS decrease the activity of HOR by decreasing the d-band center of Pt atoms. This study provides insights into the deactivation mechanism of Pt-based catalysts and is significant for the practical applications of PEMFCs.
ACS APPLIED ENERGY MATERIALS
(2022)
Article
Energy & Fuels
Artita Na Rungsi, Apanee Luengnaruemitchai, Nuwong Chollacoop, Shih-Yuan Chen, Takehisa Mochizuki, Hideyuki Takagi, Yuji Yoshimura
Summary: This study investigated the performance and sulfur poisoning of different Pd-Pt catalysts in the selective hydrogenation of soybean oil-derived fatty acid methyl esters (FAMEs). The results showed that catalysts with larger Pd-Pt alloy particles and weaker acidity favored the selective hydrogenation to produce monounsaturated esters, while catalysts with smaller Pd-Pt alloy particles and stronger acidity favored the formation of saturated esters. The performance of the catalyst physically mixed with acidic support γ-Al2O3 did not deteriorate when using a feedstock containing sulfur.
Article
Electrochemistry
Matias A. Villalba, Marc T. M. Koper
Summary: In this paper, the electrocatalytic reduction of methyl vinyl ketone on Pt(111) and Pd-modified Pt(111) electrodes was studied. The selectivity and efficiency of the reaction were calculated, while the adsorbates involved in the deactivation process were analyzed. The research found that Pd-modified Pt(111) electrode was highly active for the selective electrochemical hydrogenation of C=C, while Pt(111) was less active.
ELECTROCHIMICA ACTA
(2022)
Article
Nanoscience & Nanotechnology
Adam Prekob, Gabor Muranszky, Milan Szori, Gabor Karacs, Ferenc Kristaly, Tibor Ferenczi, Bela Fiser, Bela Viskolcz, Laszlo Vanyorek
Summary: Carbon black-supported palladium-platinum catalysts were prepared with and without nickel(II) oxide or iron(III) oxide promoter materials using ultrasonic cavitation technology. The one-step catalyst preparation method without the need for post-treatments showed excellent catalytic activity in the hydrogenation of nitrobenzene, with no significant differences in selectivity and aniline yield observed even when promoters were present.
Article
Chemistry, Multidisciplinary
Limin He, Yangdong Wang, Can Wang, Zhicheng Liu, Zaiku Xie
Summary: In this study, ZIF-8 derived carbon materials with adjustable N types were used as the supports of Pd catalysts for the hydrogenation of 4-carboxylbenzaldehyde. The Pd catalyst supported on NC with 50.5% pyridinic N showed the best hydrogenation activity. The nitrogen species on the CN surface were found to adjust the chemical state and dispersion of Pd nanoparticles, as well as promote the adsorption and activation capability of H2 molecules.
FRONTIERS IN CHEMISTRY
(2022)
Article
Chemistry, Physical
Haiting Cai, Ya-Huei Cathy Chin
Summary: The kinetic assessments of cydohexene and pyridine hydrogenation on metallic Pd and Pt surfaces covered with chemisorbed sulfur species provide insight into the catalytic involvement of sulfur in H-addition events. The distribution of irreversible and reversible sulfur species on surfaces influences the hydrogenation reactivity towards pyridine under different conditions.
Article
Chemistry, Physical
Shuo Wang, Sheng Wang, Xupeng Zong, Shudong Wang, Xiaoli Dong
Summary: Insights on CO oxidation and sulfur tolerance over supported Pt catalysts were obtained. Results showed that the presence of water promoted CO oxidation, with Pt/TiO2 and Pt/SnO2 catalysts exhibiting superior catalytic activity. Higher dispersion and strong metal support interaction (SMSI) were found to be crucial for the excellent catalytic activity. The sulfation of the support led to catalyst deactivation in the presence of both water and SO2. TiO2 with low sulfate decomposition temperature improved sulfur resistance, while the special core-shell structure of Pt/SnO2 catalyst contributed to its superior sulfur tolerance. These findings provide guidelines for the development of catalysts with excellent CO catalytic activity and sulfur tolerance.
APPLIED CATALYSIS A-GENERAL
(2023)
Article
Chemistry, Physical
Ke Jin, Chengyan Wen, Qian Jiang, Xiuzheng Zhuang, Lungang Chen, Longlong Ma, Chenguang Wang, Qi Zhang
Summary: Thermal catalytic conversion of CO2 to produce high-value gasoline is a promising and sustainable way to deal with greenhouse gases and alleviate the energy crisis and environmental problems. An Fe/C catalyst coupled with HZSM-5 as a tandem catalyst has been developed, showing a high gasoline space-time yield of 91.2 mu mol(CO2) g(Fe)(-1) s(-1). The catalyst contains three active sites (Fe3O4, Fe5C2, and acid sites) that synergistically catalyze a tandem reaction, providing a green and efficient catalyst for the conversion of CO2 to gasoline.
SUSTAINABLE ENERGY & FUELS
(2023)
Article
Chemistry, Physical
Xiaoyan Liu, Yiqi Ren, Maodi Wang, Xiaomin Ren, Jian Liu, Qihua Yang
Summary: In this study, efficient nitrobenzothiazole hydrogenation was achieved using Pt/TiO2 as a catalyst. The presence of the strong metal-support interaction (SMSI) effect in Pt/TiO2 was found to enhance its activity compared to Pt/TiO2 without the SMSI effect. The activation of the -NO2 group mainly occurs through the oxygen vacancy (O-v) of TiOx in the presence of sulfur compounds, and H species dissociate on Pt to reduce -NO2. The cooperative effect between Pt and TiOx contributes to the high hydrogenation activity of Pt/TiO2.
Article
Chemistry, Physical
Renjie Xiong, Wenqiang Ren, Zhiqiang Wang, Minghui Zhang
Summary: The study found that the addition of triphenylphosphine (TPP) can greatly enhance the catalytic performance of sulfur-poisoned Pd/C catalyst in sulfur-containing systems, proving to be an efficient antidote for Pd/C hydrogenation catalyst poisoning.
Article
Chemistry, Multidisciplinary
Qiang Liu, Niklas Pfriem, Guanhua Cheng, Eszter Barath, Yue Liu, Johannes A. Lercher
Summary: The ionic environment inside microporous zeolites can significantly affect the catalytic turnover rates by modifying the chemical potential of the reactants and transition states. However, zeolites with high ionic strength seem to have a limit to the rate enhancement for the aqueous-phase dehydration of alcohols. This limitation is hypothesized to be caused by spatial constraints in the pores, such as size exclusion effects. This study demonstrates that the increase in turnover rate, the formation of a maximum, and the subsequent rate drop are intrinsic consequences of the increasingly dense ionic environment in zeolite.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Laura Loebbert, Saumil Chheda, Jian Zheng, Navneet Khetrapal, Julian Schmid, Ruixue Zhao, Carlo A. Gaggioli, Donald M. Camaioni, Ricardo Bermejo-Deval, Oliver Y. Gutierrez, Yue Liu, J. Ilja Siepmann, Matthew Neurock, Laura Gagliardi, Johannes A. Lercher
Summary: Grafting metal cations to missing linker defect sites in zirconium-based metal-organic frameworks can produce well-defined and homotopic catalytically active sites. This study focuses on the synthesis and characterization of a group of metal catalysts supported by UiO-66, which showed varying catalytic activities for alkene dimerization. The removal of molecular water from the active site significantly increased the catalytic activity for 1-butene dimerization, and density functional theory calculations provided a molecular level understanding of the differences in activity among different metal catalysts.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Ruixue Zhao, Rachit Khare, Yang Zhang, Maricruz Sanchez-Sanchez, Ricardo Bermejo-Deval, Yue Liu, Johannes A. Lercher
Summary: Steric confinement in zeolites affects the catalytic conversion of alkanes. Silica species grafted near Bronsted acid sites in H-ZSM-5 zeolite enhance the binding of bases and increase the reaction rate of protolytic cracking of n-pentane with a lower activation energy. The presence of extra-framework silica leads to an earlier transition state and better stabilization of carbonium ions compared to extra-framework alumina.
Article
Multidisciplinary Sciences
Wei Zhang, Sungmin Kim, Lennart Wahl, Rachit Khare, Lillian Hale, Jianzhi Hu, Donald M. Camaioni, Oliver Y. Gutierrez, Yue Liu, Johannes A. Lercher
Summary: We propose a unique approach to selectively upcycle polyolefin waste by utilizing a highly ionic reaction environment, which increases polymer reactivity and reduces energy required for breaking carbon-carbon bonds. By catalyzing endothermic cleavage and exothermic alkylation reactions, we are able to convert polyethylene and polypropylene to liquid isoalkanes at temperatures below 100 degrees C. This process offers a high yield conversion of unprocessed postconsumer items into high-quality liquid alkanes.
Article
Chemistry, Physical
Yong Wang, Xiaofeng Chen, Hui Shi, Johannes A. Lercher
Summary: Metal oxides of group 4-6 elements are found to be active and stable catalysts for H2S reforming of methane, with dynamical binding of sulfur species (S*) to metal cations as the key active sites. Analysis of kinetic data and isotopic substitution effects reveals that S*-mediated C-H bond cleavage is the most plausible rate-limiting step common for all catalysts, with subtle yet essential differences in the thermodynamic stability of S* between 3d and 4d/5d catalysts.
Article
Chemistry, Applied
Feng Chen, Sungmin Kim, Dushyant Barpaga, John. L. L. Fulton, Radha Kishan Motkuri, Oliver. Y. Y. Gutierrez, Donald. M. M. Camaioni, Johannes. A. A. Lercher
Summary: Bronsted-acid sites are introduced on the ZrO2 nodes of UiO-66 MOFs via -OSO3H groups. These sites exhibit strong Bronsted acidity and are active for cyclohexanol and ethanol dehydration reactions in different phases. The activity of Bronsted acid sites at nodes is improved by increasing sulfur concentration, which leads to the formation of two interacting groups [(&mu(3)-OSO3H)(2)] through hydrogen bonding. The catalytic activity can be manipulated by functionalizing zirconia nodes of the MOF framework.
TOPICS IN CATALYSIS
(2023)
Article
Chemistry, Physical
Benjamin Yeh, Saumil Chheda, Jian Zheng, Julian Schmid, Laura Loebbert, Ricardo Bermejo-Deval, Oliver Y. Gutierrez, Johannes A. Lercher, Laura Gagliardi, Aditya Bhan
Summary: In this study, the steady state propylene oligomerization rates and selectivities were measured on Ni/UiO-66 metal organic framework (MOF), demonstrating the validity of the Cossee-Arlman mechanism. It was found that propylene dimerization reaction follows a first-order kinetics with respect to propylene pressure, and the selectivities are consistent with the selectivity expressions derived from the Cossee-Arlman mechanism.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Oliver Y. Gutierrez, Katarzyna Grubel, Jotheeswari Kothandaraman, Juan A. Lopez-Ruiz, Kriston P. Brooks, Mark E. Bowden, Tom Autrey
Summary: Using hydrogen to store energy is crucial for achieving sustainability and addressing climate change. Liquid hydrogen carriers can overcome the challenges of handling molecular hydrogen. The bicarbonate-formate cycle, utilizing formate ions as hydrogen and energy carriers, offers a promising solution. This system combines electrochemical and thermochemical operations and has the potential for CO2 capture and energy storage.
Article
Chemistry, Physical
Laura C. Meyer, Udishnu Sanyal, Kelsey A. Stoerzinger, Katherine Koh, John L. Fulton, Donald M. Camaioni, Oliver Y. Gutierrez, Johannes A. Lercher
Summary: In this study, the electrocatalytic hydrogenation (ECH) of aldehydes and ketones over carbon-supported Pd in the aqueous phase was investigated. The reaction mechanisms were proposed based on kinetic measurements and characterization of the catalyst. The rates of ECH and H-2 evolution reaction (HER) varied with the applied electric potential, which strongly depended on the organic substrate. The sorption of the organic compound and the rates of proton-coupled electron transfers influenced the kinetics of both ECH and HER.
Article
Chemistry, Physical
Lara Milakovic, Yue Liu, Eszter Barath, Johannes A. Lercher
Summary: This study reveals the impact of the tetragonal zirconia phase on octadecanol dehydration in zirconia supported tungstates catalysis, and finds that small concentrations of Pt can increase the acidity site concentration.
CATALYSIS SCIENCE & TECHNOLOGY
(2022)
Article
Chemistry, Multidisciplinary
Rachit Khare, Roland Weindl, Andreas Jentys, Karsten Reuter, Hui Shi, Johannes A. Lercher
Summary: NaY zeolite-encapsulated Mo2S4 molybdenum sulfide clusters stabilize hydrogen as hydride binding to Mo atoms. Each cluster can activate only one hydrogen molecule under reaction conditions, suggesting that the entire cluster acts as one active site for hydrogenation.
Article
Chemistry, Multidisciplinary
Zhiying Fan, Lena Staiger, Karina Hemmer, Zheng Wang, Weijia Wang, Qianjie Xie, Lunjia Zhang, Alexander Urstoeger, Michael Schuster, Johannes A. Lercher, Mirza Cokoja, Roland A. Fischer
Summary: The embedding of metal nanoparticles in metal-organic frameworks (MOFs) is crucial in catalysis research, as it prevents agglomeration and allows for functionalization of the MOF matrix to optimize the chemical environment. In this study, Pd nanoparticles were incorporated into the MOF CuBTC by encapsulation, and the hydrophobicity was adjusted by using functionalized linkers. These modifications significantly improved the catalytic activity, suggesting that channel engineering is an efficient way to optimize metal@MOF catalysts.
CELL REPORTS PHYSICAL SCIENCE
(2022)
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)
