Article
Chemistry, Physical
Matteo Farnesi Camellone, Filip Dvorak, Mykhailo Vorokhta, Andrii Tovt, Ivan Khalakhan, Viktor Johanek, Tomas Skala, Iva Matolinova, Stefano Fabris, Josef Myslivecek
Summary: Single-atom catalysts are important heterogeneous catalysts. Recent studies show that single-atom sites on the catalyst substrates can significantly affect the distribution of metal nanoparticles. By controlling the atmosphere, researchers can control the size of Pt nanoparticles on ceria-based single-atom catalysts, leading to changes in catalyst activity and stability. The competition between Pt single-atom sites and Pt nanoparticles determines the morphology of Pt nanoparticle population on the ceria surface. In oxidizing atmosphere, Pt single-atom sites bond strongly with Pt atoms and cause nanoparticle shrinkage, while in reducing atmosphere, Pt single-atom sites are emptied and Pt nanoparticles grow. A generic model of Pt redispersion and coarsening on ceria substrates is proposed, providing an atomic-level explanation for various dynamic processes observed in single-atom catalysts.
Article
Chemistry, Physical
Yawen Chen, Rui Ding, Jia Li, Jianguo Liu
Summary: By preparing Pt1/Co1NC single-atom catalyst on a support rich in defects, high HER activity and stability were achieved. Nitrogen/carbon defects were found to be crucial for anchoring and forming Pt active sites.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Chemistry, Physical
Yang Chen, Qiang Wan, Liru Cao, Zhe Gao, Jian Lin, Lin Li, Xiaoli Pan, Sen Lin, Xiaodong Wang, Tao Zhang
Summary: This study reveals the dependence of Pt single atoms' electronic structure on the facets of CeO2 and demonstrates the impact of such dependence on catalytic performance. By controlling the electron transfer patterns of Pt-O-Ce microstructures, the positively charged or metallic states of Pt single atoms can be achieved, resulting in enhanced complete oxidation of CO and activation of H2, respectively.
JOURNAL OF CATALYSIS
(2022)
Article
Chemistry, Physical
Weiyi Pan, Zhihe Wei, Yanhui Su, Yuebin Lian, Zhangyi Zheng, Huihong Yuan, Yongze Qin, Xulan Xie, Qianqian Bai, Zhenyang Jiao, Wei Hua, Jinzhou Chen, Wenjun Yang, Zhao Deng, Yang Peng
Summary: In this study, nanocages composed of two-dimensional metal-organic layers were constructed, and single atomic Co2+ sites were appended to enhance CO2 conversion catalytic activity. The outstanding photocatalytic performance is mainly attributed to the unique nanocage morphology and abundant surface hydroxyl groups.
Article
Chemistry, Multidisciplinary
Dagmar Zaoralova, Radim Mach, Petr Lazar, Miroslav Medved', Michal Otyepka
Summary: The study explores the bond strength between metal atoms and graphene derivatives, which is related to charge transfer. Graphene derivatives can reduce metal cations and oxidize metal atoms due to their pi-conjugated structure.
ADVANCED MATERIALS INTERFACES
(2021)
Article
Chemistry, Physical
Jing Li, Yanan Zhou, Weijing Tang, Jian Zheng, Xiaoping Gao, Ning Wang, Xiao Chen, Min Wei, Xin Xiao, Wei Chu
Summary: The study demonstrates the tunability of Pt single atoms coordination through a cold-plasma technique and predicts a strong correlation between Pt-N coordination concentration and adsorption free energy of H* atoms for the hydrogen evolution reaction (HER). The sample with N, O co-dopant introduced by air plasma shows significantly enhanced performance, with a high turnover frequency and outstanding mass activity, suggesting that the optimized electronic structure of active carbon site plays a key role in improving the catalyst's efficiency.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2021)
Article
Chemistry, Physical
Congwen Duan, Yating Tian, Xinya Wang, Jinhui Wu, Bogu Liu, Dong Fu, Yuling Zhang, Wei Lv, Lianxi Hu, Fei Wang, Xu Zhang, Ying Wu
Summary: By constructing N-doping carbon nanotubes (N-CNTs) supported Mo single atoms (MoSA-N-CNTs), the hydrogenation/dehydrogenation properties of the Mg/MgH2 system are improved. Mg@MoSA-N-CNTs can absorb 7.37 wt.% H2 during the milling within 15 h with an activation energy reduced to 21.2 kJ/mol. MgH2@MoSA-N-CNTs releases 7.23 wt.% H2 at 325°C for 5 min, nearly 3 times that of pristine MgH2. The synergistic effect of N-CNTs and MoSA on hydrogenation/dehydrogenation properties of Mg/MgH2 is proposed.
Article
Multidisciplinary Sciences
Qiaowan Chang, Youngmin Hong, Hye Jin Lee, Ji Hoon Lee, Damilola Ologunagba, Zhixiu Liang, Jeonghyeon Kim, Mi Ji Kim, Jong Wook Hong, Liang Song, Shyam Kattel, Zheng Chen, Jingguang G. Chen, Sang-Il Choi
Summary: A new type of unalloyed single-atom electrocatalyst has been reported, which can completely oxidize ethanol to CO2 at a low potential. In situ X-ray absorption fine structure measurements and density functional theory calculations have revealed the working mechanism of this catalyst. This work contributes to the fundamental understanding of ethanol oxidation reaction and offers a new approach to tune the activity and selectivity for complicated catalytic reactions using low-coordination active sites.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2022)
Article
Chemistry, Applied
Zhe Xue, Xinyu Zhang, Jiaqian Qin, Riping Liu
Summary: The study introduces a new method of anchoring a single Mo atom on the C9N4 substrate to form an efficient single-atom catalyst for converting N-2 to NH3. Density functional theory calculations demonstrate the effectiveness and stability of this catalyst. The research provides a promising platform for designing Mo-based single-atom catalysts for electrochemical N-2 fixation.
JOURNAL OF ENERGY CHEMISTRY
(2021)
Article
Chemistry, Physical
Mingyu Ma, Xu Cheng, Zude Shi, Chenglan Zhang, Yan Li, Yifan Yang, Chengshi Gong, Zhenxing Zhang, Huilong Fei, Chao Zhu, Yongmin He, Erqing Xie
Summary: This study explores the role of nitrogen in transition metal nitrides for anchoring single metal atoms, and discovers that a pore-rich metallic vanadium nitride nanosheet can effectively anchor platinum-group single atoms and exhibit excellent catalytic performance. This finding provides a possible support material for constructing platinum-group single-atom catalysts.
Article
Chemistry, Multidisciplinary
Meiping Li, Qing Lv, Wenyan Si, Zhufeng Hou, Changshui Huang
Summary: Iron single-atom catalysts synthesized using graphdiyne as the carbon substrate exhibit excellent catalytic performance. The catalyst accelerates the reaction kinetics and enhances its oxygen reduction reaction (ORR) activity by regulating the electronic structure of iron atoms and optimizing the adsorption energy of ORR intermediates on the active sites. Furthermore, high power density and long-term performance are demonstrated in a zinc-air battery application.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Rongjuan Feng, Kaiwei Wan, Xinyu Sui, Na Zhao, Huaxing Li, Wanying Lei, Jiaguo Yu, Xinfeng Liu, Xinghua Shi, Maolin Zhai, Gang Liu, Hui Wang, Lirong Zheng, Minghua Liu
Summary: In this study, a novel dual co-catalyst of black phosphorene (BP) and single Pt atoms on CdS nanospheres was prepared for efficient visible-light-driven hydrogen generation. The single Pt atoms interacted strongly with BP and CdS surfaces through photo-reduction and covalent bonds, enhancing the photocatalytic performance. The results demonstrate the synergistic effect of single Pt atoms and BP on spatial charge separation, leading to a significant improvement in the hydrogen evolution rate.
Article
Materials Science, Multidisciplinary
Cheng Liu, Wei Liu, Mao-sheng Miao, Jing-yao Liu
Summary: Graphene-based carbon allotropes, particularly egg tray graphene (ETG), have been found to be effective support materials for single-atom catalysts (SACs). In this study, three N-doped ETG supported Pd SACs were designed and their catalytic performance in formic acid dehydrogenation was investigated. The results showed that Pd@ETG-N-3 exhibited the best catalytic activity, surpassing Pd(111), and the N doping in the ETG substrate greatly enhanced the activity and selectivity of the SACs.
Article
Chemistry, Applied
Shaohua Xie, Xing Zhang, Peng Xu, Braden Hatcher, Yuxi Liu, Lu Ma, Steven N. Ehrlich, Sampyo Hong, Fudong Liu
Summary: With ideal metal utilization efficiency and homogeneous active sites, single atom catalysts (SACs) have attracted extensive attention in heterogeneous catalysis field. In this study, the surface acidity of Pt SACs was tuned through modification with acidic WO3 and basic MgO. It was found that WO3 modified Pt/Al2O3 showed superior activity in methanol decomposition, while MgO modified Pt/Al2O3 performed better in CO oxidation under the reaction condition with H2O.
Article
Chemistry, Applied
Yasutomo Goto, Shinji Inagaki
Summary: In this study, the structural changes of BPy-PMO and Pt-BPy-PMO caused by thermal treatment were investigated, and nitrogen-doped porous carbon/silica composites with high nitrogen/carbon ratios and large pore diameters were successfully prepared. The pyrolyzed BPy-PMO contained abundant graphitic nitrogen and carbon species, along with a few oxygenated species. Moreover, Pt complexes on the pore surface of BPy-PMO transformed into Pt oxide nanoparticles and a small amount of Pt metal after heating.
MICROPOROUS AND MESOPOROUS MATERIALS
(2023)
Article
Chemistry, Physical
Marketa Paloncyova, Martin Srejber, Petra Cechova, Petra Kuhrova, Filip Zaoral, Michal Otyepka
Summary: RNA-based therapies have shown promise in various applications. Encapsulation of RNA into lipid nanoparticles allows for safe and targeted delivery. Simulations of pH-sensitive RNA-carrying nanoparticles reveal their self-assembly process and internal structure, providing insights into their composition and potential interactions for improving RNA-based medicine.
JOURNAL OF PHYSICAL CHEMISTRY B
(2023)
Article
Chemistry, Medicinal
Petra Kuhrova, Vojtech Mlynsky, Michal Otyepka, Jiri Sponer, Pavel Banas
Summary: RNA molecules play a key role in biochemical processes and interact closely with ions and water molecules. Double-stranded RNA is important for RNA folding and the design of RNA-based nanostructures. This study used molecular dynamics simulations to investigate the effects of ion concentrations and solvation box size on A-RNA structure.
JOURNAL OF CHEMICAL INFORMATION AND MODELING
(2023)
Article
Multidisciplinary Sciences
Aby Cheruvathoor Poulose, Miroslav Medved, Vasudeva Rao Bakuru, Akashdeep Sharma, Deepika Singh, Suresh Babu Kalidindi, Hugo Bares, Michal Otyepka, Kolleboyina Jayaramulu, Aristides Bakandritsos, Radek Zboril
Summary: This study presents a reusable graphene catalyst that can convert glycerol, produced from biomass fermentation, to high-value chemicals at room temperature without solvents. The catalyst shows excellent activity and selectivity for glycerol conversion to solketal, and it can also convert oils to biodiesel.
NATURE COMMUNICATIONS
(2023)
Article
Nanoscience & Nanotechnology
Akshay Kumar K. Padinjareveetil, Juan V. Perales-Rondon, Dagmar Zaoralova, Michal Otyepka, Osamah Alduhaish, Martin Pumera
Summary: Electrochemical reduction of nitrate into ammonia is a promising solution to address the challenges of growing global energy demand. Metal-organic framework (MOF)-based catalysts are being investigated for their enhanced structural and compositional integrity, making them effective in catalytic reduction reactions.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Sujit Deshmukh, Kalyan Ghosh, Martin Pykal, Michal Otyepka, Martin Pumera
Summary: Microsupercapacitors with mechanical flexibility offer potential applications in portable biomonitoring devices. Researchers have developed high-energy-density micro-SCs integrated with a force sensing device using picosecond pulsed laser technology, and demonstrated their effectiveness in monitoring human body's radial artery pulses.
Article
Chemistry, Multidisciplinary
Thaylan Pinheiro Araujo, Jordi Morales-Vidal, Georgios Giannakakis, Cecilia Mondelli, Henrik Eliasson, Rolf Erni, Joseph A. Stewart, Sharon Mitchell, Nuria Lopez, Javier Perez-Ramirez
Summary: Ternary Pd-In2O3/ZrO2 catalysts prepared by wet impregnation exhibit selective and stable architecture under CO2 hydrogenation conditions, irrespective of the order of addition of Pd and In phases on the zirconia carrier. The rapid restructuring of the catalysts is driven by the metal-metal oxide interaction energetics. The presence of InPdx alloy particles decorated by InOx layers prevents performance losses associated with Pd sintering.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Biochemistry & Molecular Biology
Remi Coulon, Barbora Papouskova, Elmira Mohammadi, Michal Otyepka, Sreekar Wunnava, Jiri Sponer, Judit E. Sponer
Summary: 3',5'-Cyclic nucleotides play a fundamental role in modern biochemical processes and may have played a central role in the origin of early terrestrial life. A formamide-based systems chemistry could explain their availability on early Earth, as demonstrated by the formation of 3',5'-cyclic nucleotides in liquid formamide environments at elevated temperatures.
Article
Chemistry, Physical
Rabindranath Lo, Martin Pykal, Andreas Schneemann, Radek Zboril, Roland A. Fischer, Kolleboyina Jayaramulu, Michal Otyepka
Summary: Covalent hybrids of graphene and metal-organic frameworks (MOFs) have great potential in various technologies, especially catalysis and energy applications, due to their combination of conductivity and porosity. The formation of an amide bond between carboxylate-functionalized graphene acid (GA) and amine-functionalized UiO-66-NH2 MOF is an efficient strategy for creating such hybrids. This study used density functional theory (DFT) calculations to elucidate the mechanism of amide bond formation between GA and UiO-66-NH2, highlighting the crucial role of zirconium within UiO-66 as a catalyst. Insight into the binding interactions between graphene derivatives and MOFs can lead to tailored synthesis strategies for these nanocomposite materials.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Multidisciplinary
Haibin Ma, Enric Ibanez-Ale, Ramesha Ganganahalli, Javier Perez-Ramirez, Nuria Lopez, Boon Siang Yeo
Summary: In this study, it was discovered that carbonate intermediates can be adsorbed on a copper electrode during electrochemical CO2 reduction reaction (eCO(2)RR) and can be reduced to formate. The nature of active sites and the mechanism for the reduction of carbonate to formate were also elucidated. These findings provide a potential pathway to mitigate carbonate formation during eCO(2)RR.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Chunmiao Ye, Federico Dattila, Xiaoting Chen, Nuria Lopez, Marc T. M. Koper
Summary: Understanding the role of cations in the electrochemical CO2 reduction process is crucial for practical application. This study investigates how cations influence the formation of HCOOH and CO on PdMLPt-(111) in pH 3 electrolytes. The presence of cations decreases the onset potential of HCOOH and CO, with a stronger effect on HCOOH formation. These findings provide insights for evaluating the effects of cationic electrolytes on the activity and selectivity in CO2RR on Pd-Pt catalysts.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Computer Science, Interdisciplinary Applications
Sergio Pablo-Garcia, Santiago Morandi, Rodrigo A. Vargas-Hernandez, Kjell Jorner, Zarko Ivkovic, Nuria Lopez, Alan Aspuru-Guzik
Summary: GAME-Net is a graph deep learning model trained with small molecules containing a wide set of functional groups for predicting the adsorption energy of closed-shell organic molecules on metal surfaces, avoiding expensive density functional theory simulations. The model yields a mean absolute error of 0.18 eV on the test set and is 6 orders of magnitude faster than density functional theory.
NATURE COMPUTATIONAL SCIENCE
(2023)
Article
Materials Science, Multidisciplinary
Rehan Anwar, Jan Navratil, Rajani K. Vijayaraghavan, Patrick J. McNally, Michal Otyepka, Piotr Blonski, M. Veronica Sofianos
Summary: The development of long-term renewable energy storage systems is crucial for a sustainable energy future. In this study, the use of CaZrO3 nanoadditives with tailored oxygen vacancies was investigated to improve the cycling performance of Limestone for long-term renewable energy storage. The sample mixed with 20% CaZrO3 nanoadditives showed the best performance, with enhanced ionic conductivity and the highest energy density values.
MATERIALS ADVANCES
(2023)
Article
Chemistry, Multidisciplinary
Yang Qiuyue, Emily P. Nguyen, David Panacek, Veronika Sedajova, Vitezslav Hruby, Giulio Rosati, de Carvalho Castro Silva Cecilia, Aristides Bakandritsos, Michal Otyepka, Arben Merkoci
Summary: Heavy metal pollutants are highly toxic and pose great concern in environmental monitoring. Electrochemical detection, hindered by mutual interferences of heavy metal ions, is a main technique with limited sensitivity to Cd2+ ions. This study introduces a metal-free and sustainable nanomaterial, cysteamine covalently functionalized graphene (GSH), which significantly enhances the sensitivity of screen-printed carbon electrode (SPCE) to Cd2+ ions while maintaining sensitivity to other heavy metals. The enhancement is attributed to the grafted thiols on the GSH sheets with strong affinity to Cd2+ ions, based on Pearson's principle. The GSH-modified SPCE also exhibits high reusability and outperforms existing SPCEs modified by non-covalently functionalized graphene derivatives. The GSH-SPCE is successfully validated in tap water.
Article
Chemistry, Multidisciplinary
Albert Sabadell-Rendon, Kamila Kazmierczak, Santiago Morandi, Florian Euzenat, Daniel Curulla-Ferre, Nuria Lopez
Summary: This article introduces the Automated MUltiscale Simulation Environment (AMUSE), which is a framework that integrates detailed atomistic information on materials and reactions to predict the performance of heterogeneous catalytic full-scale reactors. It demonstrates the capabilities of AMUSE in computational investigation of heterogeneous catalytic reactions and provides essential information for catalyst design.
Article
Chemistry, Physical
Vojtech Mlynsky, Petra Kuhrova, Petr Stadlbauer, Miroslav Krepl, Michal Otyepka, Pavel Banas, Jiri Sponer
Summary: Molecular dynamics simulations are commonly used to study RNA molecules. By adjusting the nonbonded parameters, the widely used AMBER OL3 ff in RNA simulations can be improved. The modified simulations show better agreement with experimental results.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
