Article
Chemistry, Physical
Yangge Guo, Guofeng Wang, Shuiyun Shen, Guanghua Wei, Guofeng Xia, Junliang Zhang
Summary: This study used first-principles density functional theory calculations to predict the activity of different single atom electrocatalysts on nitrogen doped graphene for electrochemical ammonia synthesis. Six candidate structures were identified as promising active sites for ammonia synthesis based on scaling relations and additional factors, with V-N4/graphene showing the best stability and highest activity.
APPLIED SURFACE SCIENCE
(2021)
Article
Chemistry, Physical
Jing Yang, Yu Fan, Peng-Fei Liu
Summary: The study investigates the application of single-atom Fe-1 catalyst on four graphene-based substrates in water splitting reaction, showing high catalytic activity and efficiency. The hybridization and overlap of Fe single atom 3d orbitals and O atom 2p orbitals on Fe/GS surface are responsible for the strong chemisorption of H2O molecules. Strong metal-support interactions play a crucial role in the water splitting reaction process.
APPLIED SURFACE SCIENCE
(2021)
Article
Chemistry, Physical
Anu Baby, Laura Trovato, Cristiana Di Valentin
Summary: The study explores the properties of potential single atom catalysts in graphene, including stability and reactivity towards the hydrogen evolution reaction, by introducing nitrogen atoms and transforming the graphene structure to enhance stability and catalysis.
Article
Materials Science, Multidisciplinary
Siqi Chen, Xiang Zhang, Yucui Xiang, Jing Fan, Li-Yong Gan
Summary: In this study, the potential of using single transition metal atoms embedded in graphene as efficient sensor materials for methane detection was explored using first-principles calculations. It was found that AgN4 @G exhibits outstanding sensitivity, selectivity, and recovery ability for methane detection in ambient condition. Further calculations showed that the sensitivity of the system is remarkably improved in the presence of O-2 or H2O, indicating its applicability and robustness for methane sensing in ambient or humid conditions.
MATERIALS TODAY COMMUNICATIONS
(2022)
Article
Chemistry, Physical
Chihiro Mochizuki, Yusuke Inomata, Shunsaku Yasumura, Mingyue Lin, Ayako Taketoshi, Tetsuo Honma, Norihito Sakaguchi, Masatake Haruta, Ken-ichi Shimizu, Tamao Ishida, Toru Murayama
Summary: This study investigated the structural features and catalytic properties of Au single-atom catalysts supported on NiO (Au-1/NiO). The atomic Au was dispersed on the surface of NiO with Ni vacancy sites, forming cationic single atoms. The Au-1/NiO catalyst showed higher catalytic activity and stability in CO oxidation compared to nanoparticulate Au catalysts supported on NiO.
Article
Chemistry, Physical
Shu-Long Li, Qi Li, Yutao Chen, Yong Zhao, Li-Yong Gan
Summary: Noble metals are efficient for ORR and OER, but their scarcity and high price limit commercial applications. This study screened 26 TM-GY as potential SACs for ORR/OER, revealing candidates like Fe, Ir, Co, Rh, Cu, Ni, Pd and Pt-GY, with Co-GY as the optimal bifunctional SAC.
APPLIED SURFACE SCIENCE
(2022)
Review
Chemistry, Physical
Lilai Sun, Lu Han, Juntong Huang, Xudong Luo, Xibao Li
Summary: The application of hydrogen energy is crucial for addressing the challenges of fossil energy depletion and carbon emissions. Photocatalytic hydrogen evolution is considered a green and clean method for obtaining hydrogen. Single-atom catalysts (SACs) have emerged as promising cocatalysts with abundant active sites and efficient reaction mechanisms in the fields of energy and environmental science. This review summarizes the advances of SACs in photocatalytic hydrogen evolution.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2022)
Article
Chemistry, Physical
Michael Rebarchik, Saurabh Bhandari, Thomas Kropp, Manos Mavrikakis
Summary: Using first-principles density functional theory calculations, a pH-dependent microkinetic model is developed to evaluate the performance of transition metal catalysts embedded in nitrogen-doped graphene for the oxygen evolution reaction. It is found that reaction pathways involving intermediates co-adsorbed on the metal site are preferred and lead to enhanced catalytic activity. These findings highlight the importance of investigating reaction pathways on graphene-based catalysts and other two-dimensional materials with metal active centers decorated by spectator intermediate species.
Article
Chemistry, Physical
Manos Mavrikakis, Saurabh Bhandari, Thomas Kropp, Michael Rebarchik
Summary: Using first-principles density functional theory calculations, we developed a pH-dependent microkinetic model to evaluate the performance of transition metal catalysts embedded in nitrogen-doped graphene for the oxygen evolution reaction. We found that reaction pathways involving intermediates co-adsorbed on the metal site are preferred and lead to enhanced catalytic activity compared to thermodynamics-based predictions. These findings highlight the importance of investigating reaction pathways on graphene-based catalysts and other two-dimensional materials involving metal active centers decorated by spectator intermediate species.
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, Physical
Lizhen Hu, Teng Wang, Qianqian Nie, Jiayou Liu, Yunpei Cui, Kefei Zhang, Zhongchao Tan, Hesheng Yu
Summary: Efficient, stable, and selective photocatalytic conversion of nitric oxide (NO) into nitrogen dioxide (NO2) is highly desired but challenging. In this study, a single atom catalyst (SAC) was prepared by anchoring single Pd atoms onto graphitic carbon nitride (CNPd) via chemical impregnation followed by calcination. The SAC exhibited superior performance in terms of selectivity and stability compared to previous catalysts for photocatalytic removal of NO under visible light and simulated sunlight. The experimental results and density functional theory calculations revealed that the single Pd atom promoted the photocatalytic degradation of NO and the nitrate ions accumulated on the SAC surface reacted with NO to produce NO2, enhancing the selectivity and stability of the catalyst.
Review
Nanoscience & Nanotechnology
Qin Zhang, Xiaoxiang Zhang, Junzhong Wang, Congwei Wang
Summary: Supported metal nanostructures are widely studied heterogeneous catalysts, with isolated metal atoms maximizing activity. Graphene-supported SACs offer great potential as efficient electrocatalysts, but challenges remain for further improvement.
Article
Chemistry, Physical
Haobo Li, Yunxia Liu, Ke Chen, Johannes T. Margraf, Youyong Li, Karsten Reuter
Summary: The study reveals the potential of single-atom catalysts to enhance nitrogen reduction efficiency, with early transition metals that are conventionally not associated with nitrogen reduction also showing promise.
Article
Energy & Fuels
Yanan Tang, Weiguang Chen, Mingyu Zhao, Jinlei Shi, Yingqi Cui, Zhaohan Li, Zhiwen Wang, Zhen Feng, Xianqi Dai
Summary: The electronic properties and sensitivity of different single transition metal atoms anchored to boron phosphide (BP-TM) and supported by a graphene substrate were investigated. The graphene support can regulate the adsorption strength and electronic structure of the TM atoms, resulting in stable adsorption of N-2 molecules. The potential catalytic performances for nitrogen reduction reaction (NRR) were explored, with BP-gra-Mn and BP-gra-Fe showing the lowest limiting potential.
Article
Multidisciplinary Sciences
Jiacheng Li, Miao Li, Ning An, Shuo Zhang, Qinan Song, Yilin Yang, Jing Li, Xiang Liu
Summary: Efficient activation of the n=O bond is crucial for the catalytic reduction of nitrogen compounds. In this study, a single-atom catalyst with phosphorus anchored on a cobalt active center was used to achieve n=O bond activation and generate intermediate N species. Unique phosphorus-doped discontinuous active sites exhibited better activation performance than conventional N-cooperated single-atom sites, resulting in high ammonia yield rate and Faradic efficiency.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2022)
Article
Nanoscience & Nanotechnology
Aleksandra M. Bondzi, Tamara D. Lazarevic Pasti, Igor A. Pasti, Bojan P. Bondzic, Milos D. Momcilovic, Alexandra Loosen, Tatjana N. Parac-Vogt
Summary: Organophosphate-based pesticides have negative impacts on the environment and human health. This study found that the NU-1000 metal-organic framework is an effective agent for the fast and efficient removal of organophosphate pesticides. The sorption and hydrolysis processes of NU-1000 contribute to the successful detoxification of chlorpyrifos.
ACS APPLIED NANO MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Jadranka Milikic, Nikola Nikolic, Diogo M. F. Santos, Daniele Maccio, Adriana Saccone, Mabkhoot Alsaiari, Mohammed Jalalah, M. Faisal, Farid A. Harraz, Yizhao Li, Abu Bakr Nassr, Igor Pasti, Biljana Sljukic
Summary: Platinum-dysprosium (Pt-Dy) alloys prepared by the arc melting technique were evaluated as potential electrodes for the oxygen reduction reaction (ORR) in alkaline media. The Pt40Dy60 electrode with a lower Pt content showed higher ORR activity and lower oxygen evolution reaction (OER) activity compared to the alloy with a higher Pt content.
Article
Materials Science, Composites
Christoph Unterweger, Matija Ranzinger, Jiri Duchoslav, Francesco Piana, Igor Pasti, Franz Zeppetzauer, Stefan Breitenbach, David Stifter, Christian Fuerst
Summary: In this study, biobased carbons were used as fillers in PHBV to create 100% biocomposites, and their mechanical and electrical properties were analyzed. The results showed significant improvements in the graphitic structure of carbonized wood dust and cellulose fibers with increasing temperature. The carbon content increased with temperature, while other elements were removed. Significant degradation of PHBV was observed when mixed with a specific filler. However, other fillers showed improvements in the mechanical performance, with carbonized fibers performing slightly better than wood dust analogues. The effects were even more pronounced at higher filler content, especially in terms of electrical conductivity.
JOURNAL OF COMPOSITES SCIENCE
(2022)
Article
Electrochemistry
Bojana Nedic Vasiljevic, Aleksandar Z. Z. Jovanovic, Slavko V. V. Mentus, Natalia V. V. Skorodumova, Igor A. A. Pasti
Summary: Surface modification with rhodium through galvanic displacement significantly improves the catalytic activity of cobalt for hydrogen and oxygen evolution reactions in alkaline media. The overpotential for hydrogen and oxygen generation is reduced by 0.16 V and 0.06 V, respectively, after only 20 seconds of galvanic displacement. Density Functional Theory calculations indicate that the reactivity of the Rh-modified Co(0001) surface is different from that of the clean Co(0001) surface.
JOURNAL OF SOLID STATE ELECTROCHEMISTRY
(2023)
Article
Chemistry, Physical
Marjetka Savic, Aleksandra Janosevic Lezaic, Nemanja Gavrilov, Igor Pasti, Bojana Nedic Vasiljevic, Jugoslav Krstic, Gordana Ciric-Marjanovic
Summary: Composites of N,O-doped carbon/ZnO/ZnS and N,O-doped carbon/ZnO (C-(MOF-5/PANI)) were synthesized by the carbonization of MOF-5/PANI composites. These composites were comprehensively characterized and exhibited high S-BET, electrical conductivity, and specific capacitance. Acid etching treatment further improved the surface area and capacitance, making them promising electrode materials for supercapacitors.
Article
Chemistry, Physical
Sanjin J. Gutic, Dino Metarapi, Aleksandar Z. Jovanovic, Goitom K. Gebremariam, Ana S. Dobrota, Bojana Nedic Vasiljevic, Igor A. Pasti
Summary: In order to efficiently replace fossil fuels and address the growing energy crisis, hydrogen production has become a focus. This study utilized Kinetic Monte Carlo simulations to demonstrate that hydrogen evolution reaction (HER) can be enhanced by hydrogen spillover to the support under certain conditions. Based on these findings, a series of reduced graphene-oxide-supported catalysts were synthesized and compared with pure metals for HER activity in alkaline media. The results showed that the support had a negative effect on Ag, Au, and Zn, but enhanced HER activity for Pt, Pd, Fe, Co, and Ni. The study provides insights into metal-support interface engineering for effective HER catalysts and guidelines for selecting novel catalyst-support combinations for electrocatalytic hydrogen production.
Article
Food Science & Technology
Ammar Al-Hamry, Tianqi Lu, Jing Bai, Anurag Adiraju, Tharun K. Ega, Igor A. Pasti, Olfa Kanoun
Summary: Different environmental parameters and contaminations during food processing and storage can lead to food spoilage and the loss of nutritional value. Therefore, developing reliable and cost-effective sensor devices for precise monitoring is crucial. This paper demonstrates the effectiveness of Poly-(diallyl-dimethyl ammonium chloride)/reduced Graphene oxide (PDAC/rGO) films for monitoring temperature, relative humidity, volatile organic compounds, and detecting the presence of pesticides.
Article
Nanoscience & Nanotechnology
Mila Krstajic N. Pajic, Ana S. Dobrota, Anca Mazare, Sladana Durdic, Imgon Hwang, Natalia V. Skorodumova, Dragan Manojlovic, Rastko Vasilic, Igor A. Pasti, Patrik Schmuki, Uros Lacnjevac
Summary: This study reveals that the surface effects of hydrogenated TiO2 nanotube arrays can convert Os, an unexplored platinum group metal, into a highly active electrocatalyst for the hydrogen evolution reaction (HER). The optimized Os@TNT composite exhibits low overpotential and stable performance in acidic medium, offering new possibilities for the fabrication of cost-effective PGM-based catalysts.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Ammar Al-Hamry, Tianqi Lu, Haoran Chen, Anurag Adiraju, Salem Nasraoui, Amina Brahem, Danica Bajuk-Bogdanovic, Saddam Weheabby, Igor A. Pasti, Olfa Kanoun
Summary: This study investigates the relative humidity sensor properties of graphene oxide (GO) and graphene oxide/multiwalled nanotubes (GO/MWNTs) composites. Composite sensors were fabricated using direct laser scribing and characterized using various spectroscopies and microscopy techniques. The results show that GO/MWNT-based humidity sensors are more stable and repeatable, and they have faster response/recovery times compared to GO sensors. The introduction of GO/MWNT hybrid and laser direct writing proves to be advantageous in producing stable structures and sensors.
Article
Food Science & Technology
Vedran Milankovic, Tamara Tasic, Milica Pejcic, Igor Pasti, Tamara Lazarevic-Pasti
Summary: Coffee is a popular beverage, but the disposal of spent coffee grounds (SCGs) can harm the environment. This study explored the interaction between SCGs and organophosphate pesticides, specifically malathion and chlorpyrifos. The results showed that SCGs can effectively remove these pesticides from water and fruit extracts without producing toxic byproducts.
Article
Food Science & Technology
Tamara Tasic, Vedran Milankovic, Katarina Batalovic, Stefan Breitenbach, Christoph Unterweger, Christian Fuerst, Igor A. Pasti, Tamara Lazarevic-Pasti
Summary: This study shows that carefully tuned viscose-derived activated carbon fibers can efficiently remove pesticides from liquid samples, even in complex matrices. The selected materials are not affected by complex matrices of real samples and can be regenerated multiple times without performance losses. Adsorptive removal of food contaminants can effectively improve food safety and quality, unlike other methods that negatively affect the nutritional value of food products. Data-based models can guide the synthesis of novel adsorbents for desired applications in food processing.
Article
Chemistry, Analytical
Saddam Weheabby, Zhenyn Wu, Ammar Al -Hamry, Igor A. Pasti, Adiraju Anurag, Doreen Dentel, Christoph Tegenkamp, Olfa Kanoun
Summary: This study demonstrates the voltammetric sensing of paracetamol using silver nanoparticles and carboxylated multi-walled carbon nanotubes on a screen-printed carbon electrode. The sensor shows effective sensing potential with a low detection limit under optimal conditions. Experimental and computational studies were conducted to support the findings. The proposed method shows promising applications for determining paracetamol in environmental and pharmaceutical samples.
MICROCHEMICAL JOURNAL
(2023)
Article
Chemistry, Physical
Goitom K. Gebremariam, Aleksandar Z. Jovanovic, Igor A. Pasti
Summary: This study evaluates the HER kinetic parameters of different metals in various electrolytes, showing that the shape of HER volcano curves remains largely unchanged in different electrolytes. The presence of surface oxide can have both positive and negative effects on HER kinetics, depending on the metal-electrolyte combination. The study also provides a comprehensive overview of HER kinetic data from diverse literature sources, offering practical insights for the development of new catalytic materials and optimization of electrolyte formulations for enhancing HER.
Article
Chemistry, Multidisciplinary
Daniela Neumueller, Lidija D. Rafailovic, Aleksandar Z. Jovanovic, Natalia V. Skorodumova, Igor A. Pasti, Alice Lassnig, Thomas Griesser, Christoph Gammer, Juergen Eckert
Summary: Highly efficient non-noble metal catalysts are crucial for hydrogen generation through electrolysis, and the synthesis of catalytic heterostructures containing established Ni with surface NiO, Ni(OH)(2), and NiOOH domains has shown promising results. This study investigates the intrinsic catalytic activity of pure Ni and the impact of partial electrochemical oxidation of magnetron sputter-deposited Ni surfaces through various experimental techniques and simulations. The results demonstrate that surface oxidation increases the intrinsic hydrogen evolution reaction (HER) activity of nickel and improves catalyst durability.
Article
Chemistry, Physical
Igor A. Pasti, Ana S. Dobrota, Dmitri B. Migas, Boerje Johansson, Natalia V. Skorodumova
Summary: The development of new electrochromic materials and devices, such as smart windows, has a significant impact on energy efficiency in modern society. Nickel oxide is a crucial material in this technology, and its Ni-deficient form exhibits anodic electrochromism. By using DFT+U calculations, researchers have shown that the generation of nickel vacancies leads to the formation of hole polarons localized at nearby oxygen sites. These hole polarons can be filled by Li insertion or electron injection, resulting in a transition from an oxidized (colored) to a reduced (bleached) state. This study suggests a new mechanism for Ni-deficient NiO electrochromism based on the formation and annihilation of hole polarons in oxygen p-states rather than the change in Ni oxidation states (Ni2+/Ni3+ transition).
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)