Article
Chemistry, Multidisciplinary
Bingquan Xia, Yanzhao Zhang, Jingrun Ran, Mietek Jaroniec, Shi-Zhang Qiao
Summary: Single-atom photocatalysts have shown great potential in producing value-added chemicals and fuels using sustainable solar energy. They exhibit excellent activities, selectivity, and stability, while reducing the consumption of catalytic metals and aiding in elucidating reaction mechanisms. Exciting opportunities exist for designing and fabricating high-performance single-atom photocatalysts in this area.
ACS CENTRAL SCIENCE
(2021)
Article
Chemistry, Physical
Yutaka Nagahata, Rigoberto Hernandez, Tamiki Komatsuzaki
Summary: The complexity of gas and condensed phase chemical reactions is revealed through transition state theories or trajectory integration, recognizing dynamics and geometric structures in phase space. The introduction of NHIM can lead to more accurate rates and a deeper understanding of chemical reactions. This phase space perspective offers promising techniques for the design and control of chemical reactions.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Review
Chemistry, Physical
Lan Wang, Honglei Chen, Yi Wang, Xiaokang Liu, Changli Li, Jingfu He, Tao Yao
Summary: Single-atom catalysts (SACs) with M-N-4 structure have attracted significant attention due to their easy preparation, high atom efficiency, unique electronic properties, uniform active sites, and excellent activity. The M-N-4 structure is flexible and can be modified with other species to improve its catalytic performance. However, rational design and controllable synthesis of suitable SACs still pose challenges. This review discusses the progress and strategies in modulating the M-N-4 structure, as well as the preparation, structure characterization, and reaction mechanism of M-N-4-derived catalysts.
Review
Chemistry, Multidisciplinary
Markus Meuwly
Summary: Machine learning techniques have a long history in the field of chemical reactions, being able to address complex problems involving both computation and experiments. These techniques can develop models consistent with experimental knowledge, handle problems intractable to conventional approaches, and simulate reactive networks in combustion.
Review
Engineering, Chemical
Huimin Liu, Yuqiao Li, Xavier Djitcheu, Lequan Liu
Summary: Single-atom catalysts (SACs) offer various advantages in catalysis, including maximized atom-utilization efficiency, singly dispersed active sites with tailorable electronic states for achieving high catalytic activity, and specific structural geometry for tuning catalytic selectivity. This review focuses on the applications of SACs in traditional thermally driven catalytic reactions, providing a clear picture of recent scientific achievements and inspiring further studies in the rational design of SACs for other catalytic systems.
CHEMICAL ENGINEERING SCIENCE
(2022)
Article
Physics, Multidisciplinary
Zhendong Zhang, Shu Nagata, Kai-Xuan Yao, Cheng Chin
Summary: This study reports the coherent and collective reactions of atomic and molecular Bose-Einstein condensates at quantum degeneracy, highlighting the key features of bosonic enhancement and quantum coherence in these many-body reactions. The observation of such 'superchemistry' phenomena deepens our understanding of quantum many-body chemistry and provides insights into controlling chemical reactions at quantum degeneracy.
Review
Chemistry, Inorganic & Nuclear
Baokang Geng, Lingling Zhang, Fei Wang, Xiao Wang, Shuyan Song, Hongjie Zhang
Summary: Single-atom-alloy catalysts (SAAs) can improve the dispersion ratio of noble metals on another metal surface, while maintaining excellent heterogeneous catalytic performance. SAAs not only benefit from the metal bonds between noble metals and support metals, but also provide unique catalytic performance by constructing metallic metal single atoms. Recently, SAAs have been demonstrated to catalyze significant heterogeneous reactions. This review will discuss the synthesis methods of SAAs and summarize their applications in heterogeneous catalysis.
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
(2023)
Review
Nanoscience & Nanotechnology
Hongliang Chen, Chuancheng Jia, Xin Zhu, Chen Yang, Xuefeng Guo, J. Fraser Stoddart
Summary: Developing new materials is a long-standing goal in various fields, and understanding single-molecule reactions can deepen our understanding of chemical reactions and provide new frameworks in materials science. This review focuses on state-of-the-art chemical reactions in single-molecule junctions and highlights the advantages of real-time testbeds for studying reaction dynamics, intermediates, transition states, and solvent effects. The behavior of single-molecule reactions is compared with reactions in ensemble states, and the potential of leveraging single-molecule catalysis for large-scale materials production is explored.
NATURE REVIEWS MATERIALS
(2023)
Article
Chemistry, Physical
Shunlong Ju, Chongyang Yuan, Jiening Zheng, Long Yao, Tengfei Zhang, Guanglin Xia, Xuebin Yu
Summary: This study evaluates the catalytic activities of single-atom catalysts in aluminum-sulfur batteries, and finds that stable single-atom catalysts can promote the conversion reactions and improve the specific capacity of the batteries. The unique aluminum-binding interaction between SACo@NC and AlPSs is critical for its superior catalytic activity.
ENERGY STORAGE MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Hanyu Hu, Jiangbo Xi
Summary: Metal-based catalysis, including homogeneous and heterogeneous catalysis, is widely used in the modern chemical industry. Single-atom catalysts (SACs) have emerged as a promising class of catalytic material that bridges homogeneous and heterogeneous catalytic processes. This review provides an introduction and development history of SACs in organic reactions, as well as a comprehensive overview of their recent advances and practical applications. The structure-property relationships, metal atom-utilization efficiency, and catalytic performance of SACs in organic reactions are summarized, and the limitations, trends, challenges, and future perspectives of SACs for organic reactions are discussed.
CHINESE CHEMICAL LETTERS
(2023)
Review
Chemistry, Multidisciplinary
Zechuan Xu, Qingcheng Zhang, Zaimei Huang, Heng Chen, Jian Zhang, Wei Chen, Ge Meng, Dingsheng Wang
Summary: With the advantages of high atom utilization, low cost, unique and tunable microstructures, as well as specific catalytic behaviors, single-atom catalysts (SACs) have made significant progress in heterogeneous catalysis. However, catalyzing complex multistep reactions is challenging for a single atom center, requiring multiple catalytic sites. This review summarizes the experimental and computational advances in the construction strategies of multi-active-site SACs, classifying them as single-atom/single-atom, single-atom/nanoparticle, and single-atom/support multifunctional catalysts. The microstructures and catalytic behaviors of different active centers are highlighted, and the challenges and opportunities in this field are discussed. This review focuses on the design of multifunctional SACs for multistep reactions, providing insights for further development in heterogeneous catalysis and beyond.
SCIENCE CHINA-CHEMISTRY
(2023)
Review
Chemistry, Multidisciplinary
Ali Han, Zedong Zhang, Jiarui Yang, Dingsheng Wang, Yadong Li
Summary: Recent research activities have focused on single-atom catalysts to enhance the catalytic performance of fuel cells as an alternative to platinum group metals, showing potential for higher efficiency and cost-effectiveness.
Article
Chemistry, Physical
Kota Hanasaki, Kazuo Takatsuka
Summary: The development of attosecond technologies has enabled real-time control of electronic dynamics. In this study, we propose the use of spin flux as a means to monitor radical bond-rearrangement reactions in real-time. Using the reaction H. + H-2 as an illustrative example, we demonstrate that spin flux induces spin-polarization in the molecular target, weakening the covalent bond and possibly leading to bond cleavage. This mechanism aligns with the three-stage mechanism proposed by Nagase et al. in radical reactions.
CHEMICAL PHYSICS LETTERS
(2022)
Article
Chemistry, Physical
Zhifeng Ma, Zeyin Yan, Xin Li, Lung Wa Chung
Summary: In this study, the effects of external electric fields (EEFs) on three reactions involving hydrogen or carbon were extensively investigated. The study revealed that oriented EEFs can significantly reduce the barrier and increase the reaction rates. Furthermore, EEFs can modulate tunneling reactions and control the site selectivity of molecules with similar reactive sites.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Review
Engineering, Chemical
Ian Bunker, Ridwan Tobi Ayinla, Kun Wang
Summary: Understanding chemical processes at the single-molecule scale is crucial in analytical chemistry. Single-molecule detection techniques provide unprecedented accuracy in revealing the dynamics and kinetics of chemical reactions. Single-molecule junction (SMJ) techniques have opened up new possibilities for probing chemical and physical processes with exquisite precision.
Article
Engineering, Environmental
Dimitrios A. Giannakoudakis, Kumar Vikrant, Alec P. LaGrow, Dmytro Lisovytskiy, Ki-Hyun Kim, Teresa J. Bandosz, Juan Carlos Colmenares
Summary: Nanocomposites (TiO-NTbs/rGO) were successfully synthesized with high adsorption capacity and excellent photocatalytic activity, achieving an optimal surface area of 359 m2/g. By combining titanate nanosheets and reduced graphite oxide using low-power/low-frequency ultrasound and hydrothermal treatment, the materials show potential applications in removing toxic vapors such as chemical warfare agents.
CHEMICAL ENGINEERING JOURNAL
(2021)
Article
Chemistry, Physical
Dimitrios A. Giannakoudakis, Abdul Qayyum, Vaishakh Nair, Ayesha Khan, Swaraj R. Pradhan, Jovana Prekodravac, Kyriazis Rekos, Alec P. LaGrow, Oleksandr Bondarchuk, Dariusz Lomot, Konstantinos S. Triantafyllidis, Juan Carlos Colmenares
Summary: The study utilized an ultrasound-assisted ultra-wet impregnation synthetic approach to successfully decorate the surface of TiO2 nanoparticles with nanometric clusters of mixed cupric and cuprous oxides, creating TiO2-CuOx nanocomposite. This nanocomposite demonstrated enhanced hydrogen generation capability and high efficiency in the selective partial oxidation of biomass-derived chemicals, outperforming the benchmark commercial TiO2 P25.
MOLECULAR CATALYSIS
(2021)
Article
Chemistry, Physical
Alec P. LaGrow, Simone Famiani, Andreas Sergides, Leonardo Lari, David C. Lloyd, Mari Takahashi, Shinya Maenosono, Edward D. Boyes, Pratibha L. Gai, Nguyen Thi Kim Thanh
Summary: The oxidation behaviors of iron and iron carbide nanoparticles under oxygen gas were investigated. Iron nanoparticles oxidized asymmetrically, with the core disappearing, while the oxidation of iron carbide nanoparticles was symmetric, with the core shrinking. Carbon in the carbide suppressed the formation of iron oxide crystallites during oxidation.
Article
Chemistry, Physical
Pratibha L. Gai, Edward D. Boyes
Summary: Real-time in situ visualization and analysis of gas-solid catalyst reactions are crucial for understanding the relationship between dynamic catalyst atomic structure and function. Single atom processes and reaction mechanisms are believed to be important in catalytic reactions, but are not well understood under extreme reaction conditions like gas and temperature.
JOURNAL OF MATERIALS CHEMISTRY A
(2022)
Article
Chemistry, Physical
Ziyu Lu, Zhixin Tai, Zhipeng Yu, Alec P. LaGrow, Oleksandr Bondarchuk, Juliana P. S. Sousa, Lijian Meng, Zhijian Peng, Lifeng Liu
Summary: The study introduces a new three-dimensional composite anode structure for lithium metal that successfully addresses challenges such as dendrite growth and volume change in rechargeable Li batteries. The anode shows improved stability and cycling performance in a carbonate electrolyte, with no dendrite growth observed, and demonstrates better rate capability and cycle performance when assembled in a full cell paired with a LiFePO4 cathode.
MATERIALS TODAY ENERGY
(2021)
Article
Chemistry, Physical
Abdul Qayyum, Dimitrios A. Giannakoudakis, Alec P. LaGrow, Oleksandr Bondarchuk, Dariusz Lomot, Juan Carlos Colmenares
Summary: In this study, one-dimensional nanostructured titanate materials decorated with nanoclusters were synthesized using an ultrasound-assisted precipitation method. These materials exhibited high yield in the selective photo-oxidation of benzyl alcohol.
CATALYSIS COMMUNICATIONS
(2022)
Article
Chemistry, Physical
Silvia Nuti, Carlos Fernandez-Lodeiro, Javier Fernandez-Lodeiro, Adrian Fernandez-Lodeiro, Jorge Perez-Juste, Isabel Pastoriza-Santos, Alec P. LaGrow, Oliver Schraidt, Jose Luis Capelo-Martinez, Carlos Lodeiro
Summary: This study synthesized highly branched gold nanoparticles using a simple seeded growth approach, with the ability to control the morphology and optical properties by adjusting the gold salt to seeds ratio or fine-tuning the solution pH. The formation of the branched morphology may be attributed to the size-dependent PAH-AuCl4- aggregates and pH-dependent gold salt speciation.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2022)
Review
Chemistry, Multidisciplinary
Catarina S. M. Martins, Alec P. LaGrow, Joao A. V. Prior
Summary: Quantum dots (QDs) with exceptional optoelectronic properties are widely used in various applications, especially in the medical field. Recent studies have shown that micro ribonucleic acids (miRNAs) play a crucial role in cancer. Therefore, using fluorescent quantum dots as biosensors for miRNA detection is of great significance. This review aims to summarize the latest methods of using QDs to detect miRNA and provide tutorial descriptions of synthesis methods, surface modification, and functionalization approaches.
Article
Chemistry, Physical
Joao Fernandes, Tiago Queiros, Joao Rodrigues, Siva Sankar Nemala, Alec P. LaGrow, Ernesto Placidi, Pedro Alpuim, Jana B. Nieder, Andrea Capasso
Summary: This study optimized the growth of large-area two-dimensional hexagonal boron nitride (hBN) with uniform fluorescence emission properties using atmospheric-pressure chemical vapor deposition (APCVD). The characterization of the hBN films showed few-layer, polycrystalline films with balanced stoichiometry and uniformity. The fluorescence emission properties of the hBN films were studied using multidimensional hyperspectral fluorescence microscopy, revealing single-photon emission characteristics. The results suggest that APCVD hBN could potentially serve as a platform for quantum technologies.
Article
Chemistry, Physical
Zhipeng Yu, Yifan Li, Andre Torres-Pinto, Alec P. LaGrow, Vlad Martin Diaconescu, Laura Simonelli, Maria J. Sampaio, Oleksandr Bondarchuk, Isilda Amorim, Ana Araujo, Adrian M. T. Silva, Claudia G. Silva, Joaquim L. Faria, Lifeng Liu
Summary: The synthesis of single-atom Ir and Ru anchored on mesoporous graphitic carbon nitride (Ir-g-CN and Ru-g-CN) is reported as efficient electrocatalysts and photocatalysts for green hydrogen production. Ru-g-CN exhibits remarkable performance with high turnover frequency and mass activity, as well as excellent catalytic stability. This study contributes to the advancement of green hydrogen production.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Chemistry, Physical
Zhipeng Yu, Chaowei Si, Alec P. LaGrow, Zhixin Tai, Wolfgang A. Caliebe, Akhil Tayal, Maria J. Sampaio, Juliana P. S. Sousa, Isilda Amorim, Ana Araujo, Lijian Meng, Joaquim L. Faria, Junyuan Xu, Bo Li, Lifeng Liu
Summary: This study reports a bimetallic iridium-iron diatomic catalyst (IrFe-N-C) that exhibits excellent performance in oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) and is used in zinc-air batteries.
Article
Chemistry, Inorganic & Nuclear
Zhipeng Yu, Chaowei Si, Francisco Javier Escobar-Bedia, Alec P. LaGrow, Junyuan Xu, Maria J. Sabater, Isilda Amorim, Ana Araujo, Juliana P. S. Sousa, Lijian Meng, Joaquim Luis Faria, Patricia Concepcion, Bo Li, Lifeng Liu
Summary: This study reports the electrocatalytic performance of atomically dispersed ruthenium catalysts (Ru ADCs) with ultralow Ru loading for hydrogen production via water electrolysis. The Ru ADCs exhibit activity for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), showing favorable bifunctionality. Ru-N bonding is found to play a crucial role in enhancing the catalytic activity. The use of the bifunctional Ru ADCs in bipolar membrane water electrolysis enables energy-saving hydrogen production with a low cell voltage and stable performance.
INORGANIC CHEMISTRY FRONTIERS
(2022)
Article
Chemistry, Inorganic & Nuclear
Bruna F. Goncalves, Pedro M. Martins, Alec P. LaGrow, Gabriela Botelho, Laura M. Salonen, Senentxu Lanceros-Mendez, Yury Kolen'ko
Summary: This study presents an environmentally friendly synthesis method for Cu(In,Ga)Se-2 (CIGS) nanoparticles, which exhibit excellent photocatalytic properties for the removal of emerging contaminants from water. The synthesized nanoparticles demonstrated high crystallinity and efficient removal capabilities for the contaminant ciprofloxacin under both UV and visible radiations.
DALTON TRANSACTIONS
(2021)
Article
Chemistry, Multidisciplinary
Maximilian O. Besenhard, Luca Panariello, Celine Kiefer, Alec P. LaGrow, Liudmyla Storozhuk, Francis Perton, Sylvie Begin, Damien Mertz, Nguyen Thi Kim Thanh, Asterios Gavriilidis
Summary: Small iron oxide nanoparticles were synthesized in water using a flow reactor with carefully timed acid addition, resulting in stable nanoparticles suitable for MRI contrast agents. This continuous synthesis method allows for scalable production of small IONPs with high T-1 contrast enhancement.
Article
Chemistry, Multidisciplinary
Nur Hanisah AbuTalib, Alec P. LaGrow, Maximilian O. Besenhard, Oleksandr Bondarchuk, Andreas Sergides, Simone Famiani, Liliana P. Ferreira, M. Margarida Cruz, Asterios Gavriilidis, Nguyen Thi Kim Thanh
Summary: This study focuses on the synthesis of iron oxide nanoparticles based on iron(m) acetylacetonate decomposition in organic solvents, leading to anisotropic IONPs. The effects of varying amounts of oleylamine and a nitrogen purge on particle morphology were fully explored. The study revealed the crucial role of oleylamine in tuning particle size and the importance of nitrogen gas purge in forming branched and multiply branched NPs.