Article
Chemistry, Inorganic & Nuclear
Brian J. J. Timmer, Oleksandr Kravchenko, Biaobiao Zhang, Tianqi Liu, Licheng Sun
Summary: This study investigates the catalytic activity of Ru(bda)L-2 family of catalysts and finds that the unique bimolecular reactivity is purely dependent on the spatial geometry of the ligand. The electronic effects of the backbone do not significantly impact the catalysis, highlighting the importance of structural features in determining catalytic activity.
INORGANIC CHEMISTRY
(2021)
Article
Biochemistry & Molecular Biology
Michal Zielinski, Ewa Janiszewska, Adrianna Drewniak, Mariusz Pietrowski
Summary: This study focuses on the catalytic properties of ruthenium catalysts supported on modified silicalite-1 with basic centers created by post-synthesis modification. The modification not only affected the basicity and porosity of the supports, but also improved the catalytic activity for CO2 methanation. The results demonstrated that ruthenium supported on silicalite-1 treated with 1.0 M NaOH showed superior catalytic performance compared to unmodified and KOH-modified silicalite-1 supported Ru catalysts.
Article
Chemistry, Multidisciplinary
David A. Cagan, Daniel Bim, Breno Silva, Nathanael P. Kazmierczak, Brendon J. McNicholas, Ryan G. Hadt
Summary: This study investigates the mechanism of Ni(II)-bpy aryl halide complexes and finds that structural control can regulate the potential energy surfaces of metal-to-ligand and ligand-to-metal charge transfer excited states, facilitating the process of excited-state bond homolysis. This provides a rational approach to utilize photonic energy in synthetic chemistry.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Inorganic & Nuclear
Husain N. Kagalwala, Mahesh S. Deshmukh, Elamparuthi Ramasamy, Neelima Nair, Rongwei Zhou, Ruifa Zong, Laura McCormik, Po-An Chen, Randolph P. Thummel
Summary: The study focuses on the design and synthesis of two dinuclear catalysts for the conversion of water to oxygen, involving metal oxide centers under specific conditions.
INORGANIC CHEMISTRY
(2021)
Article
Chemistry, Physical
Jeremy D. Griffin, David B. Vogt, J. Du Bois, Matthew S. Sigman
Summary: This study presents a straightforward C-H oxidation protocol using an acid-stable, bis(bipyridine)Ru catalyst. It reveals that electronic differences remote to the C-H functionalization site affect product selectivity, and the choice of reaction solvent also plays a role in determining site-selectivity. A statistical model is detailed to correlate product selectivity outcomes with computational parameters describing the relative electron-richness of C-H bonds.
Article
Chemistry, Inorganic & Nuclear
Dion B. Nemez, Issiah B. Lozada, Jason D. Braun, J. A. Gareth Williams, David E. Herbert
Summary: This study presents the synthesis, characterization, and coordination chemistry of a doubly pi-extended bipyridine analogue, 6,6'-biphenanthridine (biphe), as well as the emission properties of its coordination complexes in the excited state.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Inorganic & Nuclear
Melanie Guyot, Marie-Noelle Lalloz, Juan S. Aguirre-Araque, Guillaume Rogez, Cyrille Costentin, Sylvie Chardon-Noblat
Summary: The study investigates the impact of different substituents on immobilizing molecular catalysts on (photo)electrode surfaces. Carboxylic ester groups significantly affect the catalytic activity of the complex towards CO2 electroreduction, while alkyl-phosphonic ester substituents do not affect the catalytic activity of the complex.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Inorganic & Nuclear
Wan-Qiang Wang, Zhi-Qin Wang, Wei Sang, Rui Zhang, Hua Cheng, Cheng Chen, Da-Yong Peng
Summary: This study investigates the factors influencing product distribution in the metal-catalyzed dehydrogenative coupling of alcohols and amines to access amides using N-heterocyclic carbene-based Ru (NHC/Ru) complexes. The experimental results show that Ru loadings, added NHC precursors, and the electronic/steric properties of ancillary NHC ligands have a significant impact on the selectivity and yield of the catalytic process.
Article
Polymer Science
Jie Li, Yu Wang, Wen Cai, Gang Yang, Qiuhui Tian, Yongshuang Huang, Dan Peng, Chen Zou, Chen Tan
Summary: Dual-site molecular heterogeneous catalysts have gained attention for synthesizing polyolefin in-reactor blends. A self-supporting strategy based on nickel-catalyzed precipitation coordination polymerization was used to heterogenize and spatially distribute catalyst components in the particles. These polymeric heterogeneous catalysts exhibited higher activities, high molecular weights, good morphological control, and improved compatibility with polar materials. The composition and physical properties of the blend can be controlled by the molar ratio of the two catalytic components. Interestingly, different spatial distribution types resulted in significant differences in thermal, mechanical, and rheological properties and applications of the obtained blends.
Article
Chemistry, Inorganic & Nuclear
Maya Kumari, Souradip Dasgupta, Sanjib Panda, Sudip Kumar Bera, Anindya Datta, Goutam Kumar Lahiri
Summary: This article focused on the ruthenium and osmium derivatives of isomeric 1H-indazole-3-carboxylic acid/2H-indazole-3carboxylic acid and 1H-benzimidazole-2-carboxylic acid along with the pi-acidic bpy and pap co-ligands. It discussed the structures of monomeric and dimeric complexes formed, as well as the modified L2 ' 2- complex. The article also explored the chemical oxidation of the complexes and their potential applications in anion sensing.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Jiawei Chen, Han Li, Haoshang Wang, Yuhang Song, Qiming Hong, Kuan Chang, Huihui Hu, Shuhong Zhang, Lingyun Cao, Cheng Wang
Summary: In this study, phosphine-containing metal-organic layers (MOLs) were synthesized and used for the preparation of heterogeneous catalysts. The mono(phosphine)-Ir complexes generated from metalation of TPP-MOL exhibited high activity as catalysts for the C(sp(2))-H borylation of arenes. This research expands the diversity of MOL-based catalysts.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Applied
Pardeep Dahiya, Ankita Sarkar, Basker Sundararaju
Summary: An efficient method for forming C-N bonds via intramolecular amidation catalyzed by well-defined Cp*Co(N,O)I complexes is presented. The reaction is conducted under mild conditions and produces selectively regioselective amidation product without the use of a bulky counter anion or expensive fluorinated solvents. The Cp*Co(N,O)-I catalyst is highly effective for intramolecular benzylic, tertiary, and internal C(sp(3))-H bond amidation, but ineffective for intramolecular C(sp(2))-H bond amidation.
ADVANCED SYNTHESIS & CATALYSIS
(2022)
Article
Chemistry, Multidisciplinary
Sebastian Amthor, David Hernandez-Castillo, Boris Maryasin, Phillip Seeber, Alexander K. Mengele, Stefanie Graefe, Leticia Gonzalez, Sven Rau
Summary: The substitution behavior and stability of the monodentate chloride ligand in a series of ruthenium(II) terpyridine complexes were investigated, showing a correlation between chloride ligand stability and catalytic performance in water oxidation catalysis experiments. Quantum chemical calculations and theoretical models further support the experimental findings, highlighting the importance of ligand stability in catalyst design.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Inorganic & Nuclear
Laura Ibanez-Ibanez, Andres Mollar-Cuni, Edmond Apaloo-Messan, Akhilesh K. Sharma, Jose A. Mata, Feliu Maseras, Cristian Vicent
Summary: Carboxylate-assisted Pd-catalyzed C-H bond activation is a versatile synthetic method. This study demonstrates the use of mass spectrometry to evaluate the reactivity and selectivity of such systems. The results show that the identity of the X-type ligands significantly affects the regioisomer branching ratio. Ion mobility mass spectrometry was employed to investigate the regioselectivity aspects of carboxylate-assisted Pd-mediated C-H activation of N-heterocyclic carbene ligands.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Organic
Noy B. Nechmad, N. Gabriel Lemcoff
Summary: The historical development of latent sulfur-chelated ruthenium precatalysts from the Lemcoff group's perspective is summarized in this Account. These complexes exhibit a unique cis-dichloro configuration that is latent towards olefin metathesis reactions. Activation of the precatalyst, through isomerization from cis-dihalo to trans-dihalo forms, can be achieved via thermal or light stimuli, with modifications to the ligand sphere imparting unique properties used in diverse applications.
Article
Chemistry, Physical
Lei Wang, Danhua Yan, David W. Shaffer, Xinyi Ye, Bobby H. Layne, Javier J. Concepcion, Mingzhao Liu, Chang-Yong Nam
CHEMISTRY OF MATERIALS
(2018)
Article
Chemistry, Inorganic & Nuclear
Yan Xie, David W. Shaffer, Javier J. Concepcion
INORGANIC CHEMISTRY
(2018)
Article
Chemistry, Physical
M. Kyle Brennaman, Melissa K. Gish, Leila Alibabaei, Michael R. Norris, Robert A. Binstead, Animesh Nayak, Alexander M. Lapides, Wenjing Song, Robert J. Brown, Javier J. Concepcion, Joseph L. Templeton, John M. Papanikolas, Thomas J. Meyer
JOURNAL OF PHYSICAL CHEMISTRY C
(2018)
Article
Chemistry, Multidisciplinary
Lei Wang, Dmitry E. Polyansky, Javier J. Concepcion
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2019)
Article
Chemistry, Physical
Degao Wang, Lei Wang, Matthew D. Brady, Christopher J. Dares, Gerald J. Meyer, Thomas J. Meyer, Javier J. Concepcion
JOURNAL OF PHYSICAL CHEMISTRY C
(2019)
Article
Chemistry, Physical
Lei Wang, David W. Shaffer, Gerald F. Manbeck, Dmitry E. Polyansky, Javier J. Concepcion
Article
Chemistry, Inorganic & Nuclear
Mehmed Z. Ertem, Javier J. Concepcion
INORGANIC CHEMISTRY
(2020)
Article
Nanoscience & Nanotechnology
Yosra M. Badiei, Christian Traba, Rina Rosales, Anthony Lopez Rojas, Claudio Amaya, Mohammed Shahid, Carolina Vera-Rolong, Javier J. Concepcion
Summary: The successful immobilization of Ru(II)-based WOCs and Ru(II) polypyridyl chromophore onto a plasma-grafted poly(acrylic acid) surface on FTO demonstrated higher surface stability and electrocatalytic properties in neutral aqueous solutions, indicating potential applications in solar-to-fuel energy conversion.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Inorganic & Nuclear
Renato N. Sampaio, Brian N. DiMarco, Javier J. Concepcion
Summary: By electrochemically activating an organometallic Ruthenium(II) complex in acetonitrile solutions, the movement of protons from weak Brønsted acids to carbon dioxide (CO2) was coupled with the generation of a metal-hydride complex and a carbonate species, providing key intermediates for CO2 and proton reduction catalysis. These pathways may offer alternative approaches in electrosynthesis of chemical commodities through alkylation and carboxylation reactions.
INORGANIC CHEMISTRY
(2021)
Article
Chemistry, Inorganic & Nuclear
Xiaofan Jia, Hannah S. Nedzbala, Samuel R. Bottum, James F. Cahoon, Javier J. Concepcion, Carrie L. Donley, Albert Gang, Qi Han, Nilay Hazari, Matthew C. Kessinger, Matthew R. Lockett, James M. Mayer, Brandon Q. Mercado, Gerald J. Meyer, Adam J. Pearce, Conor L. Rooney, Renato N. Sampaio, Bo Shang, Hailiang Wang
Summary: In this study, functionalized 2,2'-bipyridine (bpy) ligands were synthesized for covalent immobilization on silicon surfaces. The ligands featured attachment groups for connection to metal oxide coatings or hydrogen-terminated silicon surfaces. The ligands were then coordinated with Re(CO)5Cl to form complexes, which were immobilized on TiO2 or hydrogen-terminated silicon. Characterization of the surface-immobilized complexes showed similar CO stretching frequencies but different cyclic voltammetry behavior compared to the pure molecular complexes. Electrochemical CO2 reduction performance of the immobilized complexes was lower than the solution-phase complexes, suggesting the stability of the linker groups under reducing conditions. This work highlights the complexity of understanding the behavior of molecular catalysts attached to semiconducting silicon surfaces.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Physical
Samuel R. Bottum, Taylor S. Teitsworth, Qi Han, Andre D. Orr, Jin-Sung Park, Xiaofan Jia, Chiara Cappuccino, Bobby H. Layne, Nilay Hazari, Javier J. Concepcion, Carrie L. Donley, Dmitry E. Polyansky, Matthew R. Lockett, James F. Cahoon, David C. Grills
Summary: In situ mid-infrared spectroscopy is a powerful technique for understanding the mechanism of CO2 reduction catalysts, while hybrid photoelectrodes, composed of a semiconductor and a molecular catalyst, are promising for sunlight-driven catalysis. We developed a new strategy using ATR-IR spectroscopy coupled with electrochemistry to characterize catalysts directly integrated with a semiconductor surface under applied potential. This technique allows for the investigation of redox processes associated with CO2 reduction catalysts on Si electrode surfaces with high sensitivity.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Inorganic & Nuclear
Leandro A. A. Faustino, Antonio E. H. Machado, Pedro I. S. Maia, Javier J. J. Concepcion, Antonio Otavio T. Patrocinio
Summary: A novel terpyridine-based Ru(ii) complex was synthesized and its spectroscopic, electrochemical, and catalytic properties were investigated. The complex exhibited two reduction peaks in dry acetonitrile, attributed to consecutive 1 e(-) reduction. Under CO2 atmosphere, a catalytic wave was observed, with CO as the main reduction product. The presence of water improved the catalytic activity and formate production was detected.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Multidisciplinary
Degao Wang, Zihao Xu, Matthew V. Sheridan, Javier J. Concepcion, Fei Li, Tianquan Lian, Thomas J. Meyer
Summary: This study describes a single molecular assembly electrode that mimics the key components of PSII in nature's photosynthesis, achieving sustained light-driven water oxidation catalysis. It highlights the importance of the tyrosine-histidine pair in PSII for efficient water oxidation catalysis in artificial photosynthetic devices.
Review
Chemistry, Multidisciplinary
Ana Belen Munoz-Garcia, Iacopo Benesperi, Gerrit Boschloo, Javier J. Concepcion, Jared H. Delcamp, Elizabeth A. Gibson, Gerald J. Meyer, Michele Pavone, Henrik Pettersson, Anders Hagfeldt, Marina Freitag
Summary: Dye-sensitized solar cells (DSCs) and dye-sensitized photoelectrochemical cells (DSPECs) have seen a revival in recent years as they offer unique properties such as low cost, non-toxic materials, colorfulness, transparency, and efficiency in low light conditions. This review covers advancements in DSC technology over the past decade, including theoretical studies, characterization techniques, materials, applications, and commercialization efforts by various companies.
CHEMICAL SOCIETY REVIEWS
(2021)
Article
Chemistry, Inorganic & Nuclear
Sinval F. Sousa, Mehmed Z. Ertem, Leandro A. Faustino, Antonio Eduardo H. Machado, Javier J. Concepcion, Pedro I. S. Maia, Antonio Otavio T. Patrocinio
Summary: A new ruthenium polypyridyl complex was synthesized and characterized, showing instability and oxidation under aerobic conditions. The reaction provides insights into C-H activation with important implications for catalysis. Theoretical and experimental investigations suggest a two-step aerobic oxidative transformation with the formation of a diruthenium mu-peroxo intermediate as an alternative pathway for C-H activation.
DALTON TRANSACTIONS
(2021)