Article
Chemistry, Multidisciplinary
Ryoichi Kanega, Naoya Onishi, Shinji Tanaka, Haruo Kishimoto, Yuichiro Himeda
Summary: A novel approach using multinuclear iridium complexes for catalytic hydrogenation of CO2 to methanol in the gas-solid phase was reported. The combination of a multinuclear catalyst and gas-solid phase reaction conditions led to effective production of methanol. The catalyst showed high reactivity, with a final turnover number of 113 under specific conditions.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Physical
Arun Dixith Reddy Shada, Alexander J. M. Miller, Thomas J. Emge, Alan S. Goldman
Summary: The method of alkane dehydrogenation using iridium complexes achieves up to 97% yield and up to 15 catalytic turnovers, utilizing proton-coupled electron transfer. This approach offers a promising way to selectively dehydrogenate alkanes with practical implications.
Article
Chemistry, Multidisciplinary
Fengling Zhang, Jingning Lai, Zhengqiang Hu, Anbin Zhou, Huirong Wang, Xin Hu, Lijuan Hou, Bohua Li, Wen Sun, Nan Chen, Li Li, Feng Wu, Renjie Chen
Summary: In this study, a dilute electrolyte containing crown ether additives was tailored to improve the performance of lithium-oxygen batteries (LOBs) by promoting lithium salt dissociation and solvation of Li+ ions. This electrolyte exhibited enhanced electrochemical stability and triggered a solution-mediated Li2O2 growth pathway, leading to a high discharge capacity of 10 828.8 mAh g(carbon)(-1). Furthermore, optimized electrode/electrolyte interfaces promoted the kinetics of oxygen reduction/evolution reactions (ORR/OER) and achieved a dendrite-free Li anode, improving the cycle life of LOBs.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Inorganic & Nuclear
Jiarui Chang, Man Ding, Jia-Xue Mao, Jie Zhang, Xuenian Chen
Summary: A palladium(ii) hydride complex supported by a benzene-based PNCNP pincer ligand has been synthesized via two different routes and exhibits strong deprotonating ability and versatile catalytic activity. It can readily deprotonate acetamide to form the corresponding acetamido complex and catalyze the dehydrogenation of methanol to formaldehyde under mild conditions, as well as the direct hydration of nitriles to primary amides. The direct hydration of nitriles catalyzed by this complex is the most efficient palladium catalytic system for this type of reaction, achieving 100% selectivity and good to excellent yields.
DALTON TRANSACTIONS
(2022)
Article
Chemistry, Multidisciplinary
Matthew J. Evans, Samuel E. Neale, Mathew D. Anker, Claire L. McMullin, Martyn P. Coles
Summary: The potassium aluminyl [K{Al(NONDipp)}](2) effectively activates ethene towards carbonylation with CO under mild conditions. The study also identified important intermediates in the reaction pathway and confirmed the stabilizing influence of incorporated benzene through computational methods.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Koichiro Masada, Shuhei Kusumoto, Kyoko Nozaki
Summary: In this study, a novel method for synthesizing metallabenzenes by replacing the phosphorus atom in an aromatic phosphinine ring with transition metal fragments was reported. Iridabenzene and rhodabenzene were successfully synthesized by triggering the replacement of the phosphorus atom with iridium and rhodium fragments, respectively. The aromaticity of the newly synthesized metallabenzenes was evaluated experimentally and theoretically.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Changho Yoo, Alexander J. M. Miller
Summary: A study reported the application of an iodide-free catalyst in the production of acetic acid through methanol carbonylation, achieving methylation without the use of iodide. Experimental results showed that the catalyst mediated methylation through C-H bond activation and acetate migration, ultimately producing methyl acetate and acetic acid.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Physical
Andrew D. Newman, Yuan Wang, Samantha A. Orr, Karen Wilson, Adam F. Lee
Summary: Rh(OAc)(2)/HPW/SiO2 bifunctional catalyst exhibits promising performance in the carbonylation of methanol, showing high catalytic activity and acetic acid selectivity.
CATALYSIS SCIENCE & TECHNOLOGY
(2022)
Article
Chemistry, Physical
Soumik Biswas, Michael J. Blessent, Benjamin M. Gordon, Tian Zhou, Santanu Malakar, David Y. Wang, Karsten Krogh-Jespersen, Alan S. Goldman
Summary: The PCP-pincer iridium complexes exhibit high regioselectivity for the transfer dehydrogenation of n-alkanes, while the closely related PCOP and POCOP complexes do not. The difference in regioselectivity is a true kinetic phenomenon, not a result of isomerization subsequent to the formation of free alpha-olefin. The different regioselectivity of the POCOPIr vs PCPIr catalysts is attributable to the different rate-determining steps of their respective catalytic cycles, which can be explained in terms of different electronic effects of O versus CH2 linker exerted through the pincer aromatic ring.
Review
Chemistry, Inorganic & Nuclear
Hugo Valdes, Juan M. German-Acacio, Gerard van Koten, David Morales-Morales
Summary: This study explores the synthesis and applications of bimetallic complexes by merging a metallocene and a (cyclopentadienyl/aryl) pincer metal complex, discussing their importance in tuning electronic properties, catalytic reactions, and chiral catalysis. Various approaches to merge metallocene and pincer-metal motifs are explored, showcasing the potential for creating diastereomerically pure derivatives through post-functionalization strategies. The authors aim to inspire further research in this field by highlighting the synthetic, physico-chemical properties, and remarkable catalytic activities of metallocene-based pincer-metal complexes.
DALTON TRANSACTIONS
(2022)
Article
Chemistry, Inorganic & Nuclear
Jia-Xue Mao, Jiarui Chang, Jie Zhang, Xuenian Chen
Summary: The structures and catalytic reactivity of nickel chloride and thiolate complexes supported by benzene-pyridine-based nonsymmetrical PCN pincer ligands were investigated. The composition and substitution of the pincer backbone were found to have a significant influence on the structures and catalytic reactivity.
DALTON TRANSACTIONS
(2023)
Review
Chemistry, Multidisciplinary
Sebastian Acosta-Calle, Alexander J. M. Miller
Summary: The development of catalysts has had a significant impact on science and technology, allowing for optimized reaction conditions, improved catalytic activity, and selectivity. Controlled catalysis can be achieved by manipulating the dynamics of ligands and gating substrate access to the catalyst site. The design principles for cation-controlled catalysis have been explored and various catalysts have been developed for switchable and tunable catalysis.
ACCOUNTS OF CHEMICAL RESEARCH
(2023)
Review
Chemistry, Multidisciplinary
Sebastian Acosta-Calle, Alexander J. M. Miller
Summary: Catalysis plays a crucial role in science and technology by allowing catalysts to respond to environmental changes and alter their structure and function. Controlled catalysis offers opportunities for innovation, such as optimizing performance, executing multiple reactions, and synthesizing copolymers. By controlling the dynamics of hemilabile ligands, it is possible to regulate the substrate access to catalyst sites. This approach has significant theoretical and practical implications in synthetic chemistry.
ACCOUNTS OF CHEMICAL RESEARCH
(2023)
Article
Chemistry, Physical
Tiezheng Pan, Jiangbo Li, Bo Li, Qiangqiang Xu, Zhiliyu Cui, Jie Shang, Yan Ge, Zhenhui Qi
Summary: This study found that the sensitivity of supramolecular assemblies based on OEG to guanidinium-containing species is influenced by their cyclic and linear forms, with the cyclic form having a higher binding constant. By designing crown ether derivatives with different topologies, manipulation of the relationship between supramolecular solutes, water, and guanidinium salts is possible, providing an alternative strategy for fabricating thermal-responsive systems in ionic medium.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Chemistry, Applied
Andrea Gualandi, Giacomo Rodeghiero, Rossana Perciaccante, Thomas Paul Jansen, Cristina Moreno-Cabrerizo, Charles Foucher, Marianna Marchini, Paola Ceroni, Pier Giorgio Cozzi
Summary: The study demonstrates that under photoredox catalysis, allylation of aldehydes using organometallic cobalt species can be achieved without the need for stoichiometric amounts of zinc. The reaction proceeds in moderate to good yields under specific conditions.
ADVANCED SYNTHESIS & CATALYSIS
(2021)
Article
Chemistry, Physical
Zi-Ye Liu, Qian-Yu Wang, Ji-Ming Hu
Summary: In this study, a layered carbon dot composite catalyst (NiFe LDH@CDs) was prepared using a one-step coprecipitation method, without the need for heating or hydrothermal treatment. The CD-functionalized catalyst facilitated rapid charge transfer and accelerated the oxygen evolution reaction. Additionally, the heterojunction structure formed between NiFe LDH and CDs efficiently suppressed photoelectron-hole recombination.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
Article
Chemistry, Physical
Rohit Kumar, Ankit Kumar Srivastava, Palaniyappan Nagarasu, Vedichi Madhu, Ekambaram Balaraman
Summary: We designed and synthesized a NN-CoII bidentate complex and used it for the amination of alcohols under mild and solventless conditions. The complex exhibited good reactivity towards both primary and sterically hindered secondary alcohols, providing high yields of amines. The pyrazole moiety in the ligand played a crucial role in the reaction. Furthermore, we demonstrated the reusability of the complex as a homogeneous cobalt catalyst.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
Article
Chemistry, Physical
Shivanand Chettri, Liang-Ting Wu, Sagarmani Rasaily, Debesh Sharma, Bikram Gurung, Rajani Dewan, Sudarsan Tamang, Jyh-Chiang Jiang, Anand Pariyar
Summary: Replicating the enzymatic surface microenvironment in vitro is challenging, but constructing an analogous model could facilitate our understanding of surface effects and aid in developing an efficient bioinspired catalytic system. In this study, five unique Cu2O morphologies were generated, and the surface morphology variations were found to be a consequence of differences in the exposure of low-index facets. The reactivity of Cu2O was found to be influenced by the proportion of {110} planes, with r-Cu2O exhibiting the highest reactivity.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
Article
Chemistry, Physical
Yong Tang, Jianhao Qiu, Dingliang Dai, Guanglu Xia, Lu Zhang, Jianfeng Yao
Summary: Defect engineering has been shown to improve the photocatalytic performance. This study investigated the use of defect-rich UiO-66-NH2 wrapped by ZnIn2S4 as a catalyst for photocatalytic H2O2 production. The defects in UiO-66-NH2 enhanced O-2 adsorption and charge separation, leading to higher H2O2 yield. The insights from this work can advance the research in defect engineering of MOFs and photocatalytic H2O2 synthesis.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
Article
Chemistry, Physical
Ruiyang Qu, Shuxin Mao, Jana Weiss, Vita A. Kondratenko, Evgenii V. Kondratenko, Stephan Bartling, Haifeng Qi, Annette-Enrica Surkus, Kathrin Junge, Matthias Beller
Summary: The hydrogenation of amides, a challenging reaction usually performed at high temperatures, has been achieved under milder conditions using a new Pt-MoOx/TiO2 catalyst. This catalyst system enables the selective hydrogenation of various amides and imides.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
Article
Chemistry, Physical
Xiaoran Niu, Ao Wang, Lei Tong, Lei Wang, Yuan Kong, Chenliang Su, Hai-Wei Liang
Summary: This study introduces a novel intermetallic PdCu3 catalyst supported on defective nanodiamond-graphene (ND@G), which exhibits high selectivity (95%) and remarkable activity (turnover frequency: 2940 h(-1)), six times higher than that of the commercial Lindlar catalyst.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
Review
Chemistry, Physical
Zhiyuan Zheng, Yiming Yue, Hongying Zhuo, Qinggang Liu, Yanqiang Huang
Summary: This review presents the recent research advances on single-atom catalysis for deep reduction of CO2. Detailed introductions and summaries were classified into three categories based on proton-coupled multi-electron transfer approaches: strengthening metal-support interaction, rational design and regulation of coordination environment, and development of SACs with multi-atom active sites. The challenges and future research directions in the field of SACs for CO2 reduction are also proposed.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
Article
Chemistry, Physical
Shiv Kumar, Paramita Datta, Anup Bhunia, Swadhin K. Mandal
Summary: This article reports a transition-metal-free process for in situ denitrogenation of tosylhydrazones, resulting in the production of various sulfones. The authors used a phenalenyl-based odd alternant hydrocarbon as a photoredox catalyst, which acted as a potent oxidant to facilitate the denitrogenation reaction. The method showed wide functional-group tolerance and high yields, making it suitable for late-stage modification of natural products.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
Article
Chemistry, Physical
L. A. Luque-Alvarez, J. Gonzalez-Arias, F. Romero-Sarria, T. R. Reina, L. F. Bobadilla, J. A. Odriozola
Summary: Currently, the production of acetic acid through the carbonylation reaction of methanol has limitations, leading to the exploration of alternative methods using heterogeneous catalysts. This study investigates the methanol carbonylation reaction over a Cu-H-MOR catalyst and proposes a reaction mechanism based on the catalytic behavior and performance of the catalyst. The results provide insights into the reaction mechanism and the involvement of acid and redox centers.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)