Article
Chemistry, Inorganic & Nuclear
Takuma Kato, Ryo Tatematsu, Kenichi Nakao, Tomohiko Inomata, Tomohiro Ozawa, Hideki Masuda
Summary: The Ni(II) complexes with different counteranions exhibit distinct X-ray crystal structures and UV-vis spectra, while showing similar electrocatalytic behavior in promoting hydrogen generation. In the presence of HOAc, these three complexes demonstrate varying electrochemical performance in MeCN.
INORGANIC CHEMISTRY
(2021)
Article
Chemistry, Organic
Shiwei Xia, Linna Wu, Guizhi Zhai, Zechao Wang, Junliang Wu
Summary: Visible-light-promoted CO2 oxidative radical reactions have gained increasing attention in organic synthesis. However, current methods only result in the formation of dimer products from simple organic compounds using CO2 as an oxidant. In this study, we demonstrate a visible-light-promoted CO2 oxidative three-component 1,2-thiosulfonylation of styrenes with sodium sulfinates and thiophenols. The use of CO2 as an oxidant is crucial, and no extra stoichiometric amounts of reductants are required. Our photocatalytic strategy enables the conversion of CO2 to fuels CO and CH4, offering a new approach to combine CO2-to-fuel conversion and organic synthesis.
ORGANIC CHEMISTRY FRONTIERS
(2023)
Article
Chemistry, Physical
V. V. Zefirov, D. Gusak, V. E. Sizov, I. Elmanovich, M. S. Kondratenko
Summary: A novel method for the direct synthesis of MnO2 on multiwalled carbon nanotubes through thermal decomposition and oxidation in supercritical CO2 is proposed. The resulting composite materials exhibit improved mass activity in the oxygen reduction reaction (ORR) by controlling oxide particle dimensions and specific surface area through precursor concentration adjustment. Analysis of phase composition, morphology, and electrochemical performance in alkaline electrolyte was conducted to study the characteristics of the composites.
JOURNAL OF SUPERCRITICAL FLUIDS
(2022)
Article
Chemistry, Inorganic & Nuclear
Matthew R. Mena, Jun-Hyeong Kim, Sangho So, Hagit Ben-Daat, Tyler M. Porter, Chandrani Ghosh, Anuja Sharma, Marco Flores, Thomas L. Groy, Mu-Hyun Baik, Ryan J. Trovitch
Summary: It was recently discovered that a manganese complex with a pyridine diimine (PDI) ligand exists in two different states: a low-spin state and an antiferromagnetically coupled intermediate-spin state with a triplet PDI ligand. This finding prompted the synthesis and electronic structure evaluation of similar late first row metal variants with the same chelate. By adding the PDI ligand to iron bromide, the bromide was dissociated and a new iron complex, supported by a dianionic PDI ligand, was formed. Similar reactions were conducted with cobalt and nickel, resulting in the formation of cobalt and nickel analogs of the manganese complex. The electronic differences between these compounds were highlighted, and a computational analysis revealed the thermodynamic penalties associated with phosphine dissociation from these complexes.
INORGANIC CHEMISTRY
(2022)
Article
Environmental Sciences
J. X. Flores-Lasluisa, D. Salinas-Torres, M. Lopez-Ramon, C. Moreno-Castilla, M. A. Alvarez, E. Morallon, D. Cazorla-Amoros
Summary: The study showed that the calcination temperature of the synthesized MnFe2O4 solid nanospheres significantly influenced their electrocatalytic properties, while the presence of manganese species played a key role in the oxygen reduction reaction activity. Among the tested materials, MSN200/CB and MSN350/CB showed the best electrochemical performances and outstanding stability.
ENVIRONMENTAL RESEARCH
(2022)
Article
Chemistry, Inorganic & Nuclear
Soumen Saha, Sha Tamanna Sahil, Md Motiur R. Mazumder, Alexander M. Stephens, Bryan Cronin, Evert C. Duin, Jonah W. Jurss, Byron H. Farnum
Summary: Two NNN pincer complexes of Cu(II) and Ni(II) with BPIMe- ligands were synthesized and characterized structurally, spectroscopically, and electrochemically. The complexes displayed catalytic activity for the reduction of CO2, with the Cu(II) complex showing higher activity than the Ni(II) complex. However, both complexes decomposed into copper and nickel metal on the electrode surface during extended reductive electrolysis, indicating the role of ligand reduction in electrocatalysis and decomposition processes.
DALTON TRANSACTIONS
(2021)
Review
Materials Science, Multidisciplinary
Yue Wang, Chen Zhang, Xinjian Li, Tian Gao, Xue-Bin Wang
Summary: This paper focuses on the application of carbon nanomaterials in the field of electrocatalysis, discussing the doping effects of single elements (N, S, B, O, P) and double elements in carbon-based nonmetallic electrocatalysts, with a particular emphasis on their impact on reductions of nitrogen and carbon dioxide. Challenges and future prospects are also addressed.
MATERIALS RESEARCH BULLETIN
(2021)
Article
Chemistry, Physical
Mengen Chu, Chunjun Chen, Yahui Wu, Xupeng Yan, Shuaiqiang Jia, Ruting Feng, Haihong Wu, Mingyuan He, Buxing Han
Summary: The CuO/CeO2 composites with strong metal-support interaction were synthesized and demonstrated high efficiency and stability in electroreduction of CO2 to C2H4.
GREEN ENERGY & ENVIRONMENT
(2022)
Article
Chemistry, Multidisciplinary
Pirudhan Karak, Sanajit Kumar Mandal, Joyanta Choudhury
Summary: The use of a redox-active organic molecule as a catalyst for electrochemical hydrogen evolution reaction (HER) has not been well explored due to the challenges in strongly acidic conditions. In this study, a NADP(+)-like organic system was demonstrated to efficiently catalyze HER with mild acid as a proton source at moderate overpotential. The system achieved a high Faradaic efficiency of 85±5% and a maximum turnover frequency of 410 s(-1), which is 400 times higher than that of existing NADP(+)-like catalysts. Thorough mechanistic studies were conducted to establish a plausible catalytic cycle.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Materials Science, Multidisciplinary
Xiaoqian Wei, Zijian Li, Haeseong Jang, Min Gyu Kim, Qing Qin, Xien Liu
Summary: Surface strain tuning in a coupled heterostructure efficiently enhances the catalytic performance of Bi2O2CO3/ZnO heterojunction catalysts for CO2 electroreduction. Charge transfer from Zn atoms to Bi atoms and compressive stress on the catalyst surface are crucial in promoting CO2 capture, activation, and subsequent electrochemical reduction to formate.
SCIENCE CHINA-MATERIALS
(2023)
Article
Engineering, Chemical
Jinqiang Liu, Jiao Zhao, Ximing Deng, Yan Sun, Sarah Imhanria, Wei Wang
Summary: The study introduces a non-noble Sn, N co-doped porous carbon catalyst for electrocatalytic reduction of CO2 into syngas (CO and H2 mixture), providing a cheap, stable, and efficient route for syngas production. By adjusting the reduction potentials, the H2 / CO ratio of the generated syngas can be tuned, offering a new approach for CO2 recycling.
JOURNAL OF THE TAIWAN INSTITUTE OF CHEMICAL ENGINEERS
(2021)
Article
Chemistry, Multidisciplinary
Fan Yang, Wensheng Fang, Qingyong Wang, PeiLin Deng, Bao Yu Xia
Summary: In this study, different copper catalysts were prepared to investigate the effects of different oxidation states on the activity and selectivity of CO2 reduction. The results showed that the optimal oxidation state of copper catalysts can achieve high efficiency in converting CO2 into valuable compounds under suitable conditions.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2022)
Article
Chemistry, Physical
Yiming Chen, Zhanggui Hou, Chuan Wang, Xin Ma, Hong Yang, Wen Wang, Ling Zhou, Yi Zhang
Summary: In this work, a high-loaded Ni/Al2O3 catalyst promoted by manganese was proposed. Among them, the 20Ni(2)Mn/Al2O3 catalyst showed the best CO2 conversion (90.5%) and excellent methanation stability at 250 degrees C. The addition of Mn greatly reduced the Ni particle size and improved the Ni dispersion on the alumina support, leading to better reducibility and more medium basic sites, which favor the adsorption and activation of CO2. Manganese could promote the rapid hydrogenation of monodentate carbonate to formate, which could be quickly converted to CH4, contributing to the significantly improved activity of the Mn promoted Ni/Al2O3 catalyst.
Article
Chemistry, Organic
Meng-Qi Ping, Ming-Zhong Guo, Rui-Tao Li, Zi-Chen Wang, Cheng Ma, Li-Rong Wen, Shao-Fei Ni, Weisi Guo, Ming Li, Lin-Bao Zhang
Summary: This study has successfully developed an efficient electrochemical method for the [3 + 2] annulation of imidazo[1,2-a]pyridines with alkynes, using traceless electrons as green reagents. It leads to the synthesis of a large class of polycyclic heteroaromatics with good yields and a broad substrate scope under mild and green conditions.
Review
Chemistry, Multidisciplinary
Yiqun Zheng, Yu Wang, Yuliang Yuan, Hongwen Huang
Summary: This article reviews the recent progress and challenges of metal-based heterogeneous electrocatalysts for CO2ER into CH4, analyzing the effects of various characteristics on electrocatalytic performance.
Article
Chemistry, Inorganic & Nuclear
Raja Pal, Suyeon Kim, Woojong Lee, Matthew R. Mena, Afshan Khurshid, Chandrani Ghosh, Thomas L. Groy, Andrew V. G. Chizmeshya, Mu-Hyun Baik, Ryan J. Trovitch
Summary: This study investigated the synthesis of transition metal complexes through a series of reactions in the presence of a specific ligand, revealing the potential for CO2 coupling and other chemical transformations. Computational studies were also conducted to understand the reaction mechanisms and the importance of cis-coordination sites in selective carbon dioxide coupling reactions.
INORGANIC CHEMISTRY
(2021)
Article
Engineering, Environmental
Yinghao Wen, Ching-Hua Huang, Daniel C. Ashley, Dan Meyerstein, Dionysios D. Dionysiou, Virender K. Sharma, Xingmao Ma
Summary: This study reports the catalyst-free activation of peroxydisulfate (PDS) using visible light, which effectively degrades various organic pollutants. The formation of reactive species is different in the PDS visible light system with and without pollutants. The degradation of atrazine (ATZ) in the PDS visible light system involves both radical and nonradical processes, with O-1(2) playing an important role.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2022)
Article
Pharmacology & Pharmacy
Tufan K. Mukhopadhyay, Johannes Morstein, Dirk Trauner
Summary: This article provides an overview of signaling photolipids developed to date, focusing on their biological applications such as immunomodulation, kinase translocation, apoptosis, ion channel activation, G-protein coupled receptor activation, and neurogenesis.
CURRENT OPINION IN PHARMACOLOGY
(2022)
Article
Engineering, Environmental
Juhee Kim, Junyue Wang, Daniel C. Ashley, Virender K. Sharma, Ching-Hua Huang
Summary: This study investigates the use of the chelating agent picolinic acid (PICA) to enhance the performance of the advanced oxidation process (AOP) involving the activation of peracetic acid (PAA) with iron species. It was found that the PAA-Fe(III)-PICA system degrades micropollutants much more rapidly at higher pH values, achieving almost complete removal of parent compounds within 10 minutes. PAA is a key oxidant in this process.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2022)
Article
Chemistry, Inorganic & Nuclear
Matthew R. Mena, Jun-Hyeong Kim, Sangho So, Hagit Ben-Daat, Tyler M. Porter, Chandrani Ghosh, Anuja Sharma, Marco Flores, Thomas L. Groy, Mu-Hyun Baik, Ryan J. Trovitch
Summary: It was recently discovered that a manganese complex with a pyridine diimine (PDI) ligand exists in two different states: a low-spin state and an antiferromagnetically coupled intermediate-spin state with a triplet PDI ligand. This finding prompted the synthesis and electronic structure evaluation of similar late first row metal variants with the same chelate. By adding the PDI ligand to iron bromide, the bromide was dissociated and a new iron complex, supported by a dianionic PDI ligand, was formed. Similar reactions were conducted with cobalt and nickel, resulting in the formation of cobalt and nickel analogs of the manganese complex. The electronic differences between these compounds were highlighted, and a computational analysis revealed the thermodynamic penalties associated with phosphine dissociation from these complexes.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Thao T. Nguyen, Tufan K. Mukhopadhyay, Samantha N. MacMillan, Michael T. Janicke, Ryan J. Trovitch
Summary: This study presents a method for synthesizing aminosilane chemical vapor deposition precursors, polycarbosilazanes, and perhydropolysilazane. It is found that by using a specific catalyst, the dehydrocoupling reaction between amines and silane can be carried out at ambient temperature, achieving efficient synthesis of the target products.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2022)
Article
Chemistry, Physical
Zahid Nawaz, Habib Ullah, Nevin Gurbuz, Muhammad Naveed Zafar, Francis Verpoort, Muhammad Nawaz Tahir, Ismail Ozdemir, Ryan J. Trovitch
Summary: A series of left-to-right inequivalent 1,3-disubstituted benzimidazolium halide pro-ligands and their corresponding Ag complexes were synthesized and characterized using spectroscopic techniques. These complexes exhibited high efficiency in the addition of carbon dioxide to epoxides to yield cyclic carbonates, with the bimetallic complex showing the highest activity.
MOLECULAR CATALYSIS
(2022)
Article
Engineering, Environmental
Junyue Wang, Juhee Kim, Daniel C. Ashley, Virender K. Sharma, Ching-Hua Huang
Summary: Ferrate(VI) and peracetic acid (PAA) are two oxidants that have been found to degrade micropollutants more efficiently when applied together. This study investigated the mechanisms behind this enhanced degradation and found that Fe(IV)/Fe(V) species were the main reactive agents, while organic radicals had little contribution. The study also revealed that PAA is not an activator for Ferrate(VI), but can enhance the oxidation capacity of Fe(IV)/Fe(V), leading to increased efficiency in wastewater treatment.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2022)
Article
Chemistry, Organic
Tufan K. Mukhopadhyay, Dirk Trauner
Summary: A general strategy to quickly access glycerophospholipids is reported in this study, utilizing the opening of a phosphate triester epoxide with carboxylic acids catalyzed by Jacobsen's Co(salen) complex. This method allows for the synthesis of various glycerophosphate derivatives.
JOURNAL OF ORGANIC CHEMISTRY
(2022)
Article
Chemistry, Medicinal
Tufan K. Mukhopadhyay, Sabine Willems, Christopher J. Arp, Johannes Morstein, Caleb T. Haake, Daniel Merk, Dirk Trauner
Summary: Activation of local LXR may be a potential strategy for the treatment of metabolic diseases and cancer, and the development of photoswitchable LXR agonists based on the T0901317 scaffold can overcome the side effects of LXR agonists. The designed LXR agonist, activated in its light-induced state, sensitized human lung cancer cells to chemotherapy, supporting the potential of locally activated LXR agonists as adjuvant cancer treatment.
Article
Engineering, Environmental
Juhee Kim, Junyue Wang, Daniel C. Ashley, Virender K. Sharma, Ching-Hua Huang
Summary: This study discovers that the biodegradable chelating ligand picolinic acid (PICA) can effectively mediate the activation of peracetic acid (PAA) by manganese (II), leading to accelerated degradation of micropollutants. The PAA-Mn(II)-PICA system is capable of rapidly removing various micropollutants in clean and wastewater matrices. High-valent manganese species (Mn(V)) is identified as the main reactive species contributing to the rapid degradation of micropollutants.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Anuja Sharma, Ren H. H. Bean, Timothy E. E. Long, Ryan J. J. Trovitch
Summary: The phosphine-substituted aryl diimine cobalt catalyst efficiently mediates the dehydrocoupling of diamines or polyamines with poly(methylhydrosiloxane) to produce hydrogen and crosslinked solids. The resulting siloxane diamine and siloxane polyamine networks are stable in the presence of air or water and can withstand temperatures up to 1600°C. By reducing the catalyst loading to 0.01 mol %, the catalyst shows the highest activity ever reported for Si-N dehydrocoupling, generating a siloxane diamine foam with a turnover frequency of 157 s(-1) relative to diamine consumption. Moreover, the catalyst can produce linear siloxane diamine polymers with molecular weights up to 47,300 g/mol by reducing the number of potential branch points.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Review
Chemistry, Multidisciplinary
Brock E. Leland, Joydeb Mondal, Ryan J. Trovitch
Summary: This article explores the historical and recent efforts in catalyzing the dehydrocoupling of amines and silanes, a direct method for Si-N bond formation with hydrogen as a byproduct. The advantages of this transformation have driven the development of catalysts across the periodic table, leading to advances in efficiency and selectivity. The article highlights the formation of monomeric, oligomeric, and polymeric aminosilanes separately, and features a recent study on the manganese-catalyzed synthesis of perhydropolysilazane and commercial chemical vapor deposition precursors.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Anuja Sharma, Sangho So, Jun-Hyeong Kim, Samantha N. MacMillan, Mu-Hyun Baik, Ryan J. Trovitch
Summary: This study describes the discovery and utilization of a new cobalt catalyst that exhibits the highest reported turnover frequencies for metal-catalyzed carbonyl hydrosilylation.
CHEMICAL COMMUNICATIONS
(2022)