Review
Chemistry, Multidisciplinary
Changpeng Chen, Feng-Shou Liu, Michal Szostak
Summary: The discovery of NHCs as ancillary ligands has greatly improved catalytic processes, with BIAN-NHC ligands in particular showing enhanced reactivity due to combinations of electronic and steric properties. The development of BIAN-NHC ligands has led to major advancements in catalysis and offers a practical alternative to classical NHCs.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Inorganic & Nuclear
Hua-Qing Yin, Ming-Yang Cui, Hao Wang, Yuan-Zhao Peng, Jia Chen, Tong-Bu Lu, Zhi-Ming Zhang
Summary: Carbon dioxide cycloaddition into fine chemicals is a promising technology for solving energy crisis and environmental issues. This study investigates the effects of metal type on the performance of CO2 cycloaddition using isostructural MOF-919-Cu-Fe and MOF-919-Cu-Al as models. The results reveal that MOF-919-Cu-Fe with exposed Fe and Cu Lewis acid sites exhibits significantly higher conversion and selectivity compared to MOF-919-Cu-Al. The mechanism suggests that the exposed Fe3+ sites facilitate the ring opening of epoxide and CO2 activation, promoting the CO2 cycloaddition reaction.
INORGANIC CHEMISTRY
(2023)
Article
Biochemistry & Molecular Biology
Yaping Cheng, Geoffrey Gontard, Abderrahim Khatyr, Michael Knorr, Hani Amouri
Summary: Luminescent N-heterocyclic carbene chloride copper (I) complexes incorporating pyrene chromophore (1-Pyrenyl-NHC-R)-Cu-Cl with different substituents (methyl or naphthyl) were synthesized and characterized. X-ray diffraction confirmed the formation of the target compounds. These compounds exhibited blue emission in both solution and solid-state at room temperature, with comparable or higher quantum yields than the parent pyrene molecule. Notably, the quantum yield was increased by almost two-fold by replacing the methyl group with a naphthyl group. These compounds show potential for applications in optical displays.
Article
Engineering, Environmental
Guoliang Yang, Yijun Qian, Dan Liu, Lifeng Wang, Yuxi Ma, Jianhua Sun, Yuyu Su, Karyn Jarvis, Xungai Wang, Weiwei Lei
Summary: Functional MXene-based membranes were prepared for simultaneous electrokinetic energy conversion and organic molecular sieving. The positively charged PDDA-MXene (PMXene) composite membranes showed good rejection for positively charged methylene blue molecules, and the output current improved by around four times.
CHEMICAL ENGINEERING JOURNAL
(2022)
Review
Chemistry, Multidisciplinary
Avinash Kumar Both, Yurui Gao, Xiao Cheng Zeng, Chin Li Cheung
Summary: Gas hydrates, particularly methane hydrates, are studied for both their potential threats and as an alternative energy resource due to high methane storage capacity. Developing porous material hosts for gas hydrates is critical in materials and energy science communities.
Article
Chemistry, Multidisciplinary
Jianwen Li, Sheng Tao, Fei Chen, Min Li, Ning Liu
Summary: A variety of zero-valent molybdenum complexes and divalent molybdenum complexes with N-heterocyclic carbenes (NHC)-pyridine ligands were synthesized and their catalytic activities in the cycloaddition reaction of epoxides and CO2 were studied. The divalent molybdenum complexes showed higher catalytic activity for the synthesis of cyclic carbonates compared to the zero-valent molybdenum complexes. The divalent molybdenum complexes combined with TBAI effectively transformed various terminal and internal epoxides under specific conditions.
JOURNAL OF CO2 UTILIZATION
(2023)
Article
Chemistry, Inorganic & Nuclear
Mozhgan Parsaei, Kamran Akhbari, Jonathan White
Summary: A novel Zn(II)-based metal-organic framework, MUT-4, has been successfully synthesized and its CO2 adsorption performance can be optimized by adjusting the synthetic methods.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Inorganic & Nuclear
Fengyi Wang, Longcheng Zhang, Ting Wang, Fang Zhang, Qian Liu, Haitao Zhao, Baozhan Zheng, Juan Du, Xuping Sun
Summary: This study introduces a high-efficiency electrocatalyst Bi NPs@CRs for artificial NH3 synthesis with high FE and large NH3 yield, as well as high electrochemical durability.
INORGANIC CHEMISTRY
(2021)
Review
Chemistry, Multidisciplinary
Li-Qi Qiu, Hong-Ru Li, Liang-Nian He
Summary: CO2 conversion to valuable chemicals is an effective way to reduce CO2 emissions. We developed carbonaceous and metal-organic framework (MOF)-based catalysts for nonreductive and reductive CO2 conversion, and explored novel strategies for CO2 capture and in situ transformation. Nanomaterial-based catalysts show high stability and efficiency, and are also promising in photocatalytic CO2 reduction and electrocatalytic CO2 reduction.
ACCOUNTS OF CHEMICAL RESEARCH
(2023)
Article
Chemistry, Physical
Sangita Sahoo, Subarna Manna, Arnab Rit
Summary: Herein, a heteroditopic NHC ligand-supported environment-friendly zinc catalyst is developed for the effective N-formylation of N-H moieties with CO2 using hydrosilane as a reductant. This protocol works effortlessly under 1 bar CO2 pressure at room temperature with a low catalyst loading and is compatible with a range of N-H functionalities, offering excellent functional group tolerance and chemoselectivity. The synthetic utility of the obtained formamides is demonstrated by synthesizing biologically relevant compounds.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Engineering, Environmental
Liang Teng, Yimin Xuan, Yun Da, Chen Sun, Xianglei Liu, Yulong Ding
Summary: This study reports a modified calcium-looping (CaL) technology that utilizes solar energy to convert CO2 into syngas and methane while achieving thermal energy storage. The advantages of CaL in both carbon capture and utilization and thermal energy storage are utilized to establish a renewable energy system with near-zero carbon emissions. The results demonstrate that the proposed system achieves negative emissions of greenhouse gases and converts solar energy into hydrocarbon fuel.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Chemistry, Inorganic & Nuclear
Ai-Ling Gu, Wan-Ting Wang, Xin-Yu Cheng, Tian-Ding Hu, Zhi-Lei Wu
Summary: A novel noble-metal-free three-dimensional framework catalyst was synthesized for the efficient cyclization reaction of propargylic amines and CO2, displaying excellent solvent stability. Experimental and theoretical studies elucidate the mechanism and reaction pathway.
INORGANIC CHEMISTRY
(2021)
Article
Construction & Building Technology
Shuaichao Chen, Quantao Liu, Hanjun Wu, Chao Yang, Xing Gong, Shaopeng Wu, Yuanyuan Li
Summary: This research aims to enhance the anti-thermal oxygen and anti-ultraviolet aging properties of asphalt binder simultaneously with antioxidant intercalated UV-shielding material. The results showed that LDHs-1222 modified asphalt exhibited superior thermal oxygen aging and UV aging resistance. 4% LDHs-1222 showed the most significant enhancement effect on the anti-aging properties of asphalt.
CONSTRUCTION AND BUILDING MATERIALS
(2022)
Article
Nanoscience & Nanotechnology
Weiwei Shi, Jiao Yu, Huili Liu, Defeng Gao, Aili Yuan, Binbin Chang
Summary: Nanoporous carbons can be tailored to meet the requirements of CO2 capture and separation by optimizing their porosity and surface chemistry. The pore structure determines the CO2 adsorption capacity, while the surface chemistry affects the adsorption selectivity and heat of adsorption. Converting biowaste into high-added-value adsorbents offers an elegant solution for effective CO2 capture and utilization.
ACS APPLIED NANO MATERIALS
(2023)
Article
Chemistry, Physical
Jun Ma, Yahui Wu, Xupeng Yan, Chunjun Chen, Tianbin Wu, Honglei Fan, Zhimin Liu, Buxing Han
Summary: It is interesting to synthesize high value-added chemicals from CO2 with low energy consumption under mild conditions. A novel catalyst, Zn(betaine)(2)Br-2, is reported to efficiently promote the cycloaddition of CO2 with epoxides under ambient conditions.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Multidisciplinary
Abdul Khayum Mohammed, Pilar Pena-Sanchez, Ajmal Pandikassala, Safa Gaber, Ayesha A. AlKhoori, Tina Skorjanc, Kyriaki Polychronopoulou, Sreekumar Kurungot, Felipe Gandara, Dinesh Shetty
Summary: A new class of copper-based 2D-c-MOF was synthesized using green mechano-chemistry, with metal coordination involving salicylaldehyde functional moiety explored for the first time in MOFs. Furthermore, a semiconductive copper-based SA-MOF thin film was successfully fabricated at room temperature using an in situ salt-free method.
CHEMICAL COMMUNICATIONS
(2023)
Article
Multidisciplinary Sciences
Yan Zhao, Tianhong Zhou, Mounir Mensi, Jang Wook Choi, Ali Coskun
Summary: Fluorination of ether solvents is an effective strategy to improve the electrochemical stability of non-aqueous electrolyte solutions in lithium metal batteries. However, excessive fluorination detrimentally impacts the ionic conductivity of the electrolyte, thus limiting the battery performance.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Eunseok Park, Jongseok Park, Kyunam Lee, Yan Zhao, Tianhong Zhou, Gyuleen Park, Min-Gi Jeong, Minseok Choi, Dong-Joo Yoo, Hun-Gi Jung, Ali Coskun, Jang Wook Choi
Summary: A new low-dielectric solvent, 1,2-dimethoxypropane (DMP), was introduced as an electrolyte solvent. Compared to 1,2-dimethoxyethane (DME), DMP has decreased solvation power and increased solvation polarity, promoting anion-Li+ interactions and improving the cycling stability of the battery.
ACS ENERGY LETTERS
(2023)
Editorial Material
Energy & Fuels
Yan Zhao, Ali Coskun
Summary: Silicon-based anodes in batteries face challenges of volume change and cracks, leading to limited cycling stability. However, a hierarchically-ordered conductive binder network formed by thermal treatment of anodes with conducting polymer precursors can enhance charge-transport and mechanical properties, improving cyclability.
Article
Chemistry, Multidisciplinary
Yan Zhao, Tianhong Zhou, Lars P. H. Jeurgens, Xian Kong, Jang Wook Choi, Ali Coskun
Summary: By using a specific electrolyte, high electron transfer efficiency can be achieved, improving the stability of the lithium metal surface and its operation at high voltages.
Article
Nanoscience & Nanotechnology
Joelle Medinger, Kyung Seob Song, Pacifique Umubyeyi, Ali Coskun, Marco Lattuada
Summary: In this study, anisotropic structure of porous carbons was achieved by integrating superparamagnetic colloids and applying a uniform magnetic field during the sol-gel transition. The resulting hierarchically porous carbon monoliths showed higher porosity, higher CO2 uptake capacity, and faster adsorption kinetics compared to those synthesized without a magnetic field. Additionally, these materials were found to be effective magnetic sorbents for oil-spill cleanup.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Timur Ashirov, Patrick W. Fritz, Yanic Lauber, Claudia E. Avalos, Ali Coskun
Summary: In this study, a direct synthesis method for a fully conjugated 3D porous organic polymer (POPs) named benzyne-derived polymers (BDPs) was reported. The resulting BDPs exhibited ultramicroporous structures with surface areas up to 544 m(2) g(-1) and high CO2/N-2 selectivities. This research shows the potential of BDPs as a promising material for gas separation and storage.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Kyung Seob Song, Ali Coskun
Summary: Recycling palladium (Pd) from waste materials is crucial for meeting the increasing demand for Pd in various industries. This article focuses on the design principles of solid-sorbents, particularly porous organic polymers (POPs), which show promise for Pd recovery due to their tunable chemical functionality, stability, and porosity. The role of binding sites and porosity in Pd uptake capacity, adsorption kinetics, and selectivity is discussed, along with the sustainable use of captured Pd as a heterogeneous catalyst for cross-coupling reactions.
Article
Chemistry, Multidisciplinary
Timur Ashirov, Thamon Puangsamlee, Alexandra Robles, Patrick W. Fritz, Krzysztof Piech, Ognjen S. Miljanic, Ali Coskun
Summary: The development of porous organic polymers (POPs) with high surface areas and CO2 affinity is important for capturing CO2 and reducing its environmental impact. The synthesis of 3D macrocycle-based POPs with tunable structures and high CO2 uptake capacity was achieved through ionothermal polycondensation. The resulting polymer, 3D-mmPOP-250, exhibited a surface area of 752 m(2) g(-1), high microporosity, and excellent CO2 binding enthalpy and uptake capacity.
HELVETICA CHIMICA ACTA
(2023)
Article
Materials Science, Multidisciplinary
Sujanya Maria Ruban, Kavitha Ramadass, Gurwinder Singh, Siddulu Naidu Talapaneni, Gunda Kamalakar, Chandrakanth Rajanna Gadipelly, Lakshmi Kantham Mannepalli, Yoshihiro Sugi, Ajayan Vinu
Summary: Carbon nitrides are a type of metal-free catalytic materials with great potential for chemical transformations and organocatalysis. Their low cost, thermal and chemical stability, non-toxicity, ease of functionalization, and porosity make them versatile for catalysis. This review discusses N-rich carbon nitrides and their role in various organic catalytic reactions. It also explores the structure-property relationship and potential value of these materials compared to other catalytic materials. The review aims to provide up-to-date information on the developments in carbon nitride-based organic catalysis and their future prospects.
SCIENCE AND TECHNOLOGY OF ADVANCED MATERIALS
(2023)
Article
Chemistry, Physical
Tianhong Zhou, Yan Zhao, Kyung Seob Song, Dominika Baster, Mario El Kazzi, Ali Coskun
Summary: In this study, we demonstrated the use of captured Pd from wastewater conditions to develop a sustainable and environmentally friendly electrocatalyst for Li-S batteries. The electrocatalyst, named covalent isothiocyanurate frameworks (CITCFs), effectively suppressed the shuttling effect and promoted the kinetics of sulfur redox reactions, resulting in improved specific capacity and rate performance of Li-S batteries.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Physical
Yan Zhao, Tianhong Zhou, Dominika Baster, Mario El Kazzi, Jang Wook Choi, Ali Coskun
Summary: Understanding the degradation pathways and reactivity of electrolytes is crucial for addressing the limitations of conventional electrolytes and developing new electrolytes for high-voltage lithium metal batteries. By tuning the electronic properties of 1,3-dioxolane (DOL) through the introduction of methyl and trifluoromethyl groups, 4-methyl-1,3-dioxolane (MDOL) and 4-(trifluoromethyl)-1,3-dioxolane (TFDOL) solvents were developed. The TFDOL-based electrolyte exhibited excellent oxidation stability up to 5.0 V, while the MDOL-based electrolyte showed side reactions with metallic Li. The weak solvation power of TFDOL, along with the formation of an inorganic-rich solid electrolyte interphase, enabled a robust cycling stability in a Li|NCM811 full cell (20 μm Li foil, N/P ratio of 2.5).
ACS ENERGY LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Tianhong Zhou, Yan Zhao, Patrick W. Fritz, Timur Ashirov, Dominika Baster, Mario El Kazzi, Ali Coskun
Summary: We improved the interfacial stability of Li metal anodes in Li-S batteries by regulating the electrolytes using arylthiol additives. The tetrathiol additive had dual functionality, enhancing the interfacial stability of the Li anode, controlling the sulfur redox kinetics, and suppressing side reactions with polysulfides. This resulted in an improved capacity retention of 70% after 500 cycles at 1 C.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Omer Elmutasim, Kyriaki Polychronopoulou
Summary: Nickel phosphides have shown excellent catalytic ability and surface affinity towards probe molecules in hydrodeoxygenation reactions. This study focuses on investigating the reaction mechanism of phenol and guaiacol on the Ni5P4(001) surface using ab initio calculations. Interestingly, phenol dissociates immediately with a low activation energy, while guaiacol dissociation requires a higher activation barrier. Hydrogenation steps for both molecules have high activation energies. The study also explores the rate-limiting steps and reaction kinetics.
SUSTAINABLE ENERGY & FUELS
(2023)
Article
Chemistry, Physical
Ahmed Elabd, Jiheon Kim, Daniel Sethio, Sangho Kang, Taemin Kang, Jang Wook Choi, Ali Coskun
Summary: Electrolyte engineering is a promising strategy in lithium-sulfur batteries. This study introduces a dual functional high donor electrolyte, 3-FPN, which achieves high solubility of polysulfides and compatibility with lithium metal. This results in high specific capacity and robust cycling under lean electrolyte conditions.
ACS ENERGY LETTERS
(2022)
