Article
Chemistry, Physical
Xiaoying Sun, Xinyu Li, Yue Liu, Zhan Yu, Bo Li, Zhen Zhao
Summary: This study explores the enhanced role of Mo dopant on MgO in oxidative coupling of methane. The results reveal that subsurface Mo dopant significantly enhances the adsorption and activation of oxygen molecules. The combination of adsorbed oxygen and surface Mg exhibits a balanced activity for C-H bond activation and release of methyl radical, paving the way for methane activation with promising yield.
Article
Chemistry, Multidisciplinary
Xiao-Xi Li, Xiaoyan Lu, Jae Woo Park, Kyung-Bin Cho, Wonwoo Nam
Summary: High-valent iron-imido complexes have multiple energetically close-lying electromers and can perform efficient oxidations, unlike common iron-oxo species. The reactivity of these complexes can emulate multi-spin state reactions, and a new non-rebound mechanism is proposed for C-H activation reactions.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Inorganic & Nuclear
Ren Ying, Wang Tao, Zhang Ting-Ting, Jia Jian-Feng, Wu Hai-Shun
Summary: A systematic theoretical investigation was conducted on the Fujiwara-Moritani reaction between 3-methoxyacetanilide and n-butyl acrylate using density functional theory (DFT) calculations. The study found that the mechanism and rate-determining step of the reaction differed in two different catalytic cycles, and also investigated the roles of BQ and ligand effects.
CHINESE JOURNAL OF STRUCTURAL CHEMISTRY
(2021)
Article
Chemistry, Physical
Qingjun Zhang, Pengyuan Shi, Aiwu Zeng
Summary: Direct carboxylation of thiophene with CO2 has been achieved using a mild solvent-free carbonate and carboxylate medium. The base-mediated medium can cleave the weakly acidic C-H bond without the need for other limiting reagents. The optimal base additive for this reaction is cesium pivalate among the targeted simple carboxylate salts. The detailed mechanism of the carboxylation reaction involves initial proton abstraction and C-C bond formation by carbonate, followed by CO2 insertion. The C-H activation step has a higher energy barrier than the CO2 insertion step, indicating that the base-induced C-H deprotonation is slow and the resulting carbon-centered nucleophile rapidly reacts with CO2.
Review
Chemistry, Inorganic & Nuclear
Yongjun Liu, Ruijia Wang, Christopher K. Russell, Penglong Jia, Yi Yao, Wei Huang, Maciej Radosz, Khaled A. M. Gasem, Hertanto Adidharma, Maohong Fan
Summary: Methane has the potential to be a promising feedstock for clean fuels and chemicals. However, the direct catalytic conversion of methane into oxygenates is a significant challenge. This review summarizes the catalysts for methane synthesis of oxygenates, compares their activities and reaction mechanisms, and highlights potential catalysts and new technologies. Furthermore, future research directions are discussed.
COORDINATION CHEMISTRY REVIEWS
(2022)
Article
Chemistry, Physical
Benjamin P. Charnay, Zhihao Cui, Melissa A. Marx, Joseph Palazzo, Anne C. Co
Summary: This study investigates the electrochemical reduction of aldehydes to alcohols as a pathway for converting CO2 to alcohols. Experimental results support the proposed mechanism of reducing acetaldehyde and propionaldehyde to ethanol and 1-propanol on a Cu catalyst. Notably, acetaldehyde is selectively reduced to ethanol on Cu, but not on Au, as supported by both experimental observations and DFT calculations.
Article
Chemistry, Physical
Yuchen Zhang, Yichen Yu, Yi Dai, Yaoyuan Zhang, Qi Liu, Dong Xiong, Lixia Bao, Qin Wu, Daxin Shi, Kangcheng Chen, Yuming Li, Guiyuan Jiang, Evgenii Kondratenko, Hansheng Li
Summary: The introduction of Ga into ZrO2 catalysts alters the C-H bond activation pathway in propane, resulting in simultaneous cleavage of two C-H bonds and improved activation ability. The Ga-doped catalyst exhibits a lower reaction barrier and higher C-H bond activation ability compared to state-of-the-art metal oxide catalysts.
Article
Chemistry, Physical
Matthew Wheatley, Marco Zuccarello, Maria Tsitopoulou, Stuart A. Macgregor, Olivier Baudoin
Summary: In this study, mechanistic investigations were conducted on the reactivity of various alpha-substituted C(sp(3))-H bonds in the context of Pd-0-catalyzed C(sp(3))-H arylation. The results provide important insights into the reaction kinetics and a reactivity scale was determined, which will be useful for future studies in transition-metal-catalyzed C(sp(3))-H activation.
Article
Chemistry, Multidisciplinary
Rie Yoshimoto, Attila Taborosi, Qiyuan He, Yusuke Ano, Naoto Chatani, Seiji Mori
Summary: The reaction between aromatic amides and maleimides, catalyzed by palladium, leads to the formation of a product with double C-H bond activation, occurring at both the benzylic and meta positions. Computational chemistry studies reveal a stepwise mechanism involving a six-membered palladacycle, maleimide insertion, protonation of the Pd-N bond, and activation of the meta C-H bond. The site selectivity is determined by the interaction energy controlling the insertion of maleimide into the Pd-C(sp(3)) bond. The meta C-H bond activation step is identified as the rate-determining step based on the energetic span model. The 2-thiomethylphenyl group is found to function effectively as a directing group due to strong Pd-S bonding and the destabilizing effect of the deformation energy.
CHEMISTRY-AN ASIAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Anirudra Paul, Jae Hyun Kim, Scott D. Daniel, Daniel Seidel
Summary: Despite efforts by practitioners, direct alpha-C-H bond functionalization of unprotected alicyclic amines is rare. A new method utilizing N-lithiated alicyclic amines has been developed, providing a convenient approach to achieve functionalization reactions under mild conditions. This method offers a new pathway for the synthesis of beta-amino ketones with regioselective alpha'-alkylation, and potential for one-pot synthesis of polycyclic dihydroquinolones.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Applied
Fen Wang, Changbao Chen, Feng Zhang, Qingxi Meng
Summary: Density functional theory was used to investigate the reaction mechanism of Ni(0)-NHC-catalyzed enantioselective intramolecular C-H cyclization of indoles. The computations revealed that the C1-H bond showed the highest reactivity, and the concerted oxidative addition played a major role in the activation process. Two chiral products coexisted due to similar transition states and little difference in free energy barrier.
APPLIED ORGANOMETALLIC CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Edina Reizer, Bela Fiser
Summary: The reaction initiation points of the 16 priority polycyclic aromatic hydrocarbons (PAHs) have been determined by calculating the different C-H bond dissociation enthalpy (BDE) values. Six density functional theory methods and four basis sets were applied, and the most feasible combination was selected. Most of the hydrogen atoms are in zig-zag positions, and the BDE and bond length values for the PAHs range between certain values. The initiation points are mostly represented by armchair and peak hydrogens.
ARABIAN JOURNAL OF CHEMISTRY
(2022)
Article
Chemistry, Physical
Andrzej Bil, Michal Andrzej Kochman, Krzysztof Mierzwicki
Summary: The experimentally confirmed double proton transfer reaction in the glyoxal-methanol complex follows a complicated mechanism involving two complementary pathways, with the transition structure nearly coinciding with the dissociation of the covalent C-H bond in glyoxal. Key stages of the evolution of crucial covalent bonds along the intrinsic reaction path have been demonstrated.
JOURNAL OF MOLECULAR STRUCTURE
(2021)
Article
Multidisciplinary Sciences
Yue Liu, Wei Zhang, Cong Hao, Shuai Wang, Haichao Liu
Summary: Converting naturally occurring sugars into fuels and chemicals offers a sustainable and carbon-neutral alternative to fossil resource-based processes. Tungsten-based catalysts are efficient in selectively breaking the C-C bonds of sugars, producing oxygenate intermediates that can be used in the synthesis of various chemicals. This research reveals the mechanism of sugar conversion and provides insights for the rational design of catalytic sites and reaction pathways.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2022)
Article
Chemistry, Multidisciplinary
David Gygi, Miguel Gonzalez, Seung Jun Hwang, Kay T. Xia, Yangzhong Qin, Elizabeth J. Johnson, Francois Gygi, Yu-Sheng Chen, Daniel G. Nocera
Summary: This study overcomes the challenge of activating C-H bonds by synthesizing a specific complex that generates a chlorine radical under light irradiation. The experimental and computational results together reveal the complete reaction profile for the preferential activation of a C-H bond in the solid state.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Multidisciplinary
Fuqing Yu, Haonan Zhao, Yingzhong Li, Guomin Xia, Hongming Wang
Summary: This study demonstrates the synthesis and investigation of organic D-A-type fluorophores, Np-TPA and Np-2TPA, with strong fluorescence emission in both dilute solutions and the solid state. The conformation planarization in the excited state allows for intense emission in solution, while highly restricted pi-pi stacking permits bright emission in the crystalline state. These results suggest that dual-state emissive fluorophores represent a new paradigm for bioimaging.
MATERIALS CHEMISTRY FRONTIERS
(2022)
Article
Chemistry, Multidisciplinary
Yigang Wang, Guomin Xia, Manman Tan, Mingda Wang, Yingzhong Li, Hongming Wang
Summary: Understanding and implementing ordered supramolecular assembly in organic photothermal materials is challenging but significant. In this study, an amphipathic squaraine dye (PSQ) with a poly (ethylene glycol) chain attached was synthesized and self-assembled into nanospheres with well-defined H-dimeric substructures. Molecular dynamics simulations were conducted to illustrate the self-assembly process. The resulting H-dimeric nanospheres showed ultrahigh photothermal conversion efficiency and exhibited good stability, biocompatibility, tumor accumulation, and efficient tumor inhibition in photothermal therapy. These findings provide a unique platform for the precise design of small-molecule photothermal agents for future clinical applications of photothermal therapy.
ADVANCED FUNCTIONAL MATERIALS
(2022)
Article
Chemistry, Inorganic & Nuclear
Caiju Jin, Zijuan Chen, Shunli Shi, Ying Li, Sanmei Liu, Shuhua Wang, Hongming Wang, Chao Chen
Summary: In this study, chiral metal-organic frameworks (CMOFs) with a hierarchical micro/ mesoporous structure were synthesized using a mechanochemical process. The construction strategy was simple, green, and rapid, allowing for the solvent-free production of gram-scale CMOFs. The as-synthesized CMOFs showed excellent catalytic performance in Aldol asymmetric catalysis.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Physical
Caiju Jin, Shunli Shi, Sheng Liao, Sanmei Liu, Siyao Xia, Yanping Luo, Shuhua Wang, Hongming Wang, Chao Chen
Summary: We report a rapid synthesis of functionalized metal-organic frameworks (MOFs) by integrating post-synthetic ligand exchange (PSLE) and mechanochemistry. This mechano-PSLE approach overcomes the challenges of PSLE, such as long reaction time, excessive solvent, and PSLE failure under solvothermal conditions. The gram-scale MOF functionalized with a chiral group can be obtained easily and in an environmentally friendly manner. It exhibits excellent asymmetric catalytic performance, providing a basis for the industrial production of functionalized MOFs.
CHEMISTRY OF MATERIALS
(2023)
Review
Physics, Condensed Matter
Mingda Wang, Wenzhe Shan, Hongming Wang
Summary: This article reviews the unique properties of twisted bilayer graphene (TBG), the first experimentally discovered two-dimensional material. The main topics covered include the correlated insulating phase, superconducting phase, quantum anomalous Hall effect, and theoretical analysis. Twisted multilayer graphene, with better tunability than TBG, is also discussed, followed by conclusions and proposed research fields.
PHYSICA STATUS SOLIDI B-BASIC SOLID STATE PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Fuqing Yu, Xian Liu, Luliang Liao, Guomin Xia, Hongming Wang
Summary: Electrochemical CO2 reduction reaction (CO2RR) is an effective approach to address CO2 emission and synthesize high-value multi-carbon (C2+) chemicals. Constructing multilayer-bound nanoreactors is a promising strategy to manage intermediate CO and produce C2+ products. In this study, Ag@Cu2O nanoreactors were designed and optimized, demonstrating high Faradaic efficiency and stability during C2+ production. The study also provides insights into CO retention and ethanol generation in multilayer-bound nanoreactors.
Article
Chemistry, Multidisciplinary
G. Xia, L. Si, H. Wang
Summary: Dual-state emission refers to the phenomenon where organic molecules exhibit bright emission in both dilute solution and solid states. This concept has contributed to the understanding of photophysical areas and practical applications of mono-state emission. This review focuses on the structural features and working principles of dual-state emissive luminogens (DSEgens), highlighting the importance of intramolecular p-conjugated rigidity and twisted conformation in their efficient construction. The correlation between molecular configurations and emission properties of DSEgens is analyzed, with a focus on emission efficiency and wavelength variability. Preliminary applications and future perspectives of DSEgens are also discussed.
MATERIALS TODAY CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Xianshi Zeng, Luliang Liao, Qiming Yu, Meishan Wang, Hongming Wang
Summary: This study investigates metal-organic frameworks (MOFs) composed of transition metals and organic ligands as potential electrocatalysts for CO2 reduction. Through testing ten different catalysts, this study finds that seven of them exhibit high CO2 reduction selectivity.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Physical
Xianshi Zeng, Luliang Liao, Meishan Wang, Hongming Wang
Summary: Metal-organic frameworks (MOFs) have excellent performance in electrocatalytic reduction of CO2 and can address resource scarcity and climate issues. The two-dimensional MOF constructed from transition metal-hexaiminotriphenylene was found to be an ideal electrocatalyst based on theoretical calculations and reliable data. Various metal catalysts showed promising catalytic activity and can be used for CO2 reduction.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Weihan Guo, Mingda Wang, Leilei Si, Yigang Wang, Guomin Xia, Hongming Wang
Summary: We designed a propeller-like squaraine dye SQ-NMe2 decorated with four peripheral dimethylamines to achieve high sensitivity and wide-range color switching in piezochromic fluorescent materials. The precise peripheral design improves molecular packing and facilitates intramolecular charge transfer under mechanical stimuli. The SQ-NMe2 microcrystals exhibit significant fluorescence changes from yellow to orange to deep red, making them suitable for crytographic applications.
Article
Chemistry, Multidisciplinary
Yigang Wang, Mingda Wang, Guomin Xia, Yang Yang, Leilei Si, Hua Wang, Hongming Wang
Summary: The first acceptor-substituted squaraine fluorophore with a maximum emission wavelength beyond 1200 nm has been developed, exhibiting ultra-high brightness and photostability. It can co-assemble with bovine serum albumin to form a biocompatible dye-protein nanocomplex, leading to significant fluorescence enhancement for high-resolution vascular imaging.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Liming Hong, Xian Liu, Baozhu Chi, Guomin Xia, Hongming Wang
Summary: This study successfully designed and prepared a precise diatomic catalyst that achieves synergistic adsorption and activation of H2O and CO2 molecules through strong hydrogen bonding, thereby improving the efficiency and product selectivity of CO2 electroreduction.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Materials Science, Biomaterials
Yingzhong Li, Lizhen Chen, Leilei Si, Yang Yang, Chunlei Zhou, Fuqing Yu, Guomin Xia, Hongming Wang
Summary: By utilizing triphenylamine-equipped 1,8-naphthaolactam (NP-TPA) as a versatile scaffold, an efficient subcellular imaging agent (NP-TPA-Tar) was designed with bright and constant emissions, significant Stokes shifts, and easy modifiability. The NP-TPA-Tar can efficiently map the spatial distribution of lysosomes, mitochondria, endoplasmic reticulum, and plasma membrane in Hep G2 cells. Compared to its commercial counterpart, NP-TPA-Tar exhibits increased Stokes shift, enhanced photostability, improved targeting capability, and comparable imaging efficiency even at low concentrations (50 nM). This work will advance the development of imaging agents and improve super-resolution and real-time imaging in biological applications.
JOURNAL OF MATERIALS CHEMISTRY B
(2023)
Article
Chemistry, Organic
Wei Chen, Jingjun Fang, Jian Huang, Qin Yang, Zhibin Song, Qiuping Ding, Hongming Wang, Yiyuan Peng
Summary: An efficient method for direct regioselective acylation of quinazolines under metal-free conditions was developed. The reaction showed good to excellent yields, excellent functional group tolerance and site selectivity. The mechanism of the reaction was investigated using multiple analytical strategies.
ORGANIC & BIOMOLECULAR CHEMISTRY
(2023)
Article
Chemistry, Physical
Xian Liu, Luliang Liao, Guomin Xia, Fuqing Yu, Guangyao Zhang, Minxing Shu, Hongming Wang
Summary: This study proposes a new strategy to maintain both the precise Ni-N2C2 structure and high metal loading by using a Ni-salen polymer precursor with a confined metal position and precise coordination mode. The resulting Ni-N2C2 SAC exhibits excellent catalytic performance in the electroreduction of CO2 to CO.
JOURNAL OF MATERIALS CHEMISTRY A
(2022)
Article
Chemistry, Physical
A. Aathif Basha, Attar Kubaib, Mohammad Azam
Summary: The properties of a set of compounds were comprehensively assessed using various analytical techniques, revealing their stability and favorable drug-like characteristics. Potential antiviral and antioxidant properties were predicted, indicating promise for biological efficacy.
COMPUTATIONAL AND THEORETICAL CHEMISTRY
(2024)
Article
Chemistry, Physical
Meiqi Liu, Baoming Hou, Yuheng Li, Yuyu Pan, Bing Yang
Summary: This paper investigates the application potential of thermally activated delayed fluorescent (TADF) molecules with donor-acceptor-donor-acceptor pi-conjugated macrocycle structures in organic light-emitting diodes. The study finds that the macrocyclic structure has a smaller energy gap between the first singlet excited state and the first triplet excited state compared to the linear structure. The TADF efficiency is also analyzed and explained based on spin-orbit coupling and intersystem crossing rates.
COMPUTATIONAL AND THEORETICAL CHEMISTRY
(2024)
Article
Chemistry, Physical
Run Liu, Jiahui Liu, Jiarui Fang, Xiruo Bai, Dan Wang, Yixuan Qie, Shuqi Zu, Guancheng Wang, Xinyi Sui, Runyao Chang, Yizhu Wang, Ziheng Li
Summary: This paper investigates the remodeling effect of H2O molecules and their adsorption behavior on Co2+-doped SnO2 (221) crystal plane materials. The results show that H2O molecules remodel the crystal plane by creating oxygen defects, leading to hydroxylation. The hydroxylated crystal surface adsorbs O2 and then H2O molecules, affecting the electrical conductivity of the crystal plane.
COMPUTATIONAL AND THEORETICAL CHEMISTRY
(2024)
Article
Chemistry, Physical
Marisol Ibarra-Rodriguez, Paul Horley, Mario Sanchez
Summary: In this study, the functionalized borophene was investigated as a potential sensor or transporter of glucose for biomedical applications. The adsorption of glucose molecules on different boron-based complexes was studied, and the results showed that these complexes have high binding energies and can efficiently adsorb glucose molecules. The findings suggest that borophene-based systems with different oxidation states hold promise for intelligent drug delivery and biosensor design.
COMPUTATIONAL AND THEORETICAL CHEMISTRY
(2024)
Article
Chemistry, Physical
Syed Hassan Sarwar, Saad Jawaid Khan, Syed Faraz Jawed
Summary: The medical community is currently focusing on targeted and controlled drug delivery, and many researchers are utilizing computational resources to understand drugnanocarrier combinations and develop targeted drug delivery systems. This study used molecular dynamics to investigate the encapsulation capacity of Carbazochrome, a hemostatic drug, in Single-Walled Carbon Nanotubes of different morphological variations. The results showed that the nanotube radius and length had the most significant impact on the encapsulation capacity, followed by nanotube chirality. Temperature also affected the drug encapsulation when the nanotube radius was not very large and the chiral angle was near 30 degrees.
COMPUTATIONAL AND THEORETICAL CHEMISTRY
(2024)
Article
Chemistry, Physical
Yinquan Sui, Mengying Sun, Yongxin Wang, Zhitong Xu, Jinglu Yan, Huanpeng Liu
Summary: In this study, the structural and hydrogen storage properties of loaded Pt atoms were investigated using density functional theory (DFT) with and without substitution of B atoms on the edges of conical graphene layers (CGL). It was found that the position of the substituted B atom at the edge of the CGL has an important effect on the position of the loaded Pt atom and its hydrogen adsorption and storage properties.
COMPUTATIONAL AND THEORETICAL CHEMISTRY
(2024)
