Article
Biochemistry & Molecular Biology
Mohan Yu, Yajun Liu
Summary: Among bioluminescent organisms, fireflies are the most famous for their high luminescent efficiency. Through molecular dynamics simulation and calculations, the efficient oxygenation mechanism of luciferin in fireflies has been studied, shedding light on the high efficiency of their bioluminescence initiation.
Article
Chemistry, Physical
Ephrahime S. Traore, Aimin Liu
Summary: This study analyzes the choice of the first coordination shell of the metal center in nonheme iron oxygenases from the perspective of charge maintenance. The importance of charge maintenance after substrate binding is highlighted, and the charge analysis is extended to different types of nonheme iron oxygenases. The concept of charge maintenance is significant in promoting the reaction of the iron center and may be applicable to other oxygen-activating metalloenzymes systems.
Article
Chemistry, Physical
Cristian G. Sanchez, Matias Berdakin
Summary: The harvesting of plasmon-induced hot carriers in nanosystems has been considered a clean and efficient way to utilize light irradiation for over a decade. However, describing the full process and injection of plasmon-induced hot carriers presents challenges. By employing an atomistic and real-time approach, researchers have gained insights into the generation, injection, and photocatalytic effects of hot carriers. Future studies will continue to explore the potential applications of plasmon-induced hot carriers.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Organic
Tianwen Chen, Liyuan Wang, Shayu Li, Lichun Dong, Luxi Tan
Summary: In this study, a novel N-substituted diketopyrrolopyrrole (DPP) derivative, Ph-DPP, was synthesized, and it exhibited interaction with Lewis alkaline anions, such as F-. Both the typical electron-transfer-dominated anion-π interaction product, Ph-DPP-, and an unexpected isomer product, i-Ph-DPP, were observed. The formation mechanism of these products was investigated using density functional theory calculations, which suggested that a deprotonation initiation route is favored, providing valuable insight into the debated role of F(-) in non-covalent intermolecular interactions.
Article
Chemistry, Multidisciplinary
Naoya Haraguchi, Naoki Ogiwara, Yoshitaka Kumabe, Soichi Kikkawa, Seiji Yamazoe, Takashi Tachikawa, Sayaka Uchida
Summary: Size-controlled Ag clusters with specific colors were synthesized using porous ionic crystals (PICs) as scaffolds and redox-active polyoxometalates (POMs) as electron sources. The cluster size and color emission were controlled by the reduction time and types of ions or elements in the PICs. This method provides a convenient way to obtain ligand-free Ag clusters with high yields and stability.
Article
Chemistry, Multidisciplinary
Anqi Zhang, Ran Zhao, Yahui Wang, Jiasheng Yue, Jingjing Yang, Xinran Wang, Chuan Wu, Ying Bai
Summary: Layered manganese dioxide (delta-MnO2) is a promising cathode candidate for aqueous zinc-ion batteries, but the insertion of zinc ions has caused structural deformation, insufficient cycle stability, and limited rate capability. This study proposes a hybrid superlattice structure with improved electrochemical performance through polymer pre-intercalation, demonstrating the synergy of electron entropy stimulation and selective H+ Grotthuss intercalation.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Yanxia Wang, Jianping Sheng, Xiaoli Zhao, Ye He, Fan Dong, Yanjuan Sun
Summary: By constructing a (BiO)2CO3/beta-Bi2O3 heterostructure and introducing graphene quantum dots, efficient charge transfer dynamics are enhanced, leading to high activity and long-term stability for photocatalytic NO removal.
CHINESE CHEMICAL LETTERS
(2023)
Article
Chemistry, Inorganic & Nuclear
Santosh K. Gupta, Brindaban Modak, Pampa Modak, Yuanbing Mao
Summary: In this work, controlled energy transfer was achieved by suppressing the host to dopant energy transfer in La2Hf2O7:Eu3+ nanoparticles through co-doping with uranium ions. The co-doping creates negatively charged vacancies in the system to compensate for the excess charge in U and Eu co-doped La2Hf2O7 NPs, suppressing the formation of oxygen vacancies. This study demonstrates the potential for producing near perfect white light emission by utilizing the full color gamut in La2Hf2O7:Eu3+,U6+ nanoparticles.
INORGANIC CHEMISTRY FRONTIERS
(2021)
Article
Chemistry, Organic
Shaofa Sun, Donghui Guo, Fangyi Li, Jian Wang
Summary: The NHC-mediated oxidation of imines to amides allows for the rapid assembly of amides in good to high yields, featuring both umpolung of imines and the discovery of NHC-bound 1,2-dioxetane intermediates.
ORGANIC CHEMISTRY FRONTIERS
(2022)
Article
Chemistry, Multidisciplinary
He Li, Cheng Lin, Yilong Yang, Chaoran Dong, Yulin Min, Xiaoqin Shi, Luyang Wang, Siyu Lu, Kan Zhang
Summary: By using inter-facet edge (IFE) rich WO3 arrays in an electrolyte containing CO32-, reactive oxygen species (ROS), H2O2, and OH. are efficiently generated by water oxidation with total Faraday efficiencies of more than 90%. The IFE favors the adsorption of CO32- and reduces the adsorption energy of OH., while suppressing surface hole accumulation. In situ selective oxidation of benzyl alcohol using the formed OH. achieves a benzaldehyde production rate of approximately 768 μmolh(-1) with near 100% selectivity. This work provides a promising approach to enhance the efficiency and value-added product of oxidation reactions in aqueous solar fuel systems.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Biochemistry & Molecular Biology
Yuki Ohmuro-Matsuyama, Hayato Matsui, Masaki Kanai, Tadaomi Furuta
Summary: Researchers developed a bright luciferase, picALuc, and identified important residues and regions for its catalysis and bioluminescence through mutational analyses. These findings provide important insights into the bioluminescence mechanism of picALuc and copepod luciferases and have potential applications for sustained observations.
Article
Chemistry, Multidisciplinary
Tengyue Wang, Jiaren Du, Xiaomeng Wang, Kai Jiang, Panqin Wang, Shaoxing Lyu, Hengwei Lin
Summary: Rare earth-doped luminescent materials have wide applications in scientific research and practical use. The design of a single matrix containing multiple emitting centers is a trend in the development of luminescent materials. This study reports the design of a smart platform combining trivalent bismuth and lanthanides ions in a LuNbO4 matrix, which demonstrates multiple stimuli-responsiveness and color-tunability. The possible application of color-changeable indicators for information readouts is demonstrated, showing promise in various fields.
MATERIALS CHEMISTRY FRONTIERS
(2023)
Article
Chemistry, Multidisciplinary
Ramzi N. Massad, Thomas P. Cheshire, Chenqi Fan, Frances A. Houle
Summary: In this study, the coordination and timing of a Ru-based dye-catalyst diad in water oxidation were examined through computational stochastic kinetics. The results showed that the progress of the water oxidation catalytic cycle is controlled by the buildup of intermediates, rather than the flux of solar irradiation or charge/excitation losses. This suggests that catalytic efficiency can be improved by photostimulating all intermediates to allow the catalytic rate to be governed by charge injection under solar illumination alone.
Article
Chemistry, Multidisciplinary
Brittany R. Benlian, Pavel E. Z. Klier, Kayli N. Martinez, Marie K. Schwinn, Thomas A. Kirkland, Evan W. Miller
Summary: Q-BOLT is a small-molecule enzyme pair for optical voltage sensing that utilizes quenching of bioluminescence to visualize changes in membrane potential in live cells. It combines three distinct readouts - QRET, BRET, and the ratio between bioluminescence emission and BRET - to accurately report membrane potential oscillations in HEK 293T cells and hiPSCs, without the need for excitation light.
Article
Chemistry, Inorganic & Nuclear
Wu-Ji Wei, Ying Mu, Li Wei, Ji-Xiang Hu, Guo-Ming Wang
Summary: This study synthesized two new photochromic chain complexes through self-assembly, achieving reversible room-temperature fluorescence and phosphorescence switching by light irradiation and thermal treatment. The electron transfer photochromic behavior and generated stable radicals were found to play a key role in this process.
INORGANIC CHEMISTRY
(2021)
Article
Biochemistry & Molecular Biology
Bo-Wen Ding, Elena V. Eremeeva, Eugene S. Vysotski, Ya-Jun Liu
PHOTOCHEMISTRY AND PHOTOBIOLOGY
(2020)
Article
Chemistry, Organic
Yi-Qi Tang, Ya-Jun Liu
JOURNAL OF ORGANIC CHEMISTRY
(2020)
Article
Chemistry, Multidisciplinary
Yi-Qi Tang, Ya-Jun Liu
Summary: Bioluminescence, a visible light produced by living organisms, has been widely used in biotechnology and biomedical fields due to its high sensitivity, selectivity, and signal-to-noise ratio. Despite the unknown mechanisms of most BLs, theoretical studies in the past 14 years have uncovered the mechanisms and details of several BLs.
CHINESE JOURNAL OF CHEMISTRY
(2021)
Article
Chemistry, Multidisciplinary
Shuangqi Pi, Quansong Li, Ling Yue, Ya-Jun Liu
Summary: A recent study introduced a first-generation pair of chemiluminescent formaldehyde probes (CFAP540 and CFAP700) with high selectivity and sensitivity to formaldehyde, suitable for cellular and in vivo applications. Through density functional theory calculations, the mechanism of CFAP chemiluminescence production and the assignment of the light emitter were elucidated. By analyzing the D-pi-A architecture of the light emitters of CFAP540 and CFAP700, a theoretical design for a series of CFAPs and a scheme to modulate their chemiluminescence from visible to near-infrared region were proposed.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Organic
Ming-Yu Wang, Ya-Jun Liu
Summary: Bioluminescent fungi can emit green light continuously for days and share a common mechanism among all lineages. Detailed processes remain unknown, but theoretical calculations have provided insights into the molecular and electronic state level of the bioluminescent process. The initiation of fungal bioluminescence involves the formation of a high-energy intermediate through oxygenation of luciferin.
JOURNAL OF ORGANIC CHEMISTRY
(2021)
Article
Chemistry, Organic
Yi-Qi Tang, Li Mao, Ben-Zhan Zhu, Ya-Jun Liu
Summary: This study revealed that a strong chemiluminescence occurs in the presence of Co(II) in CA/H2O2 system. The chemiluminescence in CA/H2O2 is explained by the formation of a neutral dioxetane through six sequential reactions, followed by decomposition into a neutral excited-state product via a gradually reversible charge transfer luminescence mechanism. The key to the chemiluminescence is the generation of the intrinsically produced (OH)-O-center dot.
JOURNAL OF ORGANIC CHEMISTRY
(2021)
Article
Chemistry, Physical
Ling Yue, Ya-Jun Liu
Summary: This study theoretically investigates the rubrene-catalyzed decomposition of DDO for the first time, revealing a stepwise ET-catalyzed decomposition and three S-0/S-1 conical intersection-controlled singlet chemiexcitation. The findings not only contribute to a better understanding of high-efficiency singlet CL, but also provide some general clues for designing new high-efficient CL systems.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2021)
Article
Chemistry, Physical
Shu-Feng Chen, Eugene S. Vysotski, Ya-Jun Liu
Summary: The bioluminescence of marine organisms is regulated by CaRP, with the formation of the emitter involving a proton transfer (PT) process. Studies have shown that there is a concerted PT process between the anionic S-1-coelenteramide and the nearest histidine residue, facilitated by a water molecule. This fast PT process helps to align experimental and theoretical findings in emitter formation for CaRPs.
JOURNAL OF PHYSICAL CHEMISTRY B
(2021)
Article
Biochemistry & Molecular Biology
Mohan Yu, Yajun Liu
Summary: Among bioluminescent organisms, fireflies are the most famous for their high luminescent efficiency. Through molecular dynamics simulation and calculations, the efficient oxygenation mechanism of luciferin in fireflies has been studied, shedding light on the high efficiency of their bioluminescence initiation.
Article
Biochemistry & Molecular Biology
Ya-Jie Guo, Cheng-Xing Cui, Ya-Jun Liu
Summary: This study used density functional theory calculations to uncover the mechanism and process of storage and release reactions in the bioluminescent cycle of fireflies. The results indicated that both reactions are exergonic, favoring the storage and release processes, which is consistent with experimental observations. The computational approach utilized a model system and simulated protein environments to investigate the reactions.
PHOTOCHEMISTRY AND PHOTOBIOLOGY
(2022)
Article
Chemistry, Physical
Zhuo Quan, Li Mao, Yi-Qi Tang, Ming Lei, Ben-Zhan Zhu, Ya-Jun Liu
Summary: In this study, the mechanism of H2O2-dependent bioluminescence from TBBQ was investigated. It was found that the bioluminescence process is initiated by a nucleophilic substitution reaction, and the theoretical mechanism was supported by experimental evidence.
Article
Chemistry, Physical
Yi-Qi Tang, Yanling Luo, Ya-Jun Liu
Summary: This study explores the selectivity of RCHO chain length and the chemical reaction involving RCHO in bacterial bioluminescence through molecular docking, QM/MM calculation, and MD simulation. The research indicates that RCHO molecules with chain lengths of 8 to 16 carbon atoms participate in an enzymatic addition reaction to produce a high-energy intermediate, which is the energy source for light emission. Additionally, it is revealed that a water molecule, not alpha His44, abstracts and relays a proton to catalyze the reaction in bacterial luciferase.
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
(2021)
Review
Chemistry, Physical
Ya-Jun Liu
Summary: Bioluminescence is a fascinating natural phenomenon whose mechanism has been elucidated through computational studies. This review summarizes the theoretical investigations on bioluminescence to date and discusses the current status and future prospects of computational bioluminescence.
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY C-PHOTOCHEMISTRY REVIEWS
(2022)
Article
Chemistry, Multidisciplinary
Yu Mohan, Cheng Yuanyuan, Liu Yajun
ACTA CHIMICA SINICA
(2020)
Article
Chemistry, Physical
Ling Yue, Le Yu, Chao Xu, Chaoyuan Zhu, Yajun Liu
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2020)