Article
Chemistry, Physical
Afang Wang, Peng Zhou, Dongqi Tian, Heng Zhang, Zhaokun Xiong, Ye Du, Chuanshu He, Yue Yuan, Tingting Chen, Yang Liu, Bo Lai
Summary: This study reports the catalyst-free activation of peroxydisulfate (PDS) via visible light for the removal of fluoroquinolones (FQs). The mechanism of PDS activation by the excited triplet state of FQs ((3)FQs*) is proposed. Experimental results show that PDS can generate more ·OH in the presence of (3)FQs*. Both radical and non-radical oxidation reactions contribute to the degradation of FQs in the system. QTOF analysis and DFT calculations clarify the degradation pathways and reactive sites. The system exhibits excellent selective oxidation for FQs.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Chemistry, Multidisciplinary
Adam J. Rieth, Yangzhong Qin, Benjamin C. M. Martindale, Daniel G. Nocera
Summary: This study demonstrates the realization of a well-defined triplet excited state in cyanamide-modified carbon nitride, achieved by controlling the particle size, showing the significant role of this long-lived excited state in driving a photochemical cycle of photooxidation-reduction.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Multidisciplinary
Wooseok Lee, Sungwoo Jung, Minseok Kim, Sungwoo Hong
Summary: A novel modular photochemical platform for site-selective C-H pyridylation of unactivated hydrocarbons in chemical feedstocks has been developed, allowing for direct construction of high-value-added compounds under ambient reaction conditions. The system shows high levels of site selectivity and is applicable to a variety of linear-, branched-, and cyclo-alkanes as well as more complex molecules under visible-light conditions.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Physical
Jingyao Chen, Xiaoxiao Xiao, Shuai Li, Yuai Duan, Guo Wang, Yi Liao, Qian Peng, Hongbing Fu, Hua Geng, Zhigang Shuai
Summary: This study proposes a new design strategy to achieve thermally activated delayed fluorescence (TADF) without a typical donor-acceptor structure by controlling the processes between different excited states. Theoretical predictions and experimental synthesis show that a boron difluoride derivative synthesized using this strategy exhibits high radiative rate, fast reverse intersystem crossing rate, and large stimulated emission cross section, making it a promising material for organic amplified spontaneous emission (ASE).
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Applied
Jie Ma, Jinlong Li, Rui Yang, Weijian Xue, Qingxia Wang, Shenmiao Li
Summary: The study revealed that N-1 to N-5 exhibit significantly red-shifted UV-vis absorption and emission properties, with N-1 demonstrating dual emission, confirming their ESIPT characteristics. All compounds generated triplet excited states, with N-3 and N-4 showing longer triplet excited state lifetimes and higher photooxidative abilities than the other compounds.
Article
Chemistry, Multidisciplinary
Jeffrey T. DuBose, Andrew Christy, Jishnudas Chakkamalayath, Prashant V. Kamat
Summary: The competition between energy transfer and charge trapping in 2D halide perovskite is studied, and sensitized emission is observed in bromide-rich compositions. Broad emission from trap states is observed at low temperatures.
Article
Nanoscience & Nanotechnology
Cheng Zhang, Taotao Li, Yu Zheng, Man Zhang, Meilin Liu, Zhengjie Liu, Kui Zhang, Hengwei Lin
Summary: By introducing nitrogen heterocycles and coordinating with metal ions, room-temperature phosphorescent carbon dots have been successfully developed for applications in information encryption and anti-counterfeiting.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Biochemistry & Molecular Biology
Anam Fatima, Jad Rabah, Emmanuel Allard, Helene Fensterbank, Karen Wright, Gotard Burdzinski, Gilles Clavier, Michel Sliwa, Thomas Pino, Rachel Meallet-Renault, Karine Steenkeste, Minh-Huong Ha-Thi
Summary: This study presents the photophysical studies on a BODIPY-fullerene-distyryl BODIPY triad and its reference dyads. The association of the two chromophore units linked by a fullerene moiety leads to strong light absorption and the formation of triplet-excited states. The lifetime and formation quantum yield of the triplet-excited states are investigated, and triplet-triplet annihilation up-conversion is characterized.
PHOTOCHEMICAL & PHOTOBIOLOGICAL SCIENCES
(2022)
Article
Chemistry, Multidisciplinary
Wiebke Alex, Patrick Lorenz, Christian Henkel, Timothy Clark, Andreas Hirsch, Dirk M. Guldi
Summary: This study provides a detailed understanding of the full reaction coordinate of NBDs to QCs and reveals that the photoreversibility of NBDs is influenced by the charge-transfer character.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Akhil Bhardwaj, Bhaskar Mondal
Summary: This study strengthens the concept of weakening the N-N bond through electronic excitation and explores the potential of photochemical N-2 activation via alternate N-N pi-photoactivation route using bimetallic end-on mu(2)-eta(1):eta(1)-N-2 bridging dinitrogen complexes.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Jia-Xiong Chen, Ya-Fang Xiao, Kai Wang, Dianming Sun, Xiao-Chun Fan, Xiang Zhang, Ming Zhang, Yi-Zhong Shi, Jia Yu, Feng-Xia Geng, Chun-Sing Lee, Xiao-Hong Zhang
Summary: Developing red thermally activated delayed fluorescence (TADF) emitters for high-performance OLEDs is a challenge, but the newly designed and synthesized red TADF emitters in this study show promising results with significant efficiency enhancements. Among them, oDTBPZ-DPXZ demonstrates efficient TADF feature and high exciton utilization, achieving excellent external quantum efficiency in both vacuum-processed and solution-processed OLEDs. This work provides an effective strategy for designing red TADF molecules by managing energy level alignments to enhance exciton harvesting.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Jacob M. Garcia, Scott G. Sayres
Summary: Excited state lifetimes of neutral Cr2On clusters were measured using femtosecond pump-probe spectroscopy. Results show that dynamics of excited states are correlated with changes in the electronic structure of the clusters with increasing oxidation. The study reveals the phenomenon of long-lived response in clusters with significant d-electron character, as well as the gradual transition from semiconductor to metallic behavior at the molecular level.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Environmental Sciences
Jiangyao Chen, Xu-nuo Miao, Taicheng An
Summary: In this study, the photolysis of eleven carbonyls to produce O-1(2) was investigated. It was found that dicarbonyl compounds with both ketone and carboxyl groups connected by CC bond showed the highest O-1(2) production ability. Laser flash photolysis confirmed the production of excited triplet species from pyruvic acid and showed its dominant contribution to O-1(2) production. The addition of inorganic salt or changes in solution pH had negligible effect on the excited triplet species, but significantly decreased the steady-state concentration of O-1(2) due to reduction of hydrate content. Photolysis of a mixture of methylglyoxal and dimethylamine led to higher content of excited triplet species and enhanced O-1(2) production compared to pyruvic acid and dimethylamine mixture.
SCIENCE OF THE TOTAL ENVIRONMENT
(2022)
Article
Biochemistry & Molecular Biology
Domenic Gust, Mirko Scholz, Kawon Oum, Thomas Lenzer
Summary: In this study, thin films of a novel organic-inorganic halocuprate were prepared and their relaxation processes in the excited state were investigated. The compound exhibited blue emission with a long excited-state lifetime. Additionally, the time scales for absorption and emission, as well as the relaxation processes of carriers and phonons, were studied.
Article
Chemistry, Multidisciplinary
Shuxuan Tang, Huapeng Ruan, Zhaobo Hu, Yue Zhao, You Song, Xinping Wang
Summary: The triptycene-bridged tris(thianthrene) compound 1 was designed and synthesized. Two triradical trication salts, 2a and 2b, with different crystal packing patterns, were obtained by three-electron oxidation of 1 and subsequent crystallization. Both 2a and 2b feature triradical trications that possess a doublet ground state and can be thermally populated to a quartet state.
CHEMICAL COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Sara I. R. Costa, Yong-Seok Choi, Alistair J. Fielding, Andrew J. Naylor, John M. Griffin, Zdenek Sofer, David O. Scanlon, Nuria Tapia-Ruiz
Summary: The use of urea as a treatment method significantly enhances the cycling performance of Na2Ti3O7 by increasing Na+ ion diffusion coefficient and charge carrier density, without the need for nanosizing or complex synthetic strategies.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Biochemistry & Molecular Biology
Shaowei Zhang, Alan R. F. Godwin, Aoife Taylor, Samantha J. O. Hardman, Thomas A. Jowitt, Linus O. Johannissen, Sam Hay, Clair Baldock, Derren J. Heyes, Nigel S. Scrutton
Summary: Research shows that protochlorophyllide oxidoreductase (POR) plays a crucial role in chlorophyll biosynthesis and plant development. It was found that the binding of Pchlide triggers the formation of large oligomers of POR, likely driven by interactions of amino acid residues in the highly conserved lid regions.
Review
Biochemistry & Molecular Biology
Harshwardhan Poddar, Derren J. Heyes, Giorgio Schiro, Martin Weik, David Leys, Nigel S. Scrutton
Summary: Dynamic changes in protein structures are crucial for protein function and can be investigated with unprecedented temporal and spatial resolution using X-ray free electron lasers. Light-activated proteins are attractive targets for time-resolved structural studies, as they allow for visualization of early chemical changes and global structural changes.
Article
Chemistry, Multidisciplinary
Alexandra E. Kelly-Hunt, Aman Mehan, Sarah Brooks, Miron A. Leanca, Jack E. D. McKay, Nashad Mahamed, Daniel Lambert, Nicola M. Dempster, Robert J. Allen, Andrew R. Evans, Satyajit D. Sarker, Lutfun Nahar, George P. Sharples, Michael G. B. Drew, Alistair J. Fielding, Fyaz M. D. Ismail
Summary: This study presents a method to synthesize purpurogallin, a compound with antioxidant, anticancer, and anti-inflammatory effects. The compound's structure is identified using 1D and 2D NMR spectroscopy, FT-IR, mass spectrometry, and X-ray diffraction. The narrative highlights the shift from deductive and synthetic proof of structural identity to modern methods of structural elucidation.
JOURNAL OF CHEMICAL EDUCATION
(2022)
Article
Biochemistry & Molecular Biology
Samuel L. Freeman, Vera Skafar, Hanna Kwon, Alistair J. Fielding, Peter C. E. Moody, Alejandra Martinez, Federico M. Issoglio, Lucas Inchausti, Pablo Smircich, Ari Zeida, Lucia Piacenza, Rafael Radi, Emma L. Raven
Summary: This study solved the structure and examined the reactivity of the Trypanosoma cruzi ascorbate peroxidase-cytochrome c peroxidase enzyme (TcAPx-CcP), a hybrid heme peroxidase in the protozoan parasite Trypanosoma cruzi. The results showed that TcAPx-CcP has overall structural similarity to other peroxidases, with differences in substrate-binding regions. Additionally, TcAPx-CcP preserves the electron transfer pathway from cytochrome c to heme, preferentially oxidizing cytochrome c but still capable of oxidizing ascorbate.
JOURNAL OF BIOLOGICAL CHEMISTRY
(2022)
Article
Chemistry, Physical
Tobias M. Hedison, Andreea I. Iorgu, Donato Calabrese, Derren J. Heyes, Muralidharan Shanmugam, Nigel S. Scrutton
Summary: This study investigates the structural, dynamical, and functional relationship of copper nitrite reductases (CuNiRs) through combining crystallographic techniques and solution-state approaches. The findings shed light on the catalytic mechanisms of these enzymes and suggest the involvement of protein dynamics. The importance of integrating high-resolution crystallographic techniques and low-resolution solution-state approaches in studying metalloenzymes is emphasized.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Multidisciplinary Sciences
Jonathan S. Trimble, Rebecca Crawshaw, Florence J. Hardy, Colin W. Levy, Murray J. B. Brown, Douglas E. Fuerst, Derren J. Heyes, Richard Obexer, Anthony P. Green
Summary: The ability to program new modes of catalysis into proteins using genetic code expansion methodology has led to the development of photoenzymes that operate through triplet energy transfer catalysis. This allows for versatile reactivity in organic synthesis that is not possible with current biocatalysis methods. The study demonstrates the successful installation of a genetically encoded photosensitizer into a protein scaffold, resulting in a photoenzyme that can perform cycloadditions with high efficiency and selectivity. The photoenzyme outperforms small-molecule catalysts by being able to operate under aerobic conditions and at ambient temperatures. This research opens up new possibilities for excited-state chemistry in protein active sites and provides a foundation for the development of enantioselective photocatalysts.
Article
Electrochemistry
Alex H. Miller, Huong Thi-Thanh Nguyen, Jose G. Nery, Alistair J. Fielding
Summary: Researchers developed a modified glassy carbon electrode for the determination of bisphenol E using differential pulse voltammetry. The modified electrode showed enhanced current response compared to the unmodified electrode. Under optimized conditions, the electrode exhibited linear response to bisphenol E concentration, making it a promising sensing platform for bisphenol determination.
JOURNAL OF APPLIED ELECTROCHEMISTRY
(2023)
Correction
Multidisciplinary Sciences
Adam A. Bradlaugh, Giorgio Fedele, Anna L. Munro, Celia Napier Hansen, John M. Hares, Sanjai Patel, Charalambos P. Kyriacou, Alex R. Jones, Ezio Rosato, Richard A. Baines
Article
Multidisciplinary Sciences
Adam A. Bradlaugh, Giorgio Fedele, Anna L. Munro, Celia Napier Hansen, John M. Hares, Sanjai Patel, Charalambos P. Kyriacou, Alex R. Jones, Ezio Rosato, Richard A. Baines
Summary: Many animals, including fruit flies, use Earth's magnetic field for navigation. A study found that the C-terminal 52 amino acid residues of fruit fly CRY can facilitate magnetoreception, and increasing levels of FAD can enhance this magnetic sensitivity. These results reveal the essential components of a primary magnetoreceptor in fruit flies and suggest that non-canonical radical pairs can elicit magnetic-field responses in cells.
Article
Polymer Science
Joseph J. Dale, Joe Stanley, Romy A. Dop, Gabriela Chronowska-Bojczuk, Alistair J. Fielding, Daniel R. Neill, Tom Hasell
Summary: The build-up of elemental sulfur waste poses problems that require advancements in process and product design as solutions. Inverse vulcanisation, a process for generating high sulfur content polymeric materials, holds promise as a potential solution. However, a complete understanding of the formation of these materials is still lacking in this emerging field. This research investigates the formation mechanisms of 'dark sulfur' in order to further understand inverse vulcanisation. The detriments and benefits of dark sulfur in relation to its application and general usage are also explored.
EUROPEAN POLYMER JOURNAL
(2023)
Article
Multidisciplinary Sciences
Harshwardhan Poddar, Ronald Rios-Santacruz, Derren J. J. Heyes, Muralidharan Shanmugam, Adam Brookfield, Linus O. O. Johannissen, Colin W. W. Levy, Laura N. N. Jeffreys, Shaowei Zhang, Michiyo Sakuma, Jacques-Philippe Colletier, Sam Hay, Giorgio Schiro, Martin Weik, Nigel S. S. Scrutton, David Leys
Summary: This study provides insights into the mechanism of CarH, a photoreceptor involved in transcriptional regulation. The authors show that the response of CarH to light integrates both B-12 photochemistry and redox changes to drive large-scale conformational changes.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Ines S. Camacho, Emma Wall, Igor V. Sazanovich, Emma Gozzard, Mike Towrie, Neil T. Hunt, Sam Hay, Alex R. Jones
Summary: Time-resolved infrared spectroscopy is used to study the flow of electron density through coenzyme B-12 in the light-activated bacterial transcriptional regulator, CarH. The protein stabilizes multiple charge transfer states, resulting in a photoresponse that avoids reactive and potentially damaging radical photoproducts.
CHEMICAL COMMUNICATIONS
(2023)
Correction
Plant Sciences
Derren J. Heyes, Shaowei Zhang, Aoife Taylor, Linus O. Johannissen, Samantha J. O. Hardman, Sam Hay, Nigel S. Scrutton
Summary: A correction to this paper has been published, please refer to the link.
Review
Plant Sciences
Derren J. Heyes, Shaowei Zhang, Aoife Taylor, Linus O. Johannissen, Samantha J. O. Hardman, Sam Hay, Nigel S. Scrutton
Summary: LPOR is a light-activated enzyme essential for chlorophyll biosynthesis and plant greening. It catalyzes the conversion of protochlorophyllide to chlorophyllide, playing a crucial role in early plant development. Through photocatalysis, LPOR acts as a master switch for plant photomorphogenesis, triggering complex molecular and cellular events that lead to plant morphological changes.
