Article
Chemistry, Inorganic & Nuclear
Muhamed Amin, Divya Kaur, M. R. Gunner, Gary Brudvig
Summary: Understanding the water oxidation mechanism in Photosystem II can stimulate the design of biomimetic artificial systems for efficient conversion of solar energy into hydrogen fuel. The activity of Sr2+-substituted PSII is higher but slower compared to native Ca2+-containing PSII as an oxygen evolving catalyst. DFT calculations show that deprotonation of water bound to Ca2+ is more energetically favorable for the S-2 to S-3 transition than for Sr2+. Additionally, calculations reveal a higher pK(a) in the Mn4O5Sr2+ cluster compared to Mn4O5Ca2+ by 4 pH units.
INORGANIC CHEMISTRY COMMUNICATIONS
(2021)
Article
Chemistry, Inorganic & Nuclear
Angela A. Shiau, Heui Beom Lee, Paul H. Oyala, Theodor Agapie
Summary: This article reports the synthesis and characterization of a stable (Mn4O4)-O-IV cuboidal complex supported by a disiloxide ligand. The substitution of an anionic acetate or amidate ligand with a dianionic disiloxide ligand improves the stability and shifts the reduction potential of the complex.
INORGANIC CHEMISTRY
(2022)
Article
Multidisciplinary Sciences
Abhishek Saini, Chandan Das, Surabhi Rai, Aritra Guha, Dependu Dolui, Piyali Majumder, Arnab Dutta
Summary: This study investigates the importance of the O-2/H2O redox couple in renewable energy conversion and introduces a functional mimic compound that exhibits catalytic activity for bidirectional oxygen reduction and oxygen evolution. The compound shows high catalytic activity in neutral water and can perform both oxygen reduction and oxygen evolution under photocatalytic conditions.
Article
Biochemistry & Molecular Biology
Bernard Baituti, Sebusi Odisitse
Summary: The S-2 state in the oxygen-evolving complex of photosystem II produces two basic electron paramagnetic resonance signal types, with a focus on determining the spin states of the g4.1 signal at X-band frequencies. The multiline signal arises from a spin 1/2 center, while the g4.1 signal is proposed to originate from a spin 5/2 center with rhombic distortion. The experimental data support the g4.1 signal as originating from a near rhombic spin 5/2 of the S-2 state of the PSII manganese cluster.
Article
Energy & Fuels
Lei Zhang, Rui Sun, Zhuozhi Wang, Wenkun Zhu, Xingyi Wang, Hongliang Qi
Summary: This study investigated the emission characteristics and formation mechanisms of NH3 during the pulverized coal combustion process. Experimental results showed that H2O accelerated the conversion of HCN to NH3. The Density Functional Theory calculations revealed the formation mechanism of NH3 through the conversion of HCN and hydrogenation of coal-N. This study provides important insights into NH3 emissions and their control during coal combustion.
Article
Chemistry, Multidisciplinary
Angela A. Shiau, Heui Beom Lee, Paul H. Oyala, Theodor Agapie
Summary: This study reports the synthesis, crystal structure, electrochemistry, SQUID magnetometry, and EPR spectroscopy of a (MnMnIV)-Mn-III O-3(4) cuboidal complex featuring five-coordinate Mn-III. The cluster displays a spin ground state of S = 5/2, while conversion to a six-coordinate Mn upon treatment with water results in a spin state change to S = 1/2. These results demonstrate that coordination number has a substantial effect on spectroscopy, even without dramatic changes within the Mn4O4 core.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Multidisciplinary Sciences
Rana Hussein, Mohamed Ibrahim, Asmit Bhowmick, Philipp S. Simon, Ruchira Chatterjee, Louise Lassalle, Margaret Doyle, Isabel Bogacz, In-Sik Kim, Mun Hon Cheah, Sheraz Gul, Casper de Lichtenberg, Petko Chernev, Cindy C. Pham, Iris D. Young, Sergio Carbajo, Franklin D. Fuller, Roberto Alonso-Mori, Alex Batyuk, Kyle D. Sutherlin, Aaron S. Brewster, Robert Bolotovsky, Derek Mendez, James M. Holton, Nigel W. Moriarty, Paul D. Adams, Uwe Bergmann, Nicholas K. Sauter, Holger Dobbek, Johannes Messinger, Athina Zouni, Jan Kern, Vittal K. Yachandra, Junko Yano
Summary: The process of light-driven oxidation of water to molecular oxygen catalyzed by the oxygen-evolving complex (OEC) in Photosystem II (PS II) involves the transport of water molecules and protons. High-resolution structures and data of various time points reveal potential pathways for substrate water insertion and proton release, indicating the O1 channel as the likely water intake pathway and the Cl1 channel as the likely proton release pathway.
NATURE COMMUNICATIONS
(2021)
Article
Engineering, Chemical
Wenyue Dou, Xianjia Peng, Linghao Kong, Xingyun Hu
Summary: An improved approach of decomplexation, neutralization, and precipitation by NH3·H2O coupling with oxidation by O-2 was explored for the removal of Cu(II) and Cu(I) from acidic copper etching wastewater. The study found that Cu was effectively removed in the form of Cu-2(OH)(3)Cl precipitates under specific treatment conditions.
SEPARATION AND PURIFICATION TECHNOLOGY
(2022)
Article
Chemistry, Multidisciplinary
Bing Zhang, Xiaogang Wang, Yang Yang, Bin Hu, Lei Tong, Ying Liu, Li Zhao, Qiang Lu
Summary: This study established adsorption complexes of H2O, NH3, and O-2 on the Cs2Pb-(SCN)(2)Br-2 surface through quantum dynamics simulations, exploring the stability of perovskite structures in different atmospheres and the impact of geometric structure changes on charge transfer. The research provides insights for developing innovative perovskite sensing materials and constructing reasonable sensing mechanisms.
Article
Chemistry, Physical
Kizashi Yamaguchi, Koichi Miyagawa, Mitsuo Shoji, Hiroshi Isobe, Takashi Kawakami
Summary: A multiple S-3 intermediates model for water oxidation in the oxygen evolving complex of photosystem II is examined based on key intermediates elucidated by calculations. The results suggest that the Mn-Hydroxide configuration plays a major role in the S3 state, while Mn-Oxyl has only a partial contribution. The oxyl-radical character is significantly reduced by the coordination of the Ca ion.
CHEMICAL PHYSICS LETTERS
(2022)
Article
Plant Sciences
Khetpakorn Chakarawet, Richard J. J. Debus, R. David Britt
Summary: The D1-D170 residue plays a crucial role in linking Mn ions with the Ca ion in the Mn4CaO5 cluster of Photosystem II. However, the D1-D170E mutation alters the equilibrium between different Jahn-Teller conformers of the S-1 state and leads to the production of a high-spin form of the S-2 state instead of the low-spin form observed in the wild-type. EPR spectroscopy confirms that the D1-D170E mutant produces a high-spin form of the S-2 state, providing experimental evidence for the change in S state conformers.
PHOTOSYNTHESIS RESEARCH
(2023)
Article
Chemistry, Physical
Hiroshi Isobe, Mitsuo Shoji, Takayoshi Suzuki, Jian-Ren Shen, Kizashi Yamaguchi
Summary: In photosystem II, water is oxidized to dioxygen through a Mn4CaO5 cluster, with two competing reaction routes, stepwise and concerted, affecting the formation of the final stable closed structure.
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
(2021)
Article
Chemistry, Multidisciplinary
Manas Ranjan Dash, Mohamad Akbar Ali
Summary: This study investigates the effect of ammonia and water on the gas-phase formation of methanimine from the reaction between aminomethyl radical and oxygen. The results show that the introduction of water significantly increases the formation of methanimine. The rate coefficients for the reactions involving ammonia and water are much smaller compared to the reaction without them.
FRONTIERS IN CHEMISTRY
(2023)
Article
Chemistry, Inorganic & Nuclear
Emma N. Cook, Shelby L. Hooe, Diane A. Dickie, Charles W. Machan
Summary: A new terpyridine-based FeN3O catalyst, Fe-(tpy(tbu)pho)Cl-2, is reported for reducing O2 to H2O. Mechanistic studies suggest a 2 + 2 mechanism with hydrogen peroxide produced as an intermediate in the reduction process.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Segun V. Obisesan, Cayla Rose, Byron H. Farnum, Christian R. Goldsmith
Summary: A Co(II) complex with the polydentate quinol-containing ligand H2qp1 acts as an efficient electrocatalyst for oxygen reduction. It selectively produces H2O without any additional electron-proton transfer mediators, whereas a related complex that substitutes a phenol for the quinol instead produces mostly H2O2 under the same conditions.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Cardiac & Cardiovascular Systems
Jan R. Kraehling, Zhengrong Hao, Monica Y. Lee, David J. Vinyard, Heino Velazquez, Xinran Liu, Radu V. Stan, Gary W. Brudvig, William C. Sessa
CIRCULATION RESEARCH
(2016)
Article
Plant Sciences
David J. Vinyard, Jennifer S. Sun, Javier Gimpel, Gennady M. Ananyev, Stephen P. Mayfield, G. Charles Dismukes
PHOTOSYNTHESIS RESEARCH
(2016)
Article
Biochemistry & Molecular Biology
David J. Vinyard, Mikhail Askerka, Richard J. Debus, Victor S. Batista, Gary W. Brudvig
Article
Chemistry, Inorganic & Nuclear
Dania L. Huang, David J. Vinyard, James D. Blakemore, Sara M. Hashmi, Robert H. Crabtree
Article
Chemistry, Physical
David J. Vinyard, Sahr Khan, Mikhail Askerka, Victor S. Batista, Gary W. Brudvig
JOURNAL OF PHYSICAL CHEMISTRY B
(2017)
Article
Chemistry, Multidisciplinary
Jennifer L. Peper, David J. Vinyard, Gary W. Brudvig, James M. Mayer
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2017)
Article
Chemistry, Multidisciplinary
Megan Mohadjer Beromi, Ainara Nova, David Balcells, Ann M. Brasacchio, Gary W. Brudvig, Louise M. Guard, Nilay Hazari, David J. Vinyard
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2017)
Article
Chemistry, Multidisciplinary
Dimitar Y. Shopov, Benjamin Rudshteyn, Jesus Campos, David J. Vinyard, Victor S. Batista, Gary W. Brudvig, Robert H. Crabtree
Article
Hematology
Monica Y. Lee, Ana Gamez-Mendez, Jiasheng Zhang, Zhenwu Zhuang, David J. Vinyard, Jan Kraehling, Heino Velazquez, Gary W. Brudvig, Themis R. Kyriakides, Michael Simons, William C. Sessa
ARTERIOSCLEROSIS THROMBOSIS AND VASCULAR BIOLOGY
(2018)
Article
Multidisciplinary Sciences
Ananya Mukherjee, Chun Sing Lau, Charlotte E. Walker, Ashwani K. Rai, Camille I. Prejean, Gary Yates, Thomas Emrich-Mills, Spencer G. Lemoine, David J. Vinyard, Luke C. M. Mackinder, James V. Moroney
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2019)
Article
Multidisciplinary Sciences
David J. Vinyard, Syed Lal Badshah, M. Rita Riggio, Divya Kaur, Annaliesa R. Fanguy, M. R. Gunner
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2019)
Article
Multidisciplinary Sciences
Drew M. Hood, Ryan A. Johnson, Alex E. Carpenter, Jarod M. Younker, David J. Vinyard, George G. Stanley
Article
Biochemistry & Molecular Biology
Christopher J. Gisriel, Gaozhong Shen, Ming-Yang Ho, Vasily Kurashov, David A. Flesher, Jimin Wang, William H. Armstrong, John H. Golbeck, Marilyn R. Gunner, David J. Vinyard, Richard J. Debus, Gary W. Brudvig, Donald A. Bryant
Summary: Far-red light photoacclimation expands the range of photosynthetically active radiation for terrestrial cyanobacteria, providing a growth advantage. This process modifies the structure of photosystem II and lowers the energy required for water oxidation.
JOURNAL OF BIOLOGICAL CHEMISTRY
(2022)
Article
Plant Sciences
Brandon P. Russell, David J. Vinyard
Summary: The study found that the first Mn2+ oxidation event in the assembly of the oxygen-evolving complex in Photosystem II requires chloride-facilitated deprotonation. This process is dependent on the presence of calcium at physiologically relevant pH values.
PHOTOSYNTHESIS RESEARCH
(2022)
Article
Plant Sciences
David J. Vinyard
Summary: Unlike laboratory conditions, real environments have dynamic light intensity. Researchers have developed a simple and affordable system that uses a commercial dimmable LED panel to simulate a sinusoidal function representing daylight hours and includes stochastic shading events. The system closely replicates light intensity measurements on Earth's surface during partly cloudy days or in lower levels of plant canopies. This tool may be valuable for researchers studying photosynthetic acclimation responses.
PHOTOSYNTHESIS RESEARCH
(2023)