Article
Electrochemistry
Alina I. Inozemtseva, Artem V. Sergeev, Kirill S. Napolskii, Sergey E. Kushnir, Vladislav Belov, Daniil M. Itkis, Dmitry Yu. Usachov, Lada V. Yashina
Summary: Graphene materials offer new perspectives to electrochemical systems with high electron transfer rates and stability, but the electron transfer regime on graphene plays a critical role in its electrochemical activity. Different electron transfer regimes result in varied structure-activity relationships.
ELECTROCHIMICA ACTA
(2022)
Article
Multidisciplinary Sciences
Guang Yuan Zhu, Yi Qin, Miao Meng, Suman Mallick, Hang Gao, Xiaoli Chen, Tao Cheng, Ying Ning Tan, Xuan Xiao, Mei Juan Han, Mei Fang Sun, Chun Y. Liu
Summary: The Landau-Zener formula, a semiclassical model for nonadiabatic transitions, is shown to be valid in a broader range of conditions approaching the adiabatic regime than previously expected, as demonstrated by investigating electron transfer reactions in a series of mixed-valence complexes.
NATURE COMMUNICATIONS
(2021)
Article
Electrochemistry
Marko M. Melander
Summary: Electrochemical reactions should occur in a frozen and out of equilibrium environment, but this clashes with most theoretical and simulation approaches. Non-ergodic rate theory re-analyzes these claims and finds that in most activated electrochemical reactions, the reaction environment is completely mobile and equilibrated under constant potential conditions.
ELECTROCHIMICA ACTA
(2023)
Review
Chemistry, Multidisciplinary
Pauline J. Ollitrault, Alexander Miessen, Ivano Tavernelli
Summary: Simulating molecular dynamics within a comprehensive quantum framework is a challenge due to exponential scaling of computational cost. The Born-Oppenheimer and non-adiabatic dynamics are important for handling electron-nuclear couplings, and quantum algorithms show promise in reducing the computational complexity.
ACCOUNTS OF CHEMICAL RESEARCH
(2021)
Article
Chemistry, Physical
Thomas P. Fay
Summary: This study investigates the impact of chirality on spin during electron transfer, finding that chirality combined with spin-orbit coupling does not lead to spin polarization, but instead generates quantum coherence between spin states.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Multidisciplinary Sciences
Sindhana Pannir-Sivajothi, Jorge A. Campos-Gonzalez-Angulo, Luis A. Martinez-Martinez, Shubham Sinha, Joel Yuen-Zhou
Summary: The study focuses on molecules exhibiting laser-like phenomena at room temperature and investigates the impact of vibrational polariton condensate on chemical reactivity. It demonstrates the potential of using condensates to drive chemical reactions by bypassing the constraints of fast intramolecular vibrational redistribution typically seen in condensed phase environments.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Yaojie Lei, Can Wu, Xinxin Lu, Weibo Hua, Shaobo Li, Yaru Liang, Hanwen Liu, Wei-Hong Lai, Qinfeng Gu, Xiaolan Cai, Nana Wang, Yun-Xiao Wang, Shu-Lei Chou, Hua-Kun Liu, Guoxiu Wang, Shi-Xue Dou
Summary: It is crucial to regulate S activity dynamically for efficient and stable room-temperature sodium-sulfur (RT/Na-S) batteries. In this study, cobalt sulfide is used as an electron reservoir to enhance the activity of sulfur cathodes, and cobalt single atoms serve as double-end binding sites for stable S conversion. The rational construction of CoS2 electron reservoir enables the direct reduction of S to short-chain sodium polysulfides (Na2S4) through a streamlined redox path. Cobalt single atoms synergistically work with the electron reservoir to reinforce the streamlined redox path, immobilize in situ formed long-chain products, and catalyze their conversion, leading to high S utilization and sustainable cycling stability. The developed sulfur cathodes exhibit superior rate performance and high cycling capacity retention.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Physical
Neeraj Bangruwa, Mayra Suryansh, Mayra Peralta, Rafael Gutierrez, Gianaurelio Cuniberti, Debabrata Mishra
Summary: In this study, we investigate the sequence-dependent chiral-induced spin selectivity (CISS) in double-stranded DNA. By using time-correlated single-photon counting and electrochemical impedance spectroscopy, we find that the average lifetime of photo-excited electrons is influenced by the CISS effect generated by the DNA molecule. The observed experimental trends are supported by simulations using a tight binding method.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Multidisciplinary Sciences
Huixue Li, Lingling Lv, Kun Yuan, Sujuan Pan, Zhifeng Li
Summary: We conducted a theoretical investigation on how the molecular stacking effect affects the photophysical properties in solid phases. Our findings revealed that the aggregation of molecules led to the suppression of certain vibrations, resulting in restricted intramolecular motions and enhanced emission. Additionally, we explored the influence of charge transfer and confirmed its negligible impact on the process.
SCIENTIFIC REPORTS
(2023)
Article
Chemistry, Multidisciplinary
Yonatan Dubi
Summary: In this study, a theoretical model for the CISS effect in bio-molecular junctions is proposed, which explains the origin of the CISS effect and allows for quantitative analysis of experimental data. This is of great significance for a deeper understanding in the field of molecular electronics and nano-scale transport.
Article
Chemistry, Multidisciplinary
Fantao Kong, Xiangzhi Cui, Yifan Huang, Heliang Yao, Yafeng Chen, Han Tian, Ge Meng, Chang Chen, Ziwei Chang, Jianlin Shi
Summary: N-doped carbon materials with trace amounts of iron show excellent ORR activity and durability without significant contribution by the metal sites. The materials have a unique hollow and hierarchically porous architecture, as well as a noncovalently bonded N-deficient/N-rich heterostructure.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Physical
Sergei Tcyrulnikov, Qiuqi Cai, J. Cameron Twitty, Jianyu Xu, Abderrahman Atifi, Olivia P. Bercher, Glenn P. A. Yap, Joel Rosenthal, Mary P. Watson, Marisa C. Kozlowski
Summary: This study explores the steric and electronic effects of substituents on the canonical steps and overall process of deaminative functionalization reactions using alkyl amines as alkyl radical precursors. The research shows that while electronic effects on these steps oppose each other, steric effects are synergistic, with larger substituents favoring both reduction and radical dissociation steps. This understanding provides a framework for future design of pyridinium salts for specific catalysis or activation modes.
Article
Chemistry, Multidisciplinary
Luca D'Amario, Maria Bruna Stella, Tomas Edvinsson, Maurizio Persico, Johannes Messinger, Holger Dau
Summary: This study describes a transient spectro-electrochemical Raman setup that achieves sub-ms time resolution, allowing for the study of electrochemical processes. The technique was validated through experiments and confirmed to be effective in assigning spectral properties to transient species. This research provides a foundational contribution to the development of next generation electrolizers, fuel cells, and batteries.
Article
Multidisciplinary Sciences
Simon Bo Jensen, Sara Thodberg, Shaheena Parween, Matias E. Moses, Cecilie C. Hansen, Johannes Thomsen, Magnus B. Sletfjerding, Camilla Knudsen, Rita Del Giudice, Philip M. Lund, Patricia R. Castano, Yanet G. Bustamante, Maria Natalia Rojas Velazquez, Flemming Steen Jorgensen, Amit Pandey, Tomas Laursen, Birger Lindberg Moller, Nikos S. Hatzakis
Summary: This study identifies ligands that bind to P450 oxidoreductase (POR) and bias its specificity towards cytochromes P450 (CYP) redox partners, activating distinct metabolic cascades in cells. Single molecule FRET studies reveal that ligand binding alters the conformational sampling of POR, leading to biased activation of metabolic pathways in whole cells. This biased metabolism model may hold potential for designing pathway-specific therapeutics or personalized food to suppress unwanted, disease-related metabolic pathways.
NATURE COMMUNICATIONS
(2021)
Article
Chemistry, Multidisciplinary
Bruno Cesar da Silva, Zahra Sadre Momtaz, Eva Monroy, Hanako Okuno, Jean-Luc Rouviere, David Cooper, Martien Ilse Den Hertog
Summary: A key issue in the development of high-performance semiconductor devices is the ability to accurately measure active dopants at the nanometer scale. This study used in situ biased four-dimensional scanning transmission electron microscopy to investigate a highly doped silicon p-n specimen. The results showed that the measured junction parameters were consistent with a linearly graded junction and demonstrated that in situ biased 4D-STEM can provide a better understanding of the electrostatics of semiconductor p-n junctions at the nanometer scale.