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Jiyeon Lee Dahye Im Yajie Liu Jing Fang Xibao Tian Minsu Kim Prof. Wen-Bin Zhang Prof. Jongcheol Seo 《Angewandte Chemie (International ed. in English)》2023,62(51):e202314980
A technique combining ion mobility spectrometry-mass spectrometry (IMS-MS) and supercharging electrospray ionization (ESI) has been demonstrated to differentiate protein chemical topology effectively. Incorporating as many charges as possible into proteins via supercharging ESI allows the protein chains to be largely unfolded and stretched, revealing their hidden chemical topology. Different chemical topologies result in differing geometrical sizes of the unfolded proteins due to constraints in torsional rotations in cyclic domains. By introducing new topological indices, such as the chain-length-normalized collision cross-section (CCS) and the maximum charge state (zM) in the extensively unfolded state, we were able to successfully differentiate various protein chemical topologies, including linear chains, ring-containing topologies (lasso, tadpole, multicyclics, etc.), and mechanically interlocked rings, like catenanes. 相似文献
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Dr. Jun Wang Ganghai Ni Dr. Wanru Liao Dr. Kang Liu Jiawei Chen Prof. Fangyang Liu Prof. Zongliang Zhang Prof. Ming Jia Prof. Jie Li Prof. Junwei Fu Dr. Evangelina Pensa Prof. Liangxing Jiang Prof. Zhenfeng Bian Prof. Emiliano Cortés Prof. Min Liu 《Angewandte Chemie (International ed. in English)》2023,62(9):e202217026
Photoelectrochemical (PEC) water splitting is a promising approach for renewable solar light conversion. However, surface Fermi level pinning (FLP), caused by surface trap states, severely restricts the PEC activities. Theoretical calculations indicate subsurface oxygen vacancy (sub-Ov) could release the FLP and retain the active structure. A series of metal oxide semiconductors with sub-Ov were prepared through precisely regulated spin-coating and calcination. Etching X-ray photoelectron spectroscopy (XPS), scanning transmission electron microscopy (STEM), and electron energy loss spectra (EELS) demonstrated Ov located at sub ∼2–5 nm region. Mott–Schottky and open circuit photovoltage results confirmed the surface trap states elimination and Fermi level de-pinning. Thus, superior PEC performances of 5.1, 3.4, and 2.1 mA cm−2 at 1.23 V vs. RHE were achieved on BiVO4, Bi2O3, TiO2 with outstanding stability for 72 h, outperforming most reported works under the identical conditions. 相似文献
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Chang-Xin Zhao Prof. Xinyan Liu Jia-Ning Liu Juan Wang Dr. Xin Wan Dr. Changda Wang Xi-Yao Li Prof. Jianglan Shui Prof. Li Song Prof. Hong-Jie Peng Prof. Bo-Quan Li Prof. Qiang Zhang 《Angewandte Chemie (International ed. in English)》2023,62(48):e202313028
Coordination engineering for single-atom sites has drawn increasing attention, yet its chemical synthesis remains a tough issue, especially for tailorable coordination structures. Herein, a molecular recognition strategy is proposed to fabricate single-atom sites with regulable local coordination structures. Specifically, a heteroatom-containing ligand serves as the guest molecule to induce coordination interaction with the metal-containing host, precisely settling the heteroatoms into the local structure of single-atom sites. As a proof of concept, thiophene is selected as the guest molecule, and sulfur atoms are successfully introduced into the local coordination structure of iron single-atom sites. Ultrahigh oxygen reduction electrocatalytic activity is achieved with a half-wave potential of 0.93 V versus reversible hydrogen electrode. Furthermore, the strategy possesses excellent universality towards diversified types of single-atom sites. This work makes breakthroughs in the fabrication of single-atom sites and affords new opportunities in structural regulation at the atomic level. 相似文献
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Dr. Michael Holtmannspötter Eike Wienbeuker Dr. Timo Dellmann Isabelle Watrinet Prof. Dr. Ana J. Garcia-Sáez Prof. Dr. Kai Johnsson Dr. Rainer Kurre Prof. Dr. Jacob Piehler 《Angewandte Chemie (International ed. in English)》2023,62(18):e202219050
Self-labeling enzymes (SLE) such as the HaloTag have emerged as powerful tools in high and super-resolution fluorescence microscopy. Newly developed fluorogenic SLE substrates enable imaging in the presence of excess dye. To exploit this feature for reversible labeling, we engineered two variants of HaloTag7 with restored dehalogenase activity. Kinetic studies in vitro showed different turnover kinetics for reHaloTagS (≈0.006 s−1) and reHaloTagF (≈0.055 s−1). Imaging by confocal and stimulated emission depletion microscopy yielded 3-5-time enhanced photostability of reHaloTag labeling. Prominently, single molecule imaging with reHaloTags enabled controlled and stable labeling density over extended time periods. By combination with structured illumination, simultaneous visualization of single molecule diffusion and organellar dynamics was achieved. These applications highlight the potential of reHaloTag labeling for pushing the limits of advanced fluorescence microscopy techniques. 相似文献