Angewandte Chemie International Edition

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ISSN / EISSN : 1433-7851 / 1521-3773
Published by: Wiley (10.1002)
Total articles ≅ 74,592
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, Jan Keuter, Alexander Hepp, Constantin G Daniliuc, Milica Feldt
Angewandte Chemie International Edition; doi:10.1002/anie.202104341

Reductive debromination of {N(SiMe3)2}SiBr3 with Rieke magnesium results in the formation of the fix-vertex silicon cluster with one bromine substituent Si5{N(SiMe3)2}5Br 1 and the cyclobutadiene analogue 2 in a 1:1 ratio. The latter features a planar four-membered silicon ring with a charge-separated electronic situation. Two silicon atoms in 2 are trigonal planar and the other two trigonal pyramidal. In cycloadditions with ethylene, diethylacetylene, 1,5-cyclooctadiene and 2,3-dimethyl-1,3-butadiene cyclic unsaturated ring compounds (3-6) were formed at room temperature in quantitative reactions. Two of the products (3 and 6) show photochemical isomerization with LED light (λ = 405 nm) to afford saturated ring compounds 4e and 6’.
Ji Bian, Ziqing Zhang, Jiannan Feng, Madasamy Thangamuthu, Fan Yang, Ling Sun, Zhijun Li, Yang Qu, Dongyan Tang, Zewei Lin, et al.
Angewandte Chemie International Edition; doi:10.1002/anie.202106929

A universal strategy is developed to construct a cascade Z-scheme system, in which an effective energy platform is a core to direct charge transfer and separation, blocking the unexpected type-II charge transfer pathway. The dimension-matched (001)TiO 2 -g-C 3 N 4 /BiVO 4 nanosheet heterojunction (T-CN/BVNS) is the first such model. The optimized cascade Z-scheme exhibits ~19-fold photoactivity improvement for CO 2 reduction to CO in the absence of cocatalysts and costly sacrificial agents under visible-light irradiation, compared with BVNS, which is also superior to other reported Z-scheme systems even with noble metals as mediators. The experimental results and DFT calculations based on Van der Waals structural models on the ultrafast timescale reveal the introduced T as the platform could not only prolong the lifetimes of spatially separated electrons and holes but also did not compromise their reduction and oxidation potentials.
Andrew Tarzia, , Kim E Jelfs
Angewandte Chemie International Edition; doi:10.1002/anie.202106721

The use of unsymmetrical components in metallo-supramolecular chemistry allows for low- symmetry architectures with anisotropic cavities toward guest-binding with high specificity and affinity. Unsymmetrical ditopic ligands mixed with Pd(II) have the potential to self-assemble into reduced symmetry Pd 2 L 4 metallo-architectures. Mixtures of isomers can form, however, resulting in potentially undesirable heterogeneity within a system. Therefore it is paramount to be able to design components that preferentially form a single isomer. Previous data suggested that computational methods could predict with reasonable accuracy whether unsymmetrical ligands would preferentially self-assemble into a single isomer under constraints of geometrical mismatch. We successfully apply a collaborative computational and experimental workflow to mitigate costly trial-and-error synthetic approaches. Our low-cost computational workflow rapidly constructs new unsymmetrical ligands (and Pd 2 L 4 cage isomers) and ranks their likelihood for forming cis -Pd 2 L 4 assemblies. From this narrowed search space, we successfully synthesised four new low-symmetry, cis -Pd 2 L 4 cages, with cavities of different shapes and sizes.
Tongzhou Wang, Xuejie Cao, Hongye Qin, Long Shang, Siyu Zheng, Fang Fang, Lifang Jiao
Angewandte Chemie International Edition; doi:10.1002/anie.202108599

Main-group ( s - and p -block) metals are generally regarded as catalytically inactive due to the delocalized s / p -band. Herein, we successfully synthesized a p -block antimony single-atom catalyst (Sb SAC) with the Sb-N 4 configuration for efficient catalysis of the oxygen reduction reaction (ORR). The resulting Sb SAC exhibits superior ORR activity with a half-wave potential of 0.86 V and excellent stability, which outperforms many transition-metal (TM, d -block) based SACs and commercial Pt/C. In addition, it presents an excellent power density of 184.6 mW cm -2 and a high specific capacity (803.5 mAh g -1 ) in Zn-air battery. Both experiment and theoretical calculation manifest that the active catalytic sites are positively charged Sb-N 4 single-metal sites, which have closed d shells. Density of states (DOS) results unveil the p orbital of the atomically dispersed Sb cation in Sb SAC can easily interact with O 2 - p orbital to form hybrid states, facilitating the charge transfer and generating appropriate adsorption strength for oxygen intermediates, lowering the energy barrier and modulating the rate-determining step. This work sheds light on the atomic-level preparing p -block Sb metal catalyst for highly active ORR, and further provides valuable guidelines for the rational design of other main-group-metal SACs.
Jing‐Jing Tang, , Yi Wang, Yoshinori Yamamoto,
Angewandte Chemie International Edition, Volume 60; doi:10.1002/anie.202183062

C−H Activation In their Research Article on page 16426, Xiaoqiang Yu, Ming Bao et al. report visible-light-driven iron-catalyzed nitrene transfer reactions with dioxazolones for intermolecular C(sp3)−N, N=S and N=P bond formation.
Takahiro Iwata, Hisaaki Hirose, Kentarou Sakamoto, Yusuke Hirai, Jan Vincent V. Arafiles, Misao Akishiba, Miki Imanishi,
Angewandte Chemie International Edition; doi:10.1002/anie.202108473

Large amounts of antibodies can be rapidly delivered into cells from coacervates (lipid droplet) formed by mixing a fluorescently labeled antibody and a delivery peptide, as reported by Shiroh Futaki and co-workers in their Research Article (DOI: 10.1002/anie.202105527). The mode of delivery is a mysterious phenomenon, which is accompanied by the structural changes of the cell membranes like a drop of ink on the surface of water. The cover illustration shows a representation of the intracellular delivery of antibodies by coacervate. This research has realized the first intracellular delivery of antibodies using liquid–liquid phase separation.
Jie Li, Jiaming Wang, Qingqing Li, Mengxi Zhang, Jiani Li, Chao Sun, Shuai Yuan, , Dr. Bo Wang
Angewandte Chemie International Edition; doi:10.1002/anie.202108418

Self-healing gas separation membranes based on coordination polymers (CPs) are reported by Xiao Feng, Bo Wang et al. in their Research Article (DOI: 10.1002/anie.202102047). The low viscosity in the molten state and the low vitrification temperature equips the CPs with good processability and self-healing properties. Thin glass membranes can be prepared by hot-pressing or hot-casting methods, and they exhibit excellent molecular size-exclusive effect for gas separation.
, Yuki Kataoka, Momoko Hirata, Yuki Akinaga, Ryo Takahata, Kosuke Wakamatsu, Yu Fujiki, Miori Kataoka, Soichi Kikkawa, Abdulrahman S. Alotabi, et al.
Angewandte Chemie International Edition; doi:10.1002/anie.202108478

A ligand-desorption process during calcination was followed for metal-oxide-supported 2-phenylethanethiolate-protected gold (Au) 25-atom metal nanoclusters (NCs) using five experimental techniques by Yuichi Negishi and co-workers in their Research Article (DOI: 10.1002/anie.202104911). Based on the obtained knowledge, a method to form a metal-oxide layer on the surface of Au NCs while preventing their aggregation was established and thereby creation of a water-splitting photocatalyst with high activity and stability was achieved.
Jinhui Hao, Wei Luo, Shuaishuai Wang, Kun Zhao, Jianwen Hou, Longhua Li, Baoxin Ge, Wenshu Yang, Weidong Shi
Angewandte Chemie International Edition; doi:10.1002/anie.202108770

The fundamental understanding of the surface reconstruction induced by the applied potential is of great significance for enhancing the oxygen evolution reaction (OER). Here, we show that a previously overlooked discharge current in the low applied potential region also leads to in situ electrochemical activation of a nitrogen-doped nickel oxyhydroxide surface. We exploit the fact that doping of heteroatoms weakens the surface structure, and hence, a weak discharge current originating from the capacitive nature of nickel oxyhydroxide has a strong structure-reforming ability to promote the formation of nitrogen and oxygen vacancies. The current density at 1.4 V (vs. Hg/HgO) can dramatically increase by as much as 31.3% after discharge in the low applied potential region. This work provides insight into in situ enhancement of the OER and suggests that the low applied potential region must be a primary consideration in evaluating the origin of the activity of electrocatalysts.
, Yuming Jiang, Jie Sun, Caiqiao Xiong, Huihui Liu, Yuze Li, Xiao Wang
Angewandte Chemie International Edition; doi:10.1002/anie.202103874

The inhalation of atmospheric particles is toxicological to human health. However, as a complex mixture, tracing the behaviors of multiple components from real aerosol particles is crucial but unachievable by the existing methods. Here, taking advantage of the intrinsic fingerprints of elemental carbon (EC) and organic carbon (OC) in carbonaceous aerosol (CA) upon laser irradiation, we proposed a label-free mass spectrometry imaging method to visualize and quantify the deposition, translocation and component variation of CA in organs. With this method, the heterogeneous deposition, clearance and release behavior of CA in lung, that more OC was released in parenchyma and OC was cleared faster than EC, was observed. The translocation of CA to extrapulmonary organs including kidney, liver, spleen and even brain was also verified and quantified. By comparing the ratio of OC to EC, an organ-specific release behavior of OC from CA during circulation was revealed. In orthotopic lung and liver tumor, OC was found to penetrate more into tumor foci than EC. This technique provides deeper information for understanding the systemic health effects of aerosol particles.
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