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881.
Tianyong Liu Qian Dang Xunhui Zhou Jin Li Zhen Ge Hang Che Prof. Shaobin Tang Prof. Yi Luo Prof. Jun Jiang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(23):6945-6953
Developing the low-cost and efficient single-atom catalysts (SACs) for nitrogen reduction reaction (NRR) is of great importance while remains as a great challenge. The catalytic activity, selectivity and durability are all fundamentally related to the elaborate coordination environment of SACs. Using first-principles calculations, we investigated the SACs with single transition metal (TM) atom supported on defective boron carbide nitride nanotubes (BCNTs) as NRR electrocatalysts. Our results suggest that boron-vacancy defects on BCNTs can strongly immobilize TM atoms with large enough binding energy and high thermal/structural stability. Importantly, the synergistic effect of boron nitride (BN) and carbon domains comes up with the modifications of the charge polarization of single-TM-atom active site and the electronic properties of material, which has been proven to be the essential key to promote N2 adsorption, activation, and reduction. Specifically, six SACs (namely V, Mn, Fe, Mo, Ru, and W atoms embedded into defective BCNTs) can be used as promising candidates for NRR electrocatalysts as their NRR activity is higher than the state-of-the art Ru(0001) catalyst. In particular, single Mo atom supported on defective BCNTs with large tube diameter possesses the highest NRR activity while suppressing the competitive hydrogen evolution reaction, with a low limiting potential of −0.62 V via associative distal path. This work suggests new opportunities for driving NH3 production by carbon-based single-atom electrocatalysts under ambient conditions. 相似文献
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Dr. Benoit Colasson Dr. Thomas Devic Dr. Joël Gaubicher Dr. Charlotte Martineau-Corcos Prof. Philippe Poizot Dr. Vincent Sarou-Kanian 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(37):9589-9596
The synthesis and characterization of a polyrotaxanated covalent organic network (CON) based on the association between the viologen and pillar[5]arene (P[5]OH) units are reported. The mechanical bond allows for the irreversible insertion of n-type redox centers (P[5]OH macrocycles) within a pristine structure based on p-type viologen redox centers. Both redox units are active on a narrow potential range and, in water, the presence of P[5]OH greatly increases the electroactivity of the material. 相似文献
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Katherine M. Byrd Chitra Subramanian Jacqueline Sanchez Hashim F. Motiwala Weiya Liu Prof. Mark S. Cohen Prof. Jeffrey Holzbeierlein Prof. Brian S. J. Blagg 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(20):6921-6931
Development of heat shock protein 90 (Hsp90) C‐terminal inhibitors has emerged as an exciting strategy for the treatment of cancer. Previous efforts have focused on modifications to the natural products novobiocin and coumermycin. Moreover, variations in both the sugar and amide moieties have been extensively studied, whereas replacements for the coumarin core have received less attention. Herein, 24 cores were synthesized with varying distances and angles between the sugar and amide moieties. Compounds that exhibited good anti‐proliferative activity against multiple cancer cell lines and Hsp90 inhibitory activity, were those that placed the sugar and amide moieties between 7.7 and 12.1 Å apart along with angles of 180°. 相似文献
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Prof. Dr. Axel Schulz Dr. Alexander Villinger 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(6):2032-2038
Pure, solvent‐free Zn(N3)2 was prepared by reaction of diethyl zinc and hydrazoic acid in aprotic solvents. The single‐crystal structure determination, along with the comprehensive characterization of α‐Zn(N3)2 and two metastable polymorphs, could be achieved for the first time. Since these data disagree in large parts with the known, previously reported values, all previous syntheses of Zn(N3)2, and for comparison Zn(N3)2?2.5 H2O and Zn(OH)N3 were reinvestigated, indicating that some of the earlier work has to be revised. 相似文献