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971.
Yuan Xu Jing Xue Qing Zhou Yongjun Zheng Xinghua Chen Prof. Songqin Liu Prof. Yanfei Shen Prof. Yuanjian Zhang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(34):14606-14611
Emerging as a cost-effective and robust enzyme mimic, nanozymes have drawn increasing attention with broad applications ranging from cancer therapy to biosensing. Developing nanozymes with both accelerated and inhibited biocatalytic properties in a biological context is intriguing to peruse more advanced functions of natural enzymes, but remains challenging, because most nanozymes are lack of enzyme-like molecular structures. By re-visiting and engineering the well-known Fe-N-C electrocatalyst that has a heme-like Fe-Nx active sites, herein, it is reported that Fe-N-C could not only catalyze drug metabolization but also had inhibition behaviors similar to cytochrome P450 (CYP), endowing it a potential replacement of CYP for preliminary evaluation of massive potential chemicals, drug dosing guide, and outcome prediction. In addition, in contrast to electrocatalysts, the highly graphitic framework of Fe-N-C may not be obligatory for a competitive CYP-like activity. 相似文献
972.
Dr. Liwei Zheng Xiaojuan Dai Prof. Hongmei Su Prof. Marc M. Greenberg 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(32):13508-13515
Guanine radicals are important reactive intermediates in DNA damage. Hydroxyl radical (HO.) has long been believed to react with 2′-deoxyguanosine (dG) generating 2′-deoxyguanosin-N1-yl radical (dG(N1-H).) via addition to the nucleobase π-system and subsequent dehydration. This basic tenet was challenged by an alternative mechanism, in which the major reaction of HO. with dG was proposed to involve hydrogen atom abstraction from the N2-amine. The 2′-deoxyguanosin-N2-yl radical (dG(N2-H).) formed was proposed to rapidly tautomerize to dG(N1-H).. We report the first independent generation of dG(N2-H). in high yield via photolysis of 1 . dG(N2-H). is directly observed upon nanosecond laser flash photolysis (LFP) of 1 . The absorption spectrum of dG(N2-H). is corroborated by DFT studies, and anti- and syn-dG(N2-H). are resolved for the first time. The LFP experiments showed no evidence for tautomerization of dG(N2-H). to dG(N1-H). within hundreds of microseconds. This observation suggests that the generation of dG(N1-H). via dG(N2-H). following hydrogen atom abstraction from dG is unlikely to be a major pathway when HO. reacts with dG. 相似文献
973.
Xuan Wei Diao Zheng Ming Zhao Dr. Hongzhong Chen Xun Fan Bin Gao Dr. Long Gu Dr. Yi Guo Dr. Jianbin Qin Prof. Jing Wei Prof. Yanli Zhao Prof. Guangcheng Zhang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(34):14747-14754
Heteroatom-doped polymers or carbon nanospheres have attracted broad research interest. However, rational synthesis of these nanospheres with controllable properties is still a great challenge. Herein, we develop a template-free approach to construct cross-linked polyphosphazene nanospheres with tunable hollow structures. As comonomers, hexachlorocyclotriphosphazene provides N and P atoms, tannic acid can coordinate with metal ions, and the replaceable third comonomer can endow the materials with various properties. After carbonization, N/P-doped mesoporous carbon nanospheres were obtained with small particle size (≈50 nm) and high surface area (411.60 m2 g−1). Structural characterization confirmed uniform dispersion of the single atom transition metal sites (i.e., Co-N2P2) with N and P dual coordination. Electrochemical measurements and theoretical simulations revealed the oxygen reduction reaction performance. This work provides a solution for fabricating diverse heteroatom-containing polymer nanospheres and their derived single metal atom doped carbon catalysts. 相似文献
974.
Dr. Deng Pan Zhengzou Fang Erli Yang Zhenqiang Ning Qing Zhou Kaiyang Chen Yongjun Zheng Prof. Yuanjian Zhang Prof. Yanfei Shen 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(38):16890-16897
The exceptional nature of WO3−x dots has inspired widespread interest, but it is still a significant challenge to synthesize high-quality WO3−x dots without using unstable reactants, expensive equipment, and complex synthetic processes. Herein, the synthesis of ligand-free WO3−x dots is reported that are highly dispersible and rich in oxygen vacancies by a simple but straightforward exfoliation of bulk WS2 and a mild follow-up chemical conversion. Surprisingly, the WO3−x dots emerged as co-reactants for the electrochemiluminescence (ECL) of Ru(bpy)32+ with a comparable ECL efficiency to the well-known Ru(bpy)32+/tripropylamine (TPrA) system. Moreover, compared to TPrA, whose toxicity remains a critical issue of concern, the WO3−x dots were ca. 300-fold less toxic. The potency of WO3−x dots was further explored in the detection of circulating tumor cells (CTCs) with the most competitive limit of detection so far. 相似文献
975.
Dr. Long Jiao Dr. Weijie Yang Dr. Gang Wan Rui Zhang Dr. Xusheng Zheng Dr. Hua Zhou Prof. Dr. Shu-Hong Yu Prof. Dr. Hai-Long Jiang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(46):20770-20776
Single-atom catalysts (SACs) are of great interest because of their ultrahigh activity and selectivity. However, it is difficult to construct model SACs according to a general synthetic method, and therefore, discerning differences in activity of diverse single-atom catalysts is not straightforward. Herein, a general strategy for synthesis of single-atom metals implanted in N-doped carbon (M1-N-C; M=Fe, Co, Ni and Cu) has been developed starting from multivariate metal–organic frameworks (MOFs). The M1-N-C catalysts, featuring identical chemical environments and supports, provided an ideal platform for differentiating the activity of single-atom metal species. When employed in electrocatalytic CO2 reduction, Ni1-N-C exhibited a very high CO Faradaic efficiency (FE) up to 96.8 % that far surpassed Fe1-, Co1- and Cu1-N-C. Remarkably, the best-performer, Ni1-N-C, even demonstrated excellent CO FE at low CO2 pressures, thereby representing a promising opportunity for the direct use of dilute CO2 feedstock. 相似文献
976.
Dr. Ze-Jun Xu Yan Zong Ya-Nan Qiao Jiao-Zhen Zhang Xuyuan Liu Ming-Zhu Zhu Yuliang Xu Hongbo Zheng Liyuan Fang Dr. Xiao-ning Wang Prof. Hong-Xiang Lou 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(45):20091-20095
A divergent synthetic approach to biogenetically related diterpenoids such as ent-kauranes, ent-trachylobanes, ent-beyerane, and ent-atisane has been developed. The unified synthetic route involves the De Mayo reaction to rapidly generate the bicyclo[3.2.1]-octane moiety of ent-kaurane. The key reactions also include bioinspired nucleophilic cyclopropanation generating the [3.2.1.02,7]-tricyclic core of ent-trachylobane and regioselective cyclopropane fragmentation furnishing ent-beyerane and ent-atisane through the nucleophilic attack and protonation of the cyclopropane ring. This strategy enables the asymmetric total syntheses of six diterpenoids from the commercially available geraniol. 相似文献
977.
Ruibing An Xiaoyang Cheng Shixuan Wei Yuxuan Hu Yidan Sun Zheng Huang Prof. Hong-Yuan Chen Prof. Deju Ye 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(46):20817-20825
Stimuli-responsive smart photosensitizer (PS) nanoassemblies that allow enhanced delivery and controlled release of PSs are promising for imaging-guided photodynamic therapy (PDT) of tumors. However, the lack of high-sensitivity and spatial-resolution signals and fast washout of released PSs from tumor tissues have impeded PDT efficacy in vivo. Herein, we report tumor targeting, redox-responsive magnetic and fluorogenic PS nanoassemblies ( NP-RGD ) synthesized via self-assembly of a cRGD- and disulfide-containing fluorogenic and paramagnetic small molecule ( 1-RGD ) for fluorescence/magnetic resonance bimodal imaging-guided tumor PDT. NP-RGD show high r1 relaxivity but quenched fluorescence and PDT activity; disulfide reduction by glutathione (GSH) promotes efficient disassembly into a small-molecule probe ( 2-RGD ) and an organic PS (PPa-SH), which could further bind with intracellular albumin, allowing prolonged retention and cascade activation of fluorescence and PDT to ablate tumors. 相似文献
978.
Dr. Yan-Xia Zhao Dr. Bin Yang Dr. Hai-Fang Li Yan Zhang Yuan Yang Dr. Qing-Yu Liu Dr. Hong-Guang Xu Prof. Wei-Jun Zheng Prof. Sheng-Gui He 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(47):21402-21409
Photoassisted steam reforming and dry (CO2) reforming of methane (SRM and DRM) at room temperature with high syngas selectivity have been achieved in the gas-phase catalysis for the first time. The catalysts used are bimetallic rhodium–vanadium oxide cluster anions of Rh2VO1–3−. Both the oxidation of methane and reduction of H2O/CO2 can take place efficiently in the dark while the pivotal step to govern syngas selectivity is photo-excitation of the reaction intermediates Rh2VO2,3CH2− to specific electronically excited states that can selectively produce CO and H2. Electronic excitation over Rh2VO2,3CH2− to control the syngas selectivity is further confirmed from the comparison with the thermal excitation of Rh2VO2,3CH2−, which leads to diversity of products. The atomic-level mechanism obtained from the well-controlled cluster reactions provides insight into the process of selective syngas production from the photocatalytic SRM and DRM reactions over supported metal oxide catalysts. 相似文献
979.
Dr. Ya-Nan Chen Dr. Miao Li Yunzhi Wang Jing Wang Dr. Ming Zhang Dr. Yuanyuan Zhou Dr. Jianming Yang Dr. Yahui Liu Prof. Feng Liu Prof. Zheng Tang Prof. Qinye Bao Prof. Zhishan Bo 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(50):22903-22909
Fused-ring electron acceptors have made significant progress in recent years, while the development of fully non-fused ring acceptors has been unsatisfactory. Here, two fully non-fused ring acceptors, o-4TBC-2F and m-4TBC-2F, were designed and synthesized. By regulating the location of the hexyloxy chains, o-4TBC-2F formed planar backbones, while m-4TBC-2F displayed a twisted backbone. Additionally, the o-4TBC-2F film showed a markedly red-shifted absorption after thermal annealing, which indicated the formation of J-aggregates. For fabrication of organic solar cells (OSCs), PBDB-T was used as a donor and blended with the two acceptors. The o-4TBC-2F-based blend films displayed higher charge mobilities, lower energy loss and a higher power conversion efficiency (PCE). The optimized devices based on o-4TBC-2F gave a PCE of 10.26 %, which was much higher than those based on m-4TBC-2F at 2.63 %, and it is one of the highest reported PCE values for fully non-fused ring electron acceptors. 相似文献
980.
Yiyi Ou Dr. Weijie Zhou Dr. Zece Zhu Dr. Fengkai Ma Dr. Rongfu Zhou Fang Su Dr. Lirong Zheng Prof. Li Ma Prof. Hongbin Liang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(52):24018-24024
Optical multiplexing based on luminescent materials with tunable color/lifetime has potential applications in information storage and security. However, the available tunable luminescent materials reported so far still suffer from several drawbacks of low efficiency or poor stability, thus restraining their further applications. Herein, we demonstrate a strategy to develop efficient and stable lanthanide coordination polymers (LCPs) with tunable luminescence as a new option for optical multiplexing. Their multicolor emission from green to red and naked-eye-sensitive green emission with tunable lifetime (from ca. 300 to ca. 600 μs) can be controlled by host differential sensitization and energy transfer between lanthanide ions. The quantum efficiencies of developed samples range from around 20 % to 46 % and the luminescence intensity/lifetime appear quite stable in polar solvents up to ten weeks. Furthermore, with the aid of inkjet printing and concepts of luminescence lifetime imaging and time-gated imaging, we illustrate their promising applications of information storage and security in spatial and temporal domains. 相似文献