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941.
Dr. Shan Sun Qiao Chen Zhongdi Tang Chuang Liu Prof. Zhongjun Li Prof. Aiguo Wu Prof. Hengwei Lin 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(47):21227-21234
A method is developed to fabricate tumor microenvironment (TME) stimuli-responsive nanoplatform for fluorescence (FL) imaging and synergistic cancer therapy via assembling photosensitizer (chlorine e6, Ce6) modified carbon dots (CDs-Ce6) and Cu2+. The as-obtained nanoassemblies (named Cu/CC nanoparticles, NPs) exhibit quenched FL and photosensitization due to the aggregation of CDs-Ce6. Their FL imaging and photodynamic therapy (PDT) functions are recovered efficiently once they entering tumor sites by the stimulation of TME. Introducing of Cu2+ not only provides extra chemodynamic therapy (CDT) function through reaction with hydrogen peroxide (H2O2), but also depletes GSH in tumors by a redox reaction, thus amplifying the intracellular oxidative stress and enhancing the efficacy of reactive oxygen species (ROS) based therapy. Cu/CC NPs can act as a FL imaging guided trimodal synergistic cancer treatment agent by photothermal therapy (PTT), PDT, and thermally amplified CDT. 相似文献
942.
Xiangfeng Luan Dr. Cristina Martín Pengfei Zhang Qian Li Dr. Isabella Anna Vacchi Prof. Lucia Gemma Delogu Prof. Yiyong Mai Dr. Alberto Bianco 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(42):18673-18679
As an emerging member of the graphene family, structurally defined graphene nanoribbons (GNRs) have shown promising applications in various fields. The evaluation of the degradability of GNRs is particularly important for assessing the persistence level and risk of these materials in living organisms and the environment. However, there is a void in the study of the degradation of GNRs. Here, we report the degradation behavior of GNRs in the presence of human myeloperoxidase (hMPO) or treated with the photo-Fenton (PF) reaction. With the assistance of potassium hydroxide or imidazole, which facilitates the dispersion of GNRs in the aqueous solution, GNRs underwent only partial degradation after 25-hour incubation with hMPO, while, the PF reaction degraded GNRs almost completely after 120 hours. These results indicate that structurally precise GNRs can be efficiently degraded under suitable conditions, providing more opportunities for future applications in different fields. 相似文献
943.
Dr. Jiong Wang Dr. Xiang Huang Dr. Shibo Xi Prof. Dr. Hu Xu Prof. Dr. Xin Wang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(43):19324-19329
Efficient electron communication between molecular catalyst and support is critical for heterogeneous molecular electrocatalysis and yet it is often overlooked during the catalyst design. Taking CO2 electro-reduction on tetraphenylporphyrin cobalt (PCo) immobilized onto graphene as an example, we demonstrate that adding a relay molecule improves the interfacial electron communication. While the directly immobilized PCo on graphene exhibits relatively poor electron communications, it is found that diphenyl sulfide serves as an axial ligand for PCo and it improves the redox activity of PCo on the graphene surface to facilitate the generation of [PCo].- active sites for CO2 reduction. Thus, the turnover frequencies of the immobilized Co complexes are increased. Systematic structural analysis indicates that the benzene rings of diphenyl sulfide exhibit strong face-to-face stacking with graphene, which is proposed as an efficient medium to facilitate the interfacial electron communication. 相似文献
944.
Dr. Song Jin Youxuan Ni Zhimeng Hao Prof. Kai Zhang Dr. Yong Lu Dr. Zhenhua Yan Dr. Yajuan Wei Dr. Ying-Rui Lu Dr. Ting-Shan Chan Prof. Jun Chen 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(49):22069-22073
A general graphene quantum dot-tethering design strategy to synthesize single-atom catalysts (SACs) is presented. The strategy is applicable to different metals (Cr, Mn, Fe, Co, Ni, Cu, and Zn) and supports (0D carbon nanosphere, 1D carbon nanotube, 2D graphene nanosheet, and 3D graphite foam) with the metal loading of 3.0–4.5 wt %. The direct transmission electron microscopy imaging and X-ray absorption spectra analyses confirm the atomic dispersed metal in carbon supports. Our study reveals that the abundant oxygenated groups for complexing metal ions and the rich defective sites for incorporating nitrogen are essential to realize the synthesis of SACs. Furthermore, the carbon nanotube supported Ni SACs exhibits high electrocatalytic activity for CO2 reduction with nearly 100 % CO selectivity. This universal strategy is expected to open up new research avenues to produce SACs for diverse electrocatalytic applications. 相似文献
945.
Qi Hu Zhen Han Xiaodeng Wang Guomin Li Ziyu Wang Xiaowan Huang Hengpan Yang Xiangzhong Ren Qianling Zhang Jianhong Liu Prof. Chuanxin He 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(43):19216-19221
Previous density-functional theory (DFT) calculations show that sub-nanometric Cu clusters (i.e., 13 atoms) favorably generate CH4 from the CO2 reduction reaction (CO2RR), but experimental evidence is lacking. Herein, a facile impregnation-calcination route towards Cu clusters, having a diameter of about 1.0 nm with about 10 atoms, was developed by double confinement of carbon defects and micropores. These Cu clusters enable high selectivity for the CO2RR with a maximum Faraday efficiency of 81.7 % for CH4. Calculations and experimental results show that the Cu clusters enhance the adsorption of *H and *CO intermediates, thus promoting generation of CH4 rather than H2 and CO. The strong interactions between the Cu clusters and defective carbon optimize the electronic structure of the Cu clusters for selectivity and stability towards generation of CH4. Provided here is the first experimental evidence that sub-nanometric Cu clusters facilitate the production of CH4 from the CO2RR. 相似文献
946.
Dr. Chaohuang Chen Dr. Jun Li Dr. Constantin G. Daniliuc Dr. Christian Mück-Lichtenfeld Dr. Gerald Kehr Prof. Dr. Gerhard Erker 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(48):21644-21648
Hydride abstraction from the heterocyclic carbene borane adducts (NHC)BH2C6F5 (NHC: IMes or IMe4) gave the B−H containing [(NHC)B(H)C6F5]+ borenium cations. They added carbon monoxide to give the respective [(NHC)B(H)(C6F5)CO]+ boron carbonyl cations. Carbon nucleophiles add to the boron carbonyl to give [B](H) acyls. Hydride reduced the [B]CO cation to hydroxymethylborane derivatives. 相似文献
947.
Prof. Ping Yu Huan Wei Peipei Zhong Yifei Xue Dr. Fei Wu Dr. Yang Liu Prof. Junjie Fei Prof. Lanqun Mao 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(50):22841-22847
The development of new principles and techniques with high neuronal compatibility for quantitatively monitoring the dynamics of neurochemicals is essential for deciphering brain chemistry and function but remains a great challenge. We herein report a neuron-compatible method for in vivo neurochemical sensing by powering a single carbon fiber through spontaneous bipolar electrochemistry as a new sensing platform. By using ascorbic acid as a model target to prove the concept, we found that the single-carbon-fiber-powered microsensor exhibited a good response, high stability and, more importantly, excellent neuronal compatibility. The microsensor was also highly compatible with electrophysiological recording, thus enabling the synchronous recording of both chemical and electrical signals. The sensing principle could be developed for in vivo monitoring of various neurochemicals in the future by rationally designing and tuning the electrochemical reactions at the two poles of the carbon fiber. 相似文献
948.
为了研究La_(0.7)Sr_(0.3)CoO_(3-δ)钙钛矿催化剂对碳黑的催化氧化过程,本研究通过研究催化剂和碳黑的两种不同接触方式,即紧密接触与松散接触,讨论了其对碳黑催化氧化过程的影响。结果表明,与松散接触和无催化剂接触条件相比,紧密接触条件下碳黑的tig(起燃温度)分别下降了89.5和157.4℃,同时随着催化剂/碳黑的比例增加,碳黑氧化的tig、tm(最大转化温度)、tf(燃净温度)均向低温区域移动,表明该催化剂对碳黑有着良好的催化氧化性能。 相似文献
949.
通过扫描电子显微镜、X射线衍射仪、N2吸附分析仪及Boehm滴定法获得ZnCl2、KOH和HNO3化学处理对高纯多壁碳纳米管的结构和表面含氧官能团的影响,通过批处理实验考察吸附条件(吸附时间、初始浓度、温度)对处理前后的碳纳米管吸附苯酚行为的影响,并采用准一级、准二级、Evolich动力学模型和热力学方程拟合其吸附数据,分析其动力学行为、热力学行为和吸附机理。结果表明,虽然ZnCl2、KOH和HNO3化学处理法均未对碳纳米管BET比表面积产生显著影响,但会影响其表面化学性质(即,对于ZnCl2和KOH化学处理降低表面羧基、内酯基含量和增大碱性官能团量,而对于HNO3化学处理可以增大表面羧基、内酯基含量,而碱性官能团略有增加);改性处理影响碳纳米管去除苯酚效率:由于ZnCl2和KOH改性处理降低碳纳米管表面羧基量,故其提高了苯酚去除率,而HNO3处理则略减小碳纳米管的苯酚去除率,可能是由于碳纳米管结构和表面化学性质共同影响所致;碳纳米管的苯酚去除率均随苯酚溶液初始浓度的增大而减小;高温不利于吸附;热力学研究发现碳纳米管吸附苯酚过程是自发的和放热的,属于物理吸附;动力学研究表明,吸附过程符合准二级动力学方程。通过ZnCl2和KOH化学处理,可以显著提高碳纳米管对苯酚的吸附性能。 相似文献
950.
Integration of MnOx into the carbon matrix proves a viable strategy to improve the electrochemical performance of MnOx materials. Mn3O4 nanoparticle-decorated N-doped carbon composites (Mn3O4@N-doped carbon) were facilely prepared from a non-porous eight-fold interpenetrated ZnII-based MOF, which involves first synthesis of bimetallic Mn/Zn-MOF in one-pot reaction followed by direct pyrolysis at 1000 °C. In 0.1 m KOH solution, the optimal Mn3O4@N-doped carbon exhibits decent oxygen reduction activity with the onset potential (Eonset) of 0.94 V (vs. RHE) and half-wave potential (E1/2) of 0.81 V (vs. RHE), excellent methanol tolerance as well as good durability. 相似文献