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981.
A Bio‐inspired Cu4O4 Cubane: Effective Molecular Catalysts for Electrocatalytic Water Oxidation in Aqueous Solution 下载免费PDF全文
Xin Jiang Jian Li Bing Yang Xiang‐Zhu Wei Bo‐Wei Dong Yi Kao Mao‐Yong Huang Prof. Chen‐Ho Tung Prof. Li‐Zhu Wu 《Angewandte Chemie (International ed. in English)》2018,57(26):7850-7854
Inspired by the cubic Mn4CaO5 cluster of natural oxygen‐evolving complex in Photosystem II, tetrametallic molecular water oxidation catalysts, especially M4O4 cubane‐like clusters (M=transition metals), have aroused great interest in developing highly active and robust catalysts for water oxidation. Among these M4O4 clusters, however, copper‐based molecular catalysts are poorly understood. Now, bio‐inspired Cu4O4 cubanes are presented as effective molecular catalysts for electrocatalytic water oxidation in aqueous solution (pH 12). The exceptional catalytic activity is manifested with a turnover frequency (TOF) of 267 s?1 for [(LGly‐Cu)4] at 1.70 V and 105 s?1 for [(LGlu‐Cu)4] at 1.56 V. Electrochemical and spectroscopic study revealed a successive two‐electron transfer process in the Cu4O4 cubanes to form high‐valent CuIII and CuIIIO. intermediates during the catalysis. 相似文献
982.
Solid‐State Electrolyte Anchored with a Carboxylated Azo Compound for All‐Solid‐State Lithium Batteries 下载免费PDF全文
Dr. Chao Luo Xiao Ji Dr. Ji Chen Dr. Karen J. Gaskell Xinzi He Dr. Yujia Liang Prof. Jianjun Jiang Prof. Chunsheng Wang 《Angewandte Chemie (International ed. in English)》2018,57(28):8567-8571
Organic electrode materials are promising for green and sustainable lithium‐ion batteries. However, the high solubility of organic materials in the liquid electrolyte results in the shuttle reaction and fast capacity decay. Herein, azo compounds are firstly applied in all‐solid‐state lithium batteries (ASSLB) to suppress the dissolution challenge. Due to the high compatibility of azobenzene (AB) based compounds to Li3PS4 (LPS) solid electrolyte, the LPS solid electrolyte is used to prevent the dissolution and shuttle reaction of AB. To maintain the low interface resistance during the large volume change upon cycling, a carboxylate group is added into AB to provide 4‐(phenylazo) benzoic acid lithium salt (PBALS), which could bond with LPS solid electrolyte via the ionic bonding between oxygen in PBALS and lithium ion in LPS. The ionic bonding between the active material and solid electrolyte stabilizes the contact interface and enables the stable cycle life of PBALS in ASSLB. 相似文献
983.
Monochalcoplatin: An Actively Transported,Quickly Reducible,and Highly Potent PtIV Anticancer Prodrug 下载免费PDF全文
Dr. Lili Ma Na Wang Rong Ma Cai Li Zoufeng Xu Dr. Man‐Kit Tse Prof. Dr. Guangyu Zhu 《Angewandte Chemie (International ed. in English)》2018,57(29):9098-9102
Recently, PtIV prodrugs have attracted much attention as the next generation of platinum‐based antineoplastic drug candidates. Here we report the discovery and evaluation of monochalcoplatin, a monocarboxylated PtIV prodrug that is among the most cytotoxic PtIV prodrugs to date. Compared with its dicarboxylated counterpart chalcoplatin, monochalcoplatin accumulates astonishingly effectively and rapidly in cancer cells, which is not ascribed to its lipophilicity. The prodrug is quickly reduced, causes DNA damage, and induces apoptosis, resulting in superior cytotoxicity with IC50 values in the nanomolar range in both cisplatin‐sensitive and ‐resistant cells; these IC50 values are up to 422‐fold higher than that of cisplatin. A detailed mechanistic study reveals that monochalcoplatin actively enters cells through a transporter‐mediated process. Moreover, monochalcoplatin shows significant antitumor activity in an in vivo colorectal tumor model. Our study implies a practical strategy for the design of more effective PtIV prodrugs to conquer drug resistance by tuning both cellular uptake pathways and activation processes. 相似文献
984.
Isolated Platinum Atoms Stabilized by Amorphous Tungstenic Acid: Metal–Support Interaction for Synergistic Oxygen Activation 下载免费PDF全文
Qian Zhang Xi‐Xi Qin Fan‐Peng Duan‐Mu Prof. Hui‐Ming Ji Prof. Zhu‐Rui Shen Dr. Xiao‐Peng Han Prof. Wen‐Bin Hu 《Angewandte Chemie (International ed. in English)》2018,57(30):9351-9356
Oxygen activation plays a crucial role in many important chemical reactions such as oxidation of organic compounds and oxygen reduction. For developing highly active materials for oxygen activation, herein, we report an atomically dispersed Pt on WO3 nanoplates stabilized by in situ formed amorphous H2WO4 out‐layer and the mechanism for activating molecular oxygen. Experimental and theoretical studies demonstrate that the isolated Pt atoms coordinated with oxygen atoms from [WO6] and water of H2WO4, consequently leading to optimized surface electronic configuration and strong metal–support interaction (SMSI). In exemplified reactions of butanone oxidation sensing and oxygen reduction, the atomic Pt/WO3 hybrid exhibits superior activity than those of Pt nanoclusters/WO3 and bare WO3 as well as enhanced long‐term durability. This work will provide insight into the origin of activity and stability for atomically dispersed materials, thus promoting the development of highly efficient and durable single atom‐based catalysts. 相似文献
985.
A Rapidly Self‐Healing Host–Guest Supramolecular Hydrogel with High Mechanical Strength and Excellent Biocompatibility 下载免费PDF全文
Dr. Ye Zhu Dr. Lijing Hao Dr. Yunhua Chen Prof. Dr. Geng An Prof. Dr. Hongkai Wu Prof. Dr. Xuetao Shi Prof. Dr. Chuanbin Mao 《Angewandte Chemie (International ed. in English)》2018,57(29):9008-9012
It is still a challenge to achieve both excellent mechanical strength and biocompatibility in hydrogels. In this study, we exploited two interactions to form a novel biocompatible, slicing‐resistant, and self‐healing hydrogel. The first was molecular host–guest recognition between a host (isocyanatoethyl acrylate modified β‐cyclodextrin) and a guest (2‐(2‐(2‐(2‐(adamantyl‐1‐oxy)ethoxy)ethoxy)ethoxy)ethanol acrylate) to form “three‐arm” host–guest supramolecules (HGSMs), and the second was covalent bonding between HGSMs (achieved by UV‐initiated polymerization) to form strong cross‐links in the hydrogel. The host–guest interaction enabled the hydrogel to rapidly self‐heal. When it was cut, fresh surfaces were formed with dangling host and guest molecules (due to the breaking of host–guest recognition), which rapidly recognized each other again to heal the hydrogel by recombination of the cut surfaces. The smart hydrogels hold promise for use as biomaterials for soft‐tissue repair. 相似文献
986.
助剂Cu、K对F-T合成铁基催化剂作用的表征研究 总被引:3,自引:3,他引:3
采用连续共沉淀和喷雾干燥技术相结合的方法制备了一组Cu、K助剂单独或同时加入的微球状Fischer-Tropsch(F-T)合成铁基催化剂,借助低温N2吸附、MES、XRD、H2-TPR、CO-TPR研究了Cu和K助剂对催化剂织构、还原性能以及还原和炭化过程中的物相变化的影响。结果表明,K助剂的加入能明显提高催化剂的比表面积和铁物相在催化剂中的分散程度,增加了Fe2O3与SiO2间的相互作用;当催化剂在H2和合成气中还原时,Cu助剂的加入有利于催化剂的还原和Fe3O4的生成,在CO中还原时,Cu助剂的加入则有利于α-Fe的生成和稳定化。在H2和合成气中,单独K助剂的加入会抑制催化剂的还原或炭化,而Cu和K助剂的同时加入在H2、CO和合成气下均可使催化剂的还原或炭化能力明显提高,表明Cu和K助剂间存在一定的协同作用。 相似文献
987.
固体热载体热解淮南煤实验研究 总被引:3,自引:3,他引:3
自制处理量为1 kg煤的间歇式固体热载体热解装置,以淮南烟煤为原料,石英砂作热载体,对该煤进行热解特性评价实验。考察了热载体初始温度700 ℃~900 ℃、反应
4 min~16 min、煤粒径及热载体与煤的质量比5~9对热解产物产率和性质的影响。结果表明,提高热载体初始温度,气、液产率增加;延长反应时间和提高热载体比例,气体产率有所增加;热载体初始温度对热解气组成影响显著。提高热载体与煤的质量比和热载体初始温度,可以抑制半焦对热解反应器内壁的黏附。 相似文献
988.
989.
采用溶胶-凝胶法合成了一种V2O5/C复合材料.扫描电镜(SEM)和红外光谱(FTIR)分析表明,这是一种外层V2O5胶体包覆内层乙炔分子的多孔复合材料.以V2O5/C作正极,锌片为负极,Zn(ClO4)2溶液为电解质组成水相锌二次电池,采用循环伏安(CV)和电化学阻抗谱(EIS)等方法研究发现:V2O5:C质量比为1:1时电极具有最好的电化学性能,电池开路电压达1.64 V; Zn2+能分别在1.01 V和1.26 V处分步嵌入V2O5/C结构中A、B两种位置,其嵌入电流密度峰值最高可达70 mA•g-1,并且具有较好的循环充放电性能;在一定放电深度下,V2O5/C电极反应速率受Zn2+的扩散过程控制. 相似文献
990.