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Xiuxiu Zhang Chenyu Yang Chen Gong Meihuan Liu Wanlin Zhou Hui Su Feifan Yu Fengchun Hu Qinghua Liu Shiqiang Wei 《Angewandte Chemie (International ed. in English)》2023,62(33):e202308082
Synthesis of highly active and durable oxygen evolution reaction (OER) catalysts applied in acidic water electrolysis remains a grand challenge. Here, we construct a type of high-loading iridium single atom catalysts with tunable d-band holes character (h-HL−Ir SACs, ∼17.2 wt % Ir) realized in the early OER operation stages. The in situ X-ray absorption spectroscopy reveals that the quantity of the d-band holes of Ir active sites can be fast increased by 0.56 unit from the open circuit to a low working potential of 1.35 V. More remarkably, in situ synchrotron infrared and Raman spectroscopies demonstrate the quick accumulation of *OOH and *OH intermediates over holes-modulated Ir sites in the early reaction voltages, achieving a rapid OER kinetics. As a result, this well-designed h-HL−Ir SACs exhibits superior performance for acidic OER with overpotentials of 216 mV @10 mA cm−2 and 259 mV @100 mA cm−2, corresponding to a small Tafel slope of 43 mV dec−1. The activity of catalyst shows no evident attenuation after 60 h operation in acidic environment. This work provides some useful hints for the design of superior acidic OER catalysts. 相似文献
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本文利用间断有限元法求解非线性延迟微分方程,在拟等级网格下.给出非线性延迟微分方程间断有限元解的整体收敛阶和局部超收敛阶,数值实验验证了理论结果的正确性. 相似文献
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针对退化率较高的产品具有不稳定的退化路径以及产品个体差异对退化过程的影响,建立了一种新的随机效应退化模型,即漂移参数和扩散参数均为随机变量且两者之间呈线性关系的Wiener退化过程模型.基于该模型获得了产品剩余寿命分布与可靠度函数,同时设计了估计模型参数的EM(expectation maximization)算法.最后,通过分析钛合金疲劳裂纹数据以及与现有模型结果的比较,验证了所建模型的有效性和准确性. 相似文献
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Xiuxiu Wang Zong-Chang Han Wei Wei Hanshi Hu Pengfei Li Peiqing Sun Xiangzhi Liu Zhijia Lv Feng Wang Yi Cao Zijian Guo Jun Li Jing Zhao 《Chemical science》2022,13(24):7269
Metal clusters, such as iron–sulfur clusters, play key roles in sustaining life and are intimately involved in the functions of metalloproteins. Herein we report the formation and crystal structure of a planar square tetranuclear silver cluster when silver ions were mixed with human copper chaperone Atox1. Quantum chemical studies reveal that two Ag 5s1 electrons in the tetranuclear silver cluster fully occupy the one bonding molecular orbital, with the assumption that this Ag4 cluster is Ag42+, leading to extensive electron delocalization over the planar square and significant stabilization. This bonding pattern of the tetranuclear silver cluster represents an aromatic all-metal structure that follows a 4n + 2 electron counting rule (n = 0). This is the first time an all-metal aromatic silver cluster was observed in a protein.Metal clusters, such as iron–sulfur clusters, play key roles in sustaining life and are intimately involved in the functions of metalloproteins. 相似文献
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Nianxin Zhu Xinna Liu Kaimin Peng Hui Cao Min Yuan Tai Ye Xiuxiu Wu Fengqin Yin Jinsong Yu Liling Hao Fei Xu 《Molecules (Basel, Switzerland)》2023,28(1)
Lead contamination in aquatic products is one of the main hazard factors. The aptasensor is a promising detection method for lead ion (Pb(II)) because of its selectivity, but it is easily affected by pH. The combination of ion-imprinted polymers(IIP) with aptamers may improve their stability in different pH conditions. This paper developed a novel electrochemical biosensor for Pb(II) detection by using aptamer-imprinted polymer as a recognition element. The glassy carbon electrode was modified with gold nanoparticles and aptamers. After the aptamer was induced by Pb(II) to form a G-quadruplex conformation, a chitosan-graphene oxide was electrodeposited and cross-linked with glutaraldehyde to form an imprint layer, improving the stability of the biosensor. Under the optimal experimental conditions, the current signal change (∆I) showed a linear correlation of the content of Pb(II) in the range of 0.1–2.0 μg/mL with a detection limit of 0.0796 μg/mL (S/N = 3). The biosensor also exhibited high selectivity for the determination of Pb(II) in the presence of other interfering metal ion. At the same time, the stability of the imprinted layer made the sensor applicable to the detection environment with a pH of 6.4–8.0. Moreover, the sensor was successfully applied to the detection of Pb(II) in mantis shrimp. 相似文献
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Xiuxiu Yue Wenxiu Li Wenqiang Chen Liangliang Zhang Guofang Li Jiarong Sheng 《Tetrahedron letters》2018,59(23):2232-2237
A naphthofluorescein-based fluorescent probe with two independent reaction sites (nitro-2,1,3-benzoxadiazole and acrylate moiety) was developed. Integrating these two reaction sites into a single molecule not only can guarantee the selective detection of Cys/Hcy in an elegant fashion, but also can enable Cys/Hcy detection in a multiple-channel responsive manner. 相似文献
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