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Activating a Low Overpotential CO2 Reduction Mechanism by a Strategic Ligand Modification on a Ruthenium Polypyridyl Catalyst
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Ben A. Johnson Dr. Somnath Maji Dr. Hemlata Agarwala Dr. Travis A. White Dr. Edgar Mijangos Prof. Dr. Sascha Ott 《Angewandte Chemie (International ed. in English)》2016,55(5):1825-1829
The introduction of a simple methyl substituent on the bipyridine ligand of [Ru(tBu3tpy)(bpy)(NCCH3)]2+ (tBu3tpy=4,4′,4′′‐tri‐tert‐butyl‐2,2′:6′,2′′‐terpyridine; bpy=2,2′‐bipyridine) gives rise to a highly active electrocatalyst for the reduction of CO2 to CO. The methyl group enables CO2 binding already at the one‐electron reduced state of the complex to enter a previously not accessible catalytic cycle that operates at the potential of the first reduction. The complex turns over with a Faradaic efficiency close to unity and at an overpotential that is amongst the lowest ever reported for homogenous CO2 reduction catalysts. 相似文献
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燃料电池的阴极反应的反应动力学速率非常慢,限制了燃料电池技术的发展。因此,寻找低成本、高活性的氧还原催化剂具有重要的意义。多元金属核壳团簇表现出优良的氧还原活性。在本文中,以原子个数为19、38、55和79的八面体团簇作催化剂模型,采用密度泛函理论(GGA-PBE-PAW)方法,研究了一系列不同尺寸核壳Nim@Mn-m (n = 19, 38, 55, 79;m = 1, 6, 13, 19; M = Pt, Pd, Cu, Au, Ag)团簇催化剂的活性规律。优化*O、*OH和*OOH吸附中间体结构,计算了吸附自由能和反应吉布斯自由能,以超电势为催化活性的描述符,研究了单原子Pt嵌入Nim@Aun-m团簇的活性规律。结果表明,Ni6@Pt1Au31具有最好的ORR活性,并且Ni1@Pt1Au17、Ni6@Pt1Au31、Ni13@Pt1Au41、Ni19@Pt1Au5表现出比Pt38团簇以及Pt(111)表面更高的催化活性。Bader电荷和态密度分析表面,核壳之间的电荷转移以及单原子Pt嵌入Nim@Aun-m表面,改变了吸附位的电子性质,降低了*OH的吸附强度,提高了ORR活性。单原子Pt嵌入Nim@Aun-m表面可能是一种合适的多元金属核壳ORR催化剂设计策略。 相似文献
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基于析氢过电位解释了以下问题:Zn(s)|H2SO4(aq)|Cu(s)原电池实验中,如何避免锌表面产生H2?为什么纯锌、纯铁分别与稀硫酸反应速率几乎一样?如何解释铅蓄电池中铅与硫酸难以反应的事实?电解FeCl2溶液其阴极一定得到H2吗? 相似文献
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非晶态NiP基催化剂的制备及电催化析氢性能研究 《燃料化学学报》2018,46(4):473-478
以NaH2PO2和Ni2SO4为磷源和镍源,使用一锅法合成了非晶态NiP合金及其碳纳米(乙炔黑和石墨烯)复合催化剂。用透射电子显微镜(TEM)、X射线衍射仪(XRD)、热重分析(TGA)、电感耦合等离子体光谱仪(ICP)分别对催化剂性能和组成进行了表征和分析。通过线性扫描伏安对催化剂在酸性和碱性条件下的析氢性能进行了评价,研究结果表明,非晶态NiP/还原氧化石墨烯复合催化剂(NiP/RGO)展现出优异的电催化性能。在0.5 mol/L H2SO4中的起始过电位为89.0 mV,塔菲尔斜率为135.1 mV/decade;在1 mol/L NaOH中,起始过电位为116.1 mV,塔菲尔斜率为122.4 mV/decade,这与商业化Pt黑催化剂很接近。500次循环以后,催化剂活性没有明显下降,表明该催化剂具有良好的稳定性。该研究提供了一种简单可行的制备非贵金属磷化物方法用于电催化析氢反应。 相似文献
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Xin-Xin Zhao Zhen-Yi Gu Wen-Hao Li Xu Yang Dr. Jin-Zhi Guo Prof. Xing-Long Wu 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(35):7823-7830
Phosphate cathode materials are practical for use in sodium-ion batteries (SIBs) owing to their high stability and long-term cycle life. In this work, the temperature-dependent properties of the phosphate cathode Na3V2(PO4)2O2F (NVPOF) are studied in a wide temperature range from −25 to 55 °C. Upon cycling at general temperature (above 0 °C), the NVPOF cathode retains an excellent charge/discharge performance, and the rate capability is noteworthy, indicating that NVPOF is a competitive candidate as a temperature-adaptive cathode for SIBs. Upon decreasing the temperature below 0 °C, the cell performance deteriorates, which may be caused by the electrolyte and Na electrode, based on the study of ionic conductivity and electrode kinetics. This work proposes a new breakthrough point for the development of SIBs with high performance over a wide temperature range for advanced power systems. 相似文献
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Dr. Qian Ma Rongfeng Liao Yuheng Lu Prof. Dr. Shaohong Liu Dr. Youchen Tang Prof. Dr. Youlong Zhu Prof. Dr. Dingcai Wu 《化学:亚洲杂志》2021,16(20):3102-3106
Cobalt disulfide (CoS2) has been explored as attractive electrocatalyst for oxygen evolution reaction (OER). However, bulk CoS2 sheets have limited catalytic activity due to low exposure of active sites. Herein, through an in-situ vulcanization approach, CoS2 nanoparticles are embedded into bipyridine-containing covalent organic polymer (BP-COP). The as-prepared nanocomposite CoS2@BP-COP exhibits high catalytic activity toward OER with an ultra-low overpotential of 270 mV (vs. RHE) at a current density of 10 mA cm−2, a small Tafel slope of 36 mV dec−1, and an excellent durability for 24 h without decay. The surface of CoS2 is partially converted into CoOOH to form CoS2/CoOOH as active sites under OER conditions. CoS2@BP-COP displays superior OER catalytic activity to CoS2 nanosheets and commercially available RuO2 under the same conditions. The outstanding OER performance activity of CoS2@BP-COP could be attributed to the uniform and small particle sizes of CoS2/CoOOH distributed in BP-COP. 相似文献
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In this study, we investigated the effects of power ultrasound (26 kHz, up to ∼75 W/cm2, up to 100% acoustic amplitude, ultrasonic horn) on the hydrogen evolution reaction (HER) on a platinum (Pt) polycrystalline disc electrode in 0.5 M H2SO4 by cyclic and linear sweep voltammetry at 298 K. We also studied the formation of molecular hydrogen (H2) bubbles on a Pt wire in the absence and presence of power ultrasound using ultra-fast camera imaging. It was found that ultrasound significantly increases currents towards the HER i.e. a ∼250% increase in current density was achieved at maximum ultrasonic power. The potential at a current density of −10 mA/cm2 under silent conditions was found to be −46 mV and decreased to −27 mV at 100% acoustic amplitude i.e. a ΔE shift of ∼+20 mV, indicating the influence of ultrasound on improving the HER activity. A nearly 100% increase in the exchange current density (jo) and a 30% decrease in the Tafel slope (b) at maximum ultrasonic power, was observed in the low overpotential region, although in the high overpotential region, the Tafel slopes (b) were not significantly affected when compared to silent conditions. In our conditions, ultrasound did not greatly affect the “real” surface area (Ar) and roughness factor (R) i.e. the microscopic surface area available for electron transfer. Overall, it was found that ultrasound did not dramatically change the mechanism of HER but instead, increased currents at the Pt surface area through effective hydrogen bubble removal. 相似文献
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导电聚吡咯薄膜的大过电位是一个有趣而被忽视的现象,针对它在形成机理、膜表面微观结构等方面进行了系统实验研究。结果表明,聚吡咯薄膜大过电位现象在水相条件也存在,同时具有选择性吸附电流特点,产生这一现象与掺杂阴离子性质、种数、浓度及由此而导致的聚合有序性相关。负电位下掺杂大直径对阴离子的聚吡咯薄膜由于在还原下脱掺杂困难,Na^+、K^+、Li^+等水化小阳离子对聚吡咯链的吸附中和是导致吸附电流的产生和薄膜结构形态上变化的主要原因。 相似文献