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ChemRN: Inorganic Catalysis (Topic)最新文献

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S Doping Optimized Intermediate Energetics of FeCoOOh for Enhanced Oxygen Evolution Catalytic Activity S掺杂优化FeCoOOh中间体热力学以增强析氧催化活性
Pub Date : 2020-11-24 DOI: 10.2139/ssrn.3736398
Ding Yuan, Yuhai Dou, Chun‐Ting He, Linping Yu, Li Xu, David Adekoya, Qingbing Xia, Jianmin Ma, Shixue Dou, Shanqing Zhang
Transition metal sulfides have been demonstrated to be more active electrocatalysts than the corresponding (hydr)oxides for oxygen evolution reaction (OER). The nature of active sites, however, remains unclear. Herein, we study whether S could promote the OER activity of FeCoOOH and try to identify the catalytically active centers. Density functional theory suggests that two coordinating S could work synergistically with one adjacent Fe to optimize the electronic states of Co, resulting in decreased binding energy of OH* (ΔEOH) while little changed ΔEOH, and thus significantly lowering the catalytic overpotential. Further experimental studies validate the synergistic effect between S and Fe on tuning the electronic structure and the greatly improved catalytic activity with a small overpotential of 205.4 mV to drive 20 mA cm-2. This study unveils the origin of the high catalytic activity of transition metal sulfides and provides insights into the design of efficient OER electrocatalysts.
在析氧反应(OER)中,过渡金属硫化物已被证明是比相应的(氢)氧化物更活跃的电催化剂。然而,活性位点的性质仍不清楚。本文研究S是否能促进FeCoOOH的OER活性,并试图确定催化活性中心。密度泛函理论认为,两个配位的S可以与相邻的Fe协同作用,优化Co的电子态,使OH* (ΔEOH)的结合能降低,而ΔEOH的变化不大,从而显著降低催化过电位。进一步的实验研究证实了S和Fe在调节电子结构方面的协同作用,并大大提高了催化活性,以205.4 mV的小过电位驱动20 mA cm-2。该研究揭示了过渡金属硫化物高催化活性的起源,并为高效OER电催化剂的设计提供了见解。
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引用次数: 0
Accumulation-Driven Surfactant-Free Synthesis of Architectured Immiscible Metallic Nanoalloys with Enhanced Catalysis 积累驱动无表面活性剂的结构不混溶金属纳米合金的强化催化合成
Pub Date : 2019-04-16 DOI: 10.2139/ssrn.3372970
B. Rajeeva, Pranaw Kunal, P. Kollipara, Palash V. Acharya, M. Joe, Matthew S. Ide, K. Jarvis, Yuanyue Liu, V. Bahadur, S. M. Humphrey, Yuebing Zheng
Accumulation-mediated chemical reactions are a ubiquitous phenomenon in nature. Herein, we explore microbubble-induced accumulation of precursor ions to achieve surfactant-free synthesis of immiscible metallic nanoalloys and to simultaneously pattern the nanoalloys into targeted architectures for their enhanced catalytic applications. We name our approach as a unified spatiotemporal synthesis and structuring (US3) strategy, wherein millisecond-scale accumulation of the precursor ions in a highly confined laser-mediated microbubble trap (MBT) drives ultra-fast alloy synthesis in sync with the structuring process. As a case-in-point, we employ US3 strategy for the in-situ surfactant-free synthesis and patterning of traditionally immiscible rhodium-gold (RhAu) nanoalloys. Stochastic random walk simulations justify the millisecond-scale accumulation process, leading to a 3-order reduction in synthesis time. The catalytic activity and structure-property relationship of the structured nanoalloys were evaluated using the reduction of p-nitrophenol with NaBH4. Our in-situ synthesis and structuring strategy can be translated for high-throughput production and screening of multi-metallic systems with tailored catalytic, opto-electronic, and magnetic functions.
积累介导的化学反应是自然界中普遍存在的现象。在此,我们探索了微泡诱导的前体离子积累,以实现无表面活性剂的不混溶金属纳米合金的合成,并同时将纳米合金图案化为目标结构,以增强其催化应用。我们将我们的方法命名为统一的时空合成和结构(US3)策略,其中前体离子在高度受限的激光介导的微泡陷阱(MBT)中毫秒级的积累驱动超快速合金合成与结构过程同步。作为一个例子,我们采用US3策略进行原位无表面活性剂合成和传统不混相铑金(RhAu)纳米合金的图像化。随机漫步模拟证明了毫秒级积累过程,导致合成时间减少了3阶。利用NaBH4还原对硝基苯酚,评价了结构纳米合金的催化活性和结构性能关系。我们的原位合成和结构策略可以转化为具有定制催化,光电和磁性功能的高通量多金属体系的生产和筛选。
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引用次数: 0
A Cobalt Complex of Bis(Methylthioether)Pyridine Catalyst for Hydrogen Evolution from Water 双(甲基硫醚)吡啶钴配合物催化水析氢
Pub Date : 1900-01-01 DOI: 10.2139/ssrn.3597978
Chun‐Li Wang, Weixia Liu, Shu‐Zhong Zhan
A new cobalt-based catalyst, [(btep)CoBr 2 ] is produced by the reaction of CoBr 2 and bis(methylthioether)pyridine (btep), and its structure has been determined by X-ray crystallography. Our experiments suggest that this cobalt complex can used as a molecular catalyst for electrochemical and photochemical driven hydrogen evolution. As an electrocatalyst, this cobalt complex can provide 591.9 moles of hydrogen per mole of catalyst per hour (mol H 2 /mol catalyst/h) from a neutral water under an overpotential (OP) of 837.6 mV. As a co-catalyst, it was mixed with CdS nanorods (CdS NRs) as a photosensitizer, and ascorbic acid (H 2 A) as a sacrificial electron donor, and [(btep)CoBr 2 ] can provide 9326.4 mol H 2 per mole of catalyst during 40 h irradiation. The highest apparent quantum yield (AQY) is ~25.5%. The catalytic mechanism for H 2 production is investigated by several measurements and analysis.
由CoBr 2与双(甲基硫醚)吡啶(btep)反应制备了一种新型钴基催化剂[(btep)CoBr 2],并通过x射线晶体学对其结构进行了测定。我们的实验表明,这种钴配合物可以作为电化学和光化学驱动析氢的分子催化剂。作为电催化剂,该钴配合物在过电位(OP)为837.6 mV的中性水中,每摩尔催化剂每小时可提供591.9摩尔氢(mol h2 /mol catalyst/ H)。以CdS纳米棒(CdS NRs)为光敏剂,抗坏血酸(h2a)为牺牲电子供体作为共催化剂,[(btep) cobr2]在40 H的辐照下,每摩尔催化剂可提供9326.4 mol h22。最高表观量子产率(AQY)为~25.5%。通过一系列的测量和分析,探讨了催化生成h2的机理。
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引用次数: 0
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ChemRN: Inorganic Catalysis (Topic)
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