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在碱性电解质中负载型小非晶态镍铁纳米颗粒上的电催化析氧

Electrocatalytic oxygen evolution over supported small amorphous Ni-Fe nanoparticles in alkaline electrolyte.

作者信息

Qiu Yang, Xin Le, Li Wenzhen

机构信息

Department of Chemical Engineering, Michigan Technological University , Houghton, Michigan 49931, United States.

出版信息

Langmuir. 2014 Jul 8;30(26):7893-901. doi: 10.1021/la501246e. Epub 2014 Jun 24.

Abstract

The electrocatalytic oxygen evolution reaction (OER) is a critical anode reaction often coupled with electron or photoelectron CO2 reduction and H2 evolution reactions at the cathode for renewable energy conversion and storage. However, the sluggish OER kinetics and the utilization of precious metal catalysts are key obstacles in the broad deployment of these energy technologies. Herein, inexpensive supported 4 nm Ni-Fe nanoparticles (NiyFe1-yOx/C) featuring amorphous structures have been prepared via a solution-phase nanocapsule method for active and durable OER electrocatalysts in alkaline electrolyte. The Ni-Fe nanoparticle catalyst containing 31% Fe (Ni0.69Fe0.31Ox/C) shows the highest activity, exhibiting a 280 mV overpotential at 10 mA cm(-2) (equivalent to 10% efficiency of solar-to-fuel conversion) and a Tafel slope of 30 mV dec(-1) in 1.0 M KOH solution. The achieved OER activity outperforms NiOx/C and commercial Ir/C catalysts and is close to the highest performance of crystalline Ni-Fe thin films reported in the literature. In addition, a Faradaic efficiency of 97% measured on Ni0.69Fe0.31Ox/C suggests that carbon support corrosion and further oxidation of nanoparticle catalysts are negligible during the electrocatalytic OER tests. Ni0.69Fe0.31Ox/C further demonstrates high stability as there is no apparent OER activity loss (based on a chronoamperometry test) or particle aggregation (based on TEM image observation) after a 6 h anodization test. The high efficiency and durability make these supported amorphous Ni-Fe nanoparticles potentially applicable in the (photo)electrochemical cells for water splitting to make H2 fuel or CO2 reduction to produce usable fuels and chemicals.

摘要

电催化析氧反应(OER)是一种关键的阳极反应,通常与阴极的电子或光电子二氧化碳还原反应以及析氢反应耦合,用于可再生能源的转换和存储。然而,缓慢的OER动力学和贵金属催化剂的使用是这些能源技术广泛应用的关键障碍。在此,通过溶液相纳米胶囊法制备了具有非晶结构的廉价负载型4 nm镍铁纳米颗粒(NiyFe1-yOx/C),用于碱性电解质中活性和耐用的OER电催化剂。含有31%铁的镍铁纳米颗粒催化剂(Ni0.69Fe0.31Ox/C)表现出最高的活性,在1.0 M KOH溶液中,在10 mA cm(-2)时过电位为280 mV(相当于太阳能到燃料转换效率的10%),塔菲尔斜率为30 mV dec(-1)。所实现的OER活性优于NiOx/C和商业Ir/C催化剂,接近文献报道的结晶镍铁薄膜的最高性能。此外,在Ni0.69Fe0.31Ox/C上测得的法拉第效率为97%,这表明在电催化OER测试期间,碳载体腐蚀和纳米颗粒催化剂的进一步氧化可以忽略不计。Ni0.69Fe0.31Ox/C进一步证明了其高稳定性,因为在6小时的阳极氧化测试后,没有明显的OER活性损失(基于计时电流法测试)或颗粒聚集(基于TEM图像观察)。高效率和耐用性使得这些负载型非晶镍铁纳米颗粒有可能应用于(光)电化学电池中,用于水分解制氢燃料或二氧化碳还原以生产可用燃料和化学品。

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