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Metal-Organic frameworks-derived multifunctional carbon encapsulated metallic nanocatalysts for catalytic peroxymonosulfate activation and electrochemical hydrogen generation
Molecular Catalysis ( IF 4.6 ) Pub Date : 2020-10-16 , DOI: 10.1016/j.mcat.2020.111241
Md Ariful Ahsan , Alain R. Puente Santiago , Aruna Narayanan Nair , J. Mark Weller , Mohammed F. Sanad , Delia J. Valles-Rosales , Candace K. Chan , Sreeprasad Sreenivasan , Juan C. Noveron

Synthesis of high-efficiency metal catalysts and their application in catalyzing critical chemical processes holds the key to the sustainable supply of water and energy. However, reaction-induced atomistic modifications of nanoclusters often result in reduced stability and efficacy. Herein, we report a highly active and multifunctional transition metal nanocatalysts encapsulated in porous carbon network (M@C where M = Cu, Ni, Fe, Co) prepared by leveraging the sacrificial templating properties of metal-organic frameworks (MOFs). The as-synthesized M@C nanocatalysts were employed for oxidative degradation of organic pollutants and electrocatalytic hydrogen generation. Fenton like catalytic studies revealed that the nanocatalysts were highly active and reusable following the order of Co@C > Fe@C > Cu@C > Ni@C. On the other hand, Ni@C electrocatalyst displayed superior activity towards hydrogen evolution reaction as compared to others, delivering a low onset potential of 61 mV, Tafel slope of 82 mV/dec and an overpotential of 286 mV at 10 mA‧cm−2. The activity was essentially unchanged even after 500 cycles, suggesting the long‐term stability under acidic conditions. The impressive multifunctional catalytic performances of M@C nanocatalysts are attributed to their unique porous carbon matrix doped by transition metal nanoparticles which provide a large number of interconnected catalytically active sites.



中文翻译:

源自金属-有机骨架的多功能碳包封的金属纳米催化剂,用于催化过氧单硫酸盐活化和电化学制氢

高效金属催化剂的合成及其在催化关键化学过程中的应用是水和能源可持续供应的关键。但是,反应引起的纳米团簇的原子修饰经常导致稳定性和功效降低。在本文中,我们报告了利用金属有机骨架(MOFs)的牺牲模板性质制备的,包裹在多孔碳网络中的高活性和多功能过渡金属纳米催化剂(M @ C,其中M = Cu,Ni,Fe,Co)。合成后的M @ C纳米催化剂用于有机污染物的氧化降解和电催化制氢。类似于Fenton的催化研究表明,纳米催化剂具有很高的活性,并且可以按Co @ C> Fe @ C> Cu @ C> Ni @ C的顺序重复使用。另一方面,−2。即使经过500次循环,其活性也基本上没有变化,这表明在酸性条件下的长期稳定性。M @ C纳米催化剂令人印象深刻的多功能催化性能归因于其独特的多孔碳基质,该基质被过渡金属纳米颗粒掺杂,从而提供了大量相互连接的催化活性位。

更新日期:2020-10-16
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