Rasaily Sagarmani, Chettri Shivanand, Sharma Debesh, Baruah Khanindram, Dewan Rajani, Tamang Sudarsan, Pariyar Anand
Department of Chemistry, School of Physical Sciences, Sikkim University, Gangtok 737102, East Sikkim, India.
Centre for Advanced Studies, Department of Chemistry, North-Eastern Hill University, Shillong 793022, Meghalaya, India.
Inorg Chem. 2024 Sep 23;63(38):17846-17855. doi: 10.1021/acs.inorgchem.4c02856. Epub 2024 Sep 12.
Bifunctional electrocatalysts, capable of efficiently driving both the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER), are crucial for advancing electrochemical processes. While noble-metal-based catalysts are widely recognized for their role in oxygen processes, current state-of-the-art designs are limited to either ORR or OER activity, presenting a notable research gap. In addressing this challenge, we have developed a novel nanocomposite catalyst derived from a nickel-based metal-organic framework (). For the ORR, the catalyst exhibits an onset potential of 0.95 V vs RHE in a 1.0 M KOH solution, coupled with a Tafel slope of -99 mV dec at 1600 rpm. Moreover, the catalyst displays excellent stability, maintaining a performance of over 90% after 10 h of continuous reaction. Furthermore, the catalyst proves effective in the OER, boasting an overpotential of 370 mV (at 10 mA cm) and a Tafel slope of 114 mV dec, highlighting its bifunctionality. The bifunctional overpotential of the composite is measured at 820 mV, surpassing that of the 20% Pt/C electrocatalyst (860 mV), highlighting its potential for practical applications. Comparative experiments establish the origin of the robust bifunctional reactivity toward the conformal hybrid structure, porous framework, and the synergistic effect operating among the constituents of the nanocomposite.
能够有效驱动氧还原反应(ORR)和析氧反应(OER)的双功能电催化剂对于推进电化学过程至关重要。虽然基于贵金属的催化剂在氧过程中的作用已得到广泛认可,但目前最先进的设计仅限于ORR或OER活性,存在明显的研究空白。为应对这一挑战,我们开发了一种源自镍基金属有机框架的新型纳米复合催化剂。对于ORR,该催化剂在1.0 M KOH溶液中相对于可逆氢电极(RHE)的起始电位为0.95 V,在1600 rpm下的塔菲尔斜率为-99 mV dec-1。此外,该催化剂表现出优异的稳定性,连续反应10小时后性能保持在90%以上。此外,该催化剂在OER中也被证明是有效的,过电位为370 mV(在10 mA cm-2时),塔菲尔斜率为114 mV dec-1,突出了其双功能特性。该复合催化剂的双功能过电位测得为820 mV,超过了20% Pt/C电催化剂(860 mV),突出了其实际应用潜力。对比实验确定了对保形杂化结构、多孔框架以及纳米复合材料各成分之间协同作用产生强大双功能反应性的根源。