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在低过电位下,纳米结构核壳催化剂上一氧化氮的电化学还原,太阳能到氨的效率为1.7%

Electrochemical Reduction of Nitric Oxide with 1.7% Solar-to-Ammonia Efficiency Over Nanostructured Core-Shell Catalyst at Low Overpotentials.

作者信息

Sethuram Markandaraj Sridhar, Muthusamy Tamilselvan, Shanmugam Sangaraju

机构信息

Department of Energy Science & Engineering, Daegu Gyeongbuk Institute of Science & Technology (DGIST), Daegu, 42988, Republic of Korea.

出版信息

Adv Sci (Weinh). 2022 Oct;9(29):e2201410. doi: 10.1002/advs.202201410. Epub 2022 Aug 18.

Abstract

Transition metals have been recognized as excellent and efficient catalysts for the electrochemical nitric oxide reduction reaction (NORR) to value-added chemicals. In this work, a class of core-shell electrocatalysts that utilize nickel nanoparticles in the core and nitrogen-doped porous carbon architecture in the shell (Ni@NC) for the efficient electroreduction of NO to ammonia (NH ) is reported. In Ni@NC, the NC prevents the dissolution of Ni nanoparticles and ensures the long-term stability of the catalyst. The Ni nanoparticles involve in the catalytic reduction of NO to NH during electrolysis. As a result, the Ni@NC achieves a faradaic efficiency (FE) of 72.3% at 0.16 V . The full-cell electrolyzer is constructed by coupling Ni@NC as cathode for NORR and RuO as an anode for oxygen evolution reaction (OER), which delivers a stable performance over 20 cycles at 1.5 V. While integrating this setup with a PV-electrolyzer cell, and it demonstrates an appreciable FE of >50%. Thus, the results exemplify that the core-shell catalyst based electrolyzer is a promising approach for the stable NO to NH electroconversion.

摘要

过渡金属已被公认为是用于将电化学一氧化氮还原反应(NORR)转化为增值化学品的优异且高效的催化剂。在这项工作中,报道了一类核壳结构电催化剂,其核心为镍纳米颗粒,外壳为氮掺杂多孔碳结构(Ni@NC),用于将NO高效电还原为氨(NH₃)。在Ni@NC中,NC可防止镍纳米颗粒溶解,并确保催化剂的长期稳定性。镍纳米颗粒在电解过程中参与将NO催化还原为NH₃的反应。结果,Ni@NC在0.16 V时实现了72.3%的法拉第效率(FE)。通过将Ni@NC用作NORR的阴极和RuO₂用作析氧反应(OER)的阳极来构建全电池电解槽,该电解槽在1.5 V下经过20个循环仍具有稳定的性能。当将此装置与光伏电解槽电池集成时,其法拉第效率>50%,表现可观。因此,这些结果表明基于核壳催化剂的电解槽是一种将NO稳定电转化为NH₃的有前景的方法。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f270/9561790/ccb75eb2858a/ADVS-9-2201410-g004.jpg

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